Enhancing Green Ammonia Electrosynthesis Through Tuning Sn Vacancies in Sn‑Based MXene/ MAX Hybrids  

作　　者：Xinyu Dai Zhen‑Yi Du Ying Sun Ping Chen Xiaoguang Duan Junjun Zhang Hui Li Yang Fu Baohua Jia Lei Zhang Wenhui Fang Jieshan Qiu Tianyi Ma 

机构地区：[1]Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning Province,College of Chemistry,Institute of Clean Energy Chemistry,Liaoning University,Shenyang 110036,People’s Republic of China [2]State Key Laboratory of Clean and Efficient Coal Utilization,Taiyuan University of Technology,Taiyuan 030024,People’s Republic of China [3]School of Chemistry and Chemical Engineering,Anhui University,Hefei 230601,People’s Republic of China [4]School of Chemical Engineering,The University of Adelaide,Adelaide,SA 5005,Australia [5]State Key Laboratory of High‑Efficiency Utilization of Coal and Green Chemical Engineering,College of Chemistry and Chemical Engineering,Ningxia University,Yinchuan 750021,Ningxia,People’s Republic of China [6]School of Science,RMIT University,Melbourne,VIC 3000,Australia [7]Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials,School of Chemistry and Chemical Engineering,South China University of Technology,Guangzhou 510640,People’s Republic of China [8]College of Chemical Engineering,State Key Laboratory of Chemical Resource Engineering,Beijing University of Chemical Technology,Beijing 100029,People’s Republic of China

出　　处：《Nano-Micro Letters》2024年第5期154-168,共15页纳微快报（英文版）

基　　金：This work was supported by the National Natural Science Foundation of China(Nos.22308139,52071171,52202248);Natural Science Foundation of Liaoning Province(2023-MS-140);Liaoning BaiQianWan Talents Program(LNBQW2018B0048);Shenyang Science and Technology Project(21-108-9-04);Young Scientific and Technological Talents Project of the Department of Education of Liaoning Province(LQN202008);Key Research Project of Department of Education of Liaoning Province(LJKZZ20220015);Foundation of State Key Laboratory of Clean and Efficient Coal Utilization,Taiyuan University of Technology(MJNYSKL202301);Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(KF2023006);Anhui Province Key Laboratory of Coal Clean Conversion and High Valued Utilization,Anhui University of Technology(CHV22-05);Australian Research Council(ARC)through Future Fellowship(FT210100298,FT210100806);Discovery Project(DP220100603);Linkage Project(LP210100467,LP210200504,LP210200345,LP220100088);Industrial Transformation Training Centre(IC180100005)schemes;the Australian Government through the Cooperative Research Centres Projects(CRCPXIII000077).

摘　　要：Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia production.However,relevant out-lab research is still in its infancy.Herein,a novel Sn-based MXene/MAX hybrid with abundant Sn vacancies,Sn@Ti_(2)CTX/Ti_(2)SnC–V,was synthesized by controlled etching Sn@Ti_(2)SnC MAX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N2 reduction.Due to the synergistic effect of MXene/MAX heterostructure,the existence of Sn vacancies and the highly dispersed Sn active sites,the obtained Sn@Ti2CTX/Ti_(2)SnC–V exhibits an optimal NH_(3) yield of 28.4μg h^(−1) mg_(cat)^(−1) with an excellent FE of 15.57% at−0.4 V versus reversible hydrogen electrode in 0.1 M Na_(2)SO_(4),as well as an ultra-long durability.Noticeably,this catalyst represents a satisfactory NH3 yield rate of 10.53μg h^(−1) mg^(−1) in the home-made simulation device,where commercial electrochemical photovoltaic cell was employed as power source,air and ultrapure water as feed stock.The as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic analysis.This work is of significance for large-scale green ammonia production.

关 键 词：Green ammonia synthesis N2 electroreduction Renewable energy SN MXene/MAX hybrid 

分 类 号：TQ113.2[化学工程—无机化工]