Constructing silicon(Si)-based composite electrodes that possess high energy density,long cycle life,and fast charging capability simultaneously is critical for the development of high performance lithium-ion batterie...Constructing silicon(Si)-based composite electrodes that possess high energy density,long cycle life,and fast charging capability simultaneously is critical for the development of high performance lithium-ion batteries for mitigating range anxiety and slow charging issues in new energy vehicles.Herein,a thick silicon/carbon composite electrode with vertically aligned channels in the thickness direction(VC-SC)is constructed by employing a bubble formation method.Both experimental characterizations and theoretical simulations confirm that the obtained vertical channel structure can effectively address the problem of sluggish ion transport caused by high tortuosity in conventional thick electrodes,conspicuously enhance reaction kinetics,reduce polarization and side reactions,mitigate stress,increase the utilization of active materials,and promote cycling stability of the thick electrode.Consequently,when paired with LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622),the VC-SC||NCM622 pouch type full cell(~6.0 mAh cm^(-2))exhibits significantly improved rate performance and capacity retention compared with the SC||NCM622 full cell with the conventional silicon/carbon composite electrode without channels(SC)as the anode.The assembled VC-SC||NCM622 pouch full cell with a high energy density of 490.3 Wh kg^(-1)also reveals a remarkable fast charging capability at a high current density of 2.0 mA cm^(-2),with a capacity retention of 72.0%after 500 cycles.展开更多
Silicon-based anode is a promising candidate for all-solid-state batteries(ASSBs).However,it must be further improved because of its tremendous volume change.In this study,various interface treatment strategies for Si...Silicon-based anode is a promising candidate for all-solid-state batteries(ASSBs).However,it must be further improved because of its tremendous volume change.In this study,various interface treatment strategies for SiO/carbon composite anodes in ASSBs were investigated using a multiphysics modeling framework.By evaluating the effects of active(carbon)and inactive coating materials,as well as the geometric and mechanical parameters,this research provides critical insights into optimizing their electrochemical performance and mechanical stability.Computational results indicate that carbon coatings can greatly enhance lithiation kinetics by regulating the interfacial electrochemical potential gradients,reducing the residual lithium concentration,and homogenizing the lithium-ion distribution compared with uncoated or inactive-coated configurations.In addition,thinner carbon coatings further improve capacity retention and stress management by balancing shorter lithium diffusion pathways with mitigated interfacial stress accumulation.Despite their ability to mechanically stabilize the anode,inactive coatings exhibit tradeoffs between lithium transport kinetics and stress modulation,with optimal performance achieved at lower Young’s moduli.Mechanical analyses highlight distinct failure mechanisms at the anode–electrolyte(shear driven)and particle-coating(tension driven)interfaces,emphasizing the need for tailored adhesion strategies.These findings provide actionable guidelines for designing robust SiO-based anodes,emphasizing the interplay among electrochemical efficiency,stress regulation,and interfacial durability in ASSBs.展开更多
Silicon （Si） has been considered as one of the most promising anode material for tHe next generation lithium-ion batteries （LIBs） with high energy densities, due to its high theoretical capacity, abundant availabi...Silicon （Si） has been considered as one of the most promising anode material for tHe next generation lithium-ion batteries （LIBs） with high energy densities, due to its high theoretical capacity, abundant availability and environmental friendliness. However. silicon materials with low intrinsic electric and ionic conductivity suffer from huge volume variation during lithiation/delithiation processes leading to the pulverization of Si and subsequently resulting in severe capacity fading of the electrodes. Coupling of Si with carbon （C） realizes a favorable combination of the two materials properties, such as high lithiation capacity of Si and excellent mechanical and conductive properties of C. making silicon/carbon composite （Si/C） ideal candidates for LIBs anodes. In this review, recent progresses of Si/C materials utilized in LIBs are summarized in terms of structural design principles, material synthesis methods, morphological characteristics and electrochemical performances by highlighting the material structures. The mechanisms behind the performance enhancement are also discussed. Moreover, other factors that affect the performance of Si/C anodes, such as prelithiation, electrolyte additives, and binders, are also discussed. We aim to present a full scope of the Si/C-based anodes, and help understand and design future structures of Si/C anodes in LIBs,展开更多
Silicon(Si)has been studied as a promising alloying type anode for lithium-ion batteries due to its high specific capacity,low operating potential and abundant resources.Nevertheless,huge volume expansion during alloy...Silicon(Si)has been studied as a promising alloying type anode for lithium-ion batteries due to its high specific capacity,low operating potential and abundant resources.Nevertheless,huge volume expansion during alloying/dealloying processes and low electronic conductivity of Si anodes restrict their electrochemical performance.Thus,carbon(C)materials with special physical and chemical properties are applied in Si anodes to effectively solve these problems.This review focuses on current status in the exploration of Si/C anodes,including the lithiation mechanism and solid electrolyte interface formation,various carbon sources in Si/C anodes,such as traditional carbon sources(graphite,pitch,biomass),and novel carbon sources(MXene,graphene,MOFs-derived carbon,graphdiyne,etc.),as well as interfacial bonding modes of Si and C in the Si/C anodes.Finally,we summarize and prospect the selection of carbonaceous materials,structural design and interface control of Si/C anodes,and application of Si/C anodes in all-solid-state lithium-ion batteries and sodium-ion batteries et al.This review will help researchers in the design of novel Si/C anodes for rechargeable batteries.展开更多
Silicon/carbon composites,which integrate the high lithium storage performance of silicon with the exceptional mechanical strength and conductivity of carbon,will replace the traditional graphite electrodes for high-e...Silicon/carbon composites,which integrate the high lithium storage performance of silicon with the exceptional mechanical strength and conductivity of carbon,will replace the traditional graphite electrodes for high-energy lithium-ion batteries.Various strategies have been designed to synthesize silicon/carbon composites for tackling the issues of anode pulverization and poor stability in the anodes,thereby improving the lithium storage ability.The effect of the regulation method at each scale on the final negative electrode performance remains unclear.However,it has not been fully clarified how the regulation methods at each scale influence the final anode performance.This review will categorize the materials structure into three scales:molecular scale,nanoscale,and microscale.First,the review will examine modification methods at the molecular scale,focusing on the interfacial bonding force between silicon and carbon.Next,it will summarize various nanostructures and special shapes in the nanoscale to explore the construction of silicon/carbon composites.Lastly,the review will provide an analysis of microscale control approaches,focusing on the formation of composite particle with micron size and the utilization of micro-Si.This review provides a comprehensive overview of the multi-scale design of silicon/carbon composite anode materials and their optimization strategies to enhance the performance of lithium-ion batteries.展开更多
Silicon (Si) is regarded as a promising material for lithium-ion battery anode because of high theoretical capacity. Nevertheless, Si faces particle pulverization and rapid capacity fading due to serious volume change...Silicon (Si) is regarded as a promising material for lithium-ion battery anode because of high theoretical capacity. Nevertheless, Si faces particle pulverization and rapid capacity fading due to serious volume change during the lithiation and the delithiation process. In this work, a silicon/carbon composite constituted to Si powder and carbon nanofiber (CNF) is produced to solve the above issues as a new design structure of anode material. The Si powder was recycled from the silicon slicing waste in photovoltaic industry and the CNF was from dry rice straws. By mixing the purified Si powder with CNF, the composite was synthesized by the freeze-drying method and calcination. In the cyclic test, Si adding with 1 wt% CNF showed 3091 mAh/g capacity in the first cycle and 1079 mAh/g capacity after 100 cycles at the current density of 0.5 A/g, which were both better than pristine Si. SEM images also show the composite structure can eliminate cracks on the surface of the electrode during cycling. CNF attaching on Si particles can increase specific surface area, so binder can easily combine the active materials and the conductive materials together. This strategy enhances the structure stability and prevents the electrode from delamination.展开更多
Silicon anodes are promising for use in lithium-ion batteries.However,their practical application is severely limited by their large volume expansion leading to irreversible material fracture and electrical disconnect...Silicon anodes are promising for use in lithium-ion batteries.However,their practical application is severely limited by their large volume expansion leading to irreversible material fracture and electrical disconnects.This study proposes a new top-down strategy for preparing microsize porous silicon and introduces polyacrylonitrile(PAN)for a nitrogen-doped carbon coating,which is designed to maintain the internal pore volume and lower the expansion of the anode during lithiation and delithiation.We then explore the effect of temperature on the evolution of the structure of PAN and the electrochemical behavior of the composite electrode.After treatment at 400℃,the PAN coating retains a high nitrogen content of 11.35 at%,confirming the presence of C—N and C—O bonds that improve the ionic-electronic transport properties.This treatment not only results in a more intact carbon layer structure,but also introduces carbon defects,and produces a material that has remarkable stable cycling even at high rates.When cycled at 4 A g^(-1),the anode had a specific capacity of 857.6 mAh g^(-1) even after 200 cycles,demonstrating great potential for high-capacity energy storage applications.展开更多
There is an urgent need to develop high-areal-capacity silicon(Si)anodes with good cycling stability and rate capability for high-energy-density lithium-ion batteries(LIBs).However,this remains a huge challenge due to...There is an urgent need to develop high-areal-capacity silicon(Si)anodes with good cycling stability and rate capability for high-energy-density lithium-ion batteries(LIBs).However,this remains a huge challenge due to large volume expansion-induced mechanical degradation and electrical connectivity loss in thick electrodes.Here,a three-in-one strategy is proposed to achieve high-areal-capacity silicon anodes by constructing a multi-level interconnected 3D porous and robust conductive network that carbon nanofibers and vertical carbon nanosheets tightly encapsulate on the surface of Si nanoparticles(Si NPs)anchored in porous carbon felts.This network accommodates large volume expansion of Si NPs to significantly improve electrode mechanical stability and creates excellent electrical connectivity to boost charge transport in thick electrodes,revealed through Multiphysics field simulations and in situ electrochemical techniques.Therefore,the designed Si anodes achieve superior long-term stability with a capacity of 8.13 mAh cm^(-2)after 500 cycles and an ultrahigh areal capacity of 45.8 mAh cm^(-2).In particular,Ah-level pouch cells demonstrate an impressive capacity retention of 79.34%after 500 cycles at 1 C.Our study offers novel insights and directions for understanding and optimizing high-areal-capacity silicon-carbon composite anodes.展开更多
The development of materials with excellent microwave absorption(MWA)and electromagnetic interference(EMI)shielding performances has currently received attention.Herein,mesophase pitch-based carbon foam(MPCF)with 3D i...The development of materials with excellent microwave absorption(MWA)and electromagnetic interference(EMI)shielding performances has currently received attention.Herein,mesophase pitch-based carbon foam(MPCF)with 3D interconnected pore structure was prepared through the high pressure pyrolysis of mesophase coal tar pitch.It is found that the 3D interconnected cellular pores of MPCF facilitate multiple reflections of electromagnetic waves,which results in the minimum reflection loss(RLmin)value of MPCF reaches-37.84 dB with the effective absorption bandwidth(EAB)of 5.44 GHz at a thickness of 2.70 mm,and the total average electromagnetic shielding effectiveness(SE_(T))under 3.00 mm thickness achieves 26.52 dB in X-band.Subsequently,MPCF is activated by KOH to obtain activated carbon foam(A-MPCF).The average SE_(T)of A-MPCF achieves 103.00 dB for abundant nanopores on the pore cell walls,which leads to a transition from the multiple reflections of electromagnetic waves on the walls to diffuse reflection.Unfortunately,the reflection coefficient(R)of A-MPCF increases from 0.78 to 0.90.To reduce the R value,Fe_(3)O_(4)/A-MPCF was fabricated via the in situ growth of nano Fe_(3)O_(4)on A-MPCF.Consequently,the R value of Fe_(3)O_(4)/A-MPCF was reduced from 0.90 to 0.74,whereas the MWA performance was only slightly decreased.This work proposes a simple strategy for simultaneously adjusting MWA and EMI shielding performances of materials.展开更多
Ship operations are crucial to global trade,and their decarbonization is essential to mitigate climate change.This study evaluates the economic viability of existing and emerging decarbonization technologies in mariti...Ship operations are crucial to global trade,and their decarbonization is essential to mitigate climate change.This study evaluates the economic viability of existing and emerging decarbonization technologies in maritime shipping using the levelized cost of energy methodology.It includes a detailed comparative analysis based on essential criteria and sensitivity assessments to highlight the economic impacts of technological advancements.Key factors influencing total costs include fuel costs,carbon pricing,and energy demands for carbon capture.The findings reveal that methanol is more cost-effective than heavy fuel oil(HFO)when priced below 3000 CNY/t,assuming HFO costs 4400 CNY/t.Additionally,methanol with post-combustion carbon capture is less expensive than pre-combustion carbon capture.When carbon prices rise above 480 CNY/t,carbon capture technologies prove more economical than purchasing carbon emission allowances for HFO and liquefied natural gas.Enhanc-ing the use of exhaust gas waste heat is recommended for cost savings.Post-combustion carbon capture also shows greater efficiency,requiring about 1.1 GJ/t less energy than pre-combustion methods,leading to lower overall costs.Future research should focus on market mechanisms to stabilize fuel prices and develop less energy-intensive carbon capture technologies.This study offers critical insights into effective decarbonization strategies for advancing global maritime trade in the present and future.展开更多
To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content ...To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content in coal)catalysts were prepared by the incipient wetness impregnation method,followed by acid washing to remove calcium-containing minerals.Comprehensive characterization and low-temperature denitrification tests revealed that calcite-induced structural modulation of coal-derived AC significantly enhances catalytic activity.Specifically,NO conversion increased from 88.3%of Mn-Ce/De-AC to 91.7%of Mn-Ce/De-AC-1CaCO_(3)(210℃).The improved SCR denitrification activity results from the enhancement of physicochemical properties including higher Mn^(4+)content and Ce^(4+)/Ce^(3+)ratio,an abundance of chemisorbed oxygen and acidic sites,which could strengthen the SCR reaction pathways(richer NH_(3)activated species and bidentate nitrate active species).Therefore,NO removal is enhanced.展开更多
Porous carbon microspheres are widely regarded as a superior CO_(2) adsorbent due to their exceptional efficiency and affordability.However,better adsorption performance is very attractive for porous carbon microspher...Porous carbon microspheres are widely regarded as a superior CO_(2) adsorbent due to their exceptional efficiency and affordability.However,better adsorption performance is very attractive for porous carbon microspheres.And modification of the pore structure is one of the effective strategies.In this study,multi-cavity mesoporous carbon microspheres were successfully synthesized by the synergistic method of soft and hard templates,during which a phenolic resin with superior thermal stability was employed as the carbon precursor and a mixture of silica sol and F108 as the mesoporous template.Carbon microspheres with multi-cavity mesoporous structures were prepared,and all the samples showed highly even mesopores,with diameters around 12 nm.The diameter of these microspheres decreased from 396.8 nm to about 182.5 nm with the increase of silica sol.After CO_(2) activation,these novel carbon microspheres(APCF0.5-S1.75)demonstrated high specific surface area(983.3 m^(2)/g)and remarkable CO_(2) uptake of 4.93 mmol/g at 0℃ and1 bar.This could be attributed to the unique multi-cavity structure,which offers uniform mesoporous pore channels,minimal CO_(2) transport of and a greater number of active sites for CO_(2) adsorption.展开更多
The electromagnetic wave absorption of silicon carbide nanowires is improved by their uniform and diverse cross-structures.This study introduces a sustainable and high value-added method for synthesizing silicon carbi...The electromagnetic wave absorption of silicon carbide nanowires is improved by their uniform and diverse cross-structures.This study introduces a sustainable and high value-added method for synthesizing silicon carbide nanowires using lignite and waste silicon powder as raw materials through carbothermal reduction.The staggered structure of nanowires promotes the creation of interfacial polarization,impedance matching,and multiple loss mechanisms,leading to enhanced electromagnetic absorption performance.The silicon carbide nanowires demonstrate outstanding electromagnetic absorption capabilities with the minimum reflection loss of-48.09 d B at10.08 GHz and an effective absorption bandwidth(the reflection loss less than-10 d B)ranging from 8.54 to 16.68 GHz with a thickness of 2.17 mm.This research presents an innovative approach for utilizing solid waste in an environmentally friendly manner to produce broadband silicon carbide composite absorbers.展开更多
Heteroatom-doped carbon is considered a promising alternative to commercial Pt/C as an efficient catalyst for the oxygen reduction reaction(ORR).This study presents the synthesis of iron-loaded,sulfur and nitrogen co-...Heteroatom-doped carbon is considered a promising alternative to commercial Pt/C as an efficient catalyst for the oxygen reduction reaction(ORR).This study presents the synthesis of iron-loaded,sulfur and nitrogen co-doped carbon(Fe/SNC)via in situ incorporation of 2-aminothiazole molecules into zeolitic imidazolate framework-8(ZIF-8)through coordination between metal ions and organic ligands.Sulfur and nitrogen doping in carbon supports effectively modulates the electronic structure of the catalyst,increases the Brunauer-Emmett-Teller surface area,and exposes more Fe-N_(x)active centers.Fe-loaded,S and N co-doped carbon with Fe/S molar ratio of 1:10(Fe/SNC-10)exhibits a half-wave potential of 0.902 V vs.RHE.After 5000 cycles of cyclic voltammetry,its half-wave potential decreases by only 20 mV vs.RHE,indicating excellent stability.Due to sulfur s lower electronegativity,the electronic structure of the Fe-N_(x)active center is modulated.Additionally,the larger atomic radius of sulfur introduces defects into the carbon support.As a result,Fe/SNC-10 demonstrates superior ORR activity and stability in alkaline solution compared with Fe-loaded N-doped carbon(Fe/NC).Furthermore,the zinc-air battery assembled with the Fe/SNC-10 catalyst shows enhanced performance relative to those assembled with Fe/NC and Pt/C catalysts.This work offers a novel design strategy for advanced energy storage and conversion applications.展开更多
Nanoconfinement is a promising approach to simultaneously enhance the thermodynamics,kinetics,and cycling stability of hydrogen storage materials.The introduction of supporting scaffolds usually causes a reduction in ...Nanoconfinement is a promising approach to simultaneously enhance the thermodynamics,kinetics,and cycling stability of hydrogen storage materials.The introduction of supporting scaffolds usually causes a reduction in the total hydrogen storage capacity due to“dead weight.”Here,we synthesize an optimized N-doped porous carbon(rN-pC)without heavy metal as supporting scaffold to confine Mg/MgH_(2) nanoparticles(Mg/MgH_(2)@rN-pC).rN-pC with 60 wt%loading capacity of Mg(denoted as 60 Mg@rN-pC)can adsorb and desorb 0.62 wt%H_(2) on the rN-pC scaffold.The nanoconfined MgH_(2) can be chemically dehydrided at 175℃,providing~3.59 wt%H_(2) with fast kinetics(fully dehydrogenated at 300℃ within 15 min).This study presents the first realization of nanoconfined Mg-based system with adsorption-active scaffolds.Besides,the nanoconfined MgH_(2) formation enthalpy is reduced to~68 kJ mol^(−1) H_(2) from~75 kJ mol^(−1) H_(2) for pure MgH_(2).The composite can be also compressed to nanostructured pellets,with volumetric H_(2) density reaching 33.4 g L^(−1) after 500 MPa compression pressure,which surpasses the 24 g L^(−1) volumetric capacity of 350 bar compressed H_(2).Our approach can be implemented to the design of hybrid H_(2) storage materials with enhanced capacity and desorption rate.展开更多
To achieve low-carbon regulation of electric vehicle(EV)charging loads under the“dual carbon”goals,this paper proposes a coordinated scheduling strategy that integrates dynamic carbon factor prediction and multiobje...To achieve low-carbon regulation of electric vehicle(EV)charging loads under the“dual carbon”goals,this paper proposes a coordinated scheduling strategy that integrates dynamic carbon factor prediction and multiobjective optimization.First,a dual-convolution enhanced improved Crossformer prediction model is constructed,which employs parallel 1×1 global and 3×3 local convolutionmodules(Integrated Convolution Block,ICB)formultiscale feature extraction,combinedwith anAdaptive Spectral Block(ASB)to enhance time-series fluctuationmodeling.Based on high-precision predictions,a carbon-electricity cost joint optimization model is further designed to balance economic,environmental,and grid-friendly objectives.The model’s superiority was validated through a case study using real-world data from a renewable-heavy grid.Simulation results show that the proposed multi-objective strategy demonstrated a superior balance compared to baseline and benchmark models,achieving a 15.8%reduction in carbon emissions and a 5.2%reduction in economic costs,while still providing a substantial 22.2%reduction in the peak-valley difference.Its balanced performance significantly outperformed both a single-objective strategy and a state-of-the-art Model Predictive Control(MPC)benchmark,highlighting the advantage of a global optimization approach.This study provides theoretical and technical pathways for dynamic carbon factor-driven EV charging optimization.展开更多
Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-...Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-C_(3)N_(4) suffers from limited visible-light absorption and low charge-carrier mobility.In this study,a phosphorus-doped tubular carbon nitride(5P-TCN)was synthesized via a precursor self-assembly method using phosphoric acid and melamine as raw materials,eliminating the need for organic solvents or templates.The 5P-TCN catalyst demonstrated enhanced visible-light absorption,improved charge transfer capability,and a 5.25-fold increase in specific surface area(31.092 m^(2)/g),which provided abundant active sites to efficiently drive the PMS-assisted photocatalytic reaction.The 5P-TCN/vis/PMS system exhibited exceptional degradation performance for organic pollutants across a broad pH range(3–9),achieving over 92%degradation of Rhodamine B(RhB)within 15 min.Notably,the system retained>98%RhB degradation efficiency after three consecutive operational cycles,demonstrating robust operational stability and reusability.Moreover,key parameters influencing,active radi-cals,degradation pathways,and potential mechanisms for RhB degradation were systematically investigated.This work proposes a green and cost-effective strategy for developing high-efficiency photocatalysts,while demon-strating the exceptional capability of a PMS-assisted photocatalytic system for rapid degradation of RhB.展开更多
Global land monsoon precipitation(GLMP)is highly sensitive to changes in interhemispheric thermal contrast(ITC).Amplified interhemispheric asymmetries of GLMP due to enhanced ITC driven by high-level anthropogenic emi...Global land monsoon precipitation(GLMP)is highly sensitive to changes in interhemispheric thermal contrast(ITC).Amplified interhemispheric asymmetries of GLMP due to enhanced ITC driven by high-level anthropogenic emissions are expected to simultaneously increase the probability of regional floods and droughts,threatening ecosystems within global terrestrial monsoon regions and the freshwater supply for billions of residents in these areas.In this study,the responses of GLMP to the evolution of ITC toward the carbon neutrality goal are assessed using multimodel outputs from a new model intercomparison project(CovidMIP).The results show that the Northern Hemisphere-Southern Hemisphere(NH-SH)asymmetry of GLMP in boreal summer weakens during the 2040s,as a persistent reduction in well-mixed greenhouse gas(WMGHG)emissions leads to a downward trend in the ITC after 2040.At the same time,the reduction in WMGHG emissions dampens the Eastern Hemisphere-Western Hemisphere(EH-WH)asymmetry of GLMP by inducing La Niña-like cooling and enhancing moisture transport to Inner America.The resulting increases in land monsoon precipitation(LMP)may alleviate drought under the global warming scenario by about 19%-25%and 7%-9%in the WH and SH monsoon regions,respectively.However,a persistent reduction in aerosol emissions in Asia will dominate the increases in LMP in this region until the mid-21st century,and these increases may be approximately 23%-60%of the growth under the global warming scenario.Our results highlight the different rates of response of aerosol and WMGHG concentrations to the carbon neutrality goal,leading to various changes in LMP at global and regional scales.展开更多
Flash Joule heating(FJH),as a high-efficiency and low-energy consumption technology for advanced materials synthesis,has shown significant potential in the synthesis of graphene and other functional carbon materials.B...Flash Joule heating(FJH),as a high-efficiency and low-energy consumption technology for advanced materials synthesis,has shown significant potential in the synthesis of graphene and other functional carbon materials.Based on the Joule effect,the solid carbon sources can be rapidly heated to ultra-high temperatures(>3000 K)through instantaneous high-energy current pulses during FJH,thus driving the rapid rearrangement and graphitization of carbon atoms.This technology demonstrates numerous advantages,such as solvent-and catalyst-free features,high energy conversion efficiency,and a short process cycle.In this review,we have systematically summarized the technology principle and equipment design for FJH,as well as its raw materials selection and pretreatment strategies.The research progress in the FJH synthesis of flash graphene,carbon nanotubes,graphene fibers,and anode hard carbon,as well as its by-products,is also presented.FJH can precisely optimize the microstructures of carbon materials(e.g.,interlayer spacing of turbostratic graphene,defect concentration,and heteroatom doping)by regulating its operation parameters like flash voltage and flash time,thereby enhancing their performances in various applications,such as composite reinforcement,metal-ion battery electrodes,supercapacitors,and electrocatalysts.However,this technology is still challenged by low process yield,macroscopic material uniformity,and green power supply system construction.More research efforts are also required to promote the transition of FJH from laboratory to industrial-scale applications,thus providing innovative solutions for advanced carbon materials manufacturing and waste management toward carbon neutrality.展开更多
Electrocatalytic nitrate reduction reaction(NO3RR)represents a sustainable and environmentally benign route for ammonia(NH3)synthesis.However,NO3RR is still limited by the competition from hydrogen evolution reaction(...Electrocatalytic nitrate reduction reaction(NO3RR)represents a sustainable and environmentally benign route for ammonia(NH3)synthesis.However,NO3RR is still limited by the competition from hydrogen evolution reaction(HER)and the high energy barrier in the hydrogenation step of nitrogen-containing intermediates.Here,we report a selective etching strategy to construct Ru M nanoalloys(M=Fe,Co,Ni,Cu)uniformly dispersed on porous nitrogen-doped carbon substrates for efficient neutral NH3electrosynthesis.Density functional theory calculations confirm that the synergic effect between Ru and transition metal M modulates the electronic structure of the alloy,significantly lowering the energy barrier for the conversion of*NO_(2)to*HNO_(2).Experimentally,the optimized Ru Fe-NC catalyst achieves 100%Faraday efficiency with a high yield rate of 0.83 mg h^(-1)mg^(-1)catat a low potential of-0.1 V vs.RHE,outperforming most reported catalysts.In situ spectroscopic analyses further demonstrate that the Ru M-NC effectively promotes the hydrogenation of nitrogen intermediates while inhibiting the formation of hydrogen radicals,thereby reducing HER competition.The Ru FeNC assembled Zn-NO_(3)^(-)battery achieved a high open-circuit voltage and an outstanding power density and capacity,which drive selective NO_(3)^(-)conversion to NH3.This work provides a powerful synergistic design strategy for efficient NH3electrosynthesis and a general framework for the development of advanced multi-component catalysts for sustainable nitrogen conversion.展开更多
基金National Key R&D Program of China,Grant/Award Number:2023YFB2503900National Natural Science Foundation of China,Grant/Award Number:12172143Shenzhen Science and Technology Program,Grant/Award Numbers:JCYJ20220818100418040,JCYJ20220530160816038。
文摘Constructing silicon(Si)-based composite electrodes that possess high energy density,long cycle life,and fast charging capability simultaneously is critical for the development of high performance lithium-ion batteries for mitigating range anxiety and slow charging issues in new energy vehicles.Herein,a thick silicon/carbon composite electrode with vertically aligned channels in the thickness direction(VC-SC)is constructed by employing a bubble formation method.Both experimental characterizations and theoretical simulations confirm that the obtained vertical channel structure can effectively address the problem of sluggish ion transport caused by high tortuosity in conventional thick electrodes,conspicuously enhance reaction kinetics,reduce polarization and side reactions,mitigate stress,increase the utilization of active materials,and promote cycling stability of the thick electrode.Consequently,when paired with LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622),the VC-SC||NCM622 pouch type full cell(~6.0 mAh cm^(-2))exhibits significantly improved rate performance and capacity retention compared with the SC||NCM622 full cell with the conventional silicon/carbon composite electrode without channels(SC)as the anode.The assembled VC-SC||NCM622 pouch full cell with a high energy density of 490.3 Wh kg^(-1)also reveals a remarkable fast charging capability at a high current density of 2.0 mA cm^(-2),with a capacity retention of 72.0%after 500 cycles.
基金supported by the startup funding from Shanghai Jiao Tong University(Grant No.WH220402052).
文摘Silicon-based anode is a promising candidate for all-solid-state batteries(ASSBs).However,it must be further improved because of its tremendous volume change.In this study,various interface treatment strategies for SiO/carbon composite anodes in ASSBs were investigated using a multiphysics modeling framework.By evaluating the effects of active(carbon)and inactive coating materials,as well as the geometric and mechanical parameters,this research provides critical insights into optimizing their electrochemical performance and mechanical stability.Computational results indicate that carbon coatings can greatly enhance lithiation kinetics by regulating the interfacial electrochemical potential gradients,reducing the residual lithium concentration,and homogenizing the lithium-ion distribution compared with uncoated or inactive-coated configurations.In addition,thinner carbon coatings further improve capacity retention and stress management by balancing shorter lithium diffusion pathways with mitigated interfacial stress accumulation.Despite their ability to mechanically stabilize the anode,inactive coatings exhibit tradeoffs between lithium transport kinetics and stress modulation,with optimal performance achieved at lower Young’s moduli.Mechanical analyses highlight distinct failure mechanisms at the anode–electrolyte(shear driven)and particle-coating(tension driven)interfaces,emphasizing the need for tailored adhesion strategies.These findings provide actionable guidelines for designing robust SiO-based anodes,emphasizing the interplay among electrochemical efficiency,stress regulation,and interfacial durability in ASSBs.
文摘Silicon （Si） has been considered as one of the most promising anode material for tHe next generation lithium-ion batteries （LIBs） with high energy densities, due to its high theoretical capacity, abundant availability and environmental friendliness. However. silicon materials with low intrinsic electric and ionic conductivity suffer from huge volume variation during lithiation/delithiation processes leading to the pulverization of Si and subsequently resulting in severe capacity fading of the electrodes. Coupling of Si with carbon （C） realizes a favorable combination of the two materials properties, such as high lithiation capacity of Si and excellent mechanical and conductive properties of C. making silicon/carbon composite （Si/C） ideal candidates for LIBs anodes. In this review, recent progresses of Si/C materials utilized in LIBs are summarized in terms of structural design principles, material synthesis methods, morphological characteristics and electrochemical performances by highlighting the material structures. The mechanisms behind the performance enhancement are also discussed. Moreover, other factors that affect the performance of Si/C anodes, such as prelithiation, electrolyte additives, and binders, are also discussed. We aim to present a full scope of the Si/C-based anodes, and help understand and design future structures of Si/C anodes in LIBs,
基金supported by the National Natural Science Foundation of China(5197219862133007)the Taishan Scholars Program of Shandong Province(tsqn201812002,ts20190908)+1 种基金the Shenzhen Fundamental Research Program(JCYJ20190807093405503)The Natural Science Foundation of Shandong Province(No.ZR2020JQ19)。
文摘Silicon(Si)has been studied as a promising alloying type anode for lithium-ion batteries due to its high specific capacity,low operating potential and abundant resources.Nevertheless,huge volume expansion during alloying/dealloying processes and low electronic conductivity of Si anodes restrict their electrochemical performance.Thus,carbon(C)materials with special physical and chemical properties are applied in Si anodes to effectively solve these problems.This review focuses on current status in the exploration of Si/C anodes,including the lithiation mechanism and solid electrolyte interface formation,various carbon sources in Si/C anodes,such as traditional carbon sources(graphite,pitch,biomass),and novel carbon sources(MXene,graphene,MOFs-derived carbon,graphdiyne,etc.),as well as interfacial bonding modes of Si and C in the Si/C anodes.Finally,we summarize and prospect the selection of carbonaceous materials,structural design and interface control of Si/C anodes,and application of Si/C anodes in all-solid-state lithium-ion batteries and sodium-ion batteries et al.This review will help researchers in the design of novel Si/C anodes for rechargeable batteries.
基金funded by the Research Fund of State Key Laboratory of Mesoscience and Engineering (MESO-23-T03)the National Natural Science Foundation (22278423)+1 种基金the National Key Research and Development Program of China (2022YFB3805602)the Science Foundation of China University of Petroleum,Beijing (2462021QNXZ007)。
文摘Silicon/carbon composites,which integrate the high lithium storage performance of silicon with the exceptional mechanical strength and conductivity of carbon,will replace the traditional graphite electrodes for high-energy lithium-ion batteries.Various strategies have been designed to synthesize silicon/carbon composites for tackling the issues of anode pulverization and poor stability in the anodes,thereby improving the lithium storage ability.The effect of the regulation method at each scale on the final negative electrode performance remains unclear.However,it has not been fully clarified how the regulation methods at each scale influence the final anode performance.This review will categorize the materials structure into three scales:molecular scale,nanoscale,and microscale.First,the review will examine modification methods at the molecular scale,focusing on the interfacial bonding force between silicon and carbon.Next,it will summarize various nanostructures and special shapes in the nanoscale to explore the construction of silicon/carbon composites.Lastly,the review will provide an analysis of microscale control approaches,focusing on the formation of composite particle with micron size and the utilization of micro-Si.This review provides a comprehensive overview of the multi-scale design of silicon/carbon composite anode materials and their optimization strategies to enhance the performance of lithium-ion batteries.
文摘Silicon (Si) is regarded as a promising material for lithium-ion battery anode because of high theoretical capacity. Nevertheless, Si faces particle pulverization and rapid capacity fading due to serious volume change during the lithiation and the delithiation process. In this work, a silicon/carbon composite constituted to Si powder and carbon nanofiber (CNF) is produced to solve the above issues as a new design structure of anode material. The Si powder was recycled from the silicon slicing waste in photovoltaic industry and the CNF was from dry rice straws. By mixing the purified Si powder with CNF, the composite was synthesized by the freeze-drying method and calcination. In the cyclic test, Si adding with 1 wt% CNF showed 3091 mAh/g capacity in the first cycle and 1079 mAh/g capacity after 100 cycles at the current density of 0.5 A/g, which were both better than pristine Si. SEM images also show the composite structure can eliminate cracks on the surface of the electrode during cycling. CNF attaching on Si particles can increase specific surface area, so binder can easily combine the active materials and the conductive materials together. This strategy enhances the structure stability and prevents the electrode from delamination.
文摘Silicon anodes are promising for use in lithium-ion batteries.However,their practical application is severely limited by their large volume expansion leading to irreversible material fracture and electrical disconnects.This study proposes a new top-down strategy for preparing microsize porous silicon and introduces polyacrylonitrile(PAN)for a nitrogen-doped carbon coating,which is designed to maintain the internal pore volume and lower the expansion of the anode during lithiation and delithiation.We then explore the effect of temperature on the evolution of the structure of PAN and the electrochemical behavior of the composite electrode.After treatment at 400℃,the PAN coating retains a high nitrogen content of 11.35 at%,confirming the presence of C—N and C—O bonds that improve the ionic-electronic transport properties.This treatment not only results in a more intact carbon layer structure,but also introduces carbon defects,and produces a material that has remarkable stable cycling even at high rates.When cycled at 4 A g^(-1),the anode had a specific capacity of 857.6 mAh g^(-1) even after 200 cycles,demonstrating great potential for high-capacity energy storage applications.
基金supported by the Jiangyin-SUSTech Innovation Fundthe National Natural Science Foundation of China (No. 22309078 and 52302261)+3 种基金the Shenzhen Key Laboratory of Advanced Energy Storage (ZDSYS20220401141000001)the Shenzhen Science and Technology Plan Project(No. SGDX20230116091644003)the Guangdong Basic and Applied Basic Research Foundation (2023B1515120069)the Pico Center at SUSTech Core Research Facilities,which is supported by the Presidential Fund and the Development and Reform Commission of Shenzhen Municipality
文摘There is an urgent need to develop high-areal-capacity silicon(Si)anodes with good cycling stability and rate capability for high-energy-density lithium-ion batteries(LIBs).However,this remains a huge challenge due to large volume expansion-induced mechanical degradation and electrical connectivity loss in thick electrodes.Here,a three-in-one strategy is proposed to achieve high-areal-capacity silicon anodes by constructing a multi-level interconnected 3D porous and robust conductive network that carbon nanofibers and vertical carbon nanosheets tightly encapsulate on the surface of Si nanoparticles(Si NPs)anchored in porous carbon felts.This network accommodates large volume expansion of Si NPs to significantly improve electrode mechanical stability and creates excellent electrical connectivity to boost charge transport in thick electrodes,revealed through Multiphysics field simulations and in situ electrochemical techniques.Therefore,the designed Si anodes achieve superior long-term stability with a capacity of 8.13 mAh cm^(-2)after 500 cycles and an ultrahigh areal capacity of 45.8 mAh cm^(-2).In particular,Ah-level pouch cells demonstrate an impressive capacity retention of 79.34%after 500 cycles at 1 C.Our study offers novel insights and directions for understanding and optimizing high-areal-capacity silicon-carbon composite anodes.
基金Supported by the National Natural Science Foundation of China(22378181).
文摘The development of materials with excellent microwave absorption(MWA)and electromagnetic interference(EMI)shielding performances has currently received attention.Herein,mesophase pitch-based carbon foam(MPCF)with 3D interconnected pore structure was prepared through the high pressure pyrolysis of mesophase coal tar pitch.It is found that the 3D interconnected cellular pores of MPCF facilitate multiple reflections of electromagnetic waves,which results in the minimum reflection loss(RLmin)value of MPCF reaches-37.84 dB with the effective absorption bandwidth(EAB)of 5.44 GHz at a thickness of 2.70 mm,and the total average electromagnetic shielding effectiveness(SE_(T))under 3.00 mm thickness achieves 26.52 dB in X-band.Subsequently,MPCF is activated by KOH to obtain activated carbon foam(A-MPCF).The average SE_(T)of A-MPCF achieves 103.00 dB for abundant nanopores on the pore cell walls,which leads to a transition from the multiple reflections of electromagnetic waves on the walls to diffuse reflection.Unfortunately,the reflection coefficient(R)of A-MPCF increases from 0.78 to 0.90.To reduce the R value,Fe_(3)O_(4)/A-MPCF was fabricated via the in situ growth of nano Fe_(3)O_(4)on A-MPCF.Consequently,the R value of Fe_(3)O_(4)/A-MPCF was reduced from 0.90 to 0.74,whereas the MWA performance was only slightly decreased.This work proposes a simple strategy for simultaneously adjusting MWA and EMI shielding performances of materials.
基金supported by the National Key R&D Program of China(No.2022YFC3701500)the Key R&D Plan Projects of Zhejiang Province(No.2024SSYS0072)Zhejiang Provincial Natural Science Foundation(No.LDT23E0601).
文摘Ship operations are crucial to global trade,and their decarbonization is essential to mitigate climate change.This study evaluates the economic viability of existing and emerging decarbonization technologies in maritime shipping using the levelized cost of energy methodology.It includes a detailed comparative analysis based on essential criteria and sensitivity assessments to highlight the economic impacts of technological advancements.Key factors influencing total costs include fuel costs,carbon pricing,and energy demands for carbon capture.The findings reveal that methanol is more cost-effective than heavy fuel oil(HFO)when priced below 3000 CNY/t,assuming HFO costs 4400 CNY/t.Additionally,methanol with post-combustion carbon capture is less expensive than pre-combustion carbon capture.When carbon prices rise above 480 CNY/t,carbon capture technologies prove more economical than purchasing carbon emission allowances for HFO and liquefied natural gas.Enhanc-ing the use of exhaust gas waste heat is recommended for cost savings.Post-combustion carbon capture also shows greater efficiency,requiring about 1.1 GJ/t less energy than pre-combustion methods,leading to lower overall costs.Future research should focus on market mechanisms to stabilize fuel prices and develop less energy-intensive carbon capture technologies.This study offers critical insights into effective decarbonization strategies for advancing global maritime trade in the present and future.
基金Supported by the Science and Technology Cooperation and Exchange special project of Cooperation of Shanxi Province(202404041101014)the Fundamental Research Program of Shanxi Province(202403021212333)+3 种基金the Joint Funds of the National Natural Science Foundation of China(U24A20555)the Lvliang Key R&D of University-Local Cooperation(2023XDHZ10)the Initiation Fund for Doctoral Research of Taiyuan University of Science and Technology(20242026)the Outstanding Doctor Funding Award of Shanxi Province(20242080).
文摘To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content in coal)catalysts were prepared by the incipient wetness impregnation method,followed by acid washing to remove calcium-containing minerals.Comprehensive characterization and low-temperature denitrification tests revealed that calcite-induced structural modulation of coal-derived AC significantly enhances catalytic activity.Specifically,NO conversion increased from 88.3%of Mn-Ce/De-AC to 91.7%of Mn-Ce/De-AC-1CaCO_(3)(210℃).The improved SCR denitrification activity results from the enhancement of physicochemical properties including higher Mn^(4+)content and Ce^(4+)/Ce^(3+)ratio,an abundance of chemisorbed oxygen and acidic sites,which could strengthen the SCR reaction pathways(richer NH_(3)activated species and bidentate nitrate active species).Therefore,NO removal is enhanced.
基金supported by the National Key R&D Program of China(No.2021YFB3501102).
文摘Porous carbon microspheres are widely regarded as a superior CO_(2) adsorbent due to their exceptional efficiency and affordability.However,better adsorption performance is very attractive for porous carbon microspheres.And modification of the pore structure is one of the effective strategies.In this study,multi-cavity mesoporous carbon microspheres were successfully synthesized by the synergistic method of soft and hard templates,during which a phenolic resin with superior thermal stability was employed as the carbon precursor and a mixture of silica sol and F108 as the mesoporous template.Carbon microspheres with multi-cavity mesoporous structures were prepared,and all the samples showed highly even mesopores,with diameters around 12 nm.The diameter of these microspheres decreased from 396.8 nm to about 182.5 nm with the increase of silica sol.After CO_(2) activation,these novel carbon microspheres(APCF0.5-S1.75)demonstrated high specific surface area(983.3 m^(2)/g)and remarkable CO_(2) uptake of 4.93 mmol/g at 0℃ and1 bar.This could be attributed to the unique multi-cavity structure,which offers uniform mesoporous pore channels,minimal CO_(2) transport of and a greater number of active sites for CO_(2) adsorption.
基金supported by the National Natural Science Foundation of China(No.52436008)the Inner Mongolia Science and Technology Projects,China(Nos.JMRHZX20210003 and 2023YFCY0009)+3 种基金the Huaneng Group Co Ltd.,China(No.HNKJ23-H50)the National Natural Science Foundation of China(No.22408044)the China Postdoctoral Science Foundation(No.2024M761877)the National Key R&D Program of China(No.SQ2024YFD2200039)。
文摘The electromagnetic wave absorption of silicon carbide nanowires is improved by their uniform and diverse cross-structures.This study introduces a sustainable and high value-added method for synthesizing silicon carbide nanowires using lignite and waste silicon powder as raw materials through carbothermal reduction.The staggered structure of nanowires promotes the creation of interfacial polarization,impedance matching,and multiple loss mechanisms,leading to enhanced electromagnetic absorption performance.The silicon carbide nanowires demonstrate outstanding electromagnetic absorption capabilities with the minimum reflection loss of-48.09 d B at10.08 GHz and an effective absorption bandwidth(the reflection loss less than-10 d B)ranging from 8.54 to 16.68 GHz with a thickness of 2.17 mm.This research presents an innovative approach for utilizing solid waste in an environmentally friendly manner to produce broadband silicon carbide composite absorbers.
基金financial support of the National Natural Science Foundation of China(No.52472271)the National Key Research and Development Program of China(No.2023YFE0115800)。
文摘Heteroatom-doped carbon is considered a promising alternative to commercial Pt/C as an efficient catalyst for the oxygen reduction reaction(ORR).This study presents the synthesis of iron-loaded,sulfur and nitrogen co-doped carbon(Fe/SNC)via in situ incorporation of 2-aminothiazole molecules into zeolitic imidazolate framework-8(ZIF-8)through coordination between metal ions and organic ligands.Sulfur and nitrogen doping in carbon supports effectively modulates the electronic structure of the catalyst,increases the Brunauer-Emmett-Teller surface area,and exposes more Fe-N_(x)active centers.Fe-loaded,S and N co-doped carbon with Fe/S molar ratio of 1:10(Fe/SNC-10)exhibits a half-wave potential of 0.902 V vs.RHE.After 5000 cycles of cyclic voltammetry,its half-wave potential decreases by only 20 mV vs.RHE,indicating excellent stability.Due to sulfur s lower electronegativity,the electronic structure of the Fe-N_(x)active center is modulated.Additionally,the larger atomic radius of sulfur introduces defects into the carbon support.As a result,Fe/SNC-10 demonstrates superior ORR activity and stability in alkaline solution compared with Fe-loaded N-doped carbon(Fe/NC).Furthermore,the zinc-air battery assembled with the Fe/SNC-10 catalyst shows enhanced performance relative to those assembled with Fe/NC and Pt/C catalysts.This work offers a novel design strategy for advanced energy storage and conversion applications.
基金supported by the National Key R&D Program of China(2022YFB3803700)National Natural Science Foundation of China(52171186)+1 种基金Young Elite Scientists Sponsorship Program by CAST(2023QNRC001)support from“Zhiyuan Honor Program”for doctoral students,Shanghai Jiao Tong University.
文摘Nanoconfinement is a promising approach to simultaneously enhance the thermodynamics,kinetics,and cycling stability of hydrogen storage materials.The introduction of supporting scaffolds usually causes a reduction in the total hydrogen storage capacity due to“dead weight.”Here,we synthesize an optimized N-doped porous carbon(rN-pC)without heavy metal as supporting scaffold to confine Mg/MgH_(2) nanoparticles(Mg/MgH_(2)@rN-pC).rN-pC with 60 wt%loading capacity of Mg(denoted as 60 Mg@rN-pC)can adsorb and desorb 0.62 wt%H_(2) on the rN-pC scaffold.The nanoconfined MgH_(2) can be chemically dehydrided at 175℃,providing~3.59 wt%H_(2) with fast kinetics(fully dehydrogenated at 300℃ within 15 min).This study presents the first realization of nanoconfined Mg-based system with adsorption-active scaffolds.Besides,the nanoconfined MgH_(2) formation enthalpy is reduced to~68 kJ mol^(−1) H_(2) from~75 kJ mol^(−1) H_(2) for pure MgH_(2).The composite can be also compressed to nanostructured pellets,with volumetric H_(2) density reaching 33.4 g L^(−1) after 500 MPa compression pressure,which surpasses the 24 g L^(−1) volumetric capacity of 350 bar compressed H_(2).Our approach can be implemented to the design of hybrid H_(2) storage materials with enhanced capacity and desorption rate.
基金Supported by State Grid Corporation of China Science and Technology Project:Research on Key Technologies for Intelligent Carbon Metrology in Vehicle-to-Grid Interaction(Project Number:B3018524000Q).
文摘To achieve low-carbon regulation of electric vehicle(EV)charging loads under the“dual carbon”goals,this paper proposes a coordinated scheduling strategy that integrates dynamic carbon factor prediction and multiobjective optimization.First,a dual-convolution enhanced improved Crossformer prediction model is constructed,which employs parallel 1×1 global and 3×3 local convolutionmodules(Integrated Convolution Block,ICB)formultiscale feature extraction,combinedwith anAdaptive Spectral Block(ASB)to enhance time-series fluctuationmodeling.Based on high-precision predictions,a carbon-electricity cost joint optimization model is further designed to balance economic,environmental,and grid-friendly objectives.The model’s superiority was validated through a case study using real-world data from a renewable-heavy grid.Simulation results show that the proposed multi-objective strategy demonstrated a superior balance compared to baseline and benchmark models,achieving a 15.8%reduction in carbon emissions and a 5.2%reduction in economic costs,while still providing a substantial 22.2%reduction in the peak-valley difference.Its balanced performance significantly outperformed both a single-objective strategy and a state-of-the-art Model Predictive Control(MPC)benchmark,highlighting the advantage of a global optimization approach.This study provides theoretical and technical pathways for dynamic carbon factor-driven EV charging optimization.
文摘Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-C_(3)N_(4) suffers from limited visible-light absorption and low charge-carrier mobility.In this study,a phosphorus-doped tubular carbon nitride(5P-TCN)was synthesized via a precursor self-assembly method using phosphoric acid and melamine as raw materials,eliminating the need for organic solvents or templates.The 5P-TCN catalyst demonstrated enhanced visible-light absorption,improved charge transfer capability,and a 5.25-fold increase in specific surface area(31.092 m^(2)/g),which provided abundant active sites to efficiently drive the PMS-assisted photocatalytic reaction.The 5P-TCN/vis/PMS system exhibited exceptional degradation performance for organic pollutants across a broad pH range(3–9),achieving over 92%degradation of Rhodamine B(RhB)within 15 min.Notably,the system retained>98%RhB degradation efficiency after three consecutive operational cycles,demonstrating robust operational stability and reusability.Moreover,key parameters influencing,active radi-cals,degradation pathways,and potential mechanisms for RhB degradation were systematically investigated.This work proposes a green and cost-effective strategy for developing high-efficiency photocatalysts,while demon-strating the exceptional capability of a PMS-assisted photocatalytic system for rapid degradation of RhB.
基金funded by the National Natural Science Foundation of China(Grant No.42275039)the Meteorological Joint Fund by NSF and CMA(Grant No.U2342224)+1 种基金the National Key R&D Program of China(Grant No.2022YFC3701202)the S&T Development Fund of CAMS(Grant No.2024KJ019)。
文摘Global land monsoon precipitation(GLMP)is highly sensitive to changes in interhemispheric thermal contrast(ITC).Amplified interhemispheric asymmetries of GLMP due to enhanced ITC driven by high-level anthropogenic emissions are expected to simultaneously increase the probability of regional floods and droughts,threatening ecosystems within global terrestrial monsoon regions and the freshwater supply for billions of residents in these areas.In this study,the responses of GLMP to the evolution of ITC toward the carbon neutrality goal are assessed using multimodel outputs from a new model intercomparison project(CovidMIP).The results show that the Northern Hemisphere-Southern Hemisphere(NH-SH)asymmetry of GLMP in boreal summer weakens during the 2040s,as a persistent reduction in well-mixed greenhouse gas(WMGHG)emissions leads to a downward trend in the ITC after 2040.At the same time,the reduction in WMGHG emissions dampens the Eastern Hemisphere-Western Hemisphere(EH-WH)asymmetry of GLMP by inducing La Niña-like cooling and enhancing moisture transport to Inner America.The resulting increases in land monsoon precipitation(LMP)may alleviate drought under the global warming scenario by about 19%-25%and 7%-9%in the WH and SH monsoon regions,respectively.However,a persistent reduction in aerosol emissions in Asia will dominate the increases in LMP in this region until the mid-21st century,and these increases may be approximately 23%-60%of the growth under the global warming scenario.Our results highlight the different rates of response of aerosol and WMGHG concentrations to the carbon neutrality goal,leading to various changes in LMP at global and regional scales.
基金supported by the National Natural Science Foundation of China(52276196)the Foundation of State Key Laboratory of Coal Combustion(FSKLCCA2508)the High-level Talent Foundation of Anhui Agricultural University(rc412307).
文摘Flash Joule heating(FJH),as a high-efficiency and low-energy consumption technology for advanced materials synthesis,has shown significant potential in the synthesis of graphene and other functional carbon materials.Based on the Joule effect,the solid carbon sources can be rapidly heated to ultra-high temperatures(>3000 K)through instantaneous high-energy current pulses during FJH,thus driving the rapid rearrangement and graphitization of carbon atoms.This technology demonstrates numerous advantages,such as solvent-and catalyst-free features,high energy conversion efficiency,and a short process cycle.In this review,we have systematically summarized the technology principle and equipment design for FJH,as well as its raw materials selection and pretreatment strategies.The research progress in the FJH synthesis of flash graphene,carbon nanotubes,graphene fibers,and anode hard carbon,as well as its by-products,is also presented.FJH can precisely optimize the microstructures of carbon materials(e.g.,interlayer spacing of turbostratic graphene,defect concentration,and heteroatom doping)by regulating its operation parameters like flash voltage and flash time,thereby enhancing their performances in various applications,such as composite reinforcement,metal-ion battery electrodes,supercapacitors,and electrocatalysts.However,this technology is still challenged by low process yield,macroscopic material uniformity,and green power supply system construction.More research efforts are also required to promote the transition of FJH from laboratory to industrial-scale applications,thus providing innovative solutions for advanced carbon materials manufacturing and waste management toward carbon neutrality.
基金financially supported by National Natural Science Foundation of China(22466010)Guizhou Provincial Basic Research Program(Natural Science)ZK[2023]47 and key program ZD[2025]075+6 种基金Innovation and Entrepreneurship Project for overseas Talents in Guizhou Province[2022]02Specific Natural Science Foundation of Guizhou University(X202207)the national undergraduate innovation and entrepreneurship training program(gzugc2023006gzusc2024012)SRT project of Guizhou university(2023SRT0292023SRT024)supported by Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University。
文摘Electrocatalytic nitrate reduction reaction(NO3RR)represents a sustainable and environmentally benign route for ammonia(NH3)synthesis.However,NO3RR is still limited by the competition from hydrogen evolution reaction(HER)and the high energy barrier in the hydrogenation step of nitrogen-containing intermediates.Here,we report a selective etching strategy to construct Ru M nanoalloys(M=Fe,Co,Ni,Cu)uniformly dispersed on porous nitrogen-doped carbon substrates for efficient neutral NH3electrosynthesis.Density functional theory calculations confirm that the synergic effect between Ru and transition metal M modulates the electronic structure of the alloy,significantly lowering the energy barrier for the conversion of*NO_(2)to*HNO_(2).Experimentally,the optimized Ru Fe-NC catalyst achieves 100%Faraday efficiency with a high yield rate of 0.83 mg h^(-1)mg^(-1)catat a low potential of-0.1 V vs.RHE,outperforming most reported catalysts.In situ spectroscopic analyses further demonstrate that the Ru M-NC effectively promotes the hydrogenation of nitrogen intermediates while inhibiting the formation of hydrogen radicals,thereby reducing HER competition.The Ru FeNC assembled Zn-NO_(3)^(-)battery achieved a high open-circuit voltage and an outstanding power density and capacity,which drive selective NO_(3)^(-)conversion to NH3.This work provides a powerful synergistic design strategy for efficient NH3electrosynthesis and a general framework for the development of advanced multi-component catalysts for sustainable nitrogen conversion.
