LiBH_(4)with high hydrogen storage density,is regarded as one of the most promising hydrogen storage materials.Nevertheless,it suffers from high dehydrogenation temperature and poor reversibility for practical use.Nan...LiBH_(4)with high hydrogen storage density,is regarded as one of the most promising hydrogen storage materials.Nevertheless,it suffers from high dehydrogenation temperature and poor reversibility for practical use.Nanoconfinement is effective in achieving low dehydrogenation temperature and favorable reversibility.Besides,graphene can serve as supporting materials for LiBH_(4)catalysts and also destabilize LiBH_(4)via interfacial reaction.However,graphene has never been used alone as a frame material for nanoconfining LiBH_(4).In this study,graphene microflowers with large pore volumes were prepared and used as nanoconfinement framework material for LiBH_(4),and the nanoconfinement effect of graphene was revealed.After loading 70 wt%of LiBH_(4) and mechanically compressed at 350 MPa,8.0 wt% of H2 can be released within 100 min at 320C,corresponding to the highest volumetric hydrogen storage density of 94.9 g H2 L^(-1)ever reported.Thanks to the nanoconfinement of graphene,the rate-limiting step of dehydrogenation of nanoconfined LiBH_(4) was changed and its apparent activation energy of the dehydrogenation(107.3 kJ mol^(-1))was 42%lower than that of pure LiBH_(4).Moreover,the formation of the intermediate Li_(2)B_(12)H_(12) was effectively inhibited,and the stable nanoconfined structure enhanced the reversibility of LiBH_(4).This work widens the understanding of graphene's nanoconfinement effect and provides new insights for developing high-density hydrogen storage materials.展开更多
Objective:This study assessed the role of the attending medical team in the cost control of the cholecystectomy DRG components.Methods:The association between team structure,workflow,and treatment outcomes was analyze...Objective:This study assessed the role of the attending medical team in the cost control of the cholecystectomy DRG components.Methods:The association between team structure,workflow,and treatment outcomes was analyzed using a mixed-methods approach combining quantitative data and qualitative interviews from 628 patients.Results:Inter-professional teamwork significantly affected length of stay,treatment costs,and recurrence rates,with experienced teams performing better in terms of emergency response and collaborative efficiency.Patient satisfaction was generally high,indicating that good teamwork enhances treatment outcomes.Significance:The study highlights the importance of optimizing team configuration to improve the quality,efficiency,and cost control of healthcare.展开更多
Hydrazine oxidation reaction(HzOR)assisted hydrogen evolution reaction(HER)offers a feasible path for low power consumption to hydrogen production.Unfortunately however,the total electrooxidation of hydrazine in anode...Hydrazine oxidation reaction(HzOR)assisted hydrogen evolution reaction(HER)offers a feasible path for low power consumption to hydrogen production.Unfortunately however,the total electrooxidation of hydrazine in anode and the dissociation kinetics of water in cathode are critically depend on the interaction between the reaction intermediates and surface of catalysts,which are still challenging due to the totally different catalytic mechanisms.Herein,the[W–O]group with strong adsorption capacity is introduced into CoP nanoflakes to fabricate bifunctional catalyst,which possesses excellent catalytic performances towards both HER(185.60 mV at 1000 mA cm^(−2))and HzOR(78.99 mV at 10,00 mA cm^(−2))with the overall electrolyzer potential of 1.634 V lower than that of the water splitting system at 100 mA cm^(−2).The introduction of[W–O]groups,working as the adsorption sites for H2O dissociation and N2H4 dehydrogenation,leads to the formation of porous structure on CoP nanoflakes and regulates the electronic structure of Co through the linked O in[W–O]group as well,resultantly boosting the hydrogen production and HzOR.Moreover,a proof-of-concept direct hydrazine fuel cell-powered H_(2) production system has been assembled,realizing H_(2)evolution at a rate of 3.53 mmol cm^(−2)h^(−1)at room temperature without external electricity supply.展开更多
Recently,research on the electrocatalytic CO_(2) reduction reaction(eCO_(2)RR)has attracted considerable attention due to its potential to resolve environmental problems caused by CO_(2) while utilizing clean energy a...Recently,research on the electrocatalytic CO_(2) reduction reaction(eCO_(2)RR)has attracted considerable attention due to its potential to resolve environmental problems caused by CO_(2) while utilizing clean energy and producing high‐value‐added products.Considerable theoretical research in the lab has demonstrated its feasibility and prospect.However,industrialization is mandatory to realize the economic and social value of eCO_(2)RR.For industrial application of eCO_(2)RR,more criteria have been proposed for eCO_(2)RR research,including high current density(above 200 mA cm^(−2)),high product selectivity(above 90%),and long‐term stability.To fulfill these criteria,the eCO_(2)RR system needs to be systematically designed and optimized.In this review,recent research on eCO_(2)RR for industrial applications is summarized.The review starts with focus on potential industrial catalysts in eCO_(2)RR.Next,potential industrial products are proposed in eCO_(2)RR.These products,including carbon monoxide,formic acid,ethylene,and ethanol,all have high market demand,and have shown high current density and product selectivity in theoretical research.Notably,the innovative components and strategy for industrializing the eCO_(2)RR system are also highlighted here,including flow cells,seawater electrolytes,solid electrolytes,and a two‐step method.Finally,some instructions and possible future avenues are presented for the prospects of future industrial application of eCO_(2)RR.展开更多
The rapid advance of mild aqueous zinc-ion batteries(ZIBs)is driving the development of the energy storage system market.But the thorny issues of Zn anodes,mainly including dendrite growth,hydrogen evolution,and corro...The rapid advance of mild aqueous zinc-ion batteries(ZIBs)is driving the development of the energy storage system market.But the thorny issues of Zn anodes,mainly including dendrite growth,hydrogen evolution,and corrosion,severely reduce the performance of ZIBs.To commercialize ZIBs,researchers must overcome formidable challenges.Research about mild aqueous ZIBs is still developing.Various technical and scientific obstacles to designing Zn anodes with high stripping efficiency and long cycling life have not been resolved.Moreover,the performance of Zn anodes is a complex scientific issue determined by various parameters,most of which are often ignored,failing to achieve the maximum performance of the cell.This review proposes a comprehensive overview of existing Zn anode issues and the corresponding strategies,frontiers,and development trends to deeply comprehend the essence and inner connection of degradation mechanism and performance.First,the formation mechanism of dendrite growth,hydrogen evolution,corrosion,and their influence on the anode are analyzed.Furthermore,various strategies for constructing stable Zn anodes are summarized and discussed in detail from multiple perspectives.These strategies are mainly divided into interface modification,structural anode,alloying anode,intercalation anode,liquid electrolyte,non-liquid electrolyte,separator design,and other strategies.Finally,research directions and prospects are put forward for Zn anodes.This contribution highlights the latest developments and provides new insights into the advanced Zn anode for future research.展开更多
Magnesium hydride(MgH2) is one of the most promising hydrogen storage materials for practical application due to its favorable reversibility, low cost and environmental benign;however, it suffers from high dehydrogena...Magnesium hydride(MgH2) is one of the most promising hydrogen storage materials for practical application due to its favorable reversibility, low cost and environmental benign;however, it suffers from high dehydrogenation temperature and slow sorption kinetics.Exploring proper catalysts with high and sustainable activity is extremely desired for substantially improving the hydrogen storage properties of MgH2. In this work, a composite catalyst with high-loading of ultrafine Ni nanoparticles(NPs) uniformly dispersed on porous hollow carbon nanospheres is developed, which shows superior catalytic activity towards the de-/hydrogenation of MgH2. With an addition of 5wt% of the composite, which contains 90 wt% Ni NPs, the onset and peak dehydrogenation temperatures of MgH2are lowered to 190 and 242 ℃, respectively. 6.2 wt% H2is rapidly released within 30 min at 250 ℃. The amount of H2that the dehydrogenation product can absorb at a low temperature of 150 ℃ in only 250 s is very close to the initial dehydrogenation value. A dehydrogenation capacity of 6.4wt% remains after 50 cycles at a moderate cyclic regime, corresponding to a capacity retention of 94.1%. The Ni NPs are highly active,reacting with MgH2and forming nanosized Mg2Ni/Mg2NiH4. They act as catalysts during hydrogen sorption cycling, and maintain a high dispersibility with the help of the dispersive role of the carbon substrate, leading to sustainably catalytic activity. The present work provides new insight into designing stable and highly active catalysts for promoting the(de)hydrogenation kinetics of MgH2.展开更多
Magnesium metal anode holds great potentials toward future high energy and safe rechargeable magnesium battery technology due to its divalent redox and dendrite-free nature. Electrolytes based on Lewis acid chemistry ...Magnesium metal anode holds great potentials toward future high energy and safe rechargeable magnesium battery technology due to its divalent redox and dendrite-free nature. Electrolytes based on Lewis acid chemistry enable the reversible Mg plating/stripping,while they fail to match most cathode materials toward highvoltage magnesium batteries. Herein,reversible Mg plating/stripping is achieved in conventional carbonate electrolytes enabled by the cooperative solvation/surface engineering. Strongly electronegative Cl from the MgCl_(2) additive of electrolyte impairs the Mg…O = C interaction to reduce the Mg^(2+) desolvation barrier for accelerated redox kinetics,while the Mg^(2+)-conducting polymer coating on the Mg surface ensures the facile Mg^(2+) migration and the e ective isolation of electrolytes. As a result,reversible plating and stripping of Mg is demonstrated with a low overpotential of 0.7 V up to 2000 cycles. Moreover,benefitting from the wide electrochemical window of carbonate electrolytes,high-voltage(> 2.0 V) rechargeable magnesium batteries are achieved through assembling the electrode couple of Mg metal anode and Prussian blue-based cathodes. The present work provides a cooperative engineering strategy to promote the application of magnesium anode in carbonate electrolytes toward high energy rechargeable batteries.展开更多
In recent years,a series of aqueous metal ion batteries(AMIBs)has been developed to improve the safety and cost-efficiency of portable electronics and electric vehicles.However,the significant gaps in energy density,p...In recent years,a series of aqueous metal ion batteries(AMIBs)has been developed to improve the safety and cost-efficiency of portable electronics and electric vehicles.However,the significant gaps in energy density,power density,and cycle stability of AMIBs directly hinder them from replacing the currently widely used non-aqueous metal ion batteries,which stems from the lack of reasonable configuration and performance optimization of electrode materials.First-row transition metal compounds(FRTMCs),with the advantages of optional voltage ranges(from low to high),adjustable crystal structures(layered and tunnel types with large spacing),and designable morphology(multi-dimensional nanostructures),are widely used to construct high-performance AMIBs.However,no comprehensive review papers were generated to highlight their specific and significant roles in AMIBs.In this review,we first summarize the superiority and characteristics of FRTMCs in AMIBs.Then,we put forward control strategies of FRTMCs from subsurface engineering to inner construction to promote capacitance control and diffusion control energy storage.After that,the electrochemical performance of the FRTMCs regulation strategies in AMIBs is reviewed.Finally,we present potential directions and challenges for further enhancements of FRTMCs in AMIBs.The review aims to provide an in-depth understanding of regulation strategies for enhancing energy storage to build high-performance AMIBs that meet practical applications.展开更多
Solid-state sodium metal batteries utilizing inorganic solid electrolytes(SEs)hold immense potentials such as intrinsical safety,high energy density,and environmental sustainability.However,the interfacial inhomogenei...Solid-state sodium metal batteries utilizing inorganic solid electrolytes(SEs)hold immense potentials such as intrinsical safety,high energy density,and environmental sustainability.However,the interfacial inhomogeneity/instability at the anode-SE interface usually triggers the penetration of sodium dendrites into the electrolyte,leading to short circuit and battery failure.Herein,confronting with the original nonuniform and high-resistance solid electrolyte interphase(SEI)at the Na-Na_(3)Zr_(2)Si_(2)PO_(12)interface,an oxygen-regulated SEI innovative approach is proposed to enhance the cycling stability of anode-SEs interface,through a spontaneous reaction between the metallic sodium(containing trace amounts of oxygen)and the Na_(3)Zr_(2)Si_(2)POi_(2)SE.The oxygen-regulated spontaneous SEI is thin,uniform,and kinetically stable to facilitate homogenous interfacial Na^+transportation,Benefitting from the optimized SEI,the assembled symmetric cell exhibits an ultra-stable sodium plating/stripping cycle for over 6600 h under a practical capacity of 3 mAh cm^(-2).Qua si-sol id-state batteries with Na_(3)V_(2)(PO_(4))_(3)cathode deliver excellent cyclability over 500 cycles at a rate of 0.5 C(1 C=117 mA cm^(-2))with a high capacity retention of95.4%.This oxygen-regulated SEI strategy may offer a potential avenue for the future development of high-energy-density solid-state metal batteries.展开更多
The storage of hydrogen in a compact,safe and cost-effective manner can be one of the key enabling technologies to power a more sustainable society.Magnesium hydride(MgH_(2))has attracted strong research interest as a...The storage of hydrogen in a compact,safe and cost-effective manner can be one of the key enabling technologies to power a more sustainable society.Magnesium hydride(MgH_(2))has attracted strong research interest as a hydrogen carrier because of its high gravimetric and volumetric hydrogen densities.However,the practical use of MgH_(2)for hydrogen storage has been limited due to high operation temperatures and sluggish kinetics.Catalysis is of crucial importance for the enhancement of hydrogen cycling kinetics of Mg/MgH_(2)and considerable work has been focused on designing,fabricating and optimizing catalysts.This review covers the recent advances in catalyzed Mg-based hydrogen storage materials.The fundamental properties and the syntheses of MgH_(2)as a hydrogen carrier are first briefly reviewed.After that,the general catalysis mechanisms and the catalysts developed for hydrogen storage in MgH_(2)are summarized in detail.Finally,the challenges and future research focus are discussed.Literature studies indicate that transition metals,rare-earth metals and their compounds are quite effective in catalyzing hydrogen storage in Mg/MgH_(2).Most metal-containing compounds were converted in situ to elemental metal or their magnesium alloys,and their particle sizes and dispersion affect their catalytic activity.The in-situ construction of catalyzed ultrasmall Mg/MgH_(2)nanostructures(<10 nm in size)is believed to be the future research focus.These important insights will help with the design and development of high-performance catalysts for hydrogen storage in Mg/MgH_(2).展开更多
Proton exchange membrane water electrolyzer(PEMWE)driven by renewable electricity is a promising technique toward green hydrogen production,but the corrosive environment and high working potential pose severe challeng...Proton exchange membrane water electrolyzer(PEMWE)driven by renewable electricity is a promising technique toward green hydrogen production,but the corrosive environment and high working potential pose severe challenges for developing advanced electrocatalysts for the oxygen evolution reaction(OER).Although Ir-based materials possess relatively balanced activity and stability for the OER,their dissolution behavior cannot be neglected,in particular under high working potentials.In this work,iridium dioxide(IrO_(2))nanoparticles(NPs)were anchored on the surface of exfoliated h-boron nitride(BN)nanosheets(NSs)toward the OER reaction in acid media.Highly active Ir(V)species were stabilized by the epitaxial interface between IrO_(2)and h-BN,and therefore the IrO_(2)/BN delivered stable performance at increased working potentials,while the activity of bare IrO_(2)NPs without h-BN support decreased rapidly.Also,the smaller lattice spacing of h-BN induced compressive strain for IrO_(2),resulting in improved activity.Our results demonstrate the feasibility of stabilizing highly active Ir(V)species for the OER in acid media by constructing robust interface and provide new possibilities toward designing advanced heterostructured electrocatalysts.展开更多
The mechanism governing the pseudocapacitive lithium storage behavior is one of the most critical unsolved issues in conversion-type anodes for lithium-ion batteries.In this work,we,for the first time,demonstrate that...The mechanism governing the pseudocapacitive lithium storage behavior is one of the most critical unsolved issues in conversion-type anodes for lithium-ion batteries.In this work,we,for the first time,demonstrate that the pseudocapacitive capability of iron oxide-based anodes is closely associated with the electronic structures of iron ions.As proof of concept,the introduction of amorphization,nitrogen doping,oxygen vacancies reduces the coordination of iron ions and contributes significantly to the pseudocapacitive lithium storage capability of iron oxide,reaching up to 96%of the specific capacity at 1 mV·s^(−1).Due to the significantly modulated coordination environment,the 3d electrons of Fe(II)are delocalized with increased spin state and the energy band gap is narrowed,accompanied by an upshift of Fermi energy.The redox activity and carrier mobility of iron oxides are substantially increased,which substantially enhance the exchange current density and thereby improve the pseudocapacitive capability of iron oxide.展开更多
Green reactions not only provide us chemical products without any pollution,but also offer us the viable technology to realize difficult tasks in normal conditions.Photo-,photoelectro-,and electrocatalytic reactions a...Green reactions not only provide us chemical products without any pollution,but also offer us the viable technology to realize difficult tasks in normal conditions.Photo-,photoelectro-,and electrocatalytic reactions are indeed powerful tools to help us to embrace bright future.Especially,some gas-involved reactions are extremely useful to change our life environments from energy systems to liquid fuels and cost-effective products,such as H2 evolution(H2 production),02 evolution/reduction,CO2 reduction,N2 reduction(or N2 fixation) reactions.We can provide fuel cells clean H2 for electric vehicles from H2 evolution reaction(HER),at the same time,we also need highly efficient 02 reduction reaction(ORR) in fuel cells for improving the reaction kinetics.Moreover,we can get the clean oxidant O2 from water through O2 evolution reaction(OER),and carry out some reactions without posing any pollution to reaction systems.Furthermore,we can translate the greenhouse gas CO2 into useful liquid fuels through CO2 reduction reaction(CRR).Last but not the least,we can get ammonia from N2 reduction reaction(NRR),which can decrease energy input compared to the traditional Hubble process.These reactions,such as HER,ORR,OER,CRR and NRR could be realized through solar-,photoelectro-and electro-assisted ways.For them,the catalysts used play crucial roles in determining the efficiency and kinds of products,so we should consider the efficiency of catalysts.However,the cost,synthetic methods of catalysts should also be considered.Nowadays,significant progress has been achieved,however,many challenges still exist,reaction systems,catalysts underlying mechanisms,and so on.As extremely active fields,we should pay attention to them.Under the background,it has motivated us to contribute with a roadmap on ’GasInvolved Photo-and Electro-Catalysis’.展开更多
在大规模储能领域中,高温钠离子电池(SIBs)受到了广泛关注.然而,较低的充放电效率和较差的循环稳定性仍是制约高温钠离子电池发展的主要因素.因此,开发性能优异的电极材料是高温钠离子电池发展的关键.本工作中,我们通过简单的钾离子插...在大规模储能领域中,高温钠离子电池(SIBs)受到了广泛关注.然而,较低的充放电效率和较差的循环稳定性仍是制约高温钠离子电池发展的主要因素.因此,开发性能优异的电极材料是高温钠离子电池发展的关键.本工作中,我们通过简单的钾离子插入法制备了KV_(3)O_(8)纳米带作为高温钠离子电池的负极材料.在60℃高温下,KV_(3)O_(8)纳米带表现出高的储钠容量(在0.1 A g^(-1)电流密度下,可逆容量为414 mAh g^(-1))、卓越的倍率性能(在20 A g^(-1)的高电流密度下为220 mA h g^(-1))和优异的循环稳定性(10 A g^(-1)的电流密度下循环1000次,容量几乎没有衰减).此外,通过非原位XRD分析发现,KV_(3)O_(8)纳米带的结构在整个充放电过程中未发生明显变化,进一步证实了其优异的稳定性.本研究表明KV_(3)O_(8)纳米带具有成为高温钠离子电池负极材料的潜力.展开更多
Zinc-ion batteries(ZIBs),in particular quasi-solid-state ZIBs,occupy a crucial position in the field of energy storage devices owing to the superiorities of abundant zinc reserve,low cost,high safety and high theoreti...Zinc-ion batteries(ZIBs),in particular quasi-solid-state ZIBs,occupy a crucial position in the field of energy storage devices owing to the superiorities of abundant zinc reserve,low cost,high safety and high theoretical capacity of zinc anode.However,as divalent Zn^(2+)ions experience strong electrostatic interactions when intercalating into the cathode materials,which poses challenges to the structural stability and higher demand in Zn^(2+)ions diffusion kinetics of the cathode materials.Here,a microwave-assisted hydrothermal method is adopted to prepare pre-potassiated hydrated vanadium pentoxide(K_(0.52)V_(2)O_(5)·0.29H_(2)O,abbreviated as KHVO)cathode material,in which the potassium ions preinserted into the interlayers can act as“pillars”to stabilize the lamellar structure,and crystal water can act as“lubricant”to improve the diffusion efficiency of Zn^(2+)ions.Consequently,the KHVO displays high electrochemical properties with high capacity(∼300 mAh/g),superior rate capability(69 mAh/g at 5 A/g)and ultralong cycling performance(>1500 cycles at 2 A/g)in quasi-solid-state ZIBs.These superior Zn storage properties result from the large diffusion coefficient and highly stable and reversible Zn^(2+)(de)intercalation reaction of KHVO.展开更多
基金supported by National Key Research and Development Program of China(2021YFB4000602)National Natural Science Foundation of PR China(Nos.52071287,52072342,52271227)+3 种基金National Outstanding Youth Foundation of China(No.52125104)Natural Science Foundation of Zhejiang Province,PR China(No.LZ23E010002)Young Talent Fund of Association for Science and Technology in Shaanxi,China(No.20220456)Young Star Project of Science and Technology of Shaanxi Province(2022KJXX-43).
文摘LiBH_(4)with high hydrogen storage density,is regarded as one of the most promising hydrogen storage materials.Nevertheless,it suffers from high dehydrogenation temperature and poor reversibility for practical use.Nanoconfinement is effective in achieving low dehydrogenation temperature and favorable reversibility.Besides,graphene can serve as supporting materials for LiBH_(4)catalysts and also destabilize LiBH_(4)via interfacial reaction.However,graphene has never been used alone as a frame material for nanoconfining LiBH_(4).In this study,graphene microflowers with large pore volumes were prepared and used as nanoconfinement framework material for LiBH_(4),and the nanoconfinement effect of graphene was revealed.After loading 70 wt%of LiBH_(4) and mechanically compressed at 350 MPa,8.0 wt% of H2 can be released within 100 min at 320C,corresponding to the highest volumetric hydrogen storage density of 94.9 g H2 L^(-1)ever reported.Thanks to the nanoconfinement of graphene,the rate-limiting step of dehydrogenation of nanoconfined LiBH_(4) was changed and its apparent activation energy of the dehydrogenation(107.3 kJ mol^(-1))was 42%lower than that of pure LiBH_(4).Moreover,the formation of the intermediate Li_(2)B_(12)H_(12) was effectively inhibited,and the stable nanoconfined structure enhanced the reversibility of LiBH_(4).This work widens the understanding of graphene's nanoconfinement effect and provides new insights for developing high-density hydrogen storage materials.
文摘Objective:This study assessed the role of the attending medical team in the cost control of the cholecystectomy DRG components.Methods:The association between team structure,workflow,and treatment outcomes was analyzed using a mixed-methods approach combining quantitative data and qualitative interviews from 628 patients.Results:Inter-professional teamwork significantly affected length of stay,treatment costs,and recurrence rates,with experienced teams performing better in terms of emergency response and collaborative efficiency.Patient satisfaction was generally high,indicating that good teamwork enhances treatment outcomes.Significance:The study highlights the importance of optimizing team configuration to improve the quality,efficiency,and cost control of healthcare.
基金support of this research by National Natural Science Foundation of China(52172110)Key Research Program of Frontier Sciences,Chinese Academy of Sciences(ZDBS-LY-SLH029)+1 种基金the“Scientific and Technical Innovation Action Plan”Hong Kong,Macao and Taiwan Science&Technology Cooperation Project of Shanghai Science and Technology Committee(21520760500)BL14W1 beamline of Shanghai Synchrotron Radiation Facility(SSRF).
文摘Hydrazine oxidation reaction(HzOR)assisted hydrogen evolution reaction(HER)offers a feasible path for low power consumption to hydrogen production.Unfortunately however,the total electrooxidation of hydrazine in anode and the dissociation kinetics of water in cathode are critically depend on the interaction between the reaction intermediates and surface of catalysts,which are still challenging due to the totally different catalytic mechanisms.Herein,the[W–O]group with strong adsorption capacity is introduced into CoP nanoflakes to fabricate bifunctional catalyst,which possesses excellent catalytic performances towards both HER(185.60 mV at 1000 mA cm^(−2))and HzOR(78.99 mV at 10,00 mA cm^(−2))with the overall electrolyzer potential of 1.634 V lower than that of the water splitting system at 100 mA cm^(−2).The introduction of[W–O]groups,working as the adsorption sites for H2O dissociation and N2H4 dehydrogenation,leads to the formation of porous structure on CoP nanoflakes and regulates the electronic structure of Co through the linked O in[W–O]group as well,resultantly boosting the hydrogen production and HzOR.Moreover,a proof-of-concept direct hydrazine fuel cell-powered H_(2) production system has been assembled,realizing H_(2)evolution at a rate of 3.53 mmol cm^(−2)h^(−1)at room temperature without external electricity supply.
基金supported by the National Natural Science Foundation of China(Grant Nos.51873085,52071171)Liaoning Revitalization Talents Program-Pan Deng Scholars(XLYC2007056,XLYC1802005)+9 种基金the Liaoning BaiQianWan Talents Program(LNBQW2018B0048)the Natural Science Fund of Liaoning Province for Excellent Young Scholars(2019-YQ-04)the Key Project of Scientific Research of the Education Department of Liaoning Province(LZD201902)the Shenyang Science and Technology Project(21-108-9-04)the Australian Research Council(ARC)through Future Fellowship(FT210100298,FT210100806)Discovery Project(DP220100603)the Linkage Project(LP210100467,LP210200504,LP210200345)Industrial Transformation Training Centre(IC180100005)schemesthe CSIRO Energy Centrethe Kick-Start Project.
文摘Recently,research on the electrocatalytic CO_(2) reduction reaction(eCO_(2)RR)has attracted considerable attention due to its potential to resolve environmental problems caused by CO_(2) while utilizing clean energy and producing high‐value‐added products.Considerable theoretical research in the lab has demonstrated its feasibility and prospect.However,industrialization is mandatory to realize the economic and social value of eCO_(2)RR.For industrial application of eCO_(2)RR,more criteria have been proposed for eCO_(2)RR research,including high current density(above 200 mA cm^(−2)),high product selectivity(above 90%),and long‐term stability.To fulfill these criteria,the eCO_(2)RR system needs to be systematically designed and optimized.In this review,recent research on eCO_(2)RR for industrial applications is summarized.The review starts with focus on potential industrial catalysts in eCO_(2)RR.Next,potential industrial products are proposed in eCO_(2)RR.These products,including carbon monoxide,formic acid,ethylene,and ethanol,all have high market demand,and have shown high current density and product selectivity in theoretical research.Notably,the innovative components and strategy for industrializing the eCO_(2)RR system are also highlighted here,including flow cells,seawater electrolytes,solid electrolytes,and a two‐step method.Finally,some instructions and possible future avenues are presented for the prospects of future industrial application of eCO_(2)RR.
基金supported by the National Natural Science Foundation of China(No.52071171)Liaoning Revitalization Talents Program-Pan Deng Scholars(XLYC1802005)+5 种基金Liaoning BaiQianWan Talents Program(LNBQW2018B0048)Natural Science Fund of Liaoning Province for Excellent Young Scholars(2019-YQ-04)Key Project of Scientific Research of the Education Department of Liaoning Province(LZD201902)Foundation for Young Scholars of Liaoning University(a252102001)Australian Research Council(ARC)Future Fellowship(FT210100298)CSIRO Energy Centre,Kick-Start Project and the Victorian Government’s support through the provision of a grant from veski-Study Melbourne Research Partnerships(SMRP)project.
文摘The rapid advance of mild aqueous zinc-ion batteries(ZIBs)is driving the development of the energy storage system market.But the thorny issues of Zn anodes,mainly including dendrite growth,hydrogen evolution,and corrosion,severely reduce the performance of ZIBs.To commercialize ZIBs,researchers must overcome formidable challenges.Research about mild aqueous ZIBs is still developing.Various technical and scientific obstacles to designing Zn anodes with high stripping efficiency and long cycling life have not been resolved.Moreover,the performance of Zn anodes is a complex scientific issue determined by various parameters,most of which are often ignored,failing to achieve the maximum performance of the cell.This review proposes a comprehensive overview of existing Zn anode issues and the corresponding strategies,frontiers,and development trends to deeply comprehend the essence and inner connection of degradation mechanism and performance.First,the formation mechanism of dendrite growth,hydrogen evolution,corrosion,and their influence on the anode are analyzed.Furthermore,various strategies for constructing stable Zn anodes are summarized and discussed in detail from multiple perspectives.These strategies are mainly divided into interface modification,structural anode,alloying anode,intercalation anode,liquid electrolyte,non-liquid electrolyte,separator design,and other strategies.Finally,research directions and prospects are put forward for Zn anodes.This contribution highlights the latest developments and provides new insights into the advanced Zn anode for future research.
基金supported by the National Key Research and Development Program of the Ministry of Science and Technology of PR China (No. 2018YFB1502103)National Natural Science Foundation of PR China (Nos. 52071287, 51571175, U1601212, 51831009)。
文摘Magnesium hydride(MgH2) is one of the most promising hydrogen storage materials for practical application due to its favorable reversibility, low cost and environmental benign;however, it suffers from high dehydrogenation temperature and slow sorption kinetics.Exploring proper catalysts with high and sustainable activity is extremely desired for substantially improving the hydrogen storage properties of MgH2. In this work, a composite catalyst with high-loading of ultrafine Ni nanoparticles(NPs) uniformly dispersed on porous hollow carbon nanospheres is developed, which shows superior catalytic activity towards the de-/hydrogenation of MgH2. With an addition of 5wt% of the composite, which contains 90 wt% Ni NPs, the onset and peak dehydrogenation temperatures of MgH2are lowered to 190 and 242 ℃, respectively. 6.2 wt% H2is rapidly released within 30 min at 250 ℃. The amount of H2that the dehydrogenation product can absorb at a low temperature of 150 ℃ in only 250 s is very close to the initial dehydrogenation value. A dehydrogenation capacity of 6.4wt% remains after 50 cycles at a moderate cyclic regime, corresponding to a capacity retention of 94.1%. The Ni NPs are highly active,reacting with MgH2and forming nanosized Mg2Ni/Mg2NiH4. They act as catalysts during hydrogen sorption cycling, and maintain a high dispersibility with the help of the dispersive role of the carbon substrate, leading to sustainably catalytic activity. The present work provides new insight into designing stable and highly active catalysts for promoting the(de)hydrogenation kinetics of MgH2.
基金supported by National Key Research and Development Program (2019YFE0111200)the National Natural Science Foundation of China (51722105)+1 种基金Zhejiang Provincial Natural Science Foundation of China (LR18B030001)the Fundamental Research Funds for the Central Universities and the Fundamental Research Funds for the Central Universities。
文摘Magnesium metal anode holds great potentials toward future high energy and safe rechargeable magnesium battery technology due to its divalent redox and dendrite-free nature. Electrolytes based on Lewis acid chemistry enable the reversible Mg plating/stripping,while they fail to match most cathode materials toward highvoltage magnesium batteries. Herein,reversible Mg plating/stripping is achieved in conventional carbonate electrolytes enabled by the cooperative solvation/surface engineering. Strongly electronegative Cl from the MgCl_(2) additive of electrolyte impairs the Mg…O = C interaction to reduce the Mg^(2+) desolvation barrier for accelerated redox kinetics,while the Mg^(2+)-conducting polymer coating on the Mg surface ensures the facile Mg^(2+) migration and the e ective isolation of electrolytes. As a result,reversible plating and stripping of Mg is demonstrated with a low overpotential of 0.7 V up to 2000 cycles. Moreover,benefitting from the wide electrochemical window of carbonate electrolytes,high-voltage(> 2.0 V) rechargeable magnesium batteries are achieved through assembling the electrode couple of Mg metal anode and Prussian blue-based cathodes. The present work provides a cooperative engineering strategy to promote the application of magnesium anode in carbonate electrolytes toward high energy rechargeable batteries.
基金supported by the National Natural Science Foundation of China(Nos.52071171,22109060)the Liaoning Revitalization Talents Program-Pan Deng Scholars(XLYC1802005)+5 种基金the Liaoning Bai Qian Wan Talents Program(LNBQW2018B0048)the Natural Science Fund of Liaoning Province for Excellent Young Scholars(2019-YQ-04)the Key Project of Scientific Research of the Education Department of Liaoning Province(LZD201902)the Research Fund for the Doctoral Program of Liaoning Province(2020-BS-085)the Australian Research Council(ARC)Future Fellowship(FT210100298)the CSIRO Energy Centre。
文摘In recent years,a series of aqueous metal ion batteries(AMIBs)has been developed to improve the safety and cost-efficiency of portable electronics and electric vehicles.However,the significant gaps in energy density,power density,and cycle stability of AMIBs directly hinder them from replacing the currently widely used non-aqueous metal ion batteries,which stems from the lack of reasonable configuration and performance optimization of electrode materials.First-row transition metal compounds(FRTMCs),with the advantages of optional voltage ranges(from low to high),adjustable crystal structures(layered and tunnel types with large spacing),and designable morphology(multi-dimensional nanostructures),are widely used to construct high-performance AMIBs.However,no comprehensive review papers were generated to highlight their specific and significant roles in AMIBs.In this review,we first summarize the superiority and characteristics of FRTMCs in AMIBs.Then,we put forward control strategies of FRTMCs from subsurface engineering to inner construction to promote capacitance control and diffusion control energy storage.After that,the electrochemical performance of the FRTMCs regulation strategies in AMIBs is reviewed.Finally,we present potential directions and challenges for further enhancements of FRTMCs in AMIBs.The review aims to provide an in-depth understanding of regulation strategies for enhancing energy storage to build high-performance AMIBs that meet practical applications.
基金Zhejiang Provincial Natural Science Foundation of China(LZ23B030003)the National Key R&D Program(2022YFB2502000)+1 种基金the National Key R&D Program(2022YFB2502000)the Fundamental Research Funds for the Central Universities(2021FZZX001-09)。
文摘Solid-state sodium metal batteries utilizing inorganic solid electrolytes(SEs)hold immense potentials such as intrinsical safety,high energy density,and environmental sustainability.However,the interfacial inhomogeneity/instability at the anode-SE interface usually triggers the penetration of sodium dendrites into the electrolyte,leading to short circuit and battery failure.Herein,confronting with the original nonuniform and high-resistance solid electrolyte interphase(SEI)at the Na-Na_(3)Zr_(2)Si_(2)PO_(12)interface,an oxygen-regulated SEI innovative approach is proposed to enhance the cycling stability of anode-SEs interface,through a spontaneous reaction between the metallic sodium(containing trace amounts of oxygen)and the Na_(3)Zr_(2)Si_(2)POi_(2)SE.The oxygen-regulated spontaneous SEI is thin,uniform,and kinetically stable to facilitate homogenous interfacial Na^+transportation,Benefitting from the optimized SEI,the assembled symmetric cell exhibits an ultra-stable sodium plating/stripping cycle for over 6600 h under a practical capacity of 3 mAh cm^(-2).Qua si-sol id-state batteries with Na_(3)V_(2)(PO_(4))_(3)cathode deliver excellent cyclability over 500 cycles at a rate of 0.5 C(1 C=117 mA cm^(-2))with a high capacity retention of95.4%.This oxygen-regulated SEI strategy may offer a potential avenue for the future development of high-energy-density solid-state metal batteries.
基金the financial support received from the National Key R&D Program of China(No.2022YFB3803700)the National Outstanding Youth Foundation of China(No.52125104)+3 种基金the Natural Science Foundation of Zhejiang Province(No.LD21E010002)the National Natural Science Foundation of China(Nos.52001277 and U22A20120)the Fundamental Research Funds for the Central Universities(Nos.2021FZZX001-09 and 226-2022-00246)the National Youth Top-Notch Talent Support Program.
文摘The storage of hydrogen in a compact,safe and cost-effective manner can be one of the key enabling technologies to power a more sustainable society.Magnesium hydride(MgH_(2))has attracted strong research interest as a hydrogen carrier because of its high gravimetric and volumetric hydrogen densities.However,the practical use of MgH_(2)for hydrogen storage has been limited due to high operation temperatures and sluggish kinetics.Catalysis is of crucial importance for the enhancement of hydrogen cycling kinetics of Mg/MgH_(2)and considerable work has been focused on designing,fabricating and optimizing catalysts.This review covers the recent advances in catalyzed Mg-based hydrogen storage materials.The fundamental properties and the syntheses of MgH_(2)as a hydrogen carrier are first briefly reviewed.After that,the general catalysis mechanisms and the catalysts developed for hydrogen storage in MgH_(2)are summarized in detail.Finally,the challenges and future research focus are discussed.Literature studies indicate that transition metals,rare-earth metals and their compounds are quite effective in catalyzing hydrogen storage in Mg/MgH_(2).Most metal-containing compounds were converted in situ to elemental metal or their magnesium alloys,and their particle sizes and dispersion affect their catalytic activity.The in-situ construction of catalyzed ultrasmall Mg/MgH_(2)nanostructures(<10 nm in size)is believed to be the future research focus.These important insights will help with the design and development of high-performance catalysts for hydrogen storage in Mg/MgH_(2).
基金supported by the Natural Science Foundation of Zhejiang Province(No.LZ22B030006)the National Natural Science Foundation of China(No.52171224)+2 种基金G.Q.Z.acknowledges the financial support from the China Postdoctoral Science Foundation(Nos.2021M690132 and 2021T140588)the Office of China Postdoc Council(No.YJ20200160)Natural Science Foundation of Zhejiang Province(No.LQ22B030005).
文摘Proton exchange membrane water electrolyzer(PEMWE)driven by renewable electricity is a promising technique toward green hydrogen production,but the corrosive environment and high working potential pose severe challenges for developing advanced electrocatalysts for the oxygen evolution reaction(OER).Although Ir-based materials possess relatively balanced activity and stability for the OER,their dissolution behavior cannot be neglected,in particular under high working potentials.In this work,iridium dioxide(IrO_(2))nanoparticles(NPs)were anchored on the surface of exfoliated h-boron nitride(BN)nanosheets(NSs)toward the OER reaction in acid media.Highly active Ir(V)species were stabilized by the epitaxial interface between IrO_(2)and h-BN,and therefore the IrO_(2)/BN delivered stable performance at increased working potentials,while the activity of bare IrO_(2)NPs without h-BN support decreased rapidly.Also,the smaller lattice spacing of h-BN induced compressive strain for IrO_(2),resulting in improved activity.Our results demonstrate the feasibility of stabilizing highly active Ir(V)species for the OER in acid media by constructing robust interface and provide new possibilities toward designing advanced heterostructured electrocatalysts.
基金the key program of National Natural Science Foundation of China(No.51831009)the general program of National Natural Science Foundation of China(No.52071285).
文摘The mechanism governing the pseudocapacitive lithium storage behavior is one of the most critical unsolved issues in conversion-type anodes for lithium-ion batteries.In this work,we,for the first time,demonstrate that the pseudocapacitive capability of iron oxide-based anodes is closely associated with the electronic structures of iron ions.As proof of concept,the introduction of amorphization,nitrogen doping,oxygen vacancies reduces the coordination of iron ions and contributes significantly to the pseudocapacitive lithium storage capability of iron oxide,reaching up to 96%of the specific capacity at 1 mV·s^(−1).Due to the significantly modulated coordination environment,the 3d electrons of Fe(II)are delocalized with increased spin state and the energy band gap is narrowed,accompanied by an upshift of Fermi energy.The redox activity and carrier mobility of iron oxides are substantially increased,which substantially enhance the exchange current density and thereby improve the pseudocapacitive capability of iron oxide.
基金funding support from “Hundred Talents Program” of Zhejiang University, Chinapartially supported by the Australian Research Council (ARC) Discovery Project (DP200100365)
基金The financial support from the National Natural Science Foundation of China (Nos. 51772312, 21671197)
文摘Green reactions not only provide us chemical products without any pollution,but also offer us the viable technology to realize difficult tasks in normal conditions.Photo-,photoelectro-,and electrocatalytic reactions are indeed powerful tools to help us to embrace bright future.Especially,some gas-involved reactions are extremely useful to change our life environments from energy systems to liquid fuels and cost-effective products,such as H2 evolution(H2 production),02 evolution/reduction,CO2 reduction,N2 reduction(or N2 fixation) reactions.We can provide fuel cells clean H2 for electric vehicles from H2 evolution reaction(HER),at the same time,we also need highly efficient 02 reduction reaction(ORR) in fuel cells for improving the reaction kinetics.Moreover,we can get the clean oxidant O2 from water through O2 evolution reaction(OER),and carry out some reactions without posing any pollution to reaction systems.Furthermore,we can translate the greenhouse gas CO2 into useful liquid fuels through CO2 reduction reaction(CRR).Last but not the least,we can get ammonia from N2 reduction reaction(NRR),which can decrease energy input compared to the traditional Hubble process.These reactions,such as HER,ORR,OER,CRR and NRR could be realized through solar-,photoelectro-and electro-assisted ways.For them,the catalysts used play crucial roles in determining the efficiency and kinds of products,so we should consider the efficiency of catalysts.However,the cost,synthetic methods of catalysts should also be considered.Nowadays,significant progress has been achieved,however,many challenges still exist,reaction systems,catalysts underlying mechanisms,and so on.As extremely active fields,we should pay attention to them.Under the background,it has motivated us to contribute with a roadmap on ’GasInvolved Photo-and Electro-Catalysis’.
基金supported by the National Natural Science Foundation of China(51801030,51902032,51802044,51902062,and 51802043)the Natural Science Foundation of Jiangsu Province(BK20191026)Guangdong Natural Science Funds for the Distinguished Young Scholar(2019B151502039)。
文摘在大规模储能领域中,高温钠离子电池(SIBs)受到了广泛关注.然而,较低的充放电效率和较差的循环稳定性仍是制约高温钠离子电池发展的主要因素.因此,开发性能优异的电极材料是高温钠离子电池发展的关键.本工作中,我们通过简单的钾离子插入法制备了KV_(3)O_(8)纳米带作为高温钠离子电池的负极材料.在60℃高温下,KV_(3)O_(8)纳米带表现出高的储钠容量(在0.1 A g^(-1)电流密度下,可逆容量为414 mAh g^(-1))、卓越的倍率性能(在20 A g^(-1)的高电流密度下为220 mA h g^(-1))和优异的循环稳定性(10 A g^(-1)的电流密度下循环1000次,容量几乎没有衰减).此外,通过非原位XRD分析发现,KV_(3)O_(8)纳米带的结构在整个充放电过程中未发生明显变化,进一步证实了其优异的稳定性.本研究表明KV_(3)O_(8)纳米带具有成为高温钠离子电池负极材料的潜力.
基金the National Natural Sci-ence Foundation of China(Nos.51972067,51802265,51802044,51902062 and 51802043)the Guangdong Natural Science Funds for Distinguished Young Scholar(No.2019B151502039).
文摘Zinc-ion batteries(ZIBs),in particular quasi-solid-state ZIBs,occupy a crucial position in the field of energy storage devices owing to the superiorities of abundant zinc reserve,low cost,high safety and high theoretical capacity of zinc anode.However,as divalent Zn^(2+)ions experience strong electrostatic interactions when intercalating into the cathode materials,which poses challenges to the structural stability and higher demand in Zn^(2+)ions diffusion kinetics of the cathode materials.Here,a microwave-assisted hydrothermal method is adopted to prepare pre-potassiated hydrated vanadium pentoxide(K_(0.52)V_(2)O_(5)·0.29H_(2)O,abbreviated as KHVO)cathode material,in which the potassium ions preinserted into the interlayers can act as“pillars”to stabilize the lamellar structure,and crystal water can act as“lubricant”to improve the diffusion efficiency of Zn^(2+)ions.Consequently,the KHVO displays high electrochemical properties with high capacity(∼300 mAh/g),superior rate capability(69 mAh/g at 5 A/g)and ultralong cycling performance(>1500 cycles at 2 A/g)in quasi-solid-state ZIBs.These superior Zn storage properties result from the large diffusion coefficient and highly stable and reversible Zn^(2+)(de)intercalation reaction of KHVO.
