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Bridge Bonded Oxygen Ligands between Approximated FeN 4 Sites Confer Catalysts with High ORR Performance
Author(s) -
Gong Liyuan,
Zhang Hao,
Wang Ying,
Luo Ergui,
Li Kui,
Gao Liqin,
Wang Yuemin,
Wu Zhijian,
Jin Zhao,
Ge Junjie,
Jiang Zheng,
Liu Changpeng,
Xing Wei
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202004534
Subject(s) - catalysis , boosting (machine learning) , chemistry , oxygen , oxygen atom , rational design , combinatorial chemistry , materials science , nanotechnology , stereochemistry , molecule , organic chemistry , computer science , machine learning
Abstract The applications of the most promising Fe—N–C catalysts are prohibited by their limited intrinsic activities. Manipulating the Fe energy level through anchoring electron‐withdrawing ligands is found effective in boosting the catalytic performance. However, such regulation remains elusive as the ligands are only uncontrollably introduced oweing to their energetically unstable nature. Herein, we report a rational manipulation strategy for introducing axial bonded O to the Fe sites, attained through hexa‐coordinating Fe with oxygen functional groups in the precursor. Moreover, the O modifier is stabilized by forming the Fe−O−Fe bridge bond, with the approximation of two FeN 4 sites. The energy level modulation thus created confers the sites with an intrinsic activity that is over 10 times higher than that of the normal FeN 4 site. Our finding opens a novel strategy to manage coordination environments at an atomic level for high activity ORR catalysts.