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
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
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
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 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.