Ammonia has been recognized as the future renewable energy fuel because of its wide-ranging applications in H2 storage and transportation sector.In order to avoid the environmentally hazardous Haber-Bosch process,recently,the third-generation ambient ammonia synthesis has drawn phenom-enal attention and thus tremendous efforts are devoted to developing efficient electrocatalysts that would circumvent the bottlenecks of the electrochemical nitrogen reduction reaction(NRR)like competitive hydrogen evolution reac-tion,poor selectivity of N2 on catalyst surface.Herein,we report the synthesis of an oxygen-functionalized boron carbonitride matrix via a two-step pyrolysis technique.The conductive BNCO(1000)architecture,the compatibility of B-2pz orbital with the N-2pz orbital and the charging effect over B due to the C and O edge-atoms in a pentagon altogether facilitate N2 adsorption on the B edge-active sites.The optimum electrolyte acidity with 0.1 M HCl and the lowered anion crowding effect aid the protonation steps of NRR via an associative alternating pathway,which gives a sufficiently high yield of ammonia(211.5 μg h-1 mgcat-1)on the optimized BNCO(1000)catalyst with a Faradaic efficiency of 34.7％at-0.1 V vs RHE.This work thus offers a cost-effective electrode material and provides a contemporary idea about reinforcing the charging effect over the secured active sites for NRR by selectively choosing the electrolyte anions and functionalizing the active edges of the BNCO(1000)catalyst.

Institute of Nano Science and Technology(INST),Sector-81,Mohali,Punjab 140306,India;Department of Physics,SRM University-AP,Amaravati,Andhra Pradesh 522240,India

[1]Ashmita Biswas;Samadhan Kapse;Ranjit Thapa;Ramendra Sundar Dey-.Oxygen Functionalization-Induced Charging Effect on Boron Active Sites for High-Yield Electrocatalytic NH3 Production)[J].纳微快报（英文）,2022(12):464-480

enal,BNCO,2pz

Oxygen,Functionalization,Induced,Charging,Effect,Boron,Active,Sites,High,Yield,Electrocatalytic,NH3,Production,Ammonia,has,been,recognized,future,renewable,energy,fuel,because,its,wide,ranging,applications,H2,storage,transportation,sector,order,avoid,environmentally,hazardous,Haber,Bosch,process,recently,third,generation,ambient,ammonia,synthesis,drawn,phenom,attention,thus,tremendous,efforts,are,devoted,developing,efficient,electrocatalysts,that,would,circumvent,bottlenecks,electrochemical,nitrogen,reduction,reaction,NRR,like,competitive,hydrogen,evolution,poor,selectivity,N2,surface,Herein,report,oxygen,functionalized,boron,carbonitride,matrix,via,two,pyrolysis,technique,conductive,architecture,compatibility,orbital,charging,over,due,atoms,pentagon,altogether,facilitate,adsorption,active,sites,optimum,electrolyte,acidity,HCl,lowered,crowding,aid,protonation,steps,associative,alternating,pathway,which,gives,sufficiently,high,yield,mgcat,optimized,Faradaic,efficiency,RHE,This,work,offers,cost,effective,electrode,material,provides,contemporary,idea,about,reinforcing,secured,by,selectively,choosing,anions,functionalizing,edges

0.690314