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Li^(+)-ion bound crown ether functionalization enables dual promotion of dynamics and thermodynamics for ambient ammonia synthesis

查看全文 作　　者：Qiyang [1]Cheng;Sisi [1]Liu;Mengfan [1]Wang;Lifang [2]Zhang;Yanzheng [1]He;Jiajie [1]Ni;Jingru [1]Zhang;Chengwei [3]Deng;Yi [3]Sun;Tao [2,4]Qian;Chenglin [1,4]Yan 高影响力作者 机构地区：[1]Collaborative Innovation Center of Suzhou Nano Science and Technology,College of Energy,Soochow University,Suzhou 215006,Jiangsu,China;[2]School of Chemistry and Chemical Engineering,Nantong University,Nantong 226019,Jiangsu,China;[3]Aerospace Hydrogen Energy Technologv(Shanghai)Co.Ltd,Shanghai 201800,China;[4]Light Industry Institute of Electrochemical Power Sources,Suzhou 215600,Jiangsu,China高影响力机构 出　　处：《Journal of Energy Chemistry》索引2023年第10期,共8页高影响力期刊 基　　金：supported by the National Natural Science Foundation of China(U21A20332,52103226,52202275,52203314,and 12204253);the Distinguished Young Scholars Fund of Jiangsu Province(BK20220061);the Fellowship of China Postdoctoral Science Foundation(2021M702382)。 摘　　要：Electrosynthesis of ammonia from the reduction of nitrogen is still confronted with the limited supply of gas reactant in dynamics as well as high activation barrier in thermodynamics.Unfortunately,despite tremendous efforts devoted to electrocatalysts themselves,they still fail to tackle the above two challenges simultaneously.Herein,we employ a heterogeneous catalyst adlayer-composed of crown ethers associated with Li^(+)ions-to achieve the dual promotion of dynamics and thermodynamics for ambient ammonia synthesis.Dynamically,the bound Li^(+)ions interact with the strong quadrupole moment of nitrogen,and trigger considerable reactant flux toward the catalyst.Thermodynamically,Li^(+)associated with the oxygen of crown ether achieves a higher density of states at the Fermi level for the catalyst,enabling effortless electron transfer from the catalysts to nitrogen and thus greatly reducing the activation barrier.As expected,the proof-of-concept system achieves an ammonia yield rate of 168.5μg h^(-1)mg^(-1)and a Faradaic efficiency of 75.3%at-0.3 V vs.RHE.This system-level approach opens up pathways for tackling the two key challenges that have limited the field of ammonia synthesis. 关 键 词：Li^(+)-ion bound crown ether DYNAMICS Thermodynamics Nitrogen reduction Ammonia synthesis
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