电催化剂
过电位
双功能
材料科学
析氧
催化作用
双金属片
杂原子
碳纤维
纳米材料基催化剂
化学工程
铼
纳米技术
金属
纳米颗粒
电极
电化学
物理化学
化学
有机化学
冶金
复合材料
工程类
戒指(化学)
复合数
作者
Xiaopeng Han,Xiaofei Ling,Deshuang Yu,Dengyu Xie,Linlin Li,Shengjie Peng,Cheng Zhong,Naiqin Zhao,Yida Deng,Wenbin Hu
标识
DOI:10.1002/adma.201905622
摘要
Abstract With the inspiration of developing bifunctional electrode materials for reversible oxygen electrocatalysis, one strategy of heteroatom doping is proposed to fabricate dual metal single‐atom catalysts. However, the identification and mechanism functions of polynary single‐atom structures remain elusive. Atomically dispersed binary Co‐Ni sites embedded in N‐doped hollow carbon nanocubes (denoted as CoNi‐SAs/NC) are synthesized via proposed pyrolysis of dopamine‐coated metal‐organic frameworks. The atomically isolated bimetallic configuration in CoNi‐SAs/NC is identified by combining microscopic and spectroscopic techniques. When employing as oxygen electrocatalysts in alkaline medium, the resultant CoNi‐SAs/NC hybrid manifests outstanding catalytic performance for bifunctional oxygen reduction/evolution reactions, boosting the realistic rechargeable zinc–air batteries with high efficiency, low overpotential, and robust reversibility, superior to other counterparts and state‐of‐the‐art precious‐metal catalysts. Theoretical computations based on density functional theory demonstrate that the homogenously dispersed single atoms and the synergistic effect of neighboring Co‐Ni dual metal center can optimize the adsorption/desorption features and decrease the overall reaction barriers, eventually promoting the reversible oxygen electrocatalysis. This work not only sheds light on the controlled synthesis of atomically isolated advanced materials, but also provides deeper understanding on the structure–performance relationships of nanocatalysts with multiple active sites for various catalytic applications.
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