Electron Donor–Acceptor Activated Single Atomic Sites for Boosting Oxygen Reduction Reaction
Shenghua Ye, Dantong Zhang, Zhi‐Jun Ou, Lirong Zheng, Wenchao Liu, Wenda Chen, Yuan Xu, Yongliang Li, Xiangzhong Ren, Xiaoping Ouyang, Dongfeng Xue, Xueqing Yan, Qianling Zhang, Jian‐Hong Liu
Abstract
Abstract Fabricating efficient non‐platinum‐group‐metal catalysts for the oxygen reduction reaction (ORR) in proton‐exchange membrane fuel cells still remains a big challenge. This study creates a unique bamboo‐like architecture of Mn and Fe single atomic sites (SASs) anchored on core‐shell structure of nanopaticles@carbon nanotubes (MnFe SASs/NPs@CNTs) via a precursor route, where the Fe nanoparticles (NPs) (identified as γ‐Fe and Austenite) are confined into CNTs, such an architecture exhibits compelling ORR activity and durability in 0.1 m HClO 4 . Experiments and calculations both reveal that the electron donor–acceptor paradigm between Mn SASs and Fe NPs launches a lattice‐electron coupling mechanism not only increasing occupation of π ‐antibonding orbital in Mn− * O intermediates but also rising Jahn–Teller effect, thereby destabilize the Mn− * O intermediate and eventually facilitate the potential‐limiting step from * O to * OH. Such a coupling activation of the ORR‐inert Mn SASs greatly improves ORR performances of MnFe SASs/NPs@CNTs.