The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution rea...The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is developed.The multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.展开更多
Metal-organic frameworks possessing relatively large pores,high surface areas,and unsaturated metal sites are attractive materials for use as electrocatalysts in the reduction of N_(2)to NH_(3).In this work,a MIL-101(...Metal-organic frameworks possessing relatively large pores,high surface areas,and unsaturated metal sites are attractive materials for use as electrocatalysts in the reduction of N_(2)to NH_(3).In this work,a MIL-101(Fe)/MoS_(3)hybrid catalyst,prepared by using a precursor-transformation strategy,is shown to be an effective electrocatalyst for the N_(2)reduction reaction(NRR).Under solvothermal conditions,micro-sized octahedral MIL-101(Fe)precursors are converted into ultra-small nanodots,while amorphous MoS_(3)derived from(NH_(4))_(2)MoS_(4)provides a surface suitable for anchoring the MIL-101(Fe)nanodots.The asprepared composite exhibits excellent electrocatalytic activity and durability for the NRR with a Faraday efficiency of 36.71%and an NH_(3)yield of 25.7μg h^(-1)mg_(cat)^(-1)at-0.1 V vs.RHE in 0.1 M HCl.The results show that the dispersion and adherence of MIL-101(Fe)nanodots on amorphous MoS_(3)improves the exposure of active centers and aids mass transfer,resulting in greatly enhanced catalytic activity and stability.展开更多
基金Collaborative Innovation Center of Suzhou Nano Science and TechnologyNational Natural Science Foundation of China,Grant/Award Numbers:21773163,22271203+3 种基金EPSRC for an Overseas Travel Grant,Grant/Award Number:EP/R023816/1State Key Laboratory of Organometallic Chemistry of Shanghai Institute of Organic Chemistry,Grant/Award Number:KF2021005Priority Academic Program Development of Jiangsu Higher Education InstitutionsProject of Scientific and Technologic Infrastructure of Suzhou,Grant/Award Number:SZS201905。
文摘The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is developed.The multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.
基金supported by the National Natural Science Foundation of China(21773163,21531006,22001021)the State Key Laboratory of Organometallic Chemistry of Shanghai Institute of Organic Chemistry(KF2021005)+3 种基金Natural Science Foundation of Jiangsu Province(BK20201048)Natural Science Research Project of Higher Education Institutions in Jiangsu Province(20KJB150008)Collaborative Innovation Center of Suzhou Nano Science and Technologythe Project of Scientific and Technologic Infrastructure of Suzhou(SZS201905)。
文摘Metal-organic frameworks possessing relatively large pores,high surface areas,and unsaturated metal sites are attractive materials for use as electrocatalysts in the reduction of N_(2)to NH_(3).In this work,a MIL-101(Fe)/MoS_(3)hybrid catalyst,prepared by using a precursor-transformation strategy,is shown to be an effective electrocatalyst for the N_(2)reduction reaction(NRR).Under solvothermal conditions,micro-sized octahedral MIL-101(Fe)precursors are converted into ultra-small nanodots,while amorphous MoS_(3)derived from(NH_(4))_(2)MoS_(4)provides a surface suitable for anchoring the MIL-101(Fe)nanodots.The asprepared composite exhibits excellent electrocatalytic activity and durability for the NRR with a Faraday efficiency of 36.71%and an NH_(3)yield of 25.7μg h^(-1)mg_(cat)^(-1)at-0.1 V vs.RHE in 0.1 M HCl.The results show that the dispersion and adherence of MIL-101(Fe)nanodots on amorphous MoS_(3)improves the exposure of active centers and aids mass transfer,resulting in greatly enhanced catalytic activity and stability.
