A spinel oxide NiCo204 prepared by thermal decomposition is of very high activity for the oxygen evolution reaction(OER)in alkaline solution.The oxygen evolution overpotential on NiCo204 is 0.252-0.262V in 10 M NaOH s...A spinel oxide NiCo204 prepared by thermal decomposition is of very high activity for the oxygen evolution reaction(OER)in alkaline solution.The oxygen evolution overpotential on NiCo204 is 0.252-0.262V in 10 M NaOH solution at 343K and current density 100 mAcm^(-2).展开更多
Green reactions not only provide us chemical products without any pollution,but also offer us the viable technology to realize difficult tasks in normal conditions.Photo-,photoelectro-,and electrocatalytic reactions a...Green reactions not only provide us chemical products without any pollution,but also offer us the viable technology to realize difficult tasks in normal conditions.Photo-,photoelectro-,and electrocatalytic reactions are indeed powerful tools to help us to embrace bright future.Especially,some gas-involved reactions are extremely useful to change our life environments from energy systems to liquid fuels and cost-effective products,such as H2 evolution(H2 production),02 evolution/reduction,CO2 reduction,N2 reduction(or N2 fixation) reactions.We can provide fuel cells clean H2 for electric vehicles from H2 evolution reaction(HER),at the same time,we also need highly efficient 02 reduction reaction(ORR) in fuel cells for improving the reaction kinetics.Moreover,we can get the clean oxidant O2 from water through O2 evolution reaction(OER),and carry out some reactions without posing any pollution to reaction systems.Furthermore,we can translate the greenhouse gas CO2 into useful liquid fuels through CO2 reduction reaction(CRR).Last but not the least,we can get ammonia from N2 reduction reaction(NRR),which can decrease energy input compared to the traditional Hubble process.These reactions,such as HER,ORR,OER,CRR and NRR could be realized through solar-,photoelectro-and electro-assisted ways.For them,the catalysts used play crucial roles in determining the efficiency and kinds of products,so we should consider the efficiency of catalysts.However,the cost,synthetic methods of catalysts should also be considered.Nowadays,significant progress has been achieved,however,many challenges still exist,reaction systems,catalysts underlying mechanisms,and so on.As extremely active fields,we should pay attention to them.Under the background,it has motivated us to contribute with a roadmap on ’GasInvolved Photo-and Electro-Catalysis’.展开更多
Fe based oxides are considered as a promising catalyst for the oxygen evolution reaction （OER） due to their low cost and high stability. Here, based on density functional theory calculations, the electrocatalytic be...Fe based oxides are considered as a promising catalyst for the oxygen evolution reaction （OER） due to their low cost and high stability. Here, based on density functional theory calculations, the electrocatalytic behaviors of pure and metal （Ni, Co） doped Fe-terminated Fe2O3（0001） are investigated. The potential-limiting step for OER is determined as the formation of O＊ by dehydrogenating surface hydroxyl and it is suggested that the doping enhances the catalytic activity of Fe2O3（0001） by reducing the free energy change of rate limiting step on doped Ni or Co atom. Especially, the calculated over-potential of Co-doped Fe2O3 （0001） surface is about 0.63 eV on Co site, which is comparable with the theoretical over-potential of 0.56 eV for RuO2.展开更多
文摘A spinel oxide NiCo204 prepared by thermal decomposition is of very high activity for the oxygen evolution reaction(OER)in alkaline solution.The oxygen evolution overpotential on NiCo204 is 0.252-0.262V in 10 M NaOH solution at 343K and current density 100 mAcm^(-2).
基金The financial support from the National Natural Science Foundation of China (Nos. 51772312, 21671197)
文摘Green reactions not only provide us chemical products without any pollution,but also offer us the viable technology to realize difficult tasks in normal conditions.Photo-,photoelectro-,and electrocatalytic reactions are indeed powerful tools to help us to embrace bright future.Especially,some gas-involved reactions are extremely useful to change our life environments from energy systems to liquid fuels and cost-effective products,such as H2 evolution(H2 production),02 evolution/reduction,CO2 reduction,N2 reduction(or N2 fixation) reactions.We can provide fuel cells clean H2 for electric vehicles from H2 evolution reaction(HER),at the same time,we also need highly efficient 02 reduction reaction(ORR) in fuel cells for improving the reaction kinetics.Moreover,we can get the clean oxidant O2 from water through O2 evolution reaction(OER),and carry out some reactions without posing any pollution to reaction systems.Furthermore,we can translate the greenhouse gas CO2 into useful liquid fuels through CO2 reduction reaction(CRR).Last but not the least,we can get ammonia from N2 reduction reaction(NRR),which can decrease energy input compared to the traditional Hubble process.These reactions,such as HER,ORR,OER,CRR and NRR could be realized through solar-,photoelectro-and electro-assisted ways.For them,the catalysts used play crucial roles in determining the efficiency and kinds of products,so we should consider the efficiency of catalysts.However,the cost,synthetic methods of catalysts should also be considered.Nowadays,significant progress has been achieved,however,many challenges still exist,reaction systems,catalysts underlying mechanisms,and so on.As extremely active fields,we should pay attention to them.Under the background,it has motivated us to contribute with a roadmap on ’GasInvolved Photo-and Electro-Catalysis’.
基金This work was supported by the National Natural Science Foundation of China （No.21573204, No.21421063, No.21473167, No.51172223）, the Ministry of Science and Technology （2016YFA0200602）, Strategic Priority Research Program of CAS （XDB01020300）, the Fundamental Research Funds for the Central Universities, National Program for Support of Top-notch Young Professional, and the USTCSCC, SCCAS, Tianjin, and Shanghai Supercomputer Centers.
文摘Fe based oxides are considered as a promising catalyst for the oxygen evolution reaction （OER） due to their low cost and high stability. Here, based on density functional theory calculations, the electrocatalytic behaviors of pure and metal （Ni, Co） doped Fe-terminated Fe2O3（0001） are investigated. The potential-limiting step for OER is determined as the formation of O＊ by dehydrogenating surface hydroxyl and it is suggested that the doping enhances the catalytic activity of Fe2O3（0001） by reducing the free energy change of rate limiting step on doped Ni or Co atom. Especially, the calculated over-potential of Co-doped Fe2O3 （0001） surface is about 0.63 eV on Co site, which is comparable with the theoretical over-potential of 0.56 eV for RuO2.
