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典型文献
Spin polarization strategy to deploy proton resource over atomic-level metal sites for highly selective CO2 electrolysis
文献摘要:
Unlocking of the extremely inert C=O bond during electrochemical CO2 reduction demands subtle regulation on a key"resource",protons,necessary for intermediate conversion but also readily trapped in water splitting,which is still challenging for developing efficient single-atom catalysts limited by their structural simplicity usually incompetent to handle this task.Incorporation of extra functional units should be viable.Herein,a proton deployment strategy is demonstrated via"atomic and nanostructured iron(A/N-Fe)pairs",comprising atomically dispersed iron active centers spin-polarized by nanostructured iron carbide ferromagnets,to boost the critical protonation steps.The as-designed catalyst displays a broad window(300 mV)for CO selectivity>90%(98%maximum),even outperforming numerous cutting-edge M-N-C systems.The well-placed control of proton dynamics by A/N-Fe can promote*COOH/*CO formation and simultaneously suppress H2 evolution,benefiting from the magnetic-proximity-induced exchange splitting(spin polarization)that properly adjusts energy levels of the Fe sites'd-shells,and further those of the adsorbed intermediates'antibonding molecular orbitals.
文献关键词:
作者姓名:
Yingjie Zhao;Xinyue Wang;Xiahan Sang;Sixing Zheng;Bin Yang;Lecheng Lei;Yang Hou;Zhongjian Li
作者机构:
Key Laboratory of Biomass Chemical Engineering of Ministry of Education,College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310027,China;Nanostructure Research Centre,Wuhan University of Technology,Wuhan 430070,China;Institute of Zhejiang University-Quzhou,Quzhou 324000,China
引用格式:
[1]Yingjie Zhao;Xinyue Wang;Xiahan Sang;Sixing Zheng;Bin Yang;Lecheng Lei;Yang Hou;Zhongjian Li-.Spin polarization strategy to deploy proton resource over atomic-level metal sites for highly selective CO2 electrolysis)[J].化学科学与工程前沿,2022(12):1772-1781
A类:
incompetent,antibonding
B类:
Spin,polarization,strategy,resource,over,metal,sites,highly,selective,electrolysis,Unlocking,extremely,inert,during,electrochemical,reduction,demands,subtle,regulation,key,protons,necessary,conversion,but,also,readily,trapped,water,splitting,which,still,challenging,developing,efficient,single,catalysts,limited,by,their,structural,simplicity,usually,handle,this,task,Incorporation,extra,functional,units,should,viable,Herein,deployment,demonstrated,nanostructured,iron,pairs,comprising,atomically,dispersed,active,centers,spin,polarized,carbide,ferromagnets,boost,critical,protonation,steps,designed,displays,broad,window,mV,selectivity,maximum,even,outperforming,numerous,cutting,edge,systems,well,placed,control,dynamics,can,promote,COOH,formation,simultaneously,suppress,H2,evolution,benefiting,from,magnetic,proximity,induced,exchange,that,properly,adjusts,energy,levels,shells,further,those,adsorbed,intermediates,molecular,orbitals
AB值:
0.723224
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