Transition metal phosphides(TMPs)have been regarded as alternative hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts owing to their comparable activity to those of noble metal-based catalysts...Transition metal phosphides(TMPs)have been regarded as alternative hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts owing to their comparable activity to those of noble metal-based catalysts.TMPs have been produced in various morphologies,including hollow and porous nanostructures,which are features deemed desirable for electrocatalytic materials.Templated synthesis routes are often responsible for such morphologies.This paper reviews the latest advances and existing challenges in the synthesis of TMP-based OER and HER catalysts through templated methods.A comprehensive review of the structure-property-performance of TMP-based HER and OER catalysts prepared using different templates is presented.The discussion proceeds according to application,first by HER and further divided among the types of templates used-from hard templates,sacrificial templates,and soft templates to the emerging dynamic hydrogen bubble template.OER catalysts are then reviewed and grouped according to their morphology.Finally,prospective research directions for the synthesis of hollow and porous TMP-based catalysts,such as improvements on both activity and stability of TMPs,design of environmentally benign templates and processes,and analysis of the reaction mechanism through advanced material characterization techniques and theoretical calculations,are suggested.展开更多
The conversion of solar energy to produce clean hydrogen fuel through water splitting is an emerging strategy for efficiently storing solar energy in the form of solar fuel.This aligns with the increasing global deman...The conversion of solar energy to produce clean hydrogen fuel through water splitting is an emerging strategy for efficiently storing solar energy in the form of solar fuel.This aligns with the increasing global demand for the development of an ideal energy alternative to fossil fuels that does not emit greenhouse gases.Electrochemical(EC) and photoelectrochemical(PEC) water splitting technologies have garnered significant attention worldwide for advanced hydrogen solar fuel production in recent decades.To achieve sustainable green H_(2) production,it is essential to create efficient catalyst materials that are low-cost and can replace expensive noble metal-based catalysts.These characteristics make them an ideal catalyst material for the process.Two-dimensional MXenes with M_(n+1)X_(n) structure have been identified as a promising option for EC and PEC water splitting due to their superior hydrophilicity,metal-like conductivity,large surface area,and adjustable surface chemistry.Here,we present a summary of recent advancements in the synthesis and performance enhancement methods for MXene hybrid materials in hydrogen production through EC and PEC water splitting.Furthermore,we examine the challenges and insights associated with the rational design of MXene-based hybrid materials to facilitate efficient water splitting for sustainable solar fuel production.展开更多
Lithium-oxygen(Li-O_(2))batteries have attracted significant attention due to their ultra-high theoretical energy density.However,serious challenges,such as potential lag,low-rate capability,round-trip efficiency,and ...Lithium-oxygen(Li-O_(2))batteries have attracted significant attention due to their ultra-high theoretical energy density.However,serious challenges,such as potential lag,low-rate capability,round-trip efficiency,and poor cycle stability,greatly limit their practical application.This review provides a comprehensive account of the development of Li-O_(2)batteries,elucidates the current discharge/charge mechanism,and highlights both the advantages and bottlenecks of this technology.In particular,recent research progress on various cathode materials,such as carbon-based materials,noble metals,and non-noble metals,for Li-O_(2)batteries is deeply reviewed,emphasizing the impact of design strategies,material structures,chemical compositions,and microphysical parameters on oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)kinetics,as well as discharge products and overall battery performance.This review will also shed light on future research directions for oxygen electrode catalysts and material construction to facilitate the development of Li-O_(2)batteries with maximized electrochemical performance.展开更多
M-N-C(M=Fe,Co,Ni,etc.) catalyst owns high catalytic activity in the oxygen catalytic reaction which is the most likely to replace the Pt-based catalysts.But it is still a challenge to further increase the active site ...M-N-C(M=Fe,Co,Ni,etc.) catalyst owns high catalytic activity in the oxygen catalytic reaction which is the most likely to replace the Pt-based catalysts.But it is still a challenge to further increase the active site density.This article constructs the high-efficiency FeMn-N/S-C-1000 catalyst to realize ORR/OER bifunctional catalysis by hetero-atom,bimetal(Fe,Mn) doped simultaneously strategy.When evaluated it as bi-functional electro-catalysts,FeMn-N/S-C-1000 exhibits excellent catalytic activity(E_(1/2)=0.924 V,E_(j=10)=1.617 V) in alkaline media,outperforms conventional Pt/C,RuO_(2) and most non-precious-metal catalysts reported recently,Such outstanding performance is owing to N,S co-coordinated with metal to form multi-types of single atom,dual atom active sites to carry out bi-catalysis.Importantly,nitrite poison test provides the proof that the active sites of FeMn-N/S-C are more than that of single-atom catalysts to promote catalytic reactions directly.To better understand the local structure of Fe and Mn active sites,XAS and DFT were employed to reveal that FeMn-N_5/S-C site plays the key role during catalysis.Notably,the FeMn-N/S-C-1000 based low-temperature rechargeable flexible Zn-air also exhibits superior discharge performance and extraordinary durability at-40℃.This work will provide a new idea to design diatomic catalysts applied in low-temperature rechargeable batteries.展开更多
Rechargeable zinc-air batteries(ZABs)are a promising energy conversion device,which rely critically on electrocatalysts to accelerate their rate-determining reactions such as oxygen reduction(ORR)and oxygen evolution ...Rechargeable zinc-air batteries(ZABs)are a promising energy conversion device,which rely critically on electrocatalysts to accelerate their rate-determining reactions such as oxygen reduction(ORR)and oxygen evolution reactions(OER).Herein,we fabricate a range of bifunctional M-N-C(metal-nitrogen-carbon)catalysts containing M-Nx coordination sites and M/MxC nanoparticles(M=Co,Fe,and Cu)using a new class ofγ-cyclodextrin(CD)based metal-organic framework as the precursor.With the two types of active sites interacting with each other in the catalysts,the obtained Fe@C-FeNC and Co@C-CoNC display superior alkaline ORR activity in terms of low half-wave(E1/2)potential(~0.917 and 0.906 V,respectively),which are higher than Cu@C-CuNC(~0.829 V)and the commercial Pt/C(~0.861 V).As a bifunctional electrocatalyst,the Co@C-CoNC exhibits the best performance,showing a bifunctional ORR/OER overpotential(ΔE)of~0.732 V,which is much lower than that of Fe@C-FeNC(~0.831 V)and Cu@C-CuNC(~1.411 V),as well as most of the robust bifunctional electrocatalysts reported to date.Synchrotron X-ray absorption spectroscopy and density functional theory simulations reveal that the strong electronic correlation between metallic Co nanoparticles and the atomic Co-N4 sites in the Co@C-CoNC catalyst can increase the d-electron density near the Fermi level and thus effectively optimize the adsorption/desorption of intermediates in ORR/OER,resulting in an enhanced bifunctional electrocatalytic performance.The Co@C-CoNC-based rechargeable ZAB exhibited a maximum power density of 162.80 mW cm^(−2) at 270.30 mA cm^(−2),higher than the combination of commercial Pt/C+RuO2(~158.90 mW cm^(−2) at 265.80 mA cm^(−2))catalysts.During the galvanostatic discharge at 10 mA cm^(−2),the ZAB delivered an almost stable discharge voltage of 1.2 V for~140 h,signifying the virtue of excellent bifunctional ORR/OER electrocatalytic activity.展开更多
Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the ...Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the most conventional and classical non-noble metal-based electrocatalysts for OER,while TM basic salts[M^(2+)(OH)_(2-x)(A_(m^(-))_(x/m),A=CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)]consisting of OH−and another anion have drawn extensive research interest due to its higher catalytic activity in the past decade.In this review,we summarize the recent advances of TM basic salts and their application in OER and further overall water splitting.We categorize TM basic salt-based OER pre-catalysts into four types(CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)according to the anion,which is a key factor for their outstanding performance towards OER.We highlight experimental and theoretical methods for understanding the structure evolution during OER and the effect of anion on catalytic performance.To develop bifunctional TM basic salts as catalyst for the practical electrolysis application,we also review the present strategies for enhancing its hydrogen evolution reaction activity and thereby improving its overall water splitting performance.Finally,we conclude this review with a summary and perspective about the remaining challenges and future opportunities of TM basic salts as catalysts for water electrolysis.展开更多
基金the support from the CIPHER Project(IIID 2018-008)funded by the Commission on Higher Education-Philippine California Advanced Research Institutes(CHED-PCARI)。
文摘Transition metal phosphides(TMPs)have been regarded as alternative hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts owing to their comparable activity to those of noble metal-based catalysts.TMPs have been produced in various morphologies,including hollow and porous nanostructures,which are features deemed desirable for electrocatalytic materials.Templated synthesis routes are often responsible for such morphologies.This paper reviews the latest advances and existing challenges in the synthesis of TMP-based OER and HER catalysts through templated methods.A comprehensive review of the structure-property-performance of TMP-based HER and OER catalysts prepared using different templates is presented.The discussion proceeds according to application,first by HER and further divided among the types of templates used-from hard templates,sacrificial templates,and soft templates to the emerging dynamic hydrogen bubble template.OER catalysts are then reviewed and grouped according to their morphology.Finally,prospective research directions for the synthesis of hollow and porous TMP-based catalysts,such as improvements on both activity and stability of TMPs,design of environmentally benign templates and processes,and analysis of the reaction mechanism through advanced material characterization techniques and theoretical calculations,are suggested.
基金the result of a research project conducted with the funds of the Open R&D program of Korea Electric Power Corporation (R23XO04)supported by the Technology Innovation Program funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea) (K_G012002238601)+2 种基金by “Regional Innovation Strategy (RIS)” through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (MOE) (2021RIS-002)by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2021M3I3A1082880)by the Korea Institute of Energy Technology Evaluation and Planning (KETEP) and the Ministry of Trade, Industry & Energy (MOTIE) of the Republic of Korea (No. 20224000000320)。
文摘The conversion of solar energy to produce clean hydrogen fuel through water splitting is an emerging strategy for efficiently storing solar energy in the form of solar fuel.This aligns with the increasing global demand for the development of an ideal energy alternative to fossil fuels that does not emit greenhouse gases.Electrochemical(EC) and photoelectrochemical(PEC) water splitting technologies have garnered significant attention worldwide for advanced hydrogen solar fuel production in recent decades.To achieve sustainable green H_(2) production,it is essential to create efficient catalyst materials that are low-cost and can replace expensive noble metal-based catalysts.These characteristics make them an ideal catalyst material for the process.Two-dimensional MXenes with M_(n+1)X_(n) structure have been identified as a promising option for EC and PEC water splitting due to their superior hydrophilicity,metal-like conductivity,large surface area,and adjustable surface chemistry.Here,we present a summary of recent advancements in the synthesis and performance enhancement methods for MXene hybrid materials in hydrogen production through EC and PEC water splitting.Furthermore,we examine the challenges and insights associated with the rational design of MXene-based hybrid materials to facilitate efficient water splitting for sustainable solar fuel production.
基金supported by the National Natural Science Foundation of China(U1663225,22293020 and 22293022)the National Key R&D Program of China(2021YFE0115800)+2 种基金the Program for Changjiang Scholars and Innovative Research Team in University(IRT_15R52)of the Chinese Ministry of Educationthe Program of Introducing Talents of Discipline to Universities-Plan 111(B20002)from the Ministry of Science and Technology and the Ministry of Education of Chinathe Belgium-China Governmental Key Cooperation Program WBI-MOST(SUB/2021/IND493971/524448)。
文摘Lithium-oxygen(Li-O_(2))batteries have attracted significant attention due to their ultra-high theoretical energy density.However,serious challenges,such as potential lag,low-rate capability,round-trip efficiency,and poor cycle stability,greatly limit their practical application.This review provides a comprehensive account of the development of Li-O_(2)batteries,elucidates the current discharge/charge mechanism,and highlights both the advantages and bottlenecks of this technology.In particular,recent research progress on various cathode materials,such as carbon-based materials,noble metals,and non-noble metals,for Li-O_(2)batteries is deeply reviewed,emphasizing the impact of design strategies,material structures,chemical compositions,and microphysical parameters on oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)kinetics,as well as discharge products and overall battery performance.This review will also shed light on future research directions for oxygen electrode catalysts and material construction to facilitate the development of Li-O_(2)batteries with maximized electrochemical performance.
基金supported by the National Natural Science Foundation of China(21603171)the Basic Research Foundation of Xi’an Jiaotong University(xjh012020027)。
文摘M-N-C(M=Fe,Co,Ni,etc.) catalyst owns high catalytic activity in the oxygen catalytic reaction which is the most likely to replace the Pt-based catalysts.But it is still a challenge to further increase the active site density.This article constructs the high-efficiency FeMn-N/S-C-1000 catalyst to realize ORR/OER bifunctional catalysis by hetero-atom,bimetal(Fe,Mn) doped simultaneously strategy.When evaluated it as bi-functional electro-catalysts,FeMn-N/S-C-1000 exhibits excellent catalytic activity(E_(1/2)=0.924 V,E_(j=10)=1.617 V) in alkaline media,outperforms conventional Pt/C,RuO_(2) and most non-precious-metal catalysts reported recently,Such outstanding performance is owing to N,S co-coordinated with metal to form multi-types of single atom,dual atom active sites to carry out bi-catalysis.Importantly,nitrite poison test provides the proof that the active sites of FeMn-N/S-C are more than that of single-atom catalysts to promote catalytic reactions directly.To better understand the local structure of Fe and Mn active sites,XAS and DFT were employed to reveal that FeMn-N_5/S-C site plays the key role during catalysis.Notably,the FeMn-N/S-C-1000 based low-temperature rechargeable flexible Zn-air also exhibits superior discharge performance and extraordinary durability at-40℃.This work will provide a new idea to design diatomic catalysts applied in low-temperature rechargeable batteries.
基金supported by the Shenzhen Government’s Plan of Science and Technology(JCYJ20190808121407676 and 20200813142301001)National Natural Science Foundation of China(22178223 and 22262010)+1 种基金Guangxi Science and Technology Fund for Distinguished High-Talent Introduction Program(No.RZ2200002233AC22035091).
文摘Rechargeable zinc-air batteries(ZABs)are a promising energy conversion device,which rely critically on electrocatalysts to accelerate their rate-determining reactions such as oxygen reduction(ORR)and oxygen evolution reactions(OER).Herein,we fabricate a range of bifunctional M-N-C(metal-nitrogen-carbon)catalysts containing M-Nx coordination sites and M/MxC nanoparticles(M=Co,Fe,and Cu)using a new class ofγ-cyclodextrin(CD)based metal-organic framework as the precursor.With the two types of active sites interacting with each other in the catalysts,the obtained Fe@C-FeNC and Co@C-CoNC display superior alkaline ORR activity in terms of low half-wave(E1/2)potential(~0.917 and 0.906 V,respectively),which are higher than Cu@C-CuNC(~0.829 V)and the commercial Pt/C(~0.861 V).As a bifunctional electrocatalyst,the Co@C-CoNC exhibits the best performance,showing a bifunctional ORR/OER overpotential(ΔE)of~0.732 V,which is much lower than that of Fe@C-FeNC(~0.831 V)and Cu@C-CuNC(~1.411 V),as well as most of the robust bifunctional electrocatalysts reported to date.Synchrotron X-ray absorption spectroscopy and density functional theory simulations reveal that the strong electronic correlation between metallic Co nanoparticles and the atomic Co-N4 sites in the Co@C-CoNC catalyst can increase the d-electron density near the Fermi level and thus effectively optimize the adsorption/desorption of intermediates in ORR/OER,resulting in an enhanced bifunctional electrocatalytic performance.The Co@C-CoNC-based rechargeable ZAB exhibited a maximum power density of 162.80 mW cm^(−2) at 270.30 mA cm^(−2),higher than the combination of commercial Pt/C+RuO2(~158.90 mW cm^(−2) at 265.80 mA cm^(−2))catalysts.During the galvanostatic discharge at 10 mA cm^(−2),the ZAB delivered an almost stable discharge voltage of 1.2 V for~140 h,signifying the virtue of excellent bifunctional ORR/OER electrocatalytic activity.
基金supported by the financial support from Natural Science Foundation of China(Nos.21871065,22209129 and 22071038)High-Level Innovation and Entrepreneurship(QCYRCXM-2022-123)+1 种基金support from the“Young Talent Support Plan”of Xi’an Jiaotong University(HG6J024)“Young Talent Lift Plan”of Xi’an city(095920221352).
文摘Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the most conventional and classical non-noble metal-based electrocatalysts for OER,while TM basic salts[M^(2+)(OH)_(2-x)(A_(m^(-))_(x/m),A=CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)]consisting of OH−and another anion have drawn extensive research interest due to its higher catalytic activity in the past decade.In this review,we summarize the recent advances of TM basic salts and their application in OER and further overall water splitting.We categorize TM basic salt-based OER pre-catalysts into four types(CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)according to the anion,which is a key factor for their outstanding performance towards OER.We highlight experimental and theoretical methods for understanding the structure evolution during OER and the effect of anion on catalytic performance.To develop bifunctional TM basic salts as catalyst for the practical electrolysis application,we also review the present strategies for enhancing its hydrogen evolution reaction activity and thereby improving its overall water splitting performance.Finally,we conclude this review with a summary and perspective about the remaining challenges and future opportunities of TM basic salts as catalysts for water electrolysis.
