化学
氧原子
还原(数学)
氧气
Atom(片上系统)
原子氧
路易斯酸
氧还原
无机化学
物理化学
分子
有机化学
催化作用
电化学
嵌入式系统
几何学
计算机科学
数学
电极
作者
Qingyun Qu,Yu Mao,Shufang Ji,Jiangwen Liao,Juncai Dong,Ligang Wang,Qichen Wang,Xiao Liang,Zedong Zhang,Jiarui Yang,Haijing Li,Yongfang Zhou,Ziyun Wang,Geoffrey I. N. Waterhouse,Dingsheng Wang,Yadong Li
摘要
Nitrogen-doped carbon-supported Fe catalysts (Fe-N-C) with Fe-N 4 active sites hold great promise for the oxygen reduction reaction (ORR). However, fine-tuning the structure of Fe-N 4 active sites to enhance their performance remains a grand challenge. Herein, we report an innovative design strategy to promote the ORR activity and kinetics of Fe-N 4 sites by engineering their Lewis acidity, which is achieved by tuning the spatial Fe coordination geometry. Theoretical calculations indicated that Fe 1 -N 4 SO 2 sites (with an axial –SO 2 group bonded to Fe) offered favorable Lewis acidity for the ORR, leading to optimized adsorption energies for the key ORR intermediates. To implement this strategy, we developed a molecular-cage-encapsulated coordination strategy to synthesize a Fe single-atom site catalyst (SAC) with Fe 1 -N 4 SO 2 sites. In agreement with theory, the Fe 1 -N 4 SO 2 /NC catalyst demonstrated outstanding ORR performance in both alkaline ( E 1/2 = 0.910 V in 0.1 M KOH) and acidic media ( E 1/2 = 0.772 V in 0.1 M HClO 4 ), surpassing commercial Pt/C and traditional Fe SACs with Fe 1 -N 4 sites or planar S-coordinated Fe 1 -N 4 -S sites. Moreover, this newly developed catalyst showed great application potential in quasi-solid-state Zn–air batteries, delivering superior performance across a wide temperature range.
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