典型文献
Actinide-uranium single-atom catalysis for electrochemical nitrogen fixation
文献摘要：
Actinide-based catalysts have been regarded as promising candidates for N2 fixation owing to their unique 5f orbital with flexible oxidation states.Herein,we report for the first time the dispersion of ura-nium(U)single atoms on TiO2 nanosheets via oxygen vacancy confinement for N2 electroreduction.The single-atom U catalyst exhibited a high NH3 yield of 40.57 μg h-1 mg-1,with a reasonably high Faraday efficiency of 25.77％,ranking first among the reported nitrogen-free catalysts.Isotope-labeling operando synchrotron infrared spectroscopy verifies that the key *N2Hy intermediate species was derived from the N2 gas of the feed.By using operando X-ray absorption spectroscopy,we found enhanced metal-support interaction between U single atoms and TiO2 lattice with more U-Olatet coordination under working con-ditions.Theoretical simulations suggest that the evolved 1Oads-U-4Olatt moieties act as a critical electron-feedback center,lowering the thermodynamic energy barrier for the N2 dissociation and the first hydro-genation step.This work provides the possibility of tailoring the interaction between metal active sites and supports for designing high-performance actinide-based single-atom catalysts.
文献关键词：
中图分类号：
作者姓名：
Tao Chen;Tong Liu;Beibei Pang;Tao Ding;Wei Zhang;Xinyi Shen;Dan Wu;Lan Wang;Xiaokang Liu;Qiquan Luo;Wenkun Zhu;Tao Yao
作者机构：
National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230029,China;State Key Laboratory of Environment-friendly Energy Materials,School of National Defense Science and Technology,Southwest University of Science and Technology,Mianyang 621010,China;Institutes of Physical Science and Information Technology,Anhui University,Hefei 230601,China
文献出处：
引用格式：
[1]Tao Chen;Tong Liu;Beibei Pang;Tao Ding;Wei Zhang;Xinyi Shen;Dan Wu;Lan Wang;Xiaokang Liu;Qiquan Luo;Wenkun Zhu;Tao Yao-.Actinide-uranium single-atom catalysis for electrochemical nitrogen fixation)[J].科学通报（英文版）,2022(19):2001-2012
A类：
Actinide,N2Hy,Olatet,1Oads,4Olatt
B类：
uranium,single,catalysis,electrochemical,nitrogen,fixation,catalysts,have,been,regarded,promising,candidates,owing,their,unique,5f,orbital,flexible,oxidation,states,Herein,first,dispersion,atoms,TiO2,nanosheets,via,oxygen,vacancy,confinement,electroreduction,exhibited,high,NH3,yield,reasonably,Faraday,efficiency,ranking,among,reported,free,Isotope,labeling,operando,synchrotron,infrared,spectroscopy,verifies,that,key,intermediate,species,was,derived,from,gas,By,using,ray,absorption,found,enhanced,metal,interaction,between,lattice,more,coordination,under,working,ditions,Theoretical,simulations,suggest,evolved,moieties,critical,electron,feedback,center,lowering,thermodynamic,energy,barrier,dissociation,hydro,genation,step,This,provides,possibility,tailoring,active,sites,supports,designing,performance,actinide
AB值：
0.607063
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