The retarded kinetics of oxygen evolution on electrodes is a bottleneck for electrochemical energy conversion and storage systems.NiFe-based electrocatalysts provide a cost-effective choice to confront this challenge....The retarded kinetics of oxygen evolution on electrodes is a bottleneck for electrochemical energy conversion and storage systems.NiFe-based electrocatalysts provide a cost-effective choice to confront this challenge.However,there is a lack of facile techniques for depositing compact catalytic films of high coverage and possessing a state-of-the-art performance,which is especially desired in photoelectrochemical(PEC)systems.Herein,we demonstrate a spray pyrolysis(SP)route to address this issue,featuring the kinetic selective preparation towards the desired catalytic-active material.Differing from reported SP protocols which only produce inactive oxides,this approach directly generates a unique composite film consisting of NiFe layered oxyhydroxides and amorphous oxides,exhibiting an overpotential as small as 255 mV(10 mA cm^(−2))and a turnover frequency of∼0.4 s^(−1)per metal atom.By using such a facile protocol,the surface rate-limiting issue of BiVO_(4)photoanodes can be effectively resolved,resulting in a charge injection efficiency of over 90%.Considering this deposition directly start from simple nitrates but only takes several seconds to complete,we believe it can be developed as a widely applicable and welcomed functionalization technique for diverse electrochemical devices.展开更多
The modern demand for an alternative material maintaining excellent catalytic activities with better stability and low toxicity for application in the field of energy remains a hotspot for the scientific community.In ...The modern demand for an alternative material maintaining excellent catalytic activities with better stability and low toxicity for application in the field of energy remains a hotspot for the scientific community.In the current work,we report a simple conjugation of BiOX with manganese because of their excellent electrical and optical properties.展开更多
Seawater splitting is a prospective approach to yield renewable and sustainable hydrogen energy.Complex preparation processes and poor repeatability are currently considered to be an insuperable impediment to the prom...Seawater splitting is a prospective approach to yield renewable and sustainable hydrogen energy.Complex preparation processes and poor repeatability are currently considered to be an insuperable impediment to the promotion of the large-scale production and application of electrocatalysts.Avoiding the use of intricate instruments,corrosion engineering is an intriguing strategy to reduce the cost and presents considerable potential for electrodes with catalytic performance.An anode comprising quinary AlCoCrFeNi layered double hydroxides uniformly decorated on an AlCoCrFeNi high-entropy alloy is proposed in this paper via a one-step corrosion engineering method,which directly serves as a remarkably active catalyst for boosting the oxygen evolution reaction(OER)in alkaline seawater.Notably,the best-performing catalyst exhibited oxygen evolution reaction activity with overpotential values of 272.3 and 332 mV to achieve the current densities of 10 and100 mA·cm^(-2),respectively.The failure mechanism of the obtained catalyst was identified for advancing the development of multicomponent catalysts.展开更多
Amorphous hydroxide on a foamed nickel substrate was fabricated by a simple and efficient electrospinning method for the first time.In untreated alkaline medium,amorphous cobalt(Co)-iron(Fe)hydroxide showed oxygen-evo...Amorphous hydroxide on a foamed nickel substrate was fabricated by a simple and efficient electrospinning method for the first time.In untreated alkaline medium,amorphous cobalt(Co)-iron(Fe)hydroxide showed oxygen-evolution advantages over the typical reference catalyst(RuO_(2)).When tested with a three-electrode system in 1 M KOH,the obtained amorphous PVP/CoFe_(1.3)nanofibers possessed remarkable catalytic activity and stability for the oxygen evolution reaction(OER)with a low overpotential of 0.267 V at 100 mA cm^(-2)and a low Tafel slope of 47.43 mV dec^(-1).The amorphous CoFe microfibers were synthesized by electrospinning,and stable CoFe hydroxides can be further formed in the alkaline environment.The synergistic effect between two different amorphous CoFe-based hydroxides contributed to excellent electrocatalytic activity.Therefore,the design of amorphous CoFe hydroxide enabled the development of a high-efficiency OER catalyst and opens possibilities for the large-scale and environmentally friendly production of water splitting.展开更多
Oxygen evolution reaction（OER） is one of the most important reactions in the energy storage devices such as metal–air batteries and unitized regenerative fuel cells（URFCs）. However, the kinetically sluggishness o...Oxygen evolution reaction（OER） is one of the most important reactions in the energy storage devices such as metal–air batteries and unitized regenerative fuel cells（URFCs）. However, the kinetically sluggishness of OER and the high prices as well as the scarcity of the most active precious metal electrocatalysts are the major bottleneck in these devices. Developing low-cost non-precious metal catalysts with high activity and stability for OER is highly desirable. A facile, in situ template method combining the dodecyl benzene sulfuric acid sodium（SDBS） assisted hydrothermal process with subsequent high-temperature treatment was developed to prepare porous Co3O4 with improved surface area and hierarchical porous structure as precious catalysts alternative for oxygen evolution reaction（OER）. Due to the unique structure, the as-prepared catalyst shows higher electrocatalytic activity than Co3O4 prepared by traditional thermal-decomposition method（noted as Co3O4-T） and commercial IrO2 catalyst for OER in 0.1M KOH aqueous solution. Moreover, it displays improved stability than Co3O4-T. The results demonstrate a highly efficient, scalable, and low cost method for developing highly active and stable OER electrocatalysts in alkaline solutions.展开更多
It is highly attractive to develop high-performance non-noble-metal electrocatalysts for water oxidation in alkaline media.In this communication,we report the hydrothermal growth of a Co-MOF nanosheet array on Ni foam...It is highly attractive to develop high-performance non-noble-metal electrocatalysts for water oxidation in alkaline media.In this communication,we report the hydrothermal growth of a Co-MOF nanosheet array on Ni foam(Co-MOF/NF)as a 3D oxygen evolution reaction catalyst in alkaline media.The Co-MOF/NF demonstrates superior activity and needs an overpotential of only 311 mV to drive a geometrical catalytic current density of 50 mA cm^(-2)in 1.0 M KOH.展开更多
The structural and compositional modulation of inexpensive hydroxides is not only important,but also an ongoing challenge for the preparation of efficient oxygen evolution reaction(OER)electrocatalysts.Herein,a three-...The structural and compositional modulation of inexpensive hydroxides is not only important,but also an ongoing challenge for the preparation of efficient oxygen evolution reaction(OER)electrocatalysts.Herein,a three-dimensional(3D)structural catalyst(Co-CAT/NiFe-LDH/CNFs)is successfully synthesized by the in situ growth of a conductive metal–organic framework on NiFe layered double hydroxide nanosheets.Density functional theory(DFT)calculations demonstrated that the sluggish kinetics of the OER can be improved by increasing the conductivity and changing the hydrophilicity of the catalyst.Accordingly,the synergistic effect between Co-CAT and NiFe LDH leads to a superior catalytic performance compared to that of Pt/C.In addition,the as-assembled Zn–air battery exhibits excellent stability and a high power density of 327.09 mW cm^(−2) for 56 h and 112.04 mW cm^(−2) for 11.5 h in both liquid and solid electrolytes,respectively.展开更多
The lack of low-cost and efficient oxygen evolution reaction(OER)catalysts in acid media has significantly limited the development of proton exchange membrane water electrolysis,which can perfectly integrate with inte...The lack of low-cost and efficient oxygen evolution reaction(OER)catalysts in acid media has significantly limited the development of proton exchange membrane water electrolysis,which can perfectly integrate with intermittent renewable energy.Recently,iridium and non-noble metal mixed oxides have been identified as promising candidates for the OER in acid media.Herein,we report a novel double mixed metal oxide BaIrO_(2.937)/La_(3)IrO_(7) with a surface of IrOx formed by Ba and La leaching as an efficient electrocatalyst for boosting the sluggish OER.In 0.1 M HClO4,a low overpotential of 290 mV is required for BaIrO_(2.937)/La_(3)IrO_(7) to achieve the benchmark of 10 mA cm^(-2),comparable to commercial IrO_(2) and most reported acidic OER electrocatalysts.Moreover,a smaller Tafel slope of BaIrO_(2.937)/La_(3)IrO_(7) signifies fast reaction kinetics.Significantly important is that the iridium based mass activity was 561.6 A g_(Ir)^(-1) at 1.63 V vs.a reversible hydrogen electrode,which is 3.9 times as high as that of commercial IrO_(2).This work highlights the smart design of double mixed metal oxides with surface reconstruction as highly active and low cost electrocatalysts for the OER in acidic media.展开更多
Reducing the Ir loading while preserving catalytic performance and mechanical robustness in anodic catalyst layers remains a critical challenge for the large-scale implementation of proton exchange membrane water elec...Reducing the Ir loading while preserving catalytic performance and mechanical robustness in anodic catalyst layers remains a critical challenge for the large-scale implementation of proton exchange membrane water electrolysis(PEMWE).Herein,we present a structural engineering strategy involving neodymium-doped Ir/IrO_(2)(Nd-Ir/IrO_(2))hollow nanospheres with precisely adjustable shell thickness and cavity dimensions.The optimized catalyst demonstrates excellent oxygen evolution reaction(OER)performance in acidic media,achieving a remarkably low overpotential of 259 mV at a benchmark current density of 10 mA cm^(-2) while exhibiting substantially enhanced durability compared to commercial IrO_(2) and Ir/IrO_(2) counterparts.Notably,the Nd-Ir/IrO_(2) catalyst delivers a mass activity of 541.6 A gIr^(-1) at 1.50 V vs RHE,representing a 74.5-fold enhancement over conventional IrO_(2).Through comprehensive electrochemical analysis and advanced characterization techniques reveal that,the hierarchical hollow architecture simultaneously addresses multiple critical requirements:(i)abundant exposed active sites enabled by an enhanced electrochemical surface area,(ii)optimized mass transport pathways through engineered porosity,and(iii)preserved structural integrity via a continuous conductive framework,collectively enabling significant Ir loading reduction without compromising catalytic layer performance.Fundamental mechanistic investigations further disclose that Nd doping induces critical interfacial Nd-O-Ir configurations that stabilize lattice oxygen,together with intensified electron effect among mixed valent Ir that inhibits the overoxidation of Ir active sites during the OER process,synergistically ensuring enhanced catalytic durability.Our work establishes a dual-modulation paradigm integrating nanoscale architectural engineering with atomic-level heteroatom doping,providing a viable pathway toward high-performance PEMWE systems with drastically reduced noble metal requirements.展开更多
The tailor-made oxygen evolution catalysts(OECs)paired with photoanodes offer a path to promote water oxidation kinetics;however,the unsatisfied interface between OECs and photoanode sets a barrier for efficient charg...The tailor-made oxygen evolution catalysts(OECs)paired with photoanodes offer a path to promote water oxidation kinetics;however,the unsatisfied interface between OECs and photoanode sets a barrier for efficient charge transfer.Herein,a graphene oxide(GO)layer to promote the charge transfer from BiVO_(4)(BVO)to NiOOH OEC is reported.It is found that GO layer inserted between BVO and NiOOH can not only serve as hole extraction layer due to its hole storage capability,but also improve the stability.Finally,the rationally designed NiOOH/GO/BVO photoanode achieves a photocurrent density of 3.81 mA·cm^(-2)at 1.23 V(vs.reversible hydrogen electrode(RHE)),which is 3.85 times as high as that of bare BVO.This work opens up low-cost auxiliary materials for enhancing photoelectrochemical water splitting.展开更多
基金financially supported by the National Natural Science Foundation of China(NSFC,21805298,21905288,51904288)the Zhejiang Provincial Natural Science Foundation(Z21B030017)+2 种基金the K.C.Wong Education Foundation(GJTD-201913)the Ningbo major special projects of the Plan‘‘Science and Technology Innovation 2025”(2018B10056,2019B10046)the Ningbo 3315 Program。
文摘The retarded kinetics of oxygen evolution on electrodes is a bottleneck for electrochemical energy conversion and storage systems.NiFe-based electrocatalysts provide a cost-effective choice to confront this challenge.However,there is a lack of facile techniques for depositing compact catalytic films of high coverage and possessing a state-of-the-art performance,which is especially desired in photoelectrochemical(PEC)systems.Herein,we demonstrate a spray pyrolysis(SP)route to address this issue,featuring the kinetic selective preparation towards the desired catalytic-active material.Differing from reported SP protocols which only produce inactive oxides,this approach directly generates a unique composite film consisting of NiFe layered oxyhydroxides and amorphous oxides,exhibiting an overpotential as small as 255 mV(10 mA cm^(−2))and a turnover frequency of∼0.4 s^(−1)per metal atom.By using such a facile protocol,the surface rate-limiting issue of BiVO_(4)photoanodes can be effectively resolved,resulting in a charge injection efficiency of over 90%.Considering this deposition directly start from simple nitrates but only takes several seconds to complete,we believe it can be developed as a widely applicable and welcomed functionalization technique for diverse electrochemical devices.
基金supported by the National Research Foundation of Korea(NRF)grant which was funded by the Korea Government(MSIP)(No.2020R1G1A1102394).
文摘The modern demand for an alternative material maintaining excellent catalytic activities with better stability and low toxicity for application in the field of energy remains a hotspot for the scientific community.In the current work,we report a simple conjugation of BiOX with manganese because of their excellent electrical and optical properties.
基金supported by the National Natural Science Foundation of China (No.51901018)the Young Elite Scientists Sponsorship Program by the China Association for Science and Technology (YESS,2019QNRC001)+1 种基金the Natural Science Foundation of Beijing Municipality (No.2212037)the National Science and Technology Resources Investigation Program of China (No.2019FY 101400)。
文摘Seawater splitting is a prospective approach to yield renewable and sustainable hydrogen energy.Complex preparation processes and poor repeatability are currently considered to be an insuperable impediment to the promotion of the large-scale production and application of electrocatalysts.Avoiding the use of intricate instruments,corrosion engineering is an intriguing strategy to reduce the cost and presents considerable potential for electrodes with catalytic performance.An anode comprising quinary AlCoCrFeNi layered double hydroxides uniformly decorated on an AlCoCrFeNi high-entropy alloy is proposed in this paper via a one-step corrosion engineering method,which directly serves as a remarkably active catalyst for boosting the oxygen evolution reaction(OER)in alkaline seawater.Notably,the best-performing catalyst exhibited oxygen evolution reaction activity with overpotential values of 272.3 and 332 mV to achieve the current densities of 10 and100 mA·cm^(-2),respectively.The failure mechanism of the obtained catalyst was identified for advancing the development of multicomponent catalysts.
基金National Natural Science Foundation of China(21473013,51203008,21771021,and 21822501)Beijing Nova Program(xx2018115)+1 种基金Fundamental Research Funds for the Central UniversitiesAnalytical and Measurements Fund of Beijing Normal University。
文摘Amorphous hydroxide on a foamed nickel substrate was fabricated by a simple and efficient electrospinning method for the first time.In untreated alkaline medium,amorphous cobalt(Co)-iron(Fe)hydroxide showed oxygen-evolution advantages over the typical reference catalyst(RuO_(2)).When tested with a three-electrode system in 1 M KOH,the obtained amorphous PVP/CoFe_(1.3)nanofibers possessed remarkable catalytic activity and stability for the oxygen evolution reaction(OER)with a low overpotential of 0.267 V at 100 mA cm^(-2)and a low Tafel slope of 47.43 mV dec^(-1).The amorphous CoFe microfibers were synthesized by electrospinning,and stable CoFe hydroxides can be further formed in the alkaline environment.The synergistic effect between two different amorphous CoFe-based hydroxides contributed to excellent electrocatalytic activity.Therefore,the design of amorphous CoFe hydroxide enabled the development of a high-efficiency OER catalyst and opens possibilities for the large-scale and environmentally friendly production of water splitting.
基金supported by the Youth Innovation Promotion Association(no.2015147)CAS and National Program on Key Basic Research Project(973 Program,2012CB215500)+1 种基金the Outstanding Youngest Scientist FoundationChinese Academy of Sciences(CAS)
文摘Oxygen evolution reaction（OER） is one of the most important reactions in the energy storage devices such as metal–air batteries and unitized regenerative fuel cells（URFCs）. However, the kinetically sluggishness of OER and the high prices as well as the scarcity of the most active precious metal electrocatalysts are the major bottleneck in these devices. Developing low-cost non-precious metal catalysts with high activity and stability for OER is highly desirable. A facile, in situ template method combining the dodecyl benzene sulfuric acid sodium（SDBS） assisted hydrothermal process with subsequent high-temperature treatment was developed to prepare porous Co3O4 with improved surface area and hierarchical porous structure as precious catalysts alternative for oxygen evolution reaction（OER）. Due to the unique structure, the as-prepared catalyst shows higher electrocatalytic activity than Co3O4 prepared by traditional thermal-decomposition method（noted as Co3O4-T） and commercial IrO2 catalyst for OER in 0.1M KOH aqueous solution. Moreover, it displays improved stability than Co3O4-T. The results demonstrate a highly efficient, scalable, and low cost method for developing highly active and stable OER electrocatalysts in alkaline solutions.
基金supported by the National Natural Science Foundation of China(No.21775089,21375076)the Key Research and Development Program of Shandong Province(2015GSF121031)the Natural Science Foundation Projects of Shandong Province(No.ZR2017JL010,ZR2017QB008,ZR2017LEE006).
文摘It is highly attractive to develop high-performance non-noble-metal electrocatalysts for water oxidation in alkaline media.In this communication,we report the hydrothermal growth of a Co-MOF nanosheet array on Ni foam(Co-MOF/NF)as a 3D oxygen evolution reaction catalyst in alkaline media.The Co-MOF/NF demonstrates superior activity and needs an overpotential of only 311 mV to drive a geometrical catalytic current density of 50 mA cm^(-2)in 1.0 M KOH.
基金support from the following sources:the National Natural Science Foundation of China(NSFC)(Grants 51772073,51762013)the Key Project of Hebei Natural Science Foundation(E2020201030)+2 种基金the Second Batch of Young Talent of Hebei Province(No.70280016160250,No.70280011808)the Key Fund in Hebei Province Department of Education China(ZD2021014)the China Postdoctoral Science Foundation(No.2021M701718).
文摘The structural and compositional modulation of inexpensive hydroxides is not only important,but also an ongoing challenge for the preparation of efficient oxygen evolution reaction(OER)electrocatalysts.Herein,a three-dimensional(3D)structural catalyst(Co-CAT/NiFe-LDH/CNFs)is successfully synthesized by the in situ growth of a conductive metal–organic framework on NiFe layered double hydroxide nanosheets.Density functional theory(DFT)calculations demonstrated that the sluggish kinetics of the OER can be improved by increasing the conductivity and changing the hydrophilicity of the catalyst.Accordingly,the synergistic effect between Co-CAT and NiFe LDH leads to a superior catalytic performance compared to that of Pt/C.In addition,the as-assembled Zn–air battery exhibits excellent stability and a high power density of 327.09 mW cm^(−2) for 56 h and 112.04 mW cm^(−2) for 11.5 h in both liquid and solid electrolytes,respectively.
基金supported by the Taishan Scholar Program of Shandong Province from the Department of Education of Shandong Province,China(ts201712045)National Natural Science Foundation of China(22102079)+1 种基金Natural Science Foundation of Shandong Province,China(ZR2021YQ10)Doctoral Found of QUST(0100229001,010029081).
文摘The lack of low-cost and efficient oxygen evolution reaction(OER)catalysts in acid media has significantly limited the development of proton exchange membrane water electrolysis,which can perfectly integrate with intermittent renewable energy.Recently,iridium and non-noble metal mixed oxides have been identified as promising candidates for the OER in acid media.Herein,we report a novel double mixed metal oxide BaIrO_(2.937)/La_(3)IrO_(7) with a surface of IrOx formed by Ba and La leaching as an efficient electrocatalyst for boosting the sluggish OER.In 0.1 M HClO4,a low overpotential of 290 mV is required for BaIrO_(2.937)/La_(3)IrO_(7) to achieve the benchmark of 10 mA cm^(-2),comparable to commercial IrO_(2) and most reported acidic OER electrocatalysts.Moreover,a smaller Tafel slope of BaIrO_(2.937)/La_(3)IrO_(7) signifies fast reaction kinetics.Significantly important is that the iridium based mass activity was 561.6 A g_(Ir)^(-1) at 1.63 V vs.a reversible hydrogen electrode,which is 3.9 times as high as that of commercial IrO_(2).This work highlights the smart design of double mixed metal oxides with surface reconstruction as highly active and low cost electrocatalysts for the OER in acidic media.
基金supported by the Taishan Scholar Program of Shandong Province,China(tsqn202211162)National Natural Science Foundation of China(22372088 and 22102079)+1 种基金Natural Science Foundation of Shandong Province of China(ZR2021YQ10)the Materials/Parts Technology Development Program(RS-2024-00432627)funded by the Ministry of Trade,Industry and Energy,Korea.
文摘Reducing the Ir loading while preserving catalytic performance and mechanical robustness in anodic catalyst layers remains a critical challenge for the large-scale implementation of proton exchange membrane water electrolysis(PEMWE).Herein,we present a structural engineering strategy involving neodymium-doped Ir/IrO_(2)(Nd-Ir/IrO_(2))hollow nanospheres with precisely adjustable shell thickness and cavity dimensions.The optimized catalyst demonstrates excellent oxygen evolution reaction(OER)performance in acidic media,achieving a remarkably low overpotential of 259 mV at a benchmark current density of 10 mA cm^(-2) while exhibiting substantially enhanced durability compared to commercial IrO_(2) and Ir/IrO_(2) counterparts.Notably,the Nd-Ir/IrO_(2) catalyst delivers a mass activity of 541.6 A gIr^(-1) at 1.50 V vs RHE,representing a 74.5-fold enhancement over conventional IrO_(2).Through comprehensive electrochemical analysis and advanced characterization techniques reveal that,the hierarchical hollow architecture simultaneously addresses multiple critical requirements:(i)abundant exposed active sites enabled by an enhanced electrochemical surface area,(ii)optimized mass transport pathways through engineered porosity,and(iii)preserved structural integrity via a continuous conductive framework,collectively enabling significant Ir loading reduction without compromising catalytic layer performance.Fundamental mechanistic investigations further disclose that Nd doping induces critical interfacial Nd-O-Ir configurations that stabilize lattice oxygen,together with intensified electron effect among mixed valent Ir that inhibits the overoxidation of Ir active sites during the OER process,synergistically ensuring enhanced catalytic durability.Our work establishes a dual-modulation paradigm integrating nanoscale architectural engineering with atomic-level heteroatom doping,providing a viable pathway toward high-performance PEMWE systems with drastically reduced noble metal requirements.
基金financially supported by the National Natural Science Foundation of China(No.22172077)the Natural Science Foundation of Jiangsu Province of China(No.BK20211573)+1 种基金Jiangsu International Science and Technology Cooperation Program(No.BZ2020063)the Fundamental Research Funds for the Central Universities(No.30921011216)。
文摘The tailor-made oxygen evolution catalysts(OECs)paired with photoanodes offer a path to promote water oxidation kinetics;however,the unsatisfied interface between OECs and photoanode sets a barrier for efficient charge transfer.Herein,a graphene oxide(GO)layer to promote the charge transfer from BiVO_(4)(BVO)to NiOOH OEC is reported.It is found that GO layer inserted between BVO and NiOOH can not only serve as hole extraction layer due to its hole storage capability,but also improve the stability.Finally,the rationally designed NiOOH/GO/BVO photoanode achieves a photocurrent density of 3.81 mA·cm^(-2)at 1.23 V(vs.reversible hydrogen electrode(RHE)),which is 3.85 times as high as that of bare BVO.This work opens up low-cost auxiliary materials for enhancing photoelectrochemical water splitting.
