The development of efficient and cost-effective catalysts to catalyze a wide variety of electrochemical reactions is key to realize the large-scale applicati on of ren ewable and clean en ergy tech no logies.Owing to ...The development of efficient and cost-effective catalysts to catalyze a wide variety of electrochemical reactions is key to realize the large-scale applicati on of ren ewable and clean en ergy tech no logies.Owing to the maximum atom-utilization efficie ncy and unique electronic and geometric structures,single atom catalysts(SACs)have exhibited superior performance in various catalytic systems.Recently,assembled from the function alized orga nic lin kers and metal no des,metal-organic frameworks(MOFs)with ultrafi ne porosity have received treme ndous attention as precursors or self-sacrificing templates for preparing porous SACs.Here,the recent advances toward the synthesis strategies for using MOF precursors/templates to con struct SACs are systematically summarized with special emphasis on the types of central metal sites.The electrochemical applications of these recently emerged MOF-derived SACs for various energy-conversion processes,such as oxygen reduction/evolution reaction(ORR/OER),hydrogen evolution reaction(HER),and CO2 reduction reaction(CO2RR),are also discussed and reviewed.Fin ally,the curre nt challe nges and prospects regardi ng the developme nt of MOF-derived SACs are proposed.展开更多
Electrochemical CO_(2)reduction is a viable,economical,and sustainable method to transform atmospheric CO_(2)into carbon-based fuels and effectively reduce climate change and the energy crisis.Constructing robust cata...Electrochemical CO_(2)reduction is a viable,economical,and sustainable method to transform atmospheric CO_(2)into carbon-based fuels and effectively reduce climate change and the energy crisis.Constructing robust catalysts through interface engineering is significant for electrocatalytic CO_(2)reduction(ECR)but remains a grand challenge.Herein,SnO2/Bi_(2)O_(2)CO_(3)heterojunction on N,S-codoped-carbon(SnO_(2)/BOC@NSC)with efficient ECR performance was firstly constructed by a facile synthetic strategy.When the SnO_(2)/BOC@NSC was utilized in ECR,it exhibits a large formic acid(HCOOH)partial current density(JHCOOH)of 86.7 mA·cm^(−2)at−1.2 V versus reversible hydrogen electrode(RHE)and maximum Faradaic efficiency(FE)of HCOOH(90.75%at−1.2 V versus RHE),respectively.Notably,the FEHCOOH of SnO_(2)/BOC@NSC is higher than 90%in the flow cell and the JHCOOH of SnO_(2)/BOC@NSC can achieve 200 mA·cm^(−2)at−0.8 V versus RHE to meet the requirements of industrialization level.The comparative experimental analysis and in-situ X-ray absorption fine structure reveal that the excellent ECR performance can be ascribed to the synergistic effect of SnO_(2)/BOC heterojunction,which enhances the activation of CO_(2)molecules and improves electron transfer.This work provides an efficient SnO_(2)-based heterojunction catalyst for effective formate production and offers a novel approach for the construction of new types of metal oxide heterostructures for other catalytic applications.展开更多
Electrochemical water splitting is a facile and effective route to generate pure hydrogen and oxygen.However,the sluggish kinetics of hydrogen evolution reaction(HER) and especially oxygen evolution reaction(OER) hind...Electrochemical water splitting is a facile and effective route to generate pure hydrogen and oxygen.However,the sluggish kinetics of hydrogen evolution reaction(HER) and especially oxygen evolution reaction(OER) hinder the water splitting efficiency.Meanwhile,the high-cost of noble-metal catalysts limit their actual application.It is thus highly urgent to exploit an economical and earthabundant bifunctional HER and OER electrocatalyst to simplify procedure and reduce cost.Herein,we synthesize the three-dimensionally ordered macro-/mesoporous(3 DOM/m) Ni_(x)Co_(100-x) alloys with distinctive structure and large surface area via a dual-templating technique.Among them,the3 DOM/m Ni61Co39 shows the lowest overpotentials of 121 mV and 241 mV at 10 mA/cm^(2) for HER and OER,respectively.Furthermore,when employed for water splitting,the Ni_(61)Co_(39) only requires 1.60 V to approach 10 mA/cm^(2) and presents excellent stability.These encouraging performances of the Ni_(61)Co_(39) render it a promising bifunctional catalyst for overall water splitting.展开更多
基金This work was supported by the National Key R&D Program of China(No.2016YFA0202801)the National Natural Science Foundation of China(Nos.21671117,21871159,21890383,and 21676018)and the China Postdoctoral Science Foundation(No.2017M610864).
文摘The development of efficient and cost-effective catalysts to catalyze a wide variety of electrochemical reactions is key to realize the large-scale applicati on of ren ewable and clean en ergy tech no logies.Owing to the maximum atom-utilization efficie ncy and unique electronic and geometric structures,single atom catalysts(SACs)have exhibited superior performance in various catalytic systems.Recently,assembled from the function alized orga nic lin kers and metal no des,metal-organic frameworks(MOFs)with ultrafi ne porosity have received treme ndous attention as precursors or self-sacrificing templates for preparing porous SACs.Here,the recent advances toward the synthesis strategies for using MOF precursors/templates to con struct SACs are systematically summarized with special emphasis on the types of central metal sites.The electrochemical applications of these recently emerged MOF-derived SACs for various energy-conversion processes,such as oxygen reduction/evolution reaction(ORR/OER),hydrogen evolution reaction(HER),and CO2 reduction reaction(CO2RR),are also discussed and reviewed.Fin ally,the curre nt challe nges and prospects regardi ng the developme nt of MOF-derived SACs are proposed.
基金supported by the National Natural Science Foundation of China(Nos.21631003 and 22001015)the Fundamental Research Funds for the Central Universities(No.2050205)University of Science and Technology Beijing.
文摘Electrochemical CO_(2)reduction is a viable,economical,and sustainable method to transform atmospheric CO_(2)into carbon-based fuels and effectively reduce climate change and the energy crisis.Constructing robust catalysts through interface engineering is significant for electrocatalytic CO_(2)reduction(ECR)but remains a grand challenge.Herein,SnO2/Bi_(2)O_(2)CO_(3)heterojunction on N,S-codoped-carbon(SnO_(2)/BOC@NSC)with efficient ECR performance was firstly constructed by a facile synthetic strategy.When the SnO_(2)/BOC@NSC was utilized in ECR,it exhibits a large formic acid(HCOOH)partial current density(JHCOOH)of 86.7 mA·cm^(−2)at−1.2 V versus reversible hydrogen electrode(RHE)and maximum Faradaic efficiency(FE)of HCOOH(90.75%at−1.2 V versus RHE),respectively.Notably,the FEHCOOH of SnO_(2)/BOC@NSC is higher than 90%in the flow cell and the JHCOOH of SnO_(2)/BOC@NSC can achieve 200 mA·cm^(−2)at−0.8 V versus RHE to meet the requirements of industrialization level.The comparative experimental analysis and in-situ X-ray absorption fine structure reveal that the excellent ECR performance can be ascribed to the synergistic effect of SnO_(2)/BOC heterojunction,which enhances the activation of CO_(2)molecules and improves electron transfer.This work provides an efficient SnO_(2)-based heterojunction catalyst for effective formate production and offers a novel approach for the construction of new types of metal oxide heterostructures for other catalytic applications.
基金financially supported by the National Natural Science Foundation of China (No.21676018 and 51172014)。
文摘Electrochemical water splitting is a facile and effective route to generate pure hydrogen and oxygen.However,the sluggish kinetics of hydrogen evolution reaction(HER) and especially oxygen evolution reaction(OER) hinder the water splitting efficiency.Meanwhile,the high-cost of noble-metal catalysts limit their actual application.It is thus highly urgent to exploit an economical and earthabundant bifunctional HER and OER electrocatalyst to simplify procedure and reduce cost.Herein,we synthesize the three-dimensionally ordered macro-/mesoporous(3 DOM/m) Ni_(x)Co_(100-x) alloys with distinctive structure and large surface area via a dual-templating technique.Among them,the3 DOM/m Ni61Co39 shows the lowest overpotentials of 121 mV and 241 mV at 10 mA/cm^(2) for HER and OER,respectively.Furthermore,when employed for water splitting,the Ni_(61)Co_(39) only requires 1.60 V to approach 10 mA/cm^(2) and presents excellent stability.These encouraging performances of the Ni_(61)Co_(39) render it a promising bifunctional catalyst for overall water splitting.