催化作用
碳纤维
材料科学
纳米技术
兴奋剂
化学工程
化学
无机化学
有机化学
光电子学
复合数
工程类
复合材料
作者
Xingmei Guo,Jing Shi,Ming Li,Junhao Zhang,Xiangjun Zheng,Yuanjun Liu,Shenglin Xiong,Xuguang An,Zhongyao Duan,Qianqian Fan,Fei Gao,Shenglin Xiong
标识
DOI:10.1002/ange.202314124
摘要
Abstract Constructing atom‐clusters (ACs) with in situ modulation of coordination environment and simultaneously hollowing carbon support are critical yet challenging for improving electrocatalytic efficiency of atomically dispersed catalysts (ADCs). Herein, a general diffusion‐controlled strategy based on spatial confining and Kirkendall effect is proposed to construct metallic ACs in N,P,S triply‐doped hollow carbon matrix (M ACs /NPS−HC, M=Mn, Fe, Co, Ni, Cu). Thereinto, Fe ACs /NPS−HC with the best catalytic activity for oxygen reduction reaction (ORR) is thoroughly investigated. Unlike the benchmark sample of symmetrical N‐surrounded iron single‐atoms in N‐doped carbon (Fe SAs /N−C), Fe ACs /NPS−HC comprises bi‐/tri‐atomic Fe centers with engineered S/N coordination. Theoretical calculation reveals that proper Fe gathering and coordination modulation could mildly delocalize the electron distribution and optimize the free energy pathways of ORR. In addition, the triple doping and hollow structure of carbon matrix could further regulate the local environment and allow sufficient exposure of active sites, resulting in more enhanced ORR kinetics on Fe ACs /NPS−HC. The zinc‐air battery assembled with Fe ACs /NPS−HC as cathodic catalyst exhibits all‐round superiority to Pt/C and most Fe‐based ADCs. This work provides an exemplary method for establishing atomic‐cluster catalysts with engineered S‐dominated coordination and hollowed carbon matrix, which paves a new avenue for the fabrication and optimization of advanced ADCs.
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