Recycling synthesis of single-atom Zn-nitrogen-carbon catalyst for electrocatalytic reduction of O_(2)to H_(2)O_(2)  

ZnNC的循环合成及其在氧还原法制备过氧化氢中的应用

作　　者：Jialun Tang Shuhui Xu Kai Sun Xueqing Gao Aibing Chen Shubo Tian Daojin Zhou Xiaoming Sun 汤加伦;徐淑慧;孙恺;高学庆;陈爱兵;田书博;周道金;孙晓明(Beijing Advanced Innovation Center for Soft Matter Science and Engineering,State Key Laboratory of Chemical Resource Engineering,College of Chemistry,Beijing University of Chemical Technology,Beijing 100029,China;College of Chemical and Pharmaceutical Engineering,Hebei University of Science and Technology,Shijiazhuang 050018,China)

机构地区：[1]Beijing Advanced Innovation Center for Soft Matter Science and Engineering,State Key Laboratory of Chemical Resource Engineering,College of Chemistry,Beijing University of Chemical Technology,Beijing 100029,China [2]College of Chemical and Pharmaceutical Engineering,Hebei University of Science and Technology,Shijiazhuang 050018,China

出　　处：《Science China Materials》2022年第12期3490-3496,共7页中国科学（材料科学（英文版）

基　　金：financially supported by the National Key Research and Development Program of China (2018YFA0702002);the National Natural Science Foundation of China (21935001, 22101015, 22175012 and 22005022);the Royal Society and Newton Fund through Newton Advanced Fellowship award (NAFR1191294);the Program for Changjiang Scholars and Innovation Research Team in the University (IRT1205);the Fundamental Research Funds for the Central Universities, Beijing Natural Science Foundation (2214062);the S&T Program of Hebei (21344601D)

摘　　要：Portable electrochemical synthesis of H_(2)O_(2),which is widely used for disinfection,sterilization,and waste treatment,has attracted increasing attention.However,low atomic utilization efficiency and by-product disposal during the synthesis of electrocatalysts are inevitable.Based on the advantages of single-atom catalysts(SACs)towards H_(2)O_(2)synthesis via a 2e−transfer oxygen reduction reaction,this work presents the synthesis of ZnNC SACs as excellent oxygen reduction catalysts with high atomic use efficiency and almost no generated waste by using formamide and metal powder as precursors.The ZnNC SACs exhibit H_(2)O_(2)selectivity exceeding 80%when working continuously for 10,000 s.The synthetic strategy described in this paper is intended to be used as a supplement to the synthesis of metal-nitrogen-carbon SACs with high atomic utilization efficiency and low waste generation for environmental and chemical applications.电催化制备过氧化氢并用于消毒、灭菌和废物处理,是一种具有可移动性且适用于家庭规模的过氧化氢制备方法.但催化剂制备过程中对于原材料的原子利用率低,制备过程涉及到大量废气、废液的排放.本文基于单原子催化剂可高效电催化制备过氧化氢的特点,提出利用甲酰胺和金属单质作为前驱物循环制备单原子锌-氮-碳催化剂的方法.该催化剂在制备过程中产生废物少,在氧还原反应中催化产生过氧化氢的选择性超过80%,连续工作超过10,000秒无明显活性衰减.本文提出的单原子材料的绿色合成策略对于其他类型单原子材料的制备具有启发性和普适性,将大力推动单原子催化剂的制备及未来应用.

关 键 词：single-atom catalysts formamide pyrolysis recycling fabrication H_(2)O_(2)production 

分 类 号：TQ123.6[化学工程—无机化工] TQ426