双功能Nb-N-C原子分散催化剂用于水系锌-空气电池驱动CO_(2)还原  

Bifunctional Nb-N-C atomic catalyst for aqueous Zn-air battery driving CO_(2) electrolysis

作　　者：高三双 王天玮 靳梦梦 张书胜 刘倩 胡广志 杨慧 罗俊 刘熙俊 Sanshuang Gao;Tianwei Wang;Mengmeng Jin;Shusheng Zhang;Qian Liu;Guangzhi Hu;Hui Yang;Jun Luo;Xijun Liu(Institute for New Energy Materials and Low-Carbon Technologies,Tianjin Key Lab for Photoelectric Materials&Devices,School of Materials Science and Engineering,Tianjin University of Technology,Tianjin 300384,China;MOE Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials,and Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials,School of Resource,Environments and Materials,Guangxi University,Nanning 530004,China;College of Chemistry,Zhengzhou University,Zhengzhou 450000,China;Institute for Advanced Study,Chengdu University,Chengdu 610106,China;Institute for Ecological Research and Pollution Control of Plateau Lakes School of Ecology and Environmental Science,Yunnan University,Kunming 650504,China;Shenzhen Institute for Advanced Study,University of Electronic Science and Technology of China,Shenzhen 518110,China)

机构地区：[1]Institute for New Energy Materials and Low-Carbon Technologies,Tianjin Key Lab for Photoelectric Materials&Devices,School of Materials Science and Engineering,Tianjin University of Technology,Tianjin 300384,China [2]MOE Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials,and Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials,School of Resource,Environments and Materials,Guangxi University,Nanning 530004,China [3]College of Chemistry,Zhengzhou University,Zhengzhou 450000,China [4]Institute for Advanced Study,Chengdu University,Chengdu 610106,China [5]Institute for Ecological Research and Pollution Control of Plateau Lakes School of Ecology and Environmental Science,Yunnan University,Kunming 650504,China [6]Shenzhen Institute for Advanced Study,University of Electronic Science and Technology of China,Shenzhen 518110,China

出　　处：《Science China Materials》2023年第3期1013-1023,共11页中国科学（材料科学（英文版）

基　　金：supported by the National Natural Science Foundation of China(22075211,21601136,22109118,51971157,and 51621003).

摘　　要：设计廉价和高效的双功能催化剂应用于CO_(2)还原和O_(2)还原反应(CO_(2)RR和ORR)是实现碳中和的理想选择.因此,本文研制出铌原子分散固定在氮掺杂有序介孔碳(Nb-N-C)上的双功能CO_(2)RR和ORR催化剂用于锌-空气电池(ZAB)自驱动CO_(2)RR.得益于高铌原子利用率和有序介孔结构,Nb-N-C催化剂展现出高达90%的CO法拉第效率,ORR的半波电位活性为0.84 V,ZAB的峰值功率活性为115.6 mW cm-2.此外,采用两个串联的ZABs单元作为自供能CO_(2)RR系统的电源,能够连续将C O_(2)转化为C O.该自供能系统前10小时的C O平均产率为3.75μmol h-1mg-1cat.理论计算表明,铌原子分散固定在氮掺杂的碳上形成Nb–N配位键,从而有效地降低CO_(2)RR的决速中间体*COOH和ORR的决速中间体*O的生成能垒.Designing efficient and cost-effective bifunctional catalysts is desirable for carbon dioxide and oxygen reduction reactions (CO_(2)RR and ORR) to address carbon neutralization and energy conversion.Herein,a bifunctional CO_(2)RR and ORR catalyst for aqueous Zn-air battery (ZAB)self-driving CO_(2)RR electrolysis is developed using atomically dispersed niobium anchored onto N-doped ordered mesoporous carbon (Nb-N-C).The Nb-N-C atomic catalyst demonstrates aqueous CO_(2)RR activity with CO Faradaic efficiency up to 90%,ORR activity with a half-wave potentia of 0.84 V vs.reversible hydrogen electrode,and ZAB activity with a peak power density of 115.6 mW cm-2,owing to the high Nb atom-utilization efficiency and ordered mesoporous structure.Furthermore,two-unit ZABs in series,serving as the power source for the self-powered CO_(2)electrolysis system continuously convert CO_(2)to CO with average productivity of3.75μmol h-1mg-1catduring the first 10 h.Moreover,theoretical calculations exhibit that atomic Nb anchored to N-doped carbon can form Nb–N coordination bonds,effectively reducing the energy barriers of potential-determining*COOH for CO_(2)RR and*O formation for ORR.

关 键 词：有序介孔碳 配位键 还原反应 双功能催化剂 半波电位 原子利用率 氮掺杂 能垒 

分 类 号：TQ426[化学工程] TM911.41[电气工程—电力电子与电力传动]