Sodium-based dual-ion batteries(SDIBs) have gained tremendous attention due to their virtues of high operating voltage and low cost, yet it remains a tough challenge for the development of ideal anode material of SDIB...Sodium-based dual-ion batteries(SDIBs) have gained tremendous attention due to their virtues of high operating voltage and low cost, yet it remains a tough challenge for the development of ideal anode material of SDIBs featuring with high kinetics and long durability. Herein, we report the design and fabrication of N-doped carbon film-modified niobium sulfur–selenium(NbSSe/NC) nanosheets architecture, which holds favorable merits for Na^(+) storage of enlarged interlayer space, improved electrical conductivity, as well as enhanced reaction reversibility, endowing it with high capacity, high-rate capability and high cycling stability. The combined electrochemical studies with density functional theory calculation reveal that the enriched defects in such nanosheets architecture can benefit for facilitating charge transfer and Na+ adsorption to speed the electrochemical kinetics. The NbSSe/NC composites are studied as the anode of a full SDIBs by pairing the expanded graphite as cathode, which shows an impressively cyclic durability with negligible capacity attenuation over 1000 cycles at 0.5 A g^(-1), as well as an outstanding energy density of 230.6 Wh kg^(-1) based on the total mass of anode and cathode.展开更多
The application of electrocatalysts for the oxygen reduction reaction(ORR) is vital in a variety of energy conversion technologies. Exploring low-cost ORR catalysts with high activity and long-term stability is highly...The application of electrocatalysts for the oxygen reduction reaction(ORR) is vital in a variety of energy conversion technologies. Exploring low-cost ORR catalysts with high activity and long-term stability is highly desirable, although it still remains challenging. Herein, we report a facile and reliable route to convert ZIF-8 modified by Fe-phenanthroline into Fe-incorporated and N-doped carbon dodecahedron nanoarchitecture(Fe-NCDNA), in which carbon nanosheets are formed in situ as the building blocks with uniform Fe-N-C species decoration. Systematic electrochemical studies demonstrate that the as-synthesized Fe-NCDNA electrocatalyst possesses highly attractive catalytic features toward the ORR in terms of activity and durability in both alkaline and neutral media. The Zn-air battery with the optimal Fe-NCDNA catalyst as the cathode performs impressively, delivering a power density of 184 m W cm^–2 and a specific capacity of 801 m Ah g^–1;thus, it exhibits great competitive advantages over those of the Zn-air devices employing a Pt-based cathode electrocatalyst.展开更多
Renewable biomass-derived carbon materials have attracted increasing research attention as promising electrode materials for electrochemical energy storage devices, such as sodium-ion batteries (SIBs), due to their ou...Renewable biomass-derived carbon materials have attracted increasing research attention as promising electrode materials for electrochemical energy storage devices, such as sodium-ion batteries (SIBs), due to their outstanding electrical conductivity, hierarchical porous structure, intrinsic heteroatom doping, and environmental friendliness. Here, we investigate the potential of hierarchical N-doped porous carbon (NPC) derived from jackfruit rags through a facile pyrolysis as an anode material for SIBs. The cycling performance of NPC at 1 A/g for 2000 cycles featured a stable reversible capacity of 122.3 mA h/g with an outstanding capacity retention of 99.1%. These excellent electrochemical properties can be attributed to the unique structure of NPC;it features hierarchical porosity with abundant carbon edge defects and large speci c surface areas. These results illuminate the potential application of jackfruit rags-derived porous carbon in SIBs.展开更多
Owing to safety issue and low energy density of liquid lithium-ion batteries(LIBs),all-solid-state lithium metal batteries(ASLMBs)with unique all-solid-state electrolytes(SEs)have attracted wide attentions.This arises...Owing to safety issue and low energy density of liquid lithium-ion batteries(LIBs),all-solid-state lithium metal batteries(ASLMBs)with unique all-solid-state electrolytes(SEs)have attracted wide attentions.This arises mainly from the advantages of the SEs in the suppression of lithium dendrite growth,long cycle life,and broad working temperature range,showing huge potential applications in electronic devices,electric vehicles,smart grids,and biomedical devices.However,SEs suffer from low lithiumion conductivity and low mechanical integrity,slowing down the development of practical ASLMBs.Nanostructure engineering is of great efficiency in tuning the structure and composition of the SEs with improved lithium-ion conductivity and mechanical integrity.Among various available technologies for nanostructure engineering,electrospinning is a promising technique because of its simple operation,cost-effectiveness,and efficient integration with different components.In this review,we will first give a simple description of the electrospinning process.Then,the use of electrospinning technique in the synthesis of various SEs is summarized,for example,organic nanofibrous matrix,organic/inorganic nanofibrous matrix,and inorganic nanofibrous matrix combined with other components.The current development of the advanced architectures of SEs through electrospinning technology is also presented to provide references and ideas for designing high-performance ASLMBs.Finally,an outlook and further challenges in the preparation of advanced SEs for ASLMBs through electrospinning engineering are given.展开更多
Potassium-ion hybrid capacitors(PIHCs)tactfully combining capacitor-type cathode with battery-type anode have recently attracted increasing attentions due to their advantages of decent energy density,high power densit...Potassium-ion hybrid capacitors(PIHCs)tactfully combining capacitor-type cathode with battery-type anode have recently attracted increasing attentions due to their advantages of decent energy density,high power density,and low cost;the mismatches of capacity and kinetics between capacitor-type cathode and battery-type anode in PIHCs yet hinder their overall performance output.Herein,based on prediction of density functional theory calculations,we find Se/N co-doped porous carbon is a promising candidate for K+storage and thus develop a simple and universal self-sacrifice template method to fabricate Se and N co-doped three-dimensional(3D)macroporous carbon(Se/N-3DMpC),which features favorable properties of connective hier-archical pores,expanded interlayer structure,and rich activity site for boosting pseudocapacitive activity and kinetics toward K^(+)storage anode and enhancing capacitance performance for the reversible anion adsorption/desorption cath-ode.As expected,the as-assembled PIHCs full cell with a working voltage as high as 4.0 V delivers a high energy density of 186 Wh kg^(−1) and a power output of 8100 W kg^(−1) as well as excellent long service life.The proof-of-concept PIHCs with excellent performance open a new avenue for the development and application of high-performance hybrid capacitors.展开更多
Electrolytic water splitting,as a promising route to hydrogen(H_(2))production,is still confronted with the sluggish anodic oxygen evolution reaction(OER)and its less value-added O2 production.Herein,we report a bifun...Electrolytic water splitting,as a promising route to hydrogen(H_(2))production,is still confronted with the sluggish anodic oxygen evolution reaction(OER)and its less value-added O2 production.Herein,we report a bifunctional electrode fabricated by in situ growth of Mn-doped CoSe_(2)nanonetworks on carbon fiber cloth(Mn-CoSe_(2)/CFC),which shows attractive electrocatalytic properties toward glycerol oxidation reaction(GOR)in alkali and hydrogen evolution reaction(HER)in acid.A flow alkali/acid hybrid electrolytic cell(fA/A-hEC)was then developed by coupling anodic GOR with cathodic HER with the Mn-CoSe_(2)/CFC bifunctional electrode.Such fA/A-hEC enables a rather low voltage of 0.54 V to achieve 10 mA cm^(-2),and maintain long-term electrolysis stability over 300-h operation at 100 mA cm^(-2)with Faraday efficiencies of over 99%for H_(2)and 90%for formate production.The designed bifunctional electrode in such innovative fA/A-hEC device provides insightful guidance for coupling energy-efficient hydrogen production with biomass upgradation.展开更多
Electrosynthesis has recently attracted intensive research attentions and holds great potential in implementing scalable green synthesis thanks to more and more readily accessible renewable electric energy.
Electrochemical energy devices serve as a vital link in the mutual conversion between chemical energy and electrical energy.This role positions them to be essential for achieving high-efficiency utilization and advanc...Electrochemical energy devices serve as a vital link in the mutual conversion between chemical energy and electrical energy.This role positions them to be essential for achieving high-efficiency utilization and advancement of renewable energy.Electrochemical reactions,including anodic and cathodic reactions,play a crucial role in facilitating the connection between two types of charge carriers:electrons circulating within the external circuit and ions transportation within the internal electrolyte,which ensures the completion of the circuit in electrochemical devices.While electrons are uniform,ions come in various types,we herein propose the concept of hybrid electrochemical energy technologies(h-EETs)characterized by the utilization of different ions as charge carriers of anodic and cathodic reactions.Accordingly,this review aims to explore the fundamentals of emerging hybrid electrochemical energy technologies and recent research advancements.We start with the introduction of the concept and foundational aspects of h-EETs,including the proposed definition,the historical background,operational principles,device configurations,and the underlying principles governing these configurations of the h-EETs.We then discuss how the integration of hybrid charge carriers influences the performance of associated h-EETs,to facilitate an insightful understanding on how ions carriers can be beneficial and effectively implemented into electrochemical energy devices.Furthermore,a special emphasis is placed on offering an overview of the research progress in emerging h-EETs over recent years,including hybrid battery capacitors that extend beyond traditional hybrid supercapacitors,as well as exploration into hybrid fuel cells and hybrid electrolytic synthesis.Finally,we highlight the major challenges and provide anticipatory insights into the future perspectives of developing high-performance h-EETs devices.展开更多
We report a relatively low-temperature molten salt strategy to prepare hollow structured N-doped noble carbon(h-NNC) with highly desirable features of ultra-large surface area(1957 m^2 g^(-1)) and high graphitization,...We report a relatively low-temperature molten salt strategy to prepare hollow structured N-doped noble carbon(h-NNC) with highly desirable features of ultra-large surface area(1957 m^2 g^(-1)) and high graphitization, endowing the h-NNC with high activity toward catalysis of oxygen reduction reaction in acidic medium. The h-NNC is applied as cathode catalyst of an asymmetrical-electrolyte Zn-air battery, which exhibits an open circuit voltage of 2.11 V, a power density up to 270 mW cm^(-2),and an energy density of 1279 W h kg^(-1), behaving advantages over the conventional Zn-air batteries.展开更多
Single-atom catalysts(SACs)have emerged as one of the most competitive catalysts toward a variety of important electrochemical reactions,thanks to their maximum atom economy,unique electronic and geometric structures....Single-atom catalysts(SACs)have emerged as one of the most competitive catalysts toward a variety of important electrochemical reactions,thanks to their maximum atom economy,unique electronic and geometric structures.However,the role of SACs supports on the catalytic performance does not receive enough research attentions.Here,we report an efficient route for synthesis of single atom Zn loading on the N-doped carbon nano-onions(ZnN/CNO).ZnN/CNO catalysts show an excellent high selectivity for CO_(2) electro-reduction to CO with a Faradaic efficiency of CO(FECO)up to 97%at -0.47 V(vs.reversible hydrogen electrode,RHE)and remarkable durability without activity decay.To our knowledge,ZnN/CNO is the best activity for the Zn based catalysts up to now,and superior to single atom Zn loading on the two-dimensional planar and porous structure of graphene substrate,although the graphene with larger surface area.The exact role of such carbon nano-onions(CNO)support is studied systematically by coupling characterizations and electrochemistry with density functional theory(DFT)calculations,which have attributed such good performance to the increased curvature.Such increased curvature modifies the surface charge,which then changes the adsorption energies of key intermediates,and improves the selectivity for CO generation accordingly.展开更多
Electroreduction of CO_(2) to target products with high activity and selectivity has techno-economic importance for renewable energy storage and CO_(2) utilization.Herein,we report a hierarchical CuS hollow polyhedron...Electroreduction of CO_(2) to target products with high activity and selectivity has techno-economic importance for renewable energy storage and CO_(2) utilization.Herein,we report a hierarchical CuS hollow polyhedron(CuS-HP)for electrocatalytic CO_(2) reduction(E-CO_(2)R)in neutral pH aqueous media.Under E-CO_(2)R conditions,CuS-HP undergoes structural reconstruction into sulfur-doped metallic Cu catalyst,which promotes formate production with Faradaic efficiency>90%in a wide potential range.展开更多
Sodium-tellurium(Na-Te)battery,thanks to high theoretical capacity and abundant sodium source,has been envisaged as one promising battery technology,its practical application yet faces daunting challenges regarding ho...Sodium-tellurium(Na-Te)battery,thanks to high theoretical capacity and abundant sodium source,has been envisaged as one promising battery technology,its practical application yet faces daunting challenges regarding how to mitigate the critical issues of uncontrollable dendrites growth at Na anode and polytellurides shuttling effect at Te cathode.We here report an elaborative design for fabrication of microsphere skeleton nanohybrids with three-dimensional(3D)hierarchical porous carbon loading CeO_(2)quantum dots(CeO_(2)-QDs/HPC),which feature highly favorable properties of sodiophilic and catalysis for hosting sodium and tellurium,respectively.The systematic investigations coupling with first-principle calculations demonstrate the CeO_(2)-QDs/HPC not only offers favorable structure and abundant electrocatalytic sites for facilitating interconversion between Te and NaxTe as a cathode host,but also can function as dendrite inhibitor anode host for reversible sodium electro-plating/deposition.Such Na-Te battery exhibits admiring electrochemical performance with an impressive specific capacity of 392 mAh g1,a long cycling stability over 1000 cycles,as well as remarkably high energy density of 192 Wh kg1 based on the total mass of anode and cathode.Such proof-of-concept bifunctional host design for active electrode materials can render a new insight and direction to the development of high-performance Na-Te batteries.展开更多
Amorphous catalysts,thanks to their uniquely coordinated unsaturated properties and abundance of defect sites,tend to possess higher activity and selectivity than their crystalline counterparts.In this work,we report ...Amorphous catalysts,thanks to their uniquely coordinated unsaturated properties and abundance of defect sites,tend to possess higher activity and selectivity than their crystalline counterparts.In this work,we report a facile and general solventcontrolled precipitation method to prepare hybrids of graphene oxide(GO)supporting amorphous metal hydroxide[A-M(OH)_(x)/GO,M=Cu,Co,and Mn],which provides us with tangible materials to study the structure–performance relationship of various amorphous oxides.The systematic investigation of A-Cu(OH)_(2)/GO by coupling ex situ/in situ characteristic techniques with electrochemical studies reveals that electrocatalytic activity and selectivity toward a two-electron oxygen reduction reaction(ORR)is highly dependent on the coordinated Cu catalytic sites and the disordered structure of A-Cu(OH)_(2).In situ X-ray absorption near-edge structure(XANES)and density functional theory(DFT)calculation verify that the degree of OH*poisoning(ΔG0 OH*)tuned by three-OH-coordinated Cu sites in amorphous structures plays a crucial role in selective catalysis of ORR for H_(2)O_(2) production.The optimized A-Cu(OH)_(2)/GO shows superior activity and high selectivity(~95%)toward H_(2)O_(2),as demonstrated by a zinc–air battery capable of on-site H_(2)O_(2) production with a rate as high as 3401.5 mmol h^(−1) g^(−1).展开更多
Efficient water splitting for H_(2) evolution over semiconductor photocatalysts is highly attractive in the field of clean energy.It is of great significance to construct heterojunctions,among which the direct Z-schem...Efficient water splitting for H_(2) evolution over semiconductor photocatalysts is highly attractive in the field of clean energy.It is of great significance to construct heterojunctions,among which the direct Z-scheme nanocomposite photocatalyst provides effective separation of photo-generated carriers to boost the photocatalytic performance.Herein,Z-scheme hydrated tungsten trioxide/ZnIn_(2)S_(4) is fabricated via an in-situ hydrothermal method where ZnIn_(2)S_(4) nanosheets are grown on WO_(3)·xH_(2)O.The close contact between WO_(3)·0.5H_(2)O and WO_(3)·0.33H_(2)O as well as ZnIn_(2)S_(4) improve the charge carrier separation and migration in the photocatalyst,where the strong reducing electrons in the conduction band of ZnIn_(2)S_(4) and the strong oxidizing holes in the valence band of WO_(3)·0.33H_(2)O are retained,leading to enhanced photocatalytic hydrogen production.The obtained WO_(3)·xH_(2)O/ZnIn_(2)S_(4) shows an excellent H_(2) production rate of 7200μmol g^(−1) h^(−1),which is 11 times higher than pure ZnIn_(2)S_(4).To the best of our knowledge,this value is higher than most of the WO_(3)-based noble metal-free semiconductor photocatalysts.The improved stability and activity are attributed to the formation of the Z-scheme heterojunction,which can markedly accelerate the interfacial charge separation for surface reaction.This work offers a promising strategy towards the design of an efficient Z-scheme photocatalyst to suppress electron–hole recombination and optimize redox potential.展开更多
Ammonia (NH3) is not only an essential chemical feedstock for the manufacture of nitrogen-rich fertilizers but also a promising carbofree energy carrier for storing H2 due to its high content of hydrogen (17.6% by mas...Ammonia (NH3) is not only an essential chemical feedstock for the manufacture of nitrogen-rich fertilizers but also a promising carbofree energy carrier for storing H2 due to its high content of hydrogen (17.6% by mass). At present, industrial NH3 is still dominantly produced by the traditional Haber-Bosch process, which reduces nitrogen (N2) to NH3 (N2+3H2←→2NH 3) at high temperatures (350-550 °C) and high pressures (150-350 atm)[1]. Such a process not only requires the raw materials of high-purity streams of nitrogen and hydrogen but also consumes tremendous energy;noting that the consumed hydrogen occupied approximately 50% of its global production that produced exclusively from transformations of fossil resources with the emission of greenhouse gas [1].展开更多
基金financially supported by the National key Research & Development Program of China (2022YFE0115900, 2021YFA1501500)the National Natural Science Foundation of China (Nos. 22225902, U22A20436, 22209185)+3 种基金the CAS-Commonwealth Scientific and Industrial Research Organization (CSIRO) Joint Research Projects (121835KYSB20200039)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy (Grant. YLUDNL Fund 2021011)Fujian Province Central Government Guides to Science and Technology Development Special Project (No. 2022L3024)Natural Science Foundation of Fujian Province, China (No. 2021J02020)。
文摘Sodium-based dual-ion batteries(SDIBs) have gained tremendous attention due to their virtues of high operating voltage and low cost, yet it remains a tough challenge for the development of ideal anode material of SDIBs featuring with high kinetics and long durability. Herein, we report the design and fabrication of N-doped carbon film-modified niobium sulfur–selenium(NbSSe/NC) nanosheets architecture, which holds favorable merits for Na^(+) storage of enlarged interlayer space, improved electrical conductivity, as well as enhanced reaction reversibility, endowing it with high capacity, high-rate capability and high cycling stability. The combined electrochemical studies with density functional theory calculation reveal that the enriched defects in such nanosheets architecture can benefit for facilitating charge transfer and Na+ adsorption to speed the electrochemical kinetics. The NbSSe/NC composites are studied as the anode of a full SDIBs by pairing the expanded graphite as cathode, which shows an impressively cyclic durability with negligible capacity attenuation over 1000 cycles at 0.5 A g^(-1), as well as an outstanding energy density of 230.6 Wh kg^(-1) based on the total mass of anode and cathode.
文摘The application of electrocatalysts for the oxygen reduction reaction(ORR) is vital in a variety of energy conversion technologies. Exploring low-cost ORR catalysts with high activity and long-term stability is highly desirable, although it still remains challenging. Herein, we report a facile and reliable route to convert ZIF-8 modified by Fe-phenanthroline into Fe-incorporated and N-doped carbon dodecahedron nanoarchitecture(Fe-NCDNA), in which carbon nanosheets are formed in situ as the building blocks with uniform Fe-N-C species decoration. Systematic electrochemical studies demonstrate that the as-synthesized Fe-NCDNA electrocatalyst possesses highly attractive catalytic features toward the ORR in terms of activity and durability in both alkaline and neutral media. The Zn-air battery with the optimal Fe-NCDNA catalyst as the cathode performs impressively, delivering a power density of 184 m W cm^–2 and a specific capacity of 801 m Ah g^–1;thus, it exhibits great competitive advantages over those of the Zn-air devices employing a Pt-based cathode electrocatalyst.
基金financially supported by National Natural Science Foundation of China (Nos. 21875253, 21703249)the 1000 Plan Professorship for Young Talents
文摘Renewable biomass-derived carbon materials have attracted increasing research attention as promising electrode materials for electrochemical energy storage devices, such as sodium-ion batteries (SIBs), due to their outstanding electrical conductivity, hierarchical porous structure, intrinsic heteroatom doping, and environmental friendliness. Here, we investigate the potential of hierarchical N-doped porous carbon (NPC) derived from jackfruit rags through a facile pyrolysis as an anode material for SIBs. The cycling performance of NPC at 1 A/g for 2000 cycles featured a stable reversible capacity of 122.3 mA h/g with an outstanding capacity retention of 99.1%. These excellent electrochemical properties can be attributed to the unique structure of NPC;it features hierarchical porosity with abundant carbon edge defects and large speci c surface areas. These results illuminate the potential application of jackfruit rags-derived porous carbon in SIBs.
基金financially supported by the National Key Research and Development Project of China for Demonstration of Integrated Utilization of Solid Waste in Distinctive Convergent Areas of Southeast Light Industry Building Materials(2019YFC1904500)the National Natural Science Foundation of China(Grant No.81770222)+4 种基金the Social Development Industry University Research Cooperation Project from the Department of Science and Technology in Fujian(2018Y4002)support by the Award Program for Fujian Minjiang Scholar Professorshipsupport from the Australian Research Grants Council(DP130104648)support from the NSERC Discovery Grant(NSERC RGPIN-2020-04463)McGill Start-Up Grant。
文摘Owing to safety issue and low energy density of liquid lithium-ion batteries(LIBs),all-solid-state lithium metal batteries(ASLMBs)with unique all-solid-state electrolytes(SEs)have attracted wide attentions.This arises mainly from the advantages of the SEs in the suppression of lithium dendrite growth,long cycle life,and broad working temperature range,showing huge potential applications in electronic devices,electric vehicles,smart grids,and biomedical devices.However,SEs suffer from low lithiumion conductivity and low mechanical integrity,slowing down the development of practical ASLMBs.Nanostructure engineering is of great efficiency in tuning the structure and composition of the SEs with improved lithium-ion conductivity and mechanical integrity.Among various available technologies for nanostructure engineering,electrospinning is a promising technique because of its simple operation,cost-effectiveness,and efficient integration with different components.In this review,we will first give a simple description of the electrospinning process.Then,the use of electrospinning technique in the synthesis of various SEs is summarized,for example,organic nanofibrous matrix,organic/inorganic nanofibrous matrix,and inorganic nanofibrous matrix combined with other components.The current development of the advanced architectures of SEs through electrospinning technology is also presented to provide references and ideas for designing high-performance ASLMBs.Finally,an outlook and further challenges in the preparation of advanced SEs for ASLMBs through electrospinning engineering are given.
基金This work was supported by the National Natural Science Foundation of China(Project No.21875253)CAS-Commonwealth Scientific and Industrial Research Organization(CSIRO)Joint Research Projects(121835KYSB20200039)Scientific Research and Equipment Development Project of CAS(YJKYYQ20190007).
文摘Potassium-ion hybrid capacitors(PIHCs)tactfully combining capacitor-type cathode with battery-type anode have recently attracted increasing attentions due to their advantages of decent energy density,high power density,and low cost;the mismatches of capacity and kinetics between capacitor-type cathode and battery-type anode in PIHCs yet hinder their overall performance output.Herein,based on prediction of density functional theory calculations,we find Se/N co-doped porous carbon is a promising candidate for K+storage and thus develop a simple and universal self-sacrifice template method to fabricate Se and N co-doped three-dimensional(3D)macroporous carbon(Se/N-3DMpC),which features favorable properties of connective hier-archical pores,expanded interlayer structure,and rich activity site for boosting pseudocapacitive activity and kinetics toward K^(+)storage anode and enhancing capacitance performance for the reversible anion adsorption/desorption cath-ode.As expected,the as-assembled PIHCs full cell with a working voltage as high as 4.0 V delivers a high energy density of 186 Wh kg^(−1) and a power output of 8100 W kg^(−1) as well as excellent long service life.The proof-of-concept PIHCs with excellent performance open a new avenue for the development and application of high-performance hybrid capacitors.
基金supported by the National Natural Science Foundation of China(Project No.21875253)the CAS Commonwealth Scientific and Industrial Research Organization(CSIRO)Joint Research Projects(121835KYSB20200039)+3 种基金the Scientific Research and Equipment Development Project of CAS(YJKYYQ20190007)Fujian Natural Science Foundation(2021J01210293)the Fujian Science and Technology Pilot Project(Project No.2020H0039)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(Grant.YLUDNL Fund 2021011)。
文摘Electrolytic water splitting,as a promising route to hydrogen(H_(2))production,is still confronted with the sluggish anodic oxygen evolution reaction(OER)and its less value-added O2 production.Herein,we report a bifunctional electrode fabricated by in situ growth of Mn-doped CoSe_(2)nanonetworks on carbon fiber cloth(Mn-CoSe_(2)/CFC),which shows attractive electrocatalytic properties toward glycerol oxidation reaction(GOR)in alkali and hydrogen evolution reaction(HER)in acid.A flow alkali/acid hybrid electrolytic cell(fA/A-hEC)was then developed by coupling anodic GOR with cathodic HER with the Mn-CoSe_(2)/CFC bifunctional electrode.Such fA/A-hEC enables a rather low voltage of 0.54 V to achieve 10 mA cm^(-2),and maintain long-term electrolysis stability over 300-h operation at 100 mA cm^(-2)with Faraday efficiencies of over 99%for H_(2)and 90%for formate production.The designed bifunctional electrode in such innovative fA/A-hEC device provides insightful guidance for coupling energy-efficient hydrogen production with biomass upgradation.
基金financially supported by the National Natural Science Foundation of China(Project No.21875253,No.51903235)。
文摘Electrosynthesis has recently attracted intensive research attentions and holds great potential in implementing scalable green synthesis thanks to more and more readily accessible renewable electric energy.
基金financially supported by the National Natural Science Foundation of China (22209183,22225902,and U22A20436)the National Key Research&Development Program of China (2022YFE0115900 and 2021YFA1501500)+2 种基金the CAS-Commonwealth Scientific and Industrial Research Organization (CSIRO)Joint Research Projects (121835KYSB20200039)Advanced Talents of Jiangsu University (23JDG027)Fujian Natural Science Foundation (2021J01210293)。
基金supported by the National Natural Science Foundation of China(22109164,22225902,and U22A20436)the National Key Research&Development Program of China(2022YFE0115900,2021YFA1501500)+2 种基金the CASCommonwealth Scientific and Industrial Research Organization(CSIRO)Joint Research Projects(121835KYSB20200039)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2021011)Fujian Province Central Government Guides to Science and Technology Development Special Project(2022L3024)。
文摘Electrochemical energy devices serve as a vital link in the mutual conversion between chemical energy and electrical energy.This role positions them to be essential for achieving high-efficiency utilization and advancement of renewable energy.Electrochemical reactions,including anodic and cathodic reactions,play a crucial role in facilitating the connection between two types of charge carriers:electrons circulating within the external circuit and ions transportation within the internal electrolyte,which ensures the completion of the circuit in electrochemical devices.While electrons are uniform,ions come in various types,we herein propose the concept of hybrid electrochemical energy technologies(h-EETs)characterized by the utilization of different ions as charge carriers of anodic and cathodic reactions.Accordingly,this review aims to explore the fundamentals of emerging hybrid electrochemical energy technologies and recent research advancements.We start with the introduction of the concept and foundational aspects of h-EETs,including the proposed definition,the historical background,operational principles,device configurations,and the underlying principles governing these configurations of the h-EETs.We then discuss how the integration of hybrid charge carriers influences the performance of associated h-EETs,to facilitate an insightful understanding on how ions carriers can be beneficial and effectively implemented into electrochemical energy devices.Furthermore,a special emphasis is placed on offering an overview of the research progress in emerging h-EETs over recent years,including hybrid battery capacitors that extend beyond traditional hybrid supercapacitors,as well as exploration into hybrid fuel cells and hybrid electrolytic synthesis.Finally,we highlight the major challenges and provide anticipatory insights into the future perspectives of developing high-performance h-EETs devices.
基金supported by the 1000 Plan Professorship for Young TalentsHundred Talents Program of Fujian Province+1 种基金the Fujian Science and Technology Key Project (2016H0043)the National Natural Science Foundation of China (21703249, 21701175)
文摘We report a relatively low-temperature molten salt strategy to prepare hollow structured N-doped noble carbon(h-NNC) with highly desirable features of ultra-large surface area(1957 m^2 g^(-1)) and high graphitization, endowing the h-NNC with high activity toward catalysis of oxygen reduction reaction in acidic medium. The h-NNC is applied as cathode catalyst of an asymmetrical-electrolyte Zn-air battery, which exhibits an open circuit voltage of 2.11 V, a power density up to 270 mW cm^(-2),and an energy density of 1279 W h kg^(-1), behaving advantages over the conventional Zn-air batteries.
基金This work was supported by the National Key R&D Program of China(2020YFA0710404)the Beijing Natural Science Foundation(2182077)the National Natural Science Foundation of China(21477136,51972281,and 21703250).
文摘Single-atom catalysts(SACs)have emerged as one of the most competitive catalysts toward a variety of important electrochemical reactions,thanks to their maximum atom economy,unique electronic and geometric structures.However,the role of SACs supports on the catalytic performance does not receive enough research attentions.Here,we report an efficient route for synthesis of single atom Zn loading on the N-doped carbon nano-onions(ZnN/CNO).ZnN/CNO catalysts show an excellent high selectivity for CO_(2) electro-reduction to CO with a Faradaic efficiency of CO(FECO)up to 97%at -0.47 V(vs.reversible hydrogen electrode,RHE)and remarkable durability without activity decay.To our knowledge,ZnN/CNO is the best activity for the Zn based catalysts up to now,and superior to single atom Zn loading on the two-dimensional planar and porous structure of graphene substrate,although the graphene with larger surface area.The exact role of such carbon nano-onions(CNO)support is studied systematically by coupling characterizations and electrochemistry with density functional theory(DFT)calculations,which have attributed such good performance to the increased curvature.Such increased curvature modifies the surface charge,which then changes the adsorption energies of key intermediates,and improves the selectivity for CO generation accordingly.
基金supported by the National Natural Science Foundation of China(nos.22002168,21975259,and 21673241)the Innovation Academy for Green Manufacture of the Chinese Academy of Sciences(no.IAGM2020C17)the Strategic Priority Research Program of the Chinese Academy of Sciences(no.XDB20000000).
文摘Electroreduction of CO_(2) to target products with high activity and selectivity has techno-economic importance for renewable energy storage and CO_(2) utilization.Herein,we report a hierarchical CuS hollow polyhedron(CuS-HP)for electrocatalytic CO_(2) reduction(E-CO_(2)R)in neutral pH aqueous media.Under E-CO_(2)R conditions,CuS-HP undergoes structural reconstruction into sulfur-doped metallic Cu catalyst,which promotes formate production with Faradaic efficiency>90%in a wide potential range.
基金National Natural Science Foundation of China,Grant/Award Numbers:21875253,51872048,52073061Natural Science Foundation of Fujian Province,Grant/Award Numbers:2021J01430167,2021J02020+2 种基金CAS-Commonwealth Scientific and Industrial Research Organization(CSIRO)Joint Research Projects,Grant/Award Number:121835KYSB20200039Scientific Research and Equipment Development Project of CAS,Grant/Award Number:YJKYYQ20190007Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy,Grant/Award Number:YLU-DNL Fund 2021011。
文摘Sodium-tellurium(Na-Te)battery,thanks to high theoretical capacity and abundant sodium source,has been envisaged as one promising battery technology,its practical application yet faces daunting challenges regarding how to mitigate the critical issues of uncontrollable dendrites growth at Na anode and polytellurides shuttling effect at Te cathode.We here report an elaborative design for fabrication of microsphere skeleton nanohybrids with three-dimensional(3D)hierarchical porous carbon loading CeO_(2)quantum dots(CeO_(2)-QDs/HPC),which feature highly favorable properties of sodiophilic and catalysis for hosting sodium and tellurium,respectively.The systematic investigations coupling with first-principle calculations demonstrate the CeO_(2)-QDs/HPC not only offers favorable structure and abundant electrocatalytic sites for facilitating interconversion between Te and NaxTe as a cathode host,but also can function as dendrite inhibitor anode host for reversible sodium electro-plating/deposition.Such Na-Te battery exhibits admiring electrochemical performance with an impressive specific capacity of 392 mAh g1,a long cycling stability over 1000 cycles,as well as remarkably high energy density of 192 Wh kg1 based on the total mass of anode and cathode.Such proof-of-concept bifunctional host design for active electrode materials can render a new insight and direction to the development of high-performance Na-Te batteries.
基金the Natural Science Foundation of Fujian Province,China(grant no.2020J05079)the National Natural Science Foundation of China(grant nos.21875253,21701175,and 21703248)+1 种基金CAS-Commonwealth Scientific and Industrial Research Organization(CSIRO)Joint Research Projects(no.121835KYSB20200039)the Scientific Research and Equipment Development Project of CAS(no.YJKYYQ20190007).
文摘Amorphous catalysts,thanks to their uniquely coordinated unsaturated properties and abundance of defect sites,tend to possess higher activity and selectivity than their crystalline counterparts.In this work,we report a facile and general solventcontrolled precipitation method to prepare hybrids of graphene oxide(GO)supporting amorphous metal hydroxide[A-M(OH)_(x)/GO,M=Cu,Co,and Mn],which provides us with tangible materials to study the structure–performance relationship of various amorphous oxides.The systematic investigation of A-Cu(OH)_(2)/GO by coupling ex situ/in situ characteristic techniques with electrochemical studies reveals that electrocatalytic activity and selectivity toward a two-electron oxygen reduction reaction(ORR)is highly dependent on the coordinated Cu catalytic sites and the disordered structure of A-Cu(OH)_(2).In situ X-ray absorption near-edge structure(XANES)and density functional theory(DFT)calculation verify that the degree of OH*poisoning(ΔG0 OH*)tuned by three-OH-coordinated Cu sites in amorphous structures plays a crucial role in selective catalysis of ORR for H_(2)O_(2) production.The optimized A-Cu(OH)_(2)/GO shows superior activity and high selectivity(~95%)toward H_(2)O_(2),as demonstrated by a zinc–air battery capable of on-site H_(2)O_(2) production with a rate as high as 3401.5 mmol h^(−1) g^(−1).
基金supported by Research Grants Council of the Hong Kong Special Administrative Region,China(PolyU152140/19E).
文摘Efficient water splitting for H_(2) evolution over semiconductor photocatalysts is highly attractive in the field of clean energy.It is of great significance to construct heterojunctions,among which the direct Z-scheme nanocomposite photocatalyst provides effective separation of photo-generated carriers to boost the photocatalytic performance.Herein,Z-scheme hydrated tungsten trioxide/ZnIn_(2)S_(4) is fabricated via an in-situ hydrothermal method where ZnIn_(2)S_(4) nanosheets are grown on WO_(3)·xH_(2)O.The close contact between WO_(3)·0.5H_(2)O and WO_(3)·0.33H_(2)O as well as ZnIn_(2)S_(4) improve the charge carrier separation and migration in the photocatalyst,where the strong reducing electrons in the conduction band of ZnIn_(2)S_(4) and the strong oxidizing holes in the valence band of WO_(3)·0.33H_(2)O are retained,leading to enhanced photocatalytic hydrogen production.The obtained WO_(3)·xH_(2)O/ZnIn_(2)S_(4) shows an excellent H_(2) production rate of 7200μmol g^(−1) h^(−1),which is 11 times higher than pure ZnIn_(2)S_(4).To the best of our knowledge,this value is higher than most of the WO_(3)-based noble metal-free semiconductor photocatalysts.The improved stability and activity are attributed to the formation of the Z-scheme heterojunction,which can markedly accelerate the interfacial charge separation for surface reaction.This work offers a promising strategy towards the design of an efficient Z-scheme photocatalyst to suppress electron–hole recombination and optimize redox potential.
基金This research was supported by the National Natural Science Foundation of China （Nos. 21635002, U1505221, and 21705023）, the Program for Changjiang Scholars and Innovative Research Team in University （No. IRT15R11）, and the Independent Research Project of State Key Laboratory of Photocatalysis on Energy and Environment （No. 2014B02）.
文摘Ammonia (NH3) is not only an essential chemical feedstock for the manufacture of nitrogen-rich fertilizers but also a promising carbofree energy carrier for storing H2 due to its high content of hydrogen (17.6% by mass). At present, industrial NH3 is still dominantly produced by the traditional Haber-Bosch process, which reduces nitrogen (N2) to NH3 (N2+3H2←→2NH 3) at high temperatures (350-550 °C) and high pressures (150-350 atm)[1]. Such a process not only requires the raw materials of high-purity streams of nitrogen and hydrogen but also consumes tremendous energy;noting that the consumed hydrogen occupied approximately 50% of its global production that produced exclusively from transformations of fossil resources with the emission of greenhouse gas [1].
