Lithium sulfur batteries have attracted much attention due to their high theoretical specific energy and environmental friendliness.However,the practical application is severely plagued by the cycling life issues resu...Lithium sulfur batteries have attracted much attention due to their high theoretical specific energy and environmental friendliness.However,the practical application is severely plagued by the cycling life issues resulting from the uncontrollable generation and growth of Li dendrites.Herein,an innovative 3D flexible self-supporting Li anode protection layer of P-Mn_(3)O_(4-x)is constructed via a facile solvothermal method followed by an annealing process.Benefiting from the rich oxygen vacancies coupled with the 3D flexible self-supporting skeleton,abundant lithiophilic sites and high ionic conductivity are obtained,which succeed in guiding Li+homogeneous adsorption and redistribution,accelerating Li+diffusion rate,inducing Li+uniform deposition and nucleation.DFT calculations and experimental results conclusively demonstrate such a protection mechanism.Meanwhile,the effective anchoring and catalytic nature of polar P-Mn_(3)O_(4-x)can also be applied as an immobilization-diffusion-conversion host to improve polysulfides redox.Taking advantage of these merits,super-stable functions for Li symmetric cell matched with P-Mn_(3)O_(4-x)layer are achieved,which exhibits an ultralong lifespan of>5000 h with an ultralow overpotential of 20 m V,far lower than that of bare Li symmetric cell(overpotential of 800 m V only after 250 h)at high current densities of 5 m A cm^(-2)and high plating/stripping capacity of 10 m A h cm^(-2).Even in Li|P-Mn_(3)O_(4-x)||S full cell at 1 C,a high initial discharge specific capacity of 843.1 m A h g^(-1)is still delivered with ultralow capacity fading rate of 0.07%per cycle after 250 cycles,further confirming the synergistic regulation of P-Mn_(3)O_(4-x)for Li nucleation behavior.This work illustrates a sufficient guarantee of 3D protection layer coupled with oxygen vacancies in guiding Li diffusion and nucleation behavior and provides new guidance for promoting the development of advanced Li-S batteries.展开更多
Two-stage underground coal gasification was studied to improve the caloric value of the syngas and to extend gas production times.A model test using the oxygen-enriched two-stage coal gasification method was carried o...Two-stage underground coal gasification was studied to improve the caloric value of the syngas and to extend gas production times.A model test using the oxygen-enriched two-stage coal gasification method was carried out.The composition of the gas produced,the time ratio of the two stages,and the role of the temperature field were analysed.The results show that oxygen-enriched two-stage gasification shortens the time of the first stage and prolongs the time of the second stage.Feed oxygen concentrations of 30%, 35%,40%,45%.60%,or 80%gave time ratios（first stage to second stage） of 1：0.12,1：0.21.1：0.51,1：0.64, 1：0.90.and 1：4.0 respectively.Cooling rates of the temperature field after steam injection decreased with time from about 19.1-27.4℃/min to 2.3-6.8℃/min.But this rate increased with increasing oxygen concentrations in the first stage.The caloric value of the syngas improves with increased oxygen concentration in the first stage.Injection of 80%oxygen-enriched air gave gas with the highest caloric value and also gave the longest production time.The caloric value of the gas obtained from the oxygenenriched two-stage gasification method lies in the range from 5.31 MJ/Nm^3 to 10.54 MJ/Nm^3.展开更多
Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capac...Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capacity fading.Herein,the dual-strategy of Cr,B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature.Density functional theory(DFT)calculations prove that stable B-O and Cr-O bonds through the local gradient doping can significantly reduce the high-energy O 2p states of interfacial lattice O,which is also effective for the near-surface lattice O,thus greatly stabilizing the LLO surface,Besides,differential electrochemical mass spectrometry(DEMS)indicates that the Cr_(x)B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions,including allowing speedy Li^(+)migration,The voltage and capacity fading of the modified cathode(LLO-C_(r)B)are adequately suppressed,which are benefited from the uniformly dense cathode electrolyte interface(CEI)composed of balanced organic/inorganic composition.Therefore,the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g^(-1)(with a retention rate of 95.1%).This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.展开更多
Many people who live in the low altitude areas are often suffered from hypoxia when they entered the high plateau. This problem may seriously influence the physical and mental state and work efficacy for the travelers...Many people who live in the low altitude areas are often suffered from hypoxia when they entered the high plateau. This problem may seriously influence the physical and mental state and work efficacy for the travelers and workers. Oxygen enrichment of a small space air at high altitude is considered as a simple way to provide lowlanders enriched oxygen for sleeping and resting, improving work efficiency, so we developed an oxygen concentration machine based on the technology of oxygen enrichment membrane. This paper tested 8 healthy male lowlanders (age 21.63±1.77 yr) who have never exposed to plateau performed an incremental exercise on cycle ergometer at sea-level in order to be used as sea-level controls. Two days later, the same subjects were taken to Lhasa (3700 m) by air and exposed to the plateau, performed the same exercise as they did at sea-level. The next day, all subjects were asked to enter the experimental tent which was enriched with oxygen (higher than 24%) by the oxygen concentration machine and sleep for 10 hours at night, then exposed to plateau and performed the same exercise twice at different time (2 hours and 10 hours after oxygen enrichment). During the tests, subjects must cycled continuously at 60 rpm beginning with a 3 min exercise intensity of 0 W followed by incremental increases of 25 W every 3 min until 150 W, pulse oxygen saturation (SpO2) and heart rate (HR) were recorded. After sleeping in an oxygen enrichment of tent air, 2 hours later, the subjects’ load capacity had no difference compared with control group, but significant difference than before (higher SpO2 and lower HR), which indicated that oxygen concentration machine is effective in increasing the oxygen concentration of the air for the tent and sleeping in the oxygen enrichment tent for l0 h might be effective in improving exercise performance during high-altitude hypoxia. At the same time, 10 hours later, when work-load exceeded 125 W, the same effects were also found. The results indicated the effects of oxygen enrichment of tent air could last a certain period of time.展开更多
Facilitating anion redox chemistry is an effective strategy to increase the capacity of layered oxides for sodium-ion batteries.Nevertheless,there remains a paucity of literature pertaining to the oxygen redox chemist...Facilitating anion redox chemistry is an effective strategy to increase the capacity of layered oxides for sodium-ion batteries.Nevertheless,there remains a paucity of literature pertaining to the oxygen redox chemistry of O3-type layered oxide cathode materials.This work systematically investigates the effect of Fe doping on the anionic oxygen redox chemistry and electrochemical reactions in O3-NaNi_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1)O_(2).The results of the density functional theory(DFT)calculations indicate that the electrons of the O 2p occupy a higher energy level.In the ex-situ X-ray photoelectron spectrometer(XPS)of O 1s,the addition of Fe facilitates the lattice oxygen(O^(n-))to exhibit enhanced activity at 4.45 V.The in-situ X-ray diffraction(XRD)demonstrates that the doping of Fe effectively suppresses the Y phase transition at high voltages.Furthermore,the Galvanostatic Intermittent Titration Technique(GITT)data indicate that Fe doping significantly increases the Na~+migration rate at high voltages.Consequently,the substitution of Fe can elevate the cut-off voltage to 4.45 V,thereby facilitating electron migration from O^(2-).The redox of O^(2-)/O^(n-)(n<2)contributes to the overall capacity.O3-Na(Ni_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1))_(0.92)Fe_(0.08)O_(2)provides an initial discharge specific capacity of 180.55 mA h g^(-1)and71.6%capacity retention at 0.5 C(1 C=240 mA g^(-1)).This work not only demonstrates the beneficial impact of Fe substitution for promoting the redox activity and reversibility of O^(2-)in 03-type layered oxides,but also guarantees the structural integrity of the cathode materials at high voltages(>4.2 V).It offers a novel avenue for investigating the anionic redox reaction in O3-type layered oxides to design advanced cathode materials.展开更多
The effects of gas composition, temperature, ore to coke ratio and prereduction rate of ore on coke degradation were studied. The results showed that 1% increment in solution loss of coke reduces coke strength by 0.6%...The effects of gas composition, temperature, ore to coke ratio and prereduction rate of ore on coke degradation were studied. The results showed that 1% increment in solution loss of coke reduces coke strength by 0.6%, and the coke degradation is accelerated with the temperature. The higher the temperature, the more coke surface is involved in reactions, and the less negative effect on coke strength is. Hydrogen exerts stronger effect on coke degradation than CO at high temperature. The coke degradation is decreased with the reduction of ore to coke ratio and increase of ore prereduction rate.展开更多
A novel Pressurized Enriched Oxygen Biological Activated Carbon （PRBAC） method in treating secondary effluent of textile dying-printing ＆ alkali peeling wastewater was configured. The PRBAC reactor simply increased...A novel Pressurized Enriched Oxygen Biological Activated Carbon （PRBAC） method in treating secondary effluent of textile dying-printing ＆ alkali peeling wastewater was configured. The PRBAC reactor simply increased reactor pressure to create an eurtched dissolved oxygen （DO） environment to stimulate the bioactivities of microbes on GAC surface for removing refractory organic matter. Rapid Small- Scaled Colunm Test （RSSCT） was carried out to evaluate the adsorption characteristics of target stream constituents, and over 80% COD components were poorly adsorbable while about 82.5% color inducing matter and 85% UV254 surrogated matter were readily adsorbable. Compared with performances of normal BAC reactor under conventional DO condition, PRBAC achieved 20%, 10% and 50% more removal in COD, color and NH3-N abatement.展开更多
Normal diffusion flame(NDF)of acid gas with a H_(2)S concentration below 50.0%(vol)generally exhibits a low flame temperature in a low-level oxygen enrichment atmosphere under Claus conditions,resulting in flame insta...Normal diffusion flame(NDF)of acid gas with a H_(2)S concentration below 50.0%(vol)generally exhibits a low flame temperature in a low-level oxygen enrichment atmosphere under Claus conditions,resulting in flame instability.This research proposed that inverse diffusion flame(IDF)was applied to acid gas combustion for enhancing flame temperature.IDF of acid gas was compared with fuel gas cocombustion(FGC),split flow of acid gas(SFAG)and high-level oxygen enrichment combustion(OEC).Additionally,the effect of CO_(2)addition on the IDF of H_(2)S was investigated.The results indicated that a stable flame could be observed in the IDF of acid gas,its peak flame temperature was about 801.0 K,which was higher than that in the OEC,FGC and SFAG with a value of about 591.0,684.0 and 734.0 K,respectively.IDF of acid gas was contributed to the formation of sulfur and H_(2),and mainly involved the oxidation zone and the chemical decomposition and oxidation zone in sequence.In the IDF,CO_(2)exhibited a better oxidation performance,and the peak flame temperature was decreased by about 21.0 K with an increase in CO_(2)addition from 50.8%to 59.5%(vol),whereas significantly enhanced the oxidation reaction rate of H_(2)S,and the peak volume fraction of SO_(2)was increased from 5.812%to 7.075%.The application of IDF to acid gas combustion achieved the objective for improving flame temperature in low-level oxygen enrichment atmosphere under Claus conditions,providing a new perspective in the sulfur recovery and hydrogen production from acid gas.展开更多
Four different pulverized coals have been used to study the effects of oxygen concentration on combustion characteristics under different enriched-oxygen conditions by entrained flow reactor experiments. The results s...Four different pulverized coals have been used to study the effects of oxygen concentration on combustion characteristics under different enriched-oxygen conditions by entrained flow reactor experiments. The results show that: with the increase of oxygen concentration, the ignition temperature of four coals greatly decreases and the low volatile coals decrease faster; with the increase of oxygen concentration, the ignition mode of pulverized coal has an obviously transformation from homogeneous ignition to heterogeneous ignition, and the corresponding oxygen concentrations are about 40% and 50%-60% respectively for bituminous coal and lignite, and both about 30% for lean coal and anthracite; with the increase of oxygen concentration, the optimal pulverized coal concentrations of bituminous coal and lignite increase firstly and then decrease, but for lean coal and anthracite, the optimal pulverized coal concentrations decrease slowly with the increase of oxygen concentration.展开更多
Infrared-transparent conductors have attracted considerable attention due to their potential applications in electromagnetic shielding,infrared sensors,and photovoltaic devices.However,most known materials face the cr...Infrared-transparent conductors have attracted considerable attention due to their potential applications in electromagnetic shielding,infrared sensors,and photovoltaic devices.However,most known materials face the critical challenge of balancing high infrared transmittance with high electrical conductivity across the broad infrared spectral band(2.5-25μm).While ultra-thin indium tin oxide(ITO)films have been demonstrated to exhibit superior infrared transmittance,their inherent low electrical conductivity necessitates additional enhancement strategies.This study systematically investigates the effects of oxygen vacancy concentration regulation and ultra-thin copper capping layer integration on the infrared optoelectronic properties of 20 nm-thick ITO films.A fundamental trade-off is revealed in ITO films that increased oxygen vacancy content enhances the electrical conductivity while compromising the infrared transmittance.Meanwhile,following the introduction of a Cu capping layer,the Cu/ITO system exhibits opposing dependencies of infrared transmittance and electrical conductivity on the capping layer thickness,with an optimum thickness of~3 nm.Finally,by constructing a Cu(3 nm)/ITO(20 nm)heterostructure with varying oxygen vacancy content,we demonstrate the combined effect of the ultra-thin Cu capping layer and moderate oxygen vacancy content on optimizing the carrier transport network.This configuration simultaneously minimizes surface/interfacial reflection and absorption losses,achieving high infrared transmittance(0.861)and a low sheet resistance of 400 W/sq.Our findings highlight the critical role of the combined effect of metal/oxide heterostructure design and defect engineering in optimizing infrared-transparent conductive properties.展开更多
Layered double hydroxides(LDHs)are potential cathode materials for aqueous magnesium-ion batteries(AMIBs).However,the low capacity and sluggish kinetics significantly limit their electrochemical performance in AMIBs.H...Layered double hydroxides(LDHs)are potential cathode materials for aqueous magnesium-ion batteries(AMIBs).However,the low capacity and sluggish kinetics significantly limit their electrochemical performance in AMIBs.Herein,we find that oxygen vacancies can significantly boost the capacity,electrochemical kinetics,and structure stability of LDHs.The corresponding structure-performance relationship and energy storage mechanism are elaborated through exhaustive in/ex-situ experimental characterizations and density functional theory(DFT)calculations.Specially,in-situ Raman and DFT calculations reveal that oxygen vacancies elevate orbital energy of O 2p and electron density of O atoms,thereby enhancing the orbital hybridization of O 2p with Ni/Co 3d.This facilitates electron transfer between O and adjacent Ni/Co atoms and improves the covalency of Ni–O and Co–O bonds,which activates Ni/Co atoms to release more capacity and stabilizes the Ov-NiCo-LDH structure.Moreover,the distribution of relaxation times(DRT)and molecular dynamics(MD)simulations disclose that the enhanced d-p orbital hybridization optimizes the electronic structure of Ov-NiCo-LDH,which distinctly reduces the diffusion energy barriers of Mg^(2+)and improves the charge transfer kinetics of Ov-NiCo-LDH.Consequently,the assembled Ov-NiCo-LDH//active carbon(AC)and Ov-NiCo-LDH//perylenediimide(PTCDI)AMIBs can both deliver high specific discharge capacity(182.7 and 59.4 mAh g^(−1)at 0.5 A g^(−1),respectively)and long-term cycling stability(85.4%and 89.0%of capacity retentions after 2500 and 2400 cycles at 1.0 A g^(−1),respectively).In addition,the practical prospects for Ov-NiCo-LDH-based AMIBs have been demonstrated in different application scenarios.This work not only provides an effective strategy for obtaining high-performance cathodes of AMIBs,but also fundamentally elucidates the inherent mechanisms.展开更多
Lithium-rich manganese-based oxide(LRMO)cathode has emerged as a particularly promising candidate for achieving high energy densities in lithium-ion batteries due to its capability to access anion redox reactions at h...Lithium-rich manganese-based oxide(LRMO)cathode has emerged as a particularly promising candidate for achieving high energy densities in lithium-ion batteries due to its capability to access anion redox reactions at high voltage.The successful implementation of LRMO in energy storage systems is contingent upon the enhancement of their rate capabilities.However,the underlying relationship between high-rate cycling and electrode degradation for LRMO,particularly concerning structural evolution,still remains unclear.Benefiting from the high time resolution abilities of liquid-metal-jet operando twodimensional X-ray diffraction,it is observed that the Li_(2)MnO_(3)phase in LRMO is gradually activated accompanied by the emergence of oxygen vacancies during cycling at 1 C(1 C=250 mA/g).Consequently,the crystal lattice flexibility of LRMO is systematically enhanced,thereby preventing the collapse of the bulk structure.While,continuous release of oxygen during extended cycling results in deteriorations of the self-adjusting damping effect of the structure,ultimately leading to a decline in capacity.The findings of this study not only contribute to a more profound understanding of the structural changes of LRMOs at high rates,but also provide novel perspectives for the rational design of LRMOs with superior rate performances.展开更多
Based on a six-cylinder direct injection diesel engine, the engine operating condition was simulated by application AVL-FIRE software coupling the n-heptane reduced mechanism containing polycyclic aromatic hydrocarbon...Based on a six-cylinder direct injection diesel engine, the engine operating condition was simulated by application AVL-FIRE software coupling the n-heptane reduced mechanism containing polycyclic aromatic hydrocarbon (PAH) formation. The simulation and its verification test were both carried out under the maximum torque point. Then, the oxygen enriched combustion was simulated on the model, and the simulated condition was oxygen volume fraction from 21% to 30%. The simulation results show that, the oxygen enrichment (from 21% to 30%) increases the peak cylinder pressure of 3.32%, advances the start of combustion of 1.6 deg and rises the peak of average temperature in cylinder and wall heat flux. Among them, at the condition of 24% O2, the change of the results is the most significant. Benzene (A1) is one of the precursors of soot generated, the analysis of its impress-cuts of the mass distribution field in cylinder shows that, the increase of oxygen concentration can significantly inhibit the formation of benzene. But the oxygen enrichment makes the combustion more sufficient, cased a rise in the cylinder temperature, an extension in high temperature area, and an increment in the NOx emission.展开更多
Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthes...Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthesized the electrode material Ce-NiCo-LDHs@SnO_(2)/NF through a two-step hydrothermal reaction,where Ce-doped NiCo-LDHs are grown on nickel foam modified by a SnO_(2) layer.Ce doping adjusts the internal electronic distribution of Ni Co-LDHs,while the introduction of the SnO_(2) layer enhances electron transfer capability.Together,these factors contribute to the reduction of the OER energy barrier and experimental evidence confirms that the reaction proceeds via the lattice oxygen evolution mechanism(LOM).Consequently,Ce-NiCo-LDHs@SnO_(2)/NF exhibits high level electrochemical performance in OER,requiring only 234 m V overpotential to achieve a current density of 10 m A/cm^(2),with a Tafel slope of just 27.39 m V/dec.When paired with Pt/C/NF,an external potential of only 1.54 V is needed to drive OWS to attain a current density amounting to 10 m A/cm^(2).Furthermore,the catalyst demonstrates stability for 100 h during the OWS stability test.This study underscores the feasibility of enhancing the OER performance through Ce doping and the introduction of a conductive SnO_(2) layer.展开更多
Layered double hydroxides(LDHs)are promising electrocatalysts for the oxygen evolution reaction(OER),yet their practical application remains limited by poor electrical conductivity and sluggish reaction kinetics.In th...Layered double hydroxides(LDHs)are promising electrocatalysts for the oxygen evolution reaction(OER),yet their practical application remains limited by poor electrical conductivity and sluggish reaction kinetics.In this work,we synthesize three high-entropy LDHs(HELDHs)featuring a hierarchical architecture of microspheres assembled from ultrathin nanosheets,via a simple hydrothermal method using a combination of low-cost,catalytically active transition metals(Fe,Co,Ni,Mn,Zn,Cu,and Cr).Among them,the FeCoNiMnZn HELDH exhibits outstanding OER performance,requiring an overpotential of only 306 mV to reach a current density of 100 mA cm^(-2).Notably,during 200 h of continuous operation,the device exhibits a stable and,in some cases,increasing current output.This exceptional activity is attributed to the formation of abundant cation vacancies,induced by Zn leaching,which enhance the intrinsic catalytic properties by optimizing the adsorption energies of key OER intermediates.Density functional theory calculations further validate that these vacancies modulate the electronic structure and lower reaction barriers,underscoring the effectiveness of cation-vacancy engineering in high-entropy systems for efficient and durable water oxidation catalysis.The optimized catalyst was further evaluated as the air cathode in a zinc-air battery,demonstrating practical electrochemical performance.展开更多
With exhaustion of fossil fuels and the deterioration of global environment,widespread and intensive researches have been concentrated on clean and sustainable alternative energy sources,such as metal-air batteries[1]...With exhaustion of fossil fuels and the deterioration of global environment,widespread and intensive researches have been concentrated on clean and sustainable alternative energy sources,such as metal-air batteries[1],fuel cells[2]and water splitting devices[3].Electrocatalytic oxidation of water to O2(oxygen evolution reaction,OER)is a vital chemical process involved in energy storage and conversion from renewable sources in form of molecular fuels such as H2 via water electrolysis,which has attracted a great amount of research efforts in the past few years[4,5].Nowadays,RuO2 and IrO2 are widely used as typical excellent OER electrocatalysts.However,their high-cost and scarce nature restricts the broadly commercial application of those materials[6,7].Hence,there is an urgent demand to develop low cost,highly efficient,and superb stable OER catalysts.展开更多
Layered double hydroxides(LDHs)have attracted tremendous research interest in widely spreading applications.Most notably,transition-metal-bearing LDHs are expected to serve as highly active electrocatalysts for oxygen...Layered double hydroxides(LDHs)have attracted tremendous research interest in widely spreading applications.Most notably,transition-metal-bearing LDHs are expected to serve as highly active electrocatalysts for oxygen evolution reaction(OER)due to their layered structure combined with versatile com-positions.Furthermore,reducing the thickness of platelet LDH crystals to nanometer or even molecular scale via cleavage or delamination provides an important clue to enhance the activity.In this review,recent progresses on rational design of LDH nanosheets are reviewed,including direct synthesis via traditional coprecipitation,homogeneous precipitation,and newly developed topochemical oxidation as well as chemical exfoliation of parent LDH crystals.In addition,diverse strategies are introduced to modulate their electrochemical activity by tuning the composition of host metal cations and intercalated counter-anions,and incorporating dopants,cavi-ties,and single atoms.In particular,hybridizing LDHs with conductive components or in situ growing them on conductive substrates to produce freestanding electrodes can further enhance their intrinsic catalytic activity.A brief discussion on future research directions and prospects is also summarized.展开更多
The Tazhong paleouplift is divided into the upper and the lower structural layers, bounded by the unconformity surface at the top of the Ordovician carbonate rock. The reservoirs in the two layers from different parts...The Tazhong paleouplift is divided into the upper and the lower structural layers, bounded by the unconformity surface at the top of the Ordovician carbonate rock. The reservoirs in the two layers from different parts vary in number, type and reserves, but the mechanism was rarely researched before. Therefore, an explanation of the mechanism will promote petroleum exploration in Tazhong paleouplift. After studying the evolution and reservoir distribution of the Tazhong paleouplift, it is concluded that the evolution in late Caledonian, late Hercynian and Himalayan periods resulted in the upper and the lower structural layers. It is also defined that in the upper structural layer, structural and stratigraphic overlap reservoirs are developed at the top and the upper part of the paleouplift, which are dominated by oil reservoirs, while for the lower structural layer, lithological reservoirs are developed in the lower part of the paleouplift, which are dominated by gas reservoirs, and more reserves are discovered in the lower structural layer than the upper. Through a comparative analysis of accumulation conditions of the upper and the lower structural layers, the mechanism of enrichment differences is clearly explained. The reservoir and seal conditions of the lower structural layer are better than those of the upper layer, which is the reason why more reservoirs have been found in the former. The differences in the carrier system types, trap types and charging periods between the upper and the lower structural layers lead to differences in the reservoir types and distribution. An accumulation model is established for the Tazhong paleouplift. For the upper structural layer, the structural reservoirs and the stratigraphic overlap reservoirs are formed at the upper part of the paleouplift, while for the lower structural layer, the weathering crust reservoirs are formed at the top, the reef-flat reservoirs are formed on the lateral margin, the karst and inside reservoirs are formed in the lower part of the paleouplift.展开更多
Compared with noble metal catalyst, Co3O4-based electrocatalysts have attracted considerable interesting as low-cost alternatives for oxygen evolution reaction (OER). However, the poor electrocatalytic activity still ...Compared with noble metal catalyst, Co3O4-based electrocatalysts have attracted considerable interesting as low-cost alternatives for oxygen evolution reaction (OER). However, the poor electrocatalytic activity still remains a huge challenge. Herein, we demonstrate a feasible approach through oxidation of CoFe layered double hydroxide (CoFe-LDH) to synthesize Fe-doped Co3O4@C nanopmrticles with size of about 30-50 nm. As OER catalyst, the as-synthesized Fe-doped Co3O4@C nanoparticles exhibited superior OER performance with a small overpotential of 260 mV at the current density of 20 mA cm^-2, a small Tafel slope of 70 mV dec^-1 and long-term durability (there was no obviously OER current density degradation for 100 h) in alkaline solution. The present work opens a new avenue to the exploration of cost-effective and excellent electrocatalysts based on transition metal oxide materials to substitute precious metal materials for water splitting.展开更多
Understanding carbon-supported Pt-catalyzed oxygen reduction reaction(ORR)from the perspective of the active sites is of fundamental and practical importance.In this study,three differently sized carbon nanotube-suppo...Understanding carbon-supported Pt-catalyzed oxygen reduction reaction(ORR)from the perspective of the active sites is of fundamental and practical importance.In this study,three differently sized carbon nanotube-supported Pt nanoparticles(Pt/CNT)are prepared by both atomic layer deposition(ALD)and impregnation methods.The performances of the catalysts toward the ORR in acidic media are comparatively studied to probe the effects of the sizes of the Pt nanoparticles together with their distributions,electronic properties,and local environments.The ALD-Pt/CNT catalysts show much higher ORR activity and selectivity than the impregnation-Pt/CNT catalysts.This outstanding ORR performance is ascribed to the well-controlled Pt particle sizes and distributions,desirable Pt^04f binding energy,and the Cl-free Pt surfaces based on the electrocatalytic measurements,catalyst characterizations,and model calculations.The insights reported here could guide the rational design and fine-tuning of carbon-supported Pt catalysts for the ORR.展开更多
基金supported by the Natural Science Foundation of Shandong Province(ZR2021MB101,ZR2021ME113,ZR2021ME177,and ZR2021QE096)。
文摘Lithium sulfur batteries have attracted much attention due to their high theoretical specific energy and environmental friendliness.However,the practical application is severely plagued by the cycling life issues resulting from the uncontrollable generation and growth of Li dendrites.Herein,an innovative 3D flexible self-supporting Li anode protection layer of P-Mn_(3)O_(4-x)is constructed via a facile solvothermal method followed by an annealing process.Benefiting from the rich oxygen vacancies coupled with the 3D flexible self-supporting skeleton,abundant lithiophilic sites and high ionic conductivity are obtained,which succeed in guiding Li+homogeneous adsorption and redistribution,accelerating Li+diffusion rate,inducing Li+uniform deposition and nucleation.DFT calculations and experimental results conclusively demonstrate such a protection mechanism.Meanwhile,the effective anchoring and catalytic nature of polar P-Mn_(3)O_(4-x)can also be applied as an immobilization-diffusion-conversion host to improve polysulfides redox.Taking advantage of these merits,super-stable functions for Li symmetric cell matched with P-Mn_(3)O_(4-x)layer are achieved,which exhibits an ultralong lifespan of>5000 h with an ultralow overpotential of 20 m V,far lower than that of bare Li symmetric cell(overpotential of 800 m V only after 250 h)at high current densities of 5 m A cm^(-2)and high plating/stripping capacity of 10 m A h cm^(-2).Even in Li|P-Mn_(3)O_(4-x)||S full cell at 1 C,a high initial discharge specific capacity of 843.1 m A h g^(-1)is still delivered with ultralow capacity fading rate of 0.07%per cycle after 250 cycles,further confirming the synergistic regulation of P-Mn_(3)O_(4-x)for Li nucleation behavior.This work illustrates a sufficient guarantee of 3D protection layer coupled with oxygen vacancies in guiding Li diffusion and nucleation behavior and provides new guidance for promoting the development of advanced Li-S batteries.
基金financial support of the National Natural Science Foundation of China(No.50876112)the Fundamental Research Funds for the Central Universities (No.2009QH13)the Program of International S&T Cooperation (No.2009DFR60180,No.2010DFR60610)
文摘Two-stage underground coal gasification was studied to improve the caloric value of the syngas and to extend gas production times.A model test using the oxygen-enriched two-stage coal gasification method was carried out.The composition of the gas produced,the time ratio of the two stages,and the role of the temperature field were analysed.The results show that oxygen-enriched two-stage gasification shortens the time of the first stage and prolongs the time of the second stage.Feed oxygen concentrations of 30%, 35%,40%,45%.60%,or 80%gave time ratios（first stage to second stage） of 1：0.12,1：0.21.1：0.51,1：0.64, 1：0.90.and 1：4.0 respectively.Cooling rates of the temperature field after steam injection decreased with time from about 19.1-27.4℃/min to 2.3-6.8℃/min.But this rate increased with increasing oxygen concentrations in the first stage.The caloric value of the syngas improves with increased oxygen concentration in the first stage.Injection of 80%oxygen-enriched air gave gas with the highest caloric value and also gave the longest production time.The caloric value of the gas obtained from the oxygenenriched two-stage gasification method lies in the range from 5.31 MJ/Nm^3 to 10.54 MJ/Nm^3.
基金financially supported by the National Natural Science Foundation of China(No.12304077)the Natural Science Foundation of Science and Technology Department of Sichuan Province(No.23NSFSC6224)+3 种基金Sichuan Science and Technology Program(No.2024NSFSC0989)the Key Laboratory of Computational Physics of Sichuan Province(No.YBUJSWL-YB-2022-03)the Material Corrosion and Protection Key Laboratory of Sichuan Province(No.2023CL14 and No.2023CL01)the National Innovation Practice Project(No.202411079005S).
文摘Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capacity fading.Herein,the dual-strategy of Cr,B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature.Density functional theory(DFT)calculations prove that stable B-O and Cr-O bonds through the local gradient doping can significantly reduce the high-energy O 2p states of interfacial lattice O,which is also effective for the near-surface lattice O,thus greatly stabilizing the LLO surface,Besides,differential electrochemical mass spectrometry(DEMS)indicates that the Cr_(x)B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions,including allowing speedy Li^(+)migration,The voltage and capacity fading of the modified cathode(LLO-C_(r)B)are adequately suppressed,which are benefited from the uniformly dense cathode electrolyte interface(CEI)composed of balanced organic/inorganic composition.Therefore,the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g^(-1)(with a retention rate of 95.1%).This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.
文摘Many people who live in the low altitude areas are often suffered from hypoxia when they entered the high plateau. This problem may seriously influence the physical and mental state and work efficacy for the travelers and workers. Oxygen enrichment of a small space air at high altitude is considered as a simple way to provide lowlanders enriched oxygen for sleeping and resting, improving work efficiency, so we developed an oxygen concentration machine based on the technology of oxygen enrichment membrane. This paper tested 8 healthy male lowlanders (age 21.63±1.77 yr) who have never exposed to plateau performed an incremental exercise on cycle ergometer at sea-level in order to be used as sea-level controls. Two days later, the same subjects were taken to Lhasa (3700 m) by air and exposed to the plateau, performed the same exercise as they did at sea-level. The next day, all subjects were asked to enter the experimental tent which was enriched with oxygen (higher than 24%) by the oxygen concentration machine and sleep for 10 hours at night, then exposed to plateau and performed the same exercise twice at different time (2 hours and 10 hours after oxygen enrichment). During the tests, subjects must cycled continuously at 60 rpm beginning with a 3 min exercise intensity of 0 W followed by incremental increases of 25 W every 3 min until 150 W, pulse oxygen saturation (SpO2) and heart rate (HR) were recorded. After sleeping in an oxygen enrichment of tent air, 2 hours later, the subjects’ load capacity had no difference compared with control group, but significant difference than before (higher SpO2 and lower HR), which indicated that oxygen concentration machine is effective in increasing the oxygen concentration of the air for the tent and sleeping in the oxygen enrichment tent for l0 h might be effective in improving exercise performance during high-altitude hypoxia. At the same time, 10 hours later, when work-load exceeded 125 W, the same effects were also found. The results indicated the effects of oxygen enrichment of tent air could last a certain period of time.
基金financial support from the Natural Science Foundation of Shandong Province of China(ZR2023ME051,ZR2019MEM020)。
文摘Facilitating anion redox chemistry is an effective strategy to increase the capacity of layered oxides for sodium-ion batteries.Nevertheless,there remains a paucity of literature pertaining to the oxygen redox chemistry of O3-type layered oxide cathode materials.This work systematically investigates the effect of Fe doping on the anionic oxygen redox chemistry and electrochemical reactions in O3-NaNi_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1)O_(2).The results of the density functional theory(DFT)calculations indicate that the electrons of the O 2p occupy a higher energy level.In the ex-situ X-ray photoelectron spectrometer(XPS)of O 1s,the addition of Fe facilitates the lattice oxygen(O^(n-))to exhibit enhanced activity at 4.45 V.The in-situ X-ray diffraction(XRD)demonstrates that the doping of Fe effectively suppresses the Y phase transition at high voltages.Furthermore,the Galvanostatic Intermittent Titration Technique(GITT)data indicate that Fe doping significantly increases the Na~+migration rate at high voltages.Consequently,the substitution of Fe can elevate the cut-off voltage to 4.45 V,thereby facilitating electron migration from O^(2-).The redox of O^(2-)/O^(n-)(n<2)contributes to the overall capacity.O3-Na(Ni_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1))_(0.92)Fe_(0.08)O_(2)provides an initial discharge specific capacity of 180.55 mA h g^(-1)and71.6%capacity retention at 0.5 C(1 C=240 mA g^(-1)).This work not only demonstrates the beneficial impact of Fe substitution for promoting the redox activity and reversibility of O^(2-)in 03-type layered oxides,but also guarantees the structural integrity of the cathode materials at high voltages(>4.2 V).It offers a novel avenue for investigating the anionic redox reaction in O3-type layered oxides to design advanced cathode materials.
文摘The effects of gas composition, temperature, ore to coke ratio and prereduction rate of ore on coke degradation were studied. The results showed that 1% increment in solution loss of coke reduces coke strength by 0.6%, and the coke degradation is accelerated with the temperature. The higher the temperature, the more coke surface is involved in reactions, and the less negative effect on coke strength is. Hydrogen exerts stronger effect on coke degradation than CO at high temperature. The coke degradation is decreased with the reduction of ore to coke ratio and increase of ore prereduction rate.
文摘A novel Pressurized Enriched Oxygen Biological Activated Carbon （PRBAC） method in treating secondary effluent of textile dying-printing ＆ alkali peeling wastewater was configured. The PRBAC reactor simply increased reactor pressure to create an eurtched dissolved oxygen （DO） environment to stimulate the bioactivities of microbes on GAC surface for removing refractory organic matter. Rapid Small- Scaled Colunm Test （RSSCT） was carried out to evaluate the adsorption characteristics of target stream constituents, and over 80% COD components were poorly adsorbable while about 82.5% color inducing matter and 85% UV254 surrogated matter were readily adsorbable. Compared with performances of normal BAC reactor under conventional DO condition, PRBAC achieved 20%, 10% and 50% more removal in COD, color and NH3-N abatement.
基金supported by the National Natural Science Foundation of China(22178114,U23A20131)the social development science and technology tackling project of 2021"Scientific and Innovative Action Plan of Shanghai"(21DZ1209000)。
文摘Normal diffusion flame(NDF)of acid gas with a H_(2)S concentration below 50.0%(vol)generally exhibits a low flame temperature in a low-level oxygen enrichment atmosphere under Claus conditions,resulting in flame instability.This research proposed that inverse diffusion flame(IDF)was applied to acid gas combustion for enhancing flame temperature.IDF of acid gas was compared with fuel gas cocombustion(FGC),split flow of acid gas(SFAG)and high-level oxygen enrichment combustion(OEC).Additionally,the effect of CO_(2)addition on the IDF of H_(2)S was investigated.The results indicated that a stable flame could be observed in the IDF of acid gas,its peak flame temperature was about 801.0 K,which was higher than that in the OEC,FGC and SFAG with a value of about 591.0,684.0 and 734.0 K,respectively.IDF of acid gas was contributed to the formation of sulfur and H_(2),and mainly involved the oxidation zone and the chemical decomposition and oxidation zone in sequence.In the IDF,CO_(2)exhibited a better oxidation performance,and the peak flame temperature was decreased by about 21.0 K with an increase in CO_(2)addition from 50.8%to 59.5%(vol),whereas significantly enhanced the oxidation reaction rate of H_(2)S,and the peak volume fraction of SO_(2)was increased from 5.812%to 7.075%.The application of IDF to acid gas combustion achieved the objective for improving flame temperature in low-level oxygen enrichment atmosphere under Claus conditions,providing a new perspective in the sulfur recovery and hydrogen production from acid gas.
文摘Four different pulverized coals have been used to study the effects of oxygen concentration on combustion characteristics under different enriched-oxygen conditions by entrained flow reactor experiments. The results show that: with the increase of oxygen concentration, the ignition temperature of four coals greatly decreases and the low volatile coals decrease faster; with the increase of oxygen concentration, the ignition mode of pulverized coal has an obviously transformation from homogeneous ignition to heterogeneous ignition, and the corresponding oxygen concentrations are about 40% and 50%-60% respectively for bituminous coal and lignite, and both about 30% for lean coal and anthracite; with the increase of oxygen concentration, the optimal pulverized coal concentrations of bituminous coal and lignite increase firstly and then decrease, but for lean coal and anthracite, the optimal pulverized coal concentrations decrease slowly with the increase of oxygen concentration.
基金supported by the National Key R&D Program of China(Grant No.2022YFB3806300).
文摘Infrared-transparent conductors have attracted considerable attention due to their potential applications in electromagnetic shielding,infrared sensors,and photovoltaic devices.However,most known materials face the critical challenge of balancing high infrared transmittance with high electrical conductivity across the broad infrared spectral band(2.5-25μm).While ultra-thin indium tin oxide(ITO)films have been demonstrated to exhibit superior infrared transmittance,their inherent low electrical conductivity necessitates additional enhancement strategies.This study systematically investigates the effects of oxygen vacancy concentration regulation and ultra-thin copper capping layer integration on the infrared optoelectronic properties of 20 nm-thick ITO films.A fundamental trade-off is revealed in ITO films that increased oxygen vacancy content enhances the electrical conductivity while compromising the infrared transmittance.Meanwhile,following the introduction of a Cu capping layer,the Cu/ITO system exhibits opposing dependencies of infrared transmittance and electrical conductivity on the capping layer thickness,with an optimum thickness of~3 nm.Finally,by constructing a Cu(3 nm)/ITO(20 nm)heterostructure with varying oxygen vacancy content,we demonstrate the combined effect of the ultra-thin Cu capping layer and moderate oxygen vacancy content on optimizing the carrier transport network.This configuration simultaneously minimizes surface/interfacial reflection and absorption losses,achieving high infrared transmittance(0.861)and a low sheet resistance of 400 W/sq.Our findings highlight the critical role of the combined effect of metal/oxide heterostructure design and defect engineering in optimizing infrared-transparent conductive properties.
基金financial support of the National Natural Science Foundation of China (22379063)
文摘Layered double hydroxides(LDHs)are potential cathode materials for aqueous magnesium-ion batteries(AMIBs).However,the low capacity and sluggish kinetics significantly limit their electrochemical performance in AMIBs.Herein,we find that oxygen vacancies can significantly boost the capacity,electrochemical kinetics,and structure stability of LDHs.The corresponding structure-performance relationship and energy storage mechanism are elaborated through exhaustive in/ex-situ experimental characterizations and density functional theory(DFT)calculations.Specially,in-situ Raman and DFT calculations reveal that oxygen vacancies elevate orbital energy of O 2p and electron density of O atoms,thereby enhancing the orbital hybridization of O 2p with Ni/Co 3d.This facilitates electron transfer between O and adjacent Ni/Co atoms and improves the covalency of Ni–O and Co–O bonds,which activates Ni/Co atoms to release more capacity and stabilizes the Ov-NiCo-LDH structure.Moreover,the distribution of relaxation times(DRT)and molecular dynamics(MD)simulations disclose that the enhanced d-p orbital hybridization optimizes the electronic structure of Ov-NiCo-LDH,which distinctly reduces the diffusion energy barriers of Mg^(2+)and improves the charge transfer kinetics of Ov-NiCo-LDH.Consequently,the assembled Ov-NiCo-LDH//active carbon(AC)and Ov-NiCo-LDH//perylenediimide(PTCDI)AMIBs can both deliver high specific discharge capacity(182.7 and 59.4 mAh g^(−1)at 0.5 A g^(−1),respectively)and long-term cycling stability(85.4%and 89.0%of capacity retentions after 2500 and 2400 cycles at 1.0 A g^(−1),respectively).In addition,the practical prospects for Ov-NiCo-LDH-based AMIBs have been demonstrated in different application scenarios.This work not only provides an effective strategy for obtaining high-performance cathodes of AMIBs,but also fundamentally elucidates the inherent mechanisms.
基金financial supports from the National Natural Science Foundation of China(52372211,52371225 and 92472115)the Guangdong Province Major Talent Introducing Program(2021QN020687)+1 种基金the Shenzhen Basic Research Foundation(JCYJ20230807112503007)the Guangdong Basic and Applied Basic Research Foundation(Grant No.2020A1515110176)。
文摘Lithium-rich manganese-based oxide(LRMO)cathode has emerged as a particularly promising candidate for achieving high energy densities in lithium-ion batteries due to its capability to access anion redox reactions at high voltage.The successful implementation of LRMO in energy storage systems is contingent upon the enhancement of their rate capabilities.However,the underlying relationship between high-rate cycling and electrode degradation for LRMO,particularly concerning structural evolution,still remains unclear.Benefiting from the high time resolution abilities of liquid-metal-jet operando twodimensional X-ray diffraction,it is observed that the Li_(2)MnO_(3)phase in LRMO is gradually activated accompanied by the emergence of oxygen vacancies during cycling at 1 C(1 C=250 mA/g).Consequently,the crystal lattice flexibility of LRMO is systematically enhanced,thereby preventing the collapse of the bulk structure.While,continuous release of oxygen during extended cycling results in deteriorations of the self-adjusting damping effect of the structure,ultimately leading to a decline in capacity.The findings of this study not only contribute to a more profound understanding of the structural changes of LRMOs at high rates,but also provide novel perspectives for the rational design of LRMOs with superior rate performances.
文摘Based on a six-cylinder direct injection diesel engine, the engine operating condition was simulated by application AVL-FIRE software coupling the n-heptane reduced mechanism containing polycyclic aromatic hydrocarbon (PAH) formation. The simulation and its verification test were both carried out under the maximum torque point. Then, the oxygen enriched combustion was simulated on the model, and the simulated condition was oxygen volume fraction from 21% to 30%. The simulation results show that, the oxygen enrichment (from 21% to 30%) increases the peak cylinder pressure of 3.32%, advances the start of combustion of 1.6 deg and rises the peak of average temperature in cylinder and wall heat flux. Among them, at the condition of 24% O2, the change of the results is the most significant. Benzene (A1) is one of the precursors of soot generated, the analysis of its impress-cuts of the mass distribution field in cylinder shows that, the increase of oxygen concentration can significantly inhibit the formation of benzene. But the oxygen enrichment makes the combustion more sufficient, cased a rise in the cylinder temperature, an extension in high temperature area, and an increment in the NOx emission.
基金supported by the National Natural Science Foundation of China (No.52274304)。
文摘Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthesized the electrode material Ce-NiCo-LDHs@SnO_(2)/NF through a two-step hydrothermal reaction,where Ce-doped NiCo-LDHs are grown on nickel foam modified by a SnO_(2) layer.Ce doping adjusts the internal electronic distribution of Ni Co-LDHs,while the introduction of the SnO_(2) layer enhances electron transfer capability.Together,these factors contribute to the reduction of the OER energy barrier and experimental evidence confirms that the reaction proceeds via the lattice oxygen evolution mechanism(LOM).Consequently,Ce-NiCo-LDHs@SnO_(2)/NF exhibits high level electrochemical performance in OER,requiring only 234 m V overpotential to achieve a current density of 10 m A/cm^(2),with a Tafel slope of just 27.39 m V/dec.When paired with Pt/C/NF,an external potential of only 1.54 V is needed to drive OWS to attain a current density amounting to 10 m A/cm^(2).Furthermore,the catalyst demonstrates stability for 100 h during the OWS stability test.This study underscores the feasibility of enhancing the OER performance through Ce doping and the introduction of a conductive SnO_(2) layer.
基金supported by the National Natural Science Foundation of China(NSFC)(22302151,52502312)Natural Science Foundation of Hubei Province(2024AFB755,2024AFB267)+1 种基金Key Project of Hubei Provincial Department of Education Scientific Research Plan(F2023007)Wuhan Institute of Technology Graduate Education Innovation Fund(CX2024285)。
文摘Layered double hydroxides(LDHs)are promising electrocatalysts for the oxygen evolution reaction(OER),yet their practical application remains limited by poor electrical conductivity and sluggish reaction kinetics.In this work,we synthesize three high-entropy LDHs(HELDHs)featuring a hierarchical architecture of microspheres assembled from ultrathin nanosheets,via a simple hydrothermal method using a combination of low-cost,catalytically active transition metals(Fe,Co,Ni,Mn,Zn,Cu,and Cr).Among them,the FeCoNiMnZn HELDH exhibits outstanding OER performance,requiring an overpotential of only 306 mV to reach a current density of 100 mA cm^(-2).Notably,during 200 h of continuous operation,the device exhibits a stable and,in some cases,increasing current output.This exceptional activity is attributed to the formation of abundant cation vacancies,induced by Zn leaching,which enhance the intrinsic catalytic properties by optimizing the adsorption energies of key OER intermediates.Density functional theory calculations further validate that these vacancies modulate the electronic structure and lower reaction barriers,underscoring the effectiveness of cation-vacancy engineering in high-entropy systems for efficient and durable water oxidation catalysis.The optimized catalyst was further evaluated as the air cathode in a zinc-air battery,demonstrating practical electrochemical performance.
基金financially supported by the National Natural Science Foundation of China(U1707603,21521005,21975013,21901017)the National Key Research and Development Program of China(2017YFA0206500,2018YFA0702000)+2 种基金Beijing Natural Science Foundation(2172042)PetroChina Innovation Foundationthe Fundamental Research Funds for the Central Universities。
文摘With exhaustion of fossil fuels and the deterioration of global environment,widespread and intensive researches have been concentrated on clean and sustainable alternative energy sources,such as metal-air batteries[1],fuel cells[2]and water splitting devices[3].Electrocatalytic oxidation of water to O2(oxygen evolution reaction,OER)is a vital chemical process involved in energy storage and conversion from renewable sources in form of molecular fuels such as H2 via water electrolysis,which has attracted a great amount of research efforts in the past few years[4,5].Nowadays,RuO2 and IrO2 are widely used as typical excellent OER electrocatalysts.However,their high-cost and scarce nature restricts the broadly commercial application of those materials[6,7].Hence,there is an urgent demand to develop low cost,highly efficient,and superb stable OER catalysts.
基金supported in part by the WPIMANA,Ministry of Education,Culture,Sports,Science and TechnologyCREST of the Japan Science and Technology Agency(JST)(Grant No.JPMJCR17N1)the support from JSPS KAKENNHI grant 15H02004 and 18H03869.
文摘Layered double hydroxides(LDHs)have attracted tremendous research interest in widely spreading applications.Most notably,transition-metal-bearing LDHs are expected to serve as highly active electrocatalysts for oxygen evolution reaction(OER)due to their layered structure combined with versatile com-positions.Furthermore,reducing the thickness of platelet LDH crystals to nanometer or even molecular scale via cleavage or delamination provides an important clue to enhance the activity.In this review,recent progresses on rational design of LDH nanosheets are reviewed,including direct synthesis via traditional coprecipitation,homogeneous precipitation,and newly developed topochemical oxidation as well as chemical exfoliation of parent LDH crystals.In addition,diverse strategies are introduced to modulate their electrochemical activity by tuning the composition of host metal cations and intercalated counter-anions,and incorporating dopants,cavi-ties,and single atoms.In particular,hybridizing LDHs with conductive components or in situ growing them on conductive substrates to produce freestanding electrodes can further enhance their intrinsic catalytic activity.A brief discussion on future research directions and prospects is also summarized.
基金supported by the National 973 Key Development Program for Basic Research of China(S/N: 2006CB202308)the National Natural Science Foundation of China(Grant No.40972088)
文摘The Tazhong paleouplift is divided into the upper and the lower structural layers, bounded by the unconformity surface at the top of the Ordovician carbonate rock. The reservoirs in the two layers from different parts vary in number, type and reserves, but the mechanism was rarely researched before. Therefore, an explanation of the mechanism will promote petroleum exploration in Tazhong paleouplift. After studying the evolution and reservoir distribution of the Tazhong paleouplift, it is concluded that the evolution in late Caledonian, late Hercynian and Himalayan periods resulted in the upper and the lower structural layers. It is also defined that in the upper structural layer, structural and stratigraphic overlap reservoirs are developed at the top and the upper part of the paleouplift, which are dominated by oil reservoirs, while for the lower structural layer, lithological reservoirs are developed in the lower part of the paleouplift, which are dominated by gas reservoirs, and more reserves are discovered in the lower structural layer than the upper. Through a comparative analysis of accumulation conditions of the upper and the lower structural layers, the mechanism of enrichment differences is clearly explained. The reservoir and seal conditions of the lower structural layer are better than those of the upper layer, which is the reason why more reservoirs have been found in the former. The differences in the carrier system types, trap types and charging periods between the upper and the lower structural layers lead to differences in the reservoir types and distribution. An accumulation model is established for the Tazhong paleouplift. For the upper structural layer, the structural reservoirs and the stratigraphic overlap reservoirs are formed at the upper part of the paleouplift, while for the lower structural layer, the weathering crust reservoirs are formed at the top, the reef-flat reservoirs are formed on the lateral margin, the karst and inside reservoirs are formed in the lower part of the paleouplift.
基金supported by the 973 Program(no.2014CB932104)the National Natural Science Foundation of China(nos:2177060378,U1707603 and 21521005)the Program for Changjiang Scholars,Innovative Research Teams in Universities(no.IRT1205)
文摘Compared with noble metal catalyst, Co3O4-based electrocatalysts have attracted considerable interesting as low-cost alternatives for oxygen evolution reaction (OER). However, the poor electrocatalytic activity still remains a huge challenge. Herein, we demonstrate a feasible approach through oxidation of CoFe layered double hydroxide (CoFe-LDH) to synthesize Fe-doped Co3O4@C nanopmrticles with size of about 30-50 nm. As OER catalyst, the as-synthesized Fe-doped Co3O4@C nanoparticles exhibited superior OER performance with a small overpotential of 260 mV at the current density of 20 mA cm^-2, a small Tafel slope of 70 mV dec^-1 and long-term durability (there was no obviously OER current density degradation for 100 h) in alkaline solution. The present work opens a new avenue to the exploration of cost-effective and excellent electrocatalysts based on transition metal oxide materials to substitute precious metal materials for water splitting.
基金financially supported by the Natural Science Foundation of China(21922803 and 21776077)the Shanghai Natural Science Foundation(17ZR1407300 and 17ZR1407500)+3 种基金the Program for the Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learningthe Shanghai Rising-Star Program(17QA1401200)the State Key Laboratory of Organic-Inorganic Composites(oic-201801007)the Open Project of State Key Laboratory of Chemical Engineering(SKLChe-15C03)。
文摘Understanding carbon-supported Pt-catalyzed oxygen reduction reaction(ORR)from the perspective of the active sites is of fundamental and practical importance.In this study,three differently sized carbon nanotube-supported Pt nanoparticles(Pt/CNT)are prepared by both atomic layer deposition(ALD)and impregnation methods.The performances of the catalysts toward the ORR in acidic media are comparatively studied to probe the effects of the sizes of the Pt nanoparticles together with their distributions,electronic properties,and local environments.The ALD-Pt/CNT catalysts show much higher ORR activity and selectivity than the impregnation-Pt/CNT catalysts.This outstanding ORR performance is ascribed to the well-controlled Pt particle sizes and distributions,desirable Pt^04f binding energy,and the Cl-free Pt surfaces based on the electrocatalytic measurements,catalyst characterizations,and model calculations.The insights reported here could guide the rational design and fine-tuning of carbon-supported Pt catalysts for the ORR.
