材料科学
Atom(片上系统)
配位复合体
协调数
配位聚合物
结晶学
纳米技术
离子
冶金
金属
计算机科学
物理
复合材料
嵌入式系统
量子力学
化学
聚合物
作者
Yan Liu,Lei Zhang,Qiaoling Xu,Shijing Zhang,Yingtang Zhou,Guangzhi Hu
标识
DOI:10.1002/adfm.202413134
摘要
Abstract The development of efficient rare earth single‐atom (SA) catalysts for the oxygen reduction reaction (ORR) is essential yet challenging for high‐performance aluminum‐air batteries (AABs). This study introduces a concept‐to‐proof strategy for synthesizing a hollow carbon‐supported gadolinium (Gd) SA catalyst using low‐coordination and second‐coordination sphere engineering. In this design, Gd atoms are coordinated to three nitrogen (N) atoms in N‐doped carbon and surrounded by six phosphorus (P) atoms, forming Gd‐N 3 ‐P 6 sites. These catalysts demonstrated exceptional ORR performance, achieving a half‐wave potential of 0.895 V and superior durability compared to the commercial Pt/C benchmark. When integrated into AABs, they delivered impressive performance, with a peak power density of 257 mW/cm 2 and an energy density of 2916 Wh/kg, alongside enhanced cycling stability. In situ characterization and theoretical calculations revealed that the strategic placement of P atoms in the second coordination sphere significantly enhanced the valence state of the Gd site. This enhancement improved the adsorption capacity for O 2 and H 2 O while facilitating the rapid desorption of * OH intermediates during the ORR. This study offers valuable insights into the development of cost‐effective ORR catalysts, emphasizing the significance of modulating the local coordination environment of metal SA sites.
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