The sealing capacity of caprock is critical for preventing CO_(2)migration and ensuring the safety of geological storage.However,existing research lacks a comprehensive overview of its sealing mechanisms and failure r...The sealing capacity of caprock is critical for preventing CO_(2)migration and ensuring the safety of geological storage.However,existing research lacks a comprehensive overview of its sealing mechanisms and failure risks.Here,recent findings on caprock sealing mechanisms,its influencing factors,failure risks,and evaluation methods are summarized.The main results include the following:(i)Caprock sealing mechanisms include capillary,hydraulic,hydrocarbon concentration,and hydrate sealing.(ii)Capillary and hydrate sealing block fluid-phase CO_(2),hydrocarbon concentration sealing prevents diffusive CO_(2),and hydraulic sealing prevents fluid and water-soluble phases.(iii)The sealing capacity is influenced by the storage site,stratigraphic environment,and caprock properties,with breakthrough pressure ranked as follows:gypsum rock>salt rock>mudstone/shale>limestone>silty mudstone.(iv)Diffusion leakage occurs when the diffusion coefficients is less than 10^(-12)m^(2)/s,the seepage leakage ranges between 10^(-8)m^(2)/s and 10^(-12)m^(2)/s,and the fracture leakage is greater than 10^(-8)m^(2)/s.(v)Hydro-mechanical(HM)coupling mechanisms,including CO_(2)diffusion,breakthrough migration,uplift deformation,and fracture flow,are essential for leakage risk simulations.Future research should address sealing mechanisms under complex conditions,define leakage risk thresholds,optimize multiphysical coupling computations,and implement effective engineering solutions to mitigate leakage risk.展开更多
Structural instability and sluggish lithium-ion(Li+) kinetics of spinel NiCo_(2)O_(4) anodes severely hinder their applications in high-energy-density lithium-ion batteries.Mesocrystalline structures exhibit promising...Structural instability and sluggish lithium-ion(Li+) kinetics of spinel NiCo_(2)O_(4) anodes severely hinder their applications in high-energy-density lithium-ion batteries.Mesocrystalline structures exhibit promising potential in balancing structural stability and enhancing reaction kinetics.However,their controlled synthesis mechanisms remain elusive.Herein,a substrate interface engineering strategy is developed to achieve controllable synthesis of mesocrystalline and polycrystalline NiCo_(2)O_(4) nanorods.Remarkably,mesocrystalline NiCo_(2)O_(4) exhibits a high capacity retention rate of 85.7% after 500 cycles at 2 A/g,attributed to its porous structure facilitating Li^(+) transport kinetics and unique stress-buffering effect validated by ex-situ TEM.Theoretical calculations and interfacial chemical analysis reveal that substratecrystal surface engineering regulates the nucleation-growth pathways:Acid-treated nickel foam enables epitaxial growth via lattice matching,acting as a low-interfacial-energy template to reduce nucleation barriers and promote low-temperature oriented crystallization.In contrast,carbon cloth requires hightemperature thermal activation to overcome surface diffusion barriers induced by elevated interfacial energy.This substrate-driven crystallization kinetic modulation overcomes the limitations of random nucleation in conventional hydrothermal synthesis.The established substrate-crystal interfacial interaction model not only clarifies the kinetic essence of crystal orientation regulation but also provides a universal theoretical framework for lattice-matching design and mesostructural optimization of advanced electrode materials.展开更多
Micro-sized anatase TiO_(2) displays inferior capacity as cathode material for magnesium ion batteries because of the higher diffusion energy barrier of Mg^(2+)in anatase TiO_(2) lattice.Herein,we report that nanosize...Micro-sized anatase TiO_(2) displays inferior capacity as cathode material for magnesium ion batteries because of the higher diffusion energy barrier of Mg^(2+)in anatase TiO_(2) lattice.Herein,we report that nanosized anatase TiO_(2) exposed(001)facet doubles the capacity compared to the micro-sized sample ascribed to the interfacial Mg^(2+)ion storage.First-principles calculations reveal that the diffusion energy barrier of Mg^(2+)on the(001)facet is significantly lower than those in the bulk phase and on(100)facet,and the adsorption energy of Mg^(2+)on the(001)facet is also considerably lower than that on(100)facet,which guarantees superior interfacial Mg^(2+)storage of(001)facet.Moreover,anatase TiO_(2) exposed(001)facet displays a significantly higher capacity of 312.9 mAh g^(−1) in Mg-Li dual-salt electrolyte compared to 234.3 mAh g^(−1) in Li salt electrolyte.The adsorption energies of Mg^(2+)on(001)facet are much lower than the adsorption energies of Li+on(001)facet,implying that the Mg^(2+)ion interfacial storage is more favorable.These results highlight that controlling the crystal facet of the nanocrystals effectively enhances the interfacial storage of multivalent ions.This work offers valuable guidance for the rational design of high-capacity storage systems.展开更多
Metal hydrides with high hydrogen density provide promising hydrogen storage paths for hydrogen transportation.However,the requirement of highly pure H_(2)for re-hydrogenation limits its wide application.Here,amorphou...Metal hydrides with high hydrogen density provide promising hydrogen storage paths for hydrogen transportation.However,the requirement of highly pure H_(2)for re-hydrogenation limits its wide application.Here,amorphous Al_(2)O_(3)shells(10 nm)were deposited on the surface of highly active hydrogen storage material particles(MgH_(2)-ZrTi)by atomic layer deposition to obtain MgH_(2)-ZrTi@Al_(2)O_(3),which have been demonstrated to be air stable with selective adsorption of H_(2)under a hydrogen atmosphere with different impurities(CH_(4),O_(2),N_(2),and CO_(2)).About 4.79 wt% H_(2)was adsorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)at 75℃under 10%CH_(4)+90%H_(2)atmosphere within 3 h with no kinetic or density decay after 5 cycles(~100%capacity retention).Furthermore,about 4 wt%of H_(2)was absorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)under 0.1%O_(2)+0.4%N_(2)+99.5%H_(2)and 0.1%CO_(2)+0.4%N_(2)+99.5%H_(2)atmospheres at 100℃within 0.5 h,respectively,demonstrating the selective hydrogen absorption of MgH_(2)-ZrTi@10nmAl_(2)O_(3)in both oxygen-containing and carbon dioxide-containing atmospheres hydrogen atmosphere.The absorption and desorption curves of MgH_(2)-ZrTi@10nmAl_(2)O_(3)with and without absorption in pure hydrogen and then in 21%O_(2)+79%N_(2)for 1 h were found to overlap,further confirming the successful shielding effect of Al_(2)O_(3)shells against O_(2)and N_(2).The MgH_(2)-ZrTi@10nmAl_(2)O_(3)has been demonstrated to be air stable and have excellent selective hydrogen absorption performance under the atmosphere with CH_(4),O_(2),N_(2),and CO_(2).展开更多
Beyond conventional methods for CO2 capture and storage, a promising technology of sub-seabed CO2 storage in the form of gas hydrate has come into the limelight nowadays. In order to estimate CO2 storage capacity in t...Beyond conventional methods for CO2 capture and storage, a promising technology of sub-seabed CO2 storage in the form of gas hydrate has come into the limelight nowadays. In order to estimate CO2 storage capacity in the real sub-seabed sediments by gas hydrate, a large-scale geological model with the radius of 100 m and the thickness of 160 m was built in this study, and the processes of CO2 injection and CO2 hydrate formation in the sediments with two-phase flow were simulated numerically at three different injection rates of 10 ton/day, 50 ton/day, and 100 ton/day for an injection period of 150 days. Then, the evolutions of CO2 reaction, free CO2, and hydrate formation over time were analyzed quantitatively, and the spatial distributions of the physical properties in the sediments were presented to investigate the behaviors of CO2 hydrate formation in the sediments with two-phase flow. For CO2 storage capacity, a total amount of 15,000-ton CO2 can be stored safely in the sediments at the injection rate of 100 ton/day for 150 days, and a maximum amount of 36,500-ton CO2 could be stored in the sub-seabed sediments per year for a CO2 storage reservoir with the thickness of 100 m. For the practical scenario, an average value of 1 ton/day/m could be used to determine the actual injection rate based on the thickness of the real sub-seabed sediments.展开更多
[ Objective ] The paper was to study the effect of controlled atmosphere stress of carbon dioxide （ CO2 ） on Superoxide dismutase （SOD） activity of in- sect, so as to analyze the biological mechanism of the action...[ Objective ] The paper was to study the effect of controlled atmosphere stress of carbon dioxide （ CO2 ） on Superoxide dismutase （SOD） activity of in- sect, so as to analyze the biological mechanism of the action of controlled atmosphere stress on insect. [ Method] Using nitrotetrazolium blue chloride （NBT） light reduction method, SOD activity of drugstore beetle （ Stegobium panlceum ）, cigarette beetle （ Lasioderma serricorne） and coffee bean beetle （Araecerus fasciculatus） was studied, and the stress response of the enzyme under controlled atmosphere stress of CO2 was analyzed. [ Result ] SOD activity of drugstore beetle, cigarette beetle and coffee bean beetle exposed to controlled atmosphere stress of high concentrations of CO2 for 3 and 6 h had certain degree of increase, and the activity sig- nificantly increased from 2.011±0.954,2.664±0.218 and 1.458±0.718 to 3. 135±0. 105,3.050±0.673 and 2.975±0.229 U/（per pest · 30 min） after treat- ment for 6 h. [ Conclusion] Controlled atmosphere stress of high concentrations of CO2 had certain activation effect on SOD activity of storage pest in Chinese me- dicinal material within the context of sub-lethal events. The results could enrich the insecticidal mechanism of controlled atmosphere and theoretical system of analy- sis on insect resistance to controlled atmosphere.展开更多
Understanding the storage mechanisms in CO_(2)flooding is crucial,as many carbon capture,utilization,and storage(CCUS)projects are related to enhanced oil recovery(EOR).CO_(2)storage in reservoirs across large timesca...Understanding the storage mechanisms in CO_(2)flooding is crucial,as many carbon capture,utilization,and storage(CCUS)projects are related to enhanced oil recovery(EOR).CO_(2)storage in reservoirs across large timescales undergoes the two storage stages of oil displacement and well shut-in,which cover mul-tiple replacement processes of injection-production synchronization,injection only with no production,and injection-production stoppage.Because the controlling mechanism of CO_(2)storage in different stages is unknown,the evolution of CO_(2)storage mechanisms over large timescales is not understood.A math-ematical model for the evaluation of CO_(2)storage,including stratigraphic,residual,solubility,and mineral trapping in low-permeability tight sandstone reservoirs,was established using experimental and theoret-ical analyses.Based on a detailed geological model of the Huaziping Oilfield,calibrated with reservoir permeability and fracture characteristic parameters obtained from well test results,a dynamic simulation of CO_(2)storage for the entire reservoir life cycle under two scenarios of continuous injection and water-gas alternation were considered.The results show that CO_(2)storage exhibits the significant stage charac-teristics of complete storage,dynamic storage,and stable storage.The CO_(2)storage capacity and storage rate under the continuous gas injection scenario(scenario 1)were 6.34×10^(4)t and 61%,while those under the water-gas alternation scenario(scenario 2)were 4.62×10^(4)t and 46%.The proportions of stor-age capacity under scenarios 1 and 2 for structural or stratigraphic,residual,solubility,and mineral trap-ping were 33.36%,33.96%,32.43%,and 0.25%;and 15.09%,38.65%,45.77%,and 0.49%,respectively.The evolution of the CO_(2)storage mechanism showed an overall trend:stratigraphic and residual trapping first increased and then decreased,whereas solubility trapping gradually decreased,and mineral trapping continuously increased.Based on these results,an evolution diagram of the CO_(2)storage mechanism of low-permeability tight sandstone reservoirs across large timescales was established.展开更多
MXene derivatives are notable two-dimensional nanomaterials with numerous prospective applications in the domains of energy development.MXene derivative,MBene,diversifies its focus on energy storage and harvesting due...MXene derivatives are notable two-dimensional nanomaterials with numerous prospective applications in the domains of energy development.MXene derivative,MBene,diversifies its focus on energy storage and harvesting due to its exceptional electrical conductivity,structural flexibility,and mechanical properties.This comprehensive review describes the sandwich-like structure of the synthesized MBene,derived from its multilayered parent material and its distinct chemical framework to date.The fields of focus encompass the investigation of novel MBenes,the study of phase-changing mechanisms,and the examination of hex-MBenes,ortho-MBenes,tetra-MBenes,tri-MBenes,and MXenes with identical transition metal components.A critical analysis is also provided on the electrochemical mechanism and performance of MBene in energy storage(Li/Na/Mg/Ca/Li–S batteries and supercapacitors),as well as conversion and harvesting(CO_(2) reduction,and nitrogen reduction reactions).The persistent difficulties associated with conducting experimental synthesis and establishing artificial intelligence-based forecasts are extensively deliberated alongside the potential and forthcoming prospects of MBenes.This review provides a single platform for an overview of the MBene’s potential in energy storage and harvesting.展开更多
Aqueous Zn-ion storage offers high capacity and safety,but practical use is hindered by dendrite formation,side reactions,and hydrogen evolution,affecting stability and efficiency.Herein,tetramethylol acetylenediurea(...Aqueous Zn-ion storage offers high capacity and safety,but practical use is hindered by dendrite formation,side reactions,and hydrogen evolution,affecting stability and efficiency.Herein,tetramethylol acetylenediurea(TA)is proposed as an effective electrolyte additive that modulates the Zn^(2+)deposition environment via coordination competition.The polar functional groups of TA restructure the solvation sheath,while its molecular dipoles generate localized electric fields that accelerate Zn^(2+)migration and promote directional(002)-oriented deposition.These effects collectively suppress side reactions and enhance Zn plating/stripping reversibility.The four hydroxyl(–OH)and conjugated ketone groups(C=O)in the TA molecule have strong coordination ability(Lewis basicity)and can form a stable[Zn(TA)(H_(2)O)_(n)]^(2+)with Zn^(2+),reducing the number of free water molecules and the proportion of active water in the solvation sheath.The TA molecules are adsorbed onto the Zn anode surface,leading to the redistribution of the local spatial electric field and homogenization of ion flux dynamics.Its conjugated planar structure can induce Zn^(2+)to preferentially deposit along the(002)crystal plane.Zn//Zn symmetric cell using TA-containing ZnSO4 electrolyte exhibits stable cycling for more than 2240 h at 1 mA cm^(−2),1 mAh cm^(−2).The Zn//activated carbon(AC)full-cell can stably cycle 30,000 cycles at 5 A g^(−1)with a capacity retention rate of 90%.This study provides important insights into electrolyte engineering strategies for stabilizing Zn anodes,highlighting the potential of molecular design additives in next-generation Zn^(2+)energy storage systems.展开更多
The magnesium based metal hydrogen storage composite system Mg(NH_(2))_(2)-2LiH has a theoretical hydro-gen storage capacity of 5.6 wt.%and is a promising hydrogen storage material for vehicles.However,its application...The magnesium based metal hydrogen storage composite system Mg(NH_(2))_(2)-2LiH has a theoretical hydro-gen storage capacity of 5.6 wt.%and is a promising hydrogen storage material for vehicles.However,its application is limited due to serious thermodynamic and kinetic barriers.Introducing efficient catalysts is an effective method to improve the hydrogen storage performance of Mg(NH_(2))_(2)-2LiH.This article in-vestigates for the first time the use of nano rare earth oxide CeO_(2)(~44.5 nm)as an efficient modifier,achieving comprehensive regulation of the hydrogen storage performance of Mg(NH_(2))_(2)-2LiH composite system through oxygen vacancy driven catalysis.The modification mechanism of nano CeO_(2) is also sys-tematically studied using density functional theory(DFT)calculations and experimental results.Research has shown that the comprehensive hydrogen storage performance of the Mg(NH_(2))_(2)-2LiH-5 wt.%CeO_(2) composite system is optimal,with high hydrogen absorption and desorption kinetics and reversible per-formance.The initial hydrogen absorption and desorption temperatures of the composite system were significantly reduced from 110/130℃to 65/80℃,and the release of by-product ammonia was signifi-cantly inhibited.Under the conditions of 170℃/50 min and 180℃/100 min,4.37 wt.%of hydrogen can be rapidly absorbed and released.After 10 cycles of hydrogen release,the hydrogen cycle retention rate increased from 85%to nearly 100%.Further mechanistic studies have shown that the nano CeO_(2-x) gen-erated in situ during hydrogen evolution can effectively weaken the Mg-N and N-H bonds of Mg(NH_(2))_(2),exhibiting good catalytic effects.Meanwhile,oxygen vacancies provide a fast pathway for the diffusion of hydrogen atoms in the composite system.In addition,nano CeO_(2-x) can effectively inhibit the polycrys-talline transformation of the hydrogen evolving product Li_(2)MgN_(2)H_(2) in the system at high temperatures,reducing the difficulty of re-hydrogenation of the system.This study provides an innovative perspective for the efficient modification of magnesium based metal hydrogen storage composite materials using rare earth based catalysts,and also provides a reference for regulating the comprehensive hydrogen storage performance of hydrogen storage materials using rare earth catalysts with oxygen vacancies.展开更多
Designing catalysts with high catalytic activity and stability is the key to achieve the commercial application of MgH_(2).Herein,the sulfur doped Ti_(3)C_(2)(S-Ti_(3)C_(2))was successfully prepared by heat treatment ...Designing catalysts with high catalytic activity and stability is the key to achieve the commercial application of MgH_(2).Herein,the sulfur doped Ti_(3)C_(2)(S-Ti_(3)C_(2))was successfully prepared by heat treatment of Ti_(3)C_(2)MXene under Ar/H_(2)S atmosphere to facilitate the hydrogen release and uptake from MgH_(2).The S-Ti_(3)C_(2)exhibited pleasant catalytic effect on the hydriding/dehydriding kinetics and cyclic stability of MgH_(2).The addition of 5 wt%S-Ti_(3)C_(2)into MgH_(2)resulted in a reduction of 114℃in the starting dehydriding temperature compared to pure MgH_(2).MgH_(2)+5 wt%S-Ti_(3)C_(2)sample could quickly release 6.6 wt%hydrogen in 17 min at 220℃,and 6.8 wt%H_(2)was absorbed in 25 min at 200℃.Cyclic testing revealed that MgH_(2)+5 wt%S-Ti_(3)C_(2)system achieved a reversible hydrogen capacity of 6.5 wt%.Characterization analysis demonstrated that Ti-species(Ti0,Ti^(2+),Ti-S,and Ti^(3+))as active species significantly lowered the dehydrogenation temperature and promoted the re-/dehydrogenation kinetics of MgH_(2),and sulfur doping can effectively improve the stability of Ti0 and Ti^(3+),contributing to the improvement of cyclic stability of MgH_(2).This study provides strategy for the construction of catalysts for hydrogen storage materials.展开更多
The role of catalysts in enhancing the hydrogen storage kinetics of the Mg/MgH_(2)system is pivotal.However,the exploration of efficient catalysts and the underlying principles of their design remain both a prominent ...The role of catalysts in enhancing the hydrogen storage kinetics of the Mg/MgH_(2)system is pivotal.However,the exploration of efficient catalysts and the underlying principles of their design remain both a prominent focus and a significant challenge in current research.In this study,we present a bimetallic oxide of Bi_(2)Ti_(2)O_(7)hollow sphere as a highly effective catalyst for MgH_(2).As a result,the Bi_(2)Ti_(2)O_(7)-catalyzed Mg/MgH_(2)system lowers the hydrogen desorption initiation temperature to 194.3℃,reduces the peak desorption temperature to 245.6℃,decreases the dehydrogenation activation energy to 82.14 kJ·mol^(−1),and can absorb 5.4 wt.%of hydrogen within 60 s at 200℃,demonstrating outstanding hydrogen ab/desorption kinetics,compared to pure MgH_(2).Additionally,it can maintain a high hydrogen capacity of 5.2 wt.%,even after 50 dehydrogenation cycles,showing good cycle stability.The characterization results show that the high-valent Bi and Ti in Bi_(2)Ti_(2)O_(7)are reduced to their low-valent or even zero-valent metallic states during the dehydrogenation and hydrogenation process,thus establishing an in-situ multivalent and multi-element catalytic environment.Density functional theory calculations further reveal that the synergistic effects between Bi and Ti in the Bi-Ti mixed oxide facilitate the cleavage of Mg-H bonds and lower the kinetic barrier for the dissociation of hydrogen molecules,thereby substantially enhancing the kinetics of the Mg/MgH_(2)system.This study presents a strategic method for developing efficient catalysts for hydrogen storage materials by harnessing the synergistic effects of metal elements.展开更多
Mg-based hydrogen storage materials have attracted much attention due to their high hydrogen content,abundant resources,and environmental friendliness.However,the high dehydrogenation temperature,slow kinetics and poo...Mg-based hydrogen storage materials have attracted much attention due to their high hydrogen content,abundant resources,and environmental friendliness.However,the high dehydrogenation temperature,slow kinetics and poor cycling stability are limiting its practical application.This work demonstrates the improved dehydrogenation kinetics and cycling stability of MgH_(2) modified by a hybrid of metallic Ni and layered MoS_(2)(denoted as“Ni-MoS_(2)”)introduced by ball milling,with Ni as the catalyst for MgH_(2) and MoS_(2) as the support for both Ni and MgH_(2).The onset dehydrogenation temperature of MgH_(2) is reduced to 198℃,and the rehydrogenation begins at a low temperature of 50℃.The MgH_(2)+10 wt%Ni-MoS_(2) composite has a fast dehydrogenation kinetics and can release 6.1 wt% hydrogen in 10 min at a constant temperature of 300℃,with the dehydrogenation activation energy significantly reduced from 151 to 85 kJ mol^(-1).During the cycling,the reversible capacity of the composite first exhibits a gradual increase for the initial 22 cycles and then maintains at 6.1 wt% from the 23th cycle to the 50th cycle.The Ni/MoS_(2) addition does not change the overall thermodynamic properties of MgH_(2) but can weaken the Mg-H bonds in the local regions as evident by theoretical calculation.Microstructure studies reveal that the metallic Ni will react with MgH_(2) to form Mg_(2)NiH_(0.3),which can act as a hydrogen pump,while the layered MoS_(2) serves as a support for the well dispersion of MgH_(2) and Ni.It is believed that the synergy of Mg_(2)NiH_(0.3) and layered MoS_(2) contributes to the significantly enhanced hydrogen storage of MgH_(2).This work provides a promising and simple strategy for enhancing the Mg-based hydrogen storage materials by combination of transition metals and layered materials introduced via simple ball milling.展开更多
At present,carbon capture and storage(CCS)is the only mature and commercialized technology capable of effectively and economically reducing greenhouse gas emissions to achieve a significant and immedi-ate impact on th...At present,carbon capture and storage(CCS)is the only mature and commercialized technology capable of effectively and economically reducing greenhouse gas emissions to achieve a significant and immedi-ate impact on the CO_(2) level on Earth.Notably,long-term geological storage of captured CO_(2) has emerged as a primary storage method,given its minimal impact on surface ecological environments and high level of safety.The integrity of CO_(2) storage wellbores can be compromised by the corrosion of steel casings and degradation of cement in supercritical CO_(2) storage environments,potentially leading to the leakage of stored CO_(2) from the sites.This critical review endeavors to establish a knowledge foundation for the cor-rosion and materials degradation associated with geological CO_(2) storage through an in-depth examina-tion and analysis of the environments,operation,and the state-of-the-art progress in research pertaining to the topic.This article discusses the physical and chemical properties of CO_(2) in its supercrit-ical phase during injection and storage.It then introduces the principle of geological CO_(2) storage,consid-erations in the construction of storage systems,and the unique geo-bio-chemical environment involving aqueous media and microbial communities in CO_(2) storage.After a comprehensive analysis of existing knowledge on corrosion in CO_(2) storage,including corrosion mechanisms,parametric effects,and corro-sion rate measurements,this review identifies technical gaps and puts forward potential avenues for fur-ther research in steel corrosion within geological CO_(2) storage systems.展开更多
Saline aquifers are considered as highly favored reservoirs for CO_(2)sequestration due to their favorable properties.Understanding the impact of saline aquifer properties on the migration and distribution of CO_(2)pl...Saline aquifers are considered as highly favored reservoirs for CO_(2)sequestration due to their favorable properties.Understanding the impact of saline aquifer properties on the migration and distribution of CO_(2)plume is crucial.This study focuses on four key parameters-permeability,porosity,formation pressure,and temperature-to characterize the reservoir and analyse the petrophysical and elastic response of CO_(2).First,we performed reservoir simulations to simulate CO_(2)saturation,using multiple sets of these four parameters to examine their significance on CO_(2)saturation and the plume migration speed.Subsequently,the effect of these parameters on the elastic properties is tested using rock physics theory.We established a relationship of compressional wave velocity(V_(p))and quality factor(Q_(p))with the four key parameters,and conducted a sensitivity analysis to test their sensitivity to V_(p) and Q_(p).Finally,we utilized visco-acoustic wave equation simulated time-lapse seismic data based on the computed V_(p) and Q_(p) models,and analysed the impact of CO_(2) saturation changes on seismic data.As for the above nu-merical simulations and analysis,we conducted sensitivity analysis using both homogeneous and heterogeneous models.Consistent results are found between homogeneous and heterogeneous models.The permeability is the most sensitive parameter to the CO_(2)saturation,while porosity emerges as the primary factor affecting both Q_(p) and V_(p).Both Q_(p) and V_(p) increase with the porosity,which contradicts the observations in gas reservoirs.The seismic simulations highlight significant variations in the seismic response to different parameters.We provided analysis for these observations,which serves as a valuable reference for comprehensive CO_(2)integrity analysis,time-lapse monitoring,injection planning and site selection.展开更多
China has pledged to peak carbon dioxide(CO_(2))emissions by 2030 and achieve carbon neutrality by 2060.Carbon capture and storage(CCS)will play a key role in these efforts.Over the past several years,the China Geolog...China has pledged to peak carbon dioxide(CO_(2))emissions by 2030 and achieve carbon neutrality by 2060.Carbon capture and storage(CCS)will play a key role in these efforts.Over the past several years,the China Geological Survey(CGS)has completed the Suitability Evaluation Map of CO_(2)Geological Storage in Main Sedimentary Basins in China and Adjacent Sea Regions in 2017.This map reflects the suitability of the first-and secondary-order tectonic units within sedimentary basins for cO_(2)geological storage for CCS planning.The Junggar Basin is recognized as an important region for future CCS projects.Results from a mesoscale evaluation using the volume method indicate that deep saline aquifers represent the most significant resources for CO_(2)storage,with potential ranging from 48×10^(9)to 164×10^(9)t(with a P50 value of 96×10^(9)t).The highest storage potential is identified in the central and northern parts of the basin,reaching up to 9.5×10^(6)t/km^(2)at the P50 probability level.In contrast,the hinterland,eastern,and western parts of the basin generally exhibit storage potential of below 1.0×10^(6)t/km^(2)at the same probability level.The CGs has also characterized historical CO_(2)plume migration in reservoirs at the storage site of the Shenhua CCS demonstration project and conducted numerical simulations of CO_(2)plume migration for periods of 10 and 20 years following the shutdown of the injection well.The CGS implemented a kiloton-scale pilot test on CO_(2)-enhanced water recovery(CO_(2)-EWR)in eastern Junggar,revealing that CO_(2)flooding can improve the pressure for fluid production,with the highest ratio of CO_(2)to produced fluids estimated at approximately 1.2.Besides,an observation field for natural CO_(2)leakage,covering about 930 m^(2),was built in Qinghai Province.In natural CO_(2)fields or at artificial CO_(2)injection research sites,cO_(2)leakage points are primarily related to the distribution of faults(especially fault crossing),which can serve as pathways for CO_(2)leakage.The observation field provides a natural analog to wellbore failure and offers an opportunity to further monitor CO_(2)geological storage sites.However,it has been inferred that borehole ZK10 at the observation field has become a leakage pathway due to the drilling activities,inadequate well-plugging,and abandonment procedures without considering CO_(2)corrosion.展开更多
Carbon dioxide enhanced oil recovery(CO_(2)-EOR)technology is used for oil production and CO_(2) storage in reservoirs.Methods are being constantly developed to optimize oil recovery and CO_(2) storage during the CO_(...Carbon dioxide enhanced oil recovery(CO_(2)-EOR)technology is used for oil production and CO_(2) storage in reservoirs.Methods are being constantly developed to optimize oil recovery and CO_(2) storage during the CO_(2) displacement process,especially for low-permeability reservoirs under varying geological conditions.In this study,long-core experiments and trans-scale numerical simulations are employed to examine the characteristics of oil production and CO_(2) storage.Optimal production parameters for the target reservoir are also proposed.The results indicate that maintaining the pressure at 1.04 to 1.10 times the minimum miscible pressure(MMP)and increasing the injection rate can enhance oil production in the early stage of reservoir development.In contrast,reducing the injection rate at the later stages prevents CO_(2) channeling,thus improving oil recovery and CO_(2) storage efficiency.A solution-doubling factor is introduced to modify the calculation method for CO_(2) storage,increasing its accuracy to approximately 90%.Before CO_(2) breakthrough,prioritizing oil production is recommended to maximize the economic benefits of this process.In the middle stage of CO_(2) displacement,decreasing the injection rate optimizes the coordination between oil displacement and CO_(2) storage.Further,in the late stage,reduced pressure and injection rates are required as the focus shifts to CO_(2) storage.展开更多
The reaction characteristics of calcium-based materials during calcium looping(CaL)process are pivotal in the efficiency of CaL thermochemical energy storage(TCES)and CO_(2)capture systems.Currently,metal oxide doping...The reaction characteristics of calcium-based materials during calcium looping(CaL)process are pivotal in the efficiency of CaL thermochemical energy storage(TCES)and CO_(2)capture systems.Currently,metal oxide doping is the primary method to enhance the reaction characteristics of calcium-based materials over multiple cycles.In particular,co-doping with variable-valence metal oxides(VVMOs)can effectively increase the oxygen vacancy content in calcium-based materials,significantly improving their cyclic reaction characteristics.However,there are so numerous VVMOs co-doping schemes that the experimental screening process is complex,consuming considerable time and economic costs.Density functional theory(DFT)calculations have been widely used to reveal the impact of metal oxide doping on the cyclic reaction characteristics of calcium-based materials,with calculation results showing good agreement with experimental conclusions.Nevertheless,there is still a lack of research on utilizing DFT to screen calcium-based materials,and a systematic research methodology has not yet been established.In this study,a systematic DFT-based screening methodology for calcium-based materials was proposed.A series of key parameters for DFT calculations including CO_(2)adsorption energy,oxygen vacancy formation energy,and sintering resistance were proposed.Furthermore,a preliminary mathematical model to predict the CaL TCES and CO_(2)capture performance of calcium-based materials was introduced.The aforementioned DFT method was employed to screen for VVMOs co-doped calcium-based materials.The results revealed that Mn and Ce co-doped calcium-based materials exhibited superior DFT-predicted reaction characteristics.These DFT predictions were validated through experimental assessments of cyclic thermochemical energy storage,CO_(2)capture,and relevant characterization.The outcomes demonstrate a high degree of consistency among DFT-based predictions,experimental results,and characterization.Hence,the DFT-based screening methodology for calcium-based materials proposed herein is a viable solution,poised to offer theoretical insights for the efficient design of calcium-based materials.展开更多
Cyclic injection holds great potential for CO_(2) emission reduction coupled with enhanced unconventional oil recovery.There is,however,a lack of a thorough understanding of carbon distribution,migration,and transform...Cyclic injection holds great potential for CO_(2) emission reduction coupled with enhanced unconventional oil recovery.There is,however,a lack of a thorough understanding of carbon distribution,migration,and transformation underground over time at the reservoir scale.To address this issue,we conducted a rig-orous numerical simulation integrating microseismic events,multi-geomechanics,and multi-geochemistry to represent the complex fracture geometry,rock stress sensitivity,and CO_(2)-oil-brine-rock interactions.The fluid model,reservoir model,and geochemical reaction kinetics were carefully validated and calibrated using experimental data.The performance of CO_(2) utilization and geological storage was comprehensively investigated in terms of changes in oil production,CO_(2) storage,carbon distribution,and petrophysical properties.The results indicate that 48.3%of the injected CO_(2) was stored stably under-ground after ten cycles(ten years),with a 3.4%increase in oil recovery.The presence of multiple CO_(2) stor-age forms,such as dissolved in water and mineralized carbonate,impeded CO_(2)-oil interaction,leading to a 25.9%reduction in the volume of the CO_(2)-oil mixing zone and a 2.2%decrease in cumulative oil pro-duction,albeit with a 7.7%increase in the storage rate.The cyclic injection mode had a significant impact on the migration and transformation of CO_(2) in the reservoir.While dissolved CO_(2) in oil accounted for over half of the total storage,it had the possibility of being released during production.After ten cycles,20%of the injected CO_(2)(approximately 12000 t)reached long-term storage in four forms:mineralized carbon-ate(6%),water-dissolved CO_(2)(6%),aqueous ions(4%),and trapped gas(4%).Notably,the non-fracture zone within the stimulated reservoir volume(SRV)served as the primary trapping area for residual gas.This work provides valuable insights into dynamic CO_(2) transport and transformation processes under cyclic injection and presents a more comprehensive and precise framework for assessing CO_(2) capture,utilization,and storage with enhanced oil recovery(CCUS-EOR)performance in unconventional reser-voirs after fracturing.展开更多
Offshore carbon dioxide(CO_(2))geological storage is a promising strategy for reducing carbon emissions and supporting sustainable development in coastal regions within a carbon neutrality framework.However,only a few...Offshore carbon dioxide(CO_(2))geological storage is a promising strategy for reducing carbon emissions and supporting sustainable development in coastal regions within a carbon neutrality framework.However,only a few works have focused on offshore basins in China.To address this gap,this study established a dual indicator system that comprises necessary and critical indices and is integrated with the analytic hierarchy process.A coupled analysis was then performed to evaluate the suitability of 10 offshore sedimentary basins in China for CO_(2)geological storage.The necessary indicator system focuses on storage potential,geological conditions,and engineering feasibility.Meanwhile,the critical indicator system emphasizes the safety of storage projects and the viability of drilling operations.Evaluation results revealed that China's offshore basins have undergone two geological evolution stages,namely,the rifting and post-rifting phases,leading to the formation of a dual-layer structure characterized by faulted lower layers and sagged upper layers.These basins have thick and widespread Cenozoic strata,generally low seismic activity,and medium-to-low geothermal gradients.They form five reservoir-caprock systems with favorable geological conditions for CO_(2)storage.The Pearl River Mouth,East China Sea Shelf,and Bohai Basins emerged as primary candidates that offer substantial storage potential to support carbon neutrality goals in the Bohai Rim Economic Zone,Yangtze River Delta Economic Zone,and Guangdong-Hong Kong-Macao Greater Bay Area.The Beibu Gulf and South Yellow Sea Basins were identified as secondary candidates,and the Qiongdongnan and Yinggehai Basins were considered potential alternatives.展开更多
基金supported by the Joint Funds of the National Natural Science Foundation of China(Grant No.U23A20671)the Major Project of Inner Mongolia Science and Technology,China(Grant No.2021ZD0034)the Creative Groups of Natural Science Foundation of Hubei Province(Grant No.2021CFA030).
文摘The sealing capacity of caprock is critical for preventing CO_(2)migration and ensuring the safety of geological storage.However,existing research lacks a comprehensive overview of its sealing mechanisms and failure risks.Here,recent findings on caprock sealing mechanisms,its influencing factors,failure risks,and evaluation methods are summarized.The main results include the following:(i)Caprock sealing mechanisms include capillary,hydraulic,hydrocarbon concentration,and hydrate sealing.(ii)Capillary and hydrate sealing block fluid-phase CO_(2),hydrocarbon concentration sealing prevents diffusive CO_(2),and hydraulic sealing prevents fluid and water-soluble phases.(iii)The sealing capacity is influenced by the storage site,stratigraphic environment,and caprock properties,with breakthrough pressure ranked as follows:gypsum rock>salt rock>mudstone/shale>limestone>silty mudstone.(iv)Diffusion leakage occurs when the diffusion coefficients is less than 10^(-12)m^(2)/s,the seepage leakage ranges between 10^(-8)m^(2)/s and 10^(-12)m^(2)/s,and the fracture leakage is greater than 10^(-8)m^(2)/s.(v)Hydro-mechanical(HM)coupling mechanisms,including CO_(2)diffusion,breakthrough migration,uplift deformation,and fracture flow,are essential for leakage risk simulations.Future research should address sealing mechanisms under complex conditions,define leakage risk thresholds,optimize multiphysical coupling computations,and implement effective engineering solutions to mitigate leakage risk.
基金financially supported by the National Nature Science Foundation of China (No.52401273)Science and Technology Department of Henan (Nos.242102241007,252102320178 and 252102321067)Training Program for Young Backbone Teachers in Higher Education Institutions in Henan Province (No.2024GGJS101)。
文摘Structural instability and sluggish lithium-ion(Li+) kinetics of spinel NiCo_(2)O_(4) anodes severely hinder their applications in high-energy-density lithium-ion batteries.Mesocrystalline structures exhibit promising potential in balancing structural stability and enhancing reaction kinetics.However,their controlled synthesis mechanisms remain elusive.Herein,a substrate interface engineering strategy is developed to achieve controllable synthesis of mesocrystalline and polycrystalline NiCo_(2)O_(4) nanorods.Remarkably,mesocrystalline NiCo_(2)O_(4) exhibits a high capacity retention rate of 85.7% after 500 cycles at 2 A/g,attributed to its porous structure facilitating Li^(+) transport kinetics and unique stress-buffering effect validated by ex-situ TEM.Theoretical calculations and interfacial chemical analysis reveal that substratecrystal surface engineering regulates the nucleation-growth pathways:Acid-treated nickel foam enables epitaxial growth via lattice matching,acting as a low-interfacial-energy template to reduce nucleation barriers and promote low-temperature oriented crystallization.In contrast,carbon cloth requires hightemperature thermal activation to overcome surface diffusion barriers induced by elevated interfacial energy.This substrate-driven crystallization kinetic modulation overcomes the limitations of random nucleation in conventional hydrothermal synthesis.The established substrate-crystal interfacial interaction model not only clarifies the kinetic essence of crystal orientation regulation but also provides a universal theoretical framework for lattice-matching design and mesostructural optimization of advanced electrode materials.
基金supported by the National Key R&D Program of China(No.2023YFB3809500)the Fundamental Research Funds for the Central Universities(No.2024CDJXY003)+1 种基金the Venture&Innovation Support Program for Chongqing Overseas Returnees(cx2023087)The Chongqing Technology Innovation and Application Development Project(No.2024TIAD-KPX0003).
文摘Micro-sized anatase TiO_(2) displays inferior capacity as cathode material for magnesium ion batteries because of the higher diffusion energy barrier of Mg^(2+)in anatase TiO_(2) lattice.Herein,we report that nanosized anatase TiO_(2) exposed(001)facet doubles the capacity compared to the micro-sized sample ascribed to the interfacial Mg^(2+)ion storage.First-principles calculations reveal that the diffusion energy barrier of Mg^(2+)on the(001)facet is significantly lower than those in the bulk phase and on(100)facet,and the adsorption energy of Mg^(2+)on the(001)facet is also considerably lower than that on(100)facet,which guarantees superior interfacial Mg^(2+)storage of(001)facet.Moreover,anatase TiO_(2) exposed(001)facet displays a significantly higher capacity of 312.9 mAh g^(−1) in Mg-Li dual-salt electrolyte compared to 234.3 mAh g^(−1) in Li salt electrolyte.The adsorption energies of Mg^(2+)on(001)facet are much lower than the adsorption energies of Li+on(001)facet,implying that the Mg^(2+)ion interfacial storage is more favorable.These results highlight that controlling the crystal facet of the nanocrystals effectively enhances the interfacial storage of multivalent ions.This work offers valuable guidance for the rational design of high-capacity storage systems.
基金supported by the National Natural Science Foundation of China(22175136)the State Key Laboratory of Electrical Insulation and Power Equipment(EIPE23127)the Fundamental Research Funds for the Central Universities(xtr052024009).
文摘Metal hydrides with high hydrogen density provide promising hydrogen storage paths for hydrogen transportation.However,the requirement of highly pure H_(2)for re-hydrogenation limits its wide application.Here,amorphous Al_(2)O_(3)shells(10 nm)were deposited on the surface of highly active hydrogen storage material particles(MgH_(2)-ZrTi)by atomic layer deposition to obtain MgH_(2)-ZrTi@Al_(2)O_(3),which have been demonstrated to be air stable with selective adsorption of H_(2)under a hydrogen atmosphere with different impurities(CH_(4),O_(2),N_(2),and CO_(2)).About 4.79 wt% H_(2)was adsorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)at 75℃under 10%CH_(4)+90%H_(2)atmosphere within 3 h with no kinetic or density decay after 5 cycles(~100%capacity retention).Furthermore,about 4 wt%of H_(2)was absorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)under 0.1%O_(2)+0.4%N_(2)+99.5%H_(2)and 0.1%CO_(2)+0.4%N_(2)+99.5%H_(2)atmospheres at 100℃within 0.5 h,respectively,demonstrating the selective hydrogen absorption of MgH_(2)-ZrTi@10nmAl_(2)O_(3)in both oxygen-containing and carbon dioxide-containing atmospheres hydrogen atmosphere.The absorption and desorption curves of MgH_(2)-ZrTi@10nmAl_(2)O_(3)with and without absorption in pure hydrogen and then in 21%O_(2)+79%N_(2)for 1 h were found to overlap,further confirming the successful shielding effect of Al_(2)O_(3)shells against O_(2)and N_(2).The MgH_(2)-ZrTi@10nmAl_(2)O_(3)has been demonstrated to be air stable and have excellent selective hydrogen absorption performance under the atmosphere with CH_(4),O_(2),N_(2),and CO_(2).
文摘Beyond conventional methods for CO2 capture and storage, a promising technology of sub-seabed CO2 storage in the form of gas hydrate has come into the limelight nowadays. In order to estimate CO2 storage capacity in the real sub-seabed sediments by gas hydrate, a large-scale geological model with the radius of 100 m and the thickness of 160 m was built in this study, and the processes of CO2 injection and CO2 hydrate formation in the sediments with two-phase flow were simulated numerically at three different injection rates of 10 ton/day, 50 ton/day, and 100 ton/day for an injection period of 150 days. Then, the evolutions of CO2 reaction, free CO2, and hydrate formation over time were analyzed quantitatively, and the spatial distributions of the physical properties in the sediments were presented to investigate the behaviors of CO2 hydrate formation in the sediments with two-phase flow. For CO2 storage capacity, a total amount of 15,000-ton CO2 can be stored safely in the sediments at the injection rate of 100 ton/day for 150 days, and a maximum amount of 36,500-ton CO2 could be stored in the sub-seabed sediments per year for a CO2 storage reservoir with the thickness of 100 m. For the practical scenario, an average value of 1 ton/day/m could be used to determine the actual injection rate based on the thickness of the real sub-seabed sediments.
基金Supported by Project of Guizhou Provincial Modernization of Chinese Medicine Material Project(QKHYZ[2011]5049Organization Department of CPCGuizhou Committee(TZJF-2009-02)Promotion Project of Key Scientific and Technological Achievements of Guiyang City([2010]1-T-4)~~
文摘[ Objective ] The paper was to study the effect of controlled atmosphere stress of carbon dioxide （ CO2 ） on Superoxide dismutase （SOD） activity of in- sect, so as to analyze the biological mechanism of the action of controlled atmosphere stress on insect. [ Method] Using nitrotetrazolium blue chloride （NBT） light reduction method, SOD activity of drugstore beetle （ Stegobium panlceum ）, cigarette beetle （ Lasioderma serricorne） and coffee bean beetle （Araecerus fasciculatus） was studied, and the stress response of the enzyme under controlled atmosphere stress of CO2 was analyzed. [ Result ] SOD activity of drugstore beetle, cigarette beetle and coffee bean beetle exposed to controlled atmosphere stress of high concentrations of CO2 for 3 and 6 h had certain degree of increase, and the activity sig- nificantly increased from 2.011±0.954,2.664±0.218 and 1.458±0.718 to 3. 135±0. 105,3.050±0.673 and 2.975±0.229 U/（per pest · 30 min） after treat- ment for 6 h. [ Conclusion] Controlled atmosphere stress of high concentrations of CO2 had certain activation effect on SOD activity of storage pest in Chinese me- dicinal material within the context of sub-lethal events. The results could enrich the insecticidal mechanism of controlled atmosphere and theoretical system of analy- sis on insect resistance to controlled atmosphere.
基金supported by the National Key Research and Development Program of China(2022YFE0206700).
文摘Understanding the storage mechanisms in CO_(2)flooding is crucial,as many carbon capture,utilization,and storage(CCUS)projects are related to enhanced oil recovery(EOR).CO_(2)storage in reservoirs across large timescales undergoes the two storage stages of oil displacement and well shut-in,which cover mul-tiple replacement processes of injection-production synchronization,injection only with no production,and injection-production stoppage.Because the controlling mechanism of CO_(2)storage in different stages is unknown,the evolution of CO_(2)storage mechanisms over large timescales is not understood.A math-ematical model for the evaluation of CO_(2)storage,including stratigraphic,residual,solubility,and mineral trapping in low-permeability tight sandstone reservoirs,was established using experimental and theoret-ical analyses.Based on a detailed geological model of the Huaziping Oilfield,calibrated with reservoir permeability and fracture characteristic parameters obtained from well test results,a dynamic simulation of CO_(2)storage for the entire reservoir life cycle under two scenarios of continuous injection and water-gas alternation were considered.The results show that CO_(2)storage exhibits the significant stage charac-teristics of complete storage,dynamic storage,and stable storage.The CO_(2)storage capacity and storage rate under the continuous gas injection scenario(scenario 1)were 6.34×10^(4)t and 61%,while those under the water-gas alternation scenario(scenario 2)were 4.62×10^(4)t and 46%.The proportions of stor-age capacity under scenarios 1 and 2 for structural or stratigraphic,residual,solubility,and mineral trap-ping were 33.36%,33.96%,32.43%,and 0.25%;and 15.09%,38.65%,45.77%,and 0.49%,respectively.The evolution of the CO_(2)storage mechanism showed an overall trend:stratigraphic and residual trapping first increased and then decreased,whereas solubility trapping gradually decreased,and mineral trapping continuously increased.Based on these results,an evolution diagram of the CO_(2)storage mechanism of low-permeability tight sandstone reservoirs across large timescales was established.
基金supported by the National Natural Science Foundation of China(No.52302241 and 22225801)the Major Science and Technology Programs of Henan Province(241100240200)the China Postdoctoral Science Foundation(No.2023M730940).
文摘MXene derivatives are notable two-dimensional nanomaterials with numerous prospective applications in the domains of energy development.MXene derivative,MBene,diversifies its focus on energy storage and harvesting due to its exceptional electrical conductivity,structural flexibility,and mechanical properties.This comprehensive review describes the sandwich-like structure of the synthesized MBene,derived from its multilayered parent material and its distinct chemical framework to date.The fields of focus encompass the investigation of novel MBenes,the study of phase-changing mechanisms,and the examination of hex-MBenes,ortho-MBenes,tetra-MBenes,tri-MBenes,and MXenes with identical transition metal components.A critical analysis is also provided on the electrochemical mechanism and performance of MBene in energy storage(Li/Na/Mg/Ca/Li–S batteries and supercapacitors),as well as conversion and harvesting(CO_(2) reduction,and nitrogen reduction reactions).The persistent difficulties associated with conducting experimental synthesis and establishing artificial intelligence-based forecasts are extensively deliberated alongside the potential and forthcoming prospects of MBenes.This review provides a single platform for an overview of the MBene’s potential in energy storage and harvesting.
基金supported by the National Natural Science Foundation of China(22269020,42167068,U23A20582)the Gansu Province Higher Education Industry Support Plan Project(2023CYZC-17,2023CYZC-68)+1 种基金the Key Project of Natural Science Foundation of Gansu Province(25JRRA004)2024 Major Cultivation Project for University Research and Innovation Platforms(2024CXPT-10).
文摘Aqueous Zn-ion storage offers high capacity and safety,but practical use is hindered by dendrite formation,side reactions,and hydrogen evolution,affecting stability and efficiency.Herein,tetramethylol acetylenediurea(TA)is proposed as an effective electrolyte additive that modulates the Zn^(2+)deposition environment via coordination competition.The polar functional groups of TA restructure the solvation sheath,while its molecular dipoles generate localized electric fields that accelerate Zn^(2+)migration and promote directional(002)-oriented deposition.These effects collectively suppress side reactions and enhance Zn plating/stripping reversibility.The four hydroxyl(–OH)and conjugated ketone groups(C=O)in the TA molecule have strong coordination ability(Lewis basicity)and can form a stable[Zn(TA)(H_(2)O)_(n)]^(2+)with Zn^(2+),reducing the number of free water molecules and the proportion of active water in the solvation sheath.The TA molecules are adsorbed onto the Zn anode surface,leading to the redistribution of the local spatial electric field and homogenization of ion flux dynamics.Its conjugated planar structure can induce Zn^(2+)to preferentially deposit along the(002)crystal plane.Zn//Zn symmetric cell using TA-containing ZnSO4 electrolyte exhibits stable cycling for more than 2240 h at 1 mA cm^(−2),1 mAh cm^(−2).The Zn//activated carbon(AC)full-cell can stably cycle 30,000 cycles at 5 A g^(−1)with a capacity retention rate of 90%.This study provides important insights into electrolyte engineering strategies for stabilizing Zn anodes,highlighting the potential of molecular design additives in next-generation Zn^(2+)energy storage systems.
基金supported by the National Natural Science Foundation of China(Nos.51971199 and 51771171).
文摘The magnesium based metal hydrogen storage composite system Mg(NH_(2))_(2)-2LiH has a theoretical hydro-gen storage capacity of 5.6 wt.%and is a promising hydrogen storage material for vehicles.However,its application is limited due to serious thermodynamic and kinetic barriers.Introducing efficient catalysts is an effective method to improve the hydrogen storage performance of Mg(NH_(2))_(2)-2LiH.This article in-vestigates for the first time the use of nano rare earth oxide CeO_(2)(~44.5 nm)as an efficient modifier,achieving comprehensive regulation of the hydrogen storage performance of Mg(NH_(2))_(2)-2LiH composite system through oxygen vacancy driven catalysis.The modification mechanism of nano CeO_(2) is also sys-tematically studied using density functional theory(DFT)calculations and experimental results.Research has shown that the comprehensive hydrogen storage performance of the Mg(NH_(2))_(2)-2LiH-5 wt.%CeO_(2) composite system is optimal,with high hydrogen absorption and desorption kinetics and reversible per-formance.The initial hydrogen absorption and desorption temperatures of the composite system were significantly reduced from 110/130℃to 65/80℃,and the release of by-product ammonia was signifi-cantly inhibited.Under the conditions of 170℃/50 min and 180℃/100 min,4.37 wt.%of hydrogen can be rapidly absorbed and released.After 10 cycles of hydrogen release,the hydrogen cycle retention rate increased from 85%to nearly 100%.Further mechanistic studies have shown that the nano CeO_(2-x) gen-erated in situ during hydrogen evolution can effectively weaken the Mg-N and N-H bonds of Mg(NH_(2))_(2),exhibiting good catalytic effects.Meanwhile,oxygen vacancies provide a fast pathway for the diffusion of hydrogen atoms in the composite system.In addition,nano CeO_(2-x) can effectively inhibit the polycrys-talline transformation of the hydrogen evolving product Li_(2)MgN_(2)H_(2) in the system at high temperatures,reducing the difficulty of re-hydrogenation of the system.This study provides an innovative perspective for the efficient modification of magnesium based metal hydrogen storage composite materials using rare earth based catalysts,and also provides a reference for regulating the comprehensive hydrogen storage performance of hydrogen storage materials using rare earth catalysts with oxygen vacancies.
基金supported by the National Natural Science Foundation of China(U22A20120,52071135,51871090,U1804135,and 52301269)the Natural Science Foundation of Hebei Province for Innovation Groups Program(C2022203003)Fundamental Research Funds for the Universities of Henan Province(NSFRF220201).
文摘Designing catalysts with high catalytic activity and stability is the key to achieve the commercial application of MgH_(2).Herein,the sulfur doped Ti_(3)C_(2)(S-Ti_(3)C_(2))was successfully prepared by heat treatment of Ti_(3)C_(2)MXene under Ar/H_(2)S atmosphere to facilitate the hydrogen release and uptake from MgH_(2).The S-Ti_(3)C_(2)exhibited pleasant catalytic effect on the hydriding/dehydriding kinetics and cyclic stability of MgH_(2).The addition of 5 wt%S-Ti_(3)C_(2)into MgH_(2)resulted in a reduction of 114℃in the starting dehydriding temperature compared to pure MgH_(2).MgH_(2)+5 wt%S-Ti_(3)C_(2)sample could quickly release 6.6 wt%hydrogen in 17 min at 220℃,and 6.8 wt%H_(2)was absorbed in 25 min at 200℃.Cyclic testing revealed that MgH_(2)+5 wt%S-Ti_(3)C_(2)system achieved a reversible hydrogen capacity of 6.5 wt%.Characterization analysis demonstrated that Ti-species(Ti0,Ti^(2+),Ti-S,and Ti^(3+))as active species significantly lowered the dehydrogenation temperature and promoted the re-/dehydrogenation kinetics of MgH_(2),and sulfur doping can effectively improve the stability of Ti0 and Ti^(3+),contributing to the improvement of cyclic stability of MgH_(2).This study provides strategy for the construction of catalysts for hydrogen storage materials.
基金supported by the National Key Research and Development Program of China(No.2024YFB4007204,2022YFB4004301)the National Natural Science Founda-tion of China(Grant Nos.52477220,52301287,22005353)+2 种基金the Two-chain Integration Key Project of Shaanxi Province(2021LLRH-09)the Key Research and Development Program of Shaanxi Province(No.2024CY2-GJHX-44,2024CY2-GJHX-53,2024GX-ZDCYL-04-06)the Key Industrial Chain Technology Research Program of Xi’an city(23LL-RHZDZX0017).
文摘The role of catalysts in enhancing the hydrogen storage kinetics of the Mg/MgH_(2)system is pivotal.However,the exploration of efficient catalysts and the underlying principles of their design remain both a prominent focus and a significant challenge in current research.In this study,we present a bimetallic oxide of Bi_(2)Ti_(2)O_(7)hollow sphere as a highly effective catalyst for MgH_(2).As a result,the Bi_(2)Ti_(2)O_(7)-catalyzed Mg/MgH_(2)system lowers the hydrogen desorption initiation temperature to 194.3℃,reduces the peak desorption temperature to 245.6℃,decreases the dehydrogenation activation energy to 82.14 kJ·mol^(−1),and can absorb 5.4 wt.%of hydrogen within 60 s at 200℃,demonstrating outstanding hydrogen ab/desorption kinetics,compared to pure MgH_(2).Additionally,it can maintain a high hydrogen capacity of 5.2 wt.%,even after 50 dehydrogenation cycles,showing good cycle stability.The characterization results show that the high-valent Bi and Ti in Bi_(2)Ti_(2)O_(7)are reduced to their low-valent or even zero-valent metallic states during the dehydrogenation and hydrogenation process,thus establishing an in-situ multivalent and multi-element catalytic environment.Density functional theory calculations further reveal that the synergistic effects between Bi and Ti in the Bi-Ti mixed oxide facilitate the cleavage of Mg-H bonds and lower the kinetic barrier for the dissociation of hydrogen molecules,thereby substantially enhancing the kinetics of the Mg/MgH_(2)system.This study presents a strategic method for developing efficient catalysts for hydrogen storage materials by harnessing the synergistic effects of metal elements.
基金supported by the Science and Technology Department of Guangxi Zhuang Autonomous[grant numbers 2025GXNSFFA069003]the National Natural Science Foundation of China[grant numbers 22379030]+1 种基金Bagui Young Scholars Program of Guangxi Zhuang Autonomous Regionthe high-performance computing platform of Guangxi University.
文摘Mg-based hydrogen storage materials have attracted much attention due to their high hydrogen content,abundant resources,and environmental friendliness.However,the high dehydrogenation temperature,slow kinetics and poor cycling stability are limiting its practical application.This work demonstrates the improved dehydrogenation kinetics and cycling stability of MgH_(2) modified by a hybrid of metallic Ni and layered MoS_(2)(denoted as“Ni-MoS_(2)”)introduced by ball milling,with Ni as the catalyst for MgH_(2) and MoS_(2) as the support for both Ni and MgH_(2).The onset dehydrogenation temperature of MgH_(2) is reduced to 198℃,and the rehydrogenation begins at a low temperature of 50℃.The MgH_(2)+10 wt%Ni-MoS_(2) composite has a fast dehydrogenation kinetics and can release 6.1 wt% hydrogen in 10 min at a constant temperature of 300℃,with the dehydrogenation activation energy significantly reduced from 151 to 85 kJ mol^(-1).During the cycling,the reversible capacity of the composite first exhibits a gradual increase for the initial 22 cycles and then maintains at 6.1 wt% from the 23th cycle to the 50th cycle.The Ni/MoS_(2) addition does not change the overall thermodynamic properties of MgH_(2) but can weaken the Mg-H bonds in the local regions as evident by theoretical calculation.Microstructure studies reveal that the metallic Ni will react with MgH_(2) to form Mg_(2)NiH_(0.3),which can act as a hydrogen pump,while the layered MoS_(2) serves as a support for the well dispersion of MgH_(2) and Ni.It is believed that the synergy of Mg_(2)NiH_(0.3) and layered MoS_(2) contributes to the significantly enhanced hydrogen storage of MgH_(2).This work provides a promising and simple strategy for enhancing the Mg-based hydrogen storage materials by combination of transition metals and layered materials introduced via simple ball milling.
文摘At present,carbon capture and storage(CCS)is the only mature and commercialized technology capable of effectively and economically reducing greenhouse gas emissions to achieve a significant and immedi-ate impact on the CO_(2) level on Earth.Notably,long-term geological storage of captured CO_(2) has emerged as a primary storage method,given its minimal impact on surface ecological environments and high level of safety.The integrity of CO_(2) storage wellbores can be compromised by the corrosion of steel casings and degradation of cement in supercritical CO_(2) storage environments,potentially leading to the leakage of stored CO_(2) from the sites.This critical review endeavors to establish a knowledge foundation for the cor-rosion and materials degradation associated with geological CO_(2) storage through an in-depth examina-tion and analysis of the environments,operation,and the state-of-the-art progress in research pertaining to the topic.This article discusses the physical and chemical properties of CO_(2) in its supercrit-ical phase during injection and storage.It then introduces the principle of geological CO_(2) storage,consid-erations in the construction of storage systems,and the unique geo-bio-chemical environment involving aqueous media and microbial communities in CO_(2) storage.After a comprehensive analysis of existing knowledge on corrosion in CO_(2) storage,including corrosion mechanisms,parametric effects,and corro-sion rate measurements,this review identifies technical gaps and puts forward potential avenues for fur-ther research in steel corrosion within geological CO_(2) storage systems.
基金supported by the State Key Laboratory of Offshore Oil and Gas Exploitation, Open Fund Project (No. CCL2023RCPS0162RQN)the primary funding, National Natural Science Foundation of China (No. ZX20230400)
文摘Saline aquifers are considered as highly favored reservoirs for CO_(2)sequestration due to their favorable properties.Understanding the impact of saline aquifer properties on the migration and distribution of CO_(2)plume is crucial.This study focuses on four key parameters-permeability,porosity,formation pressure,and temperature-to characterize the reservoir and analyse the petrophysical and elastic response of CO_(2).First,we performed reservoir simulations to simulate CO_(2)saturation,using multiple sets of these four parameters to examine their significance on CO_(2)saturation and the plume migration speed.Subsequently,the effect of these parameters on the elastic properties is tested using rock physics theory.We established a relationship of compressional wave velocity(V_(p))and quality factor(Q_(p))with the four key parameters,and conducted a sensitivity analysis to test their sensitivity to V_(p) and Q_(p).Finally,we utilized visco-acoustic wave equation simulated time-lapse seismic data based on the computed V_(p) and Q_(p) models,and analysed the impact of CO_(2) saturation changes on seismic data.As for the above nu-merical simulations and analysis,we conducted sensitivity analysis using both homogeneous and heterogeneous models.Consistent results are found between homogeneous and heterogeneous models.The permeability is the most sensitive parameter to the CO_(2)saturation,while porosity emerges as the primary factor affecting both Q_(p) and V_(p).Both Q_(p) and V_(p) increase with the porosity,which contradicts the observations in gas reservoirs.The seismic simulations highlight significant variations in the seismic response to different parameters.We provided analysis for these observations,which serves as a valuable reference for comprehensive CO_(2)integrity analysis,time-lapse monitoring,injection planning and site selection.
基金funded by the National Natural Science Foundation of China(No.42141013)China Geological Survey(DD20221818,DD20242513).
文摘China has pledged to peak carbon dioxide(CO_(2))emissions by 2030 and achieve carbon neutrality by 2060.Carbon capture and storage(CCS)will play a key role in these efforts.Over the past several years,the China Geological Survey(CGS)has completed the Suitability Evaluation Map of CO_(2)Geological Storage in Main Sedimentary Basins in China and Adjacent Sea Regions in 2017.This map reflects the suitability of the first-and secondary-order tectonic units within sedimentary basins for cO_(2)geological storage for CCS planning.The Junggar Basin is recognized as an important region for future CCS projects.Results from a mesoscale evaluation using the volume method indicate that deep saline aquifers represent the most significant resources for CO_(2)storage,with potential ranging from 48×10^(9)to 164×10^(9)t(with a P50 value of 96×10^(9)t).The highest storage potential is identified in the central and northern parts of the basin,reaching up to 9.5×10^(6)t/km^(2)at the P50 probability level.In contrast,the hinterland,eastern,and western parts of the basin generally exhibit storage potential of below 1.0×10^(6)t/km^(2)at the same probability level.The CGs has also characterized historical CO_(2)plume migration in reservoirs at the storage site of the Shenhua CCS demonstration project and conducted numerical simulations of CO_(2)plume migration for periods of 10 and 20 years following the shutdown of the injection well.The CGS implemented a kiloton-scale pilot test on CO_(2)-enhanced water recovery(CO_(2)-EWR)in eastern Junggar,revealing that CO_(2)flooding can improve the pressure for fluid production,with the highest ratio of CO_(2)to produced fluids estimated at approximately 1.2.Besides,an observation field for natural CO_(2)leakage,covering about 930 m^(2),was built in Qinghai Province.In natural CO_(2)fields or at artificial CO_(2)injection research sites,cO_(2)leakage points are primarily related to the distribution of faults(especially fault crossing),which can serve as pathways for CO_(2)leakage.The observation field provides a natural analog to wellbore failure and offers an opportunity to further monitor CO_(2)geological storage sites.However,it has been inferred that borehole ZK10 at the observation field has become a leakage pathway due to the drilling activities,inadequate well-plugging,and abandonment procedures without considering CO_(2)corrosion.
基金funded by the National Science and Technology Major Project for the Exploration and Development of New Types of Oil and Gas(No.2024ZD14066)the National Natural Science Foundation of China(No.52274053)+1 种基金the Natural Science Foundation of Beijing Municipality(No.3173044)the Xinjiang Conglomerate Reservoir Laboratory Development Foundation Project(No.2020D04045)。
文摘Carbon dioxide enhanced oil recovery(CO_(2)-EOR)technology is used for oil production and CO_(2) storage in reservoirs.Methods are being constantly developed to optimize oil recovery and CO_(2) storage during the CO_(2) displacement process,especially for low-permeability reservoirs under varying geological conditions.In this study,long-core experiments and trans-scale numerical simulations are employed to examine the characteristics of oil production and CO_(2) storage.Optimal production parameters for the target reservoir are also proposed.The results indicate that maintaining the pressure at 1.04 to 1.10 times the minimum miscible pressure(MMP)and increasing the injection rate can enhance oil production in the early stage of reservoir development.In contrast,reducing the injection rate at the later stages prevents CO_(2) channeling,thus improving oil recovery and CO_(2) storage efficiency.A solution-doubling factor is introduced to modify the calculation method for CO_(2) storage,increasing its accuracy to approximately 90%.Before CO_(2) breakthrough,prioritizing oil production is recommended to maximize the economic benefits of this process.In the middle stage of CO_(2) displacement,decreasing the injection rate optimizes the coordination between oil displacement and CO_(2) storage.Further,in the late stage,reduced pressure and injection rates are required as the focus shifts to CO_(2) storage.
基金supported by the National Natural Science Foundation of China(52276204 and U22A20435)。
文摘The reaction characteristics of calcium-based materials during calcium looping(CaL)process are pivotal in the efficiency of CaL thermochemical energy storage(TCES)and CO_(2)capture systems.Currently,metal oxide doping is the primary method to enhance the reaction characteristics of calcium-based materials over multiple cycles.In particular,co-doping with variable-valence metal oxides(VVMOs)can effectively increase the oxygen vacancy content in calcium-based materials,significantly improving their cyclic reaction characteristics.However,there are so numerous VVMOs co-doping schemes that the experimental screening process is complex,consuming considerable time and economic costs.Density functional theory(DFT)calculations have been widely used to reveal the impact of metal oxide doping on the cyclic reaction characteristics of calcium-based materials,with calculation results showing good agreement with experimental conclusions.Nevertheless,there is still a lack of research on utilizing DFT to screen calcium-based materials,and a systematic research methodology has not yet been established.In this study,a systematic DFT-based screening methodology for calcium-based materials was proposed.A series of key parameters for DFT calculations including CO_(2)adsorption energy,oxygen vacancy formation energy,and sintering resistance were proposed.Furthermore,a preliminary mathematical model to predict the CaL TCES and CO_(2)capture performance of calcium-based materials was introduced.The aforementioned DFT method was employed to screen for VVMOs co-doped calcium-based materials.The results revealed that Mn and Ce co-doped calcium-based materials exhibited superior DFT-predicted reaction characteristics.These DFT predictions were validated through experimental assessments of cyclic thermochemical energy storage,CO_(2)capture,and relevant characterization.The outcomes demonstrate a high degree of consistency among DFT-based predictions,experimental results,and characterization.Hence,the DFT-based screening methodology for calcium-based materials proposed herein is a viable solution,poised to offer theoretical insights for the efficient design of calcium-based materials.
基金support from the National Key Research and Development Program of China(2023YFE0120700)National Natural Science Foundation of China(52274041)Distinguished Young Sichuan Science Scholars(2023NSFSC1954).
文摘Cyclic injection holds great potential for CO_(2) emission reduction coupled with enhanced unconventional oil recovery.There is,however,a lack of a thorough understanding of carbon distribution,migration,and transformation underground over time at the reservoir scale.To address this issue,we conducted a rig-orous numerical simulation integrating microseismic events,multi-geomechanics,and multi-geochemistry to represent the complex fracture geometry,rock stress sensitivity,and CO_(2)-oil-brine-rock interactions.The fluid model,reservoir model,and geochemical reaction kinetics were carefully validated and calibrated using experimental data.The performance of CO_(2) utilization and geological storage was comprehensively investigated in terms of changes in oil production,CO_(2) storage,carbon distribution,and petrophysical properties.The results indicate that 48.3%of the injected CO_(2) was stored stably under-ground after ten cycles(ten years),with a 3.4%increase in oil recovery.The presence of multiple CO_(2) stor-age forms,such as dissolved in water and mineralized carbonate,impeded CO_(2)-oil interaction,leading to a 25.9%reduction in the volume of the CO_(2)-oil mixing zone and a 2.2%decrease in cumulative oil pro-duction,albeit with a 7.7%increase in the storage rate.The cyclic injection mode had a significant impact on the migration and transformation of CO_(2) in the reservoir.While dissolved CO_(2) in oil accounted for over half of the total storage,it had the possibility of being released during production.After ten cycles,20%of the injected CO_(2)(approximately 12000 t)reached long-term storage in four forms:mineralized carbon-ate(6%),water-dissolved CO_(2)(6%),aqueous ions(4%),and trapped gas(4%).Notably,the non-fracture zone within the stimulated reservoir volume(SRV)served as the primary trapping area for residual gas.This work provides valuable insights into dynamic CO_(2) transport and transformation processes under cyclic injection and presents a more comprehensive and precise framework for assessing CO_(2) capture,utilization,and storage with enhanced oil recovery(CCUS-EOR)performance in unconventional reser-voirs after fracturing.
基金the National Natural Science Foundation of China(Nos.42206234,42476228,42076220)the Key R&D Project of Shandong Province(No.2024SFGC0302)+2 种基金the Project of Laoshan Laboratory(No.LSKJ202203404)the Project of China Geology Survey(Nos.DD202503023,DD20230401)support from the Ocean Negative Carbon Emissions(ONCE)Program。
文摘Offshore carbon dioxide(CO_(2))geological storage is a promising strategy for reducing carbon emissions and supporting sustainable development in coastal regions within a carbon neutrality framework.However,only a few works have focused on offshore basins in China.To address this gap,this study established a dual indicator system that comprises necessary and critical indices and is integrated with the analytic hierarchy process.A coupled analysis was then performed to evaluate the suitability of 10 offshore sedimentary basins in China for CO_(2)geological storage.The necessary indicator system focuses on storage potential,geological conditions,and engineering feasibility.Meanwhile,the critical indicator system emphasizes the safety of storage projects and the viability of drilling operations.Evaluation results revealed that China's offshore basins have undergone two geological evolution stages,namely,the rifting and post-rifting phases,leading to the formation of a dual-layer structure characterized by faulted lower layers and sagged upper layers.These basins have thick and widespread Cenozoic strata,generally low seismic activity,and medium-to-low geothermal gradients.They form five reservoir-caprock systems with favorable geological conditions for CO_(2)storage.The Pearl River Mouth,East China Sea Shelf,and Bohai Basins emerged as primary candidates that offer substantial storage potential to support carbon neutrality goals in the Bohai Rim Economic Zone,Yangtze River Delta Economic Zone,and Guangdong-Hong Kong-Macao Greater Bay Area.The Beibu Gulf and South Yellow Sea Basins were identified as secondary candidates,and the Qiongdongnan and Yinggehai Basins were considered potential alternatives.
