Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 33, Pages 13923-13928Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202004534
Keywords
electronic structure; iron; O ligands; oxygen reduction; single-atom catalysts
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Funding
- National Natural Science Foundation of China [21633008, 21875243, 21673220, U1601211]
- National Science and Technology Major Project [2017YFB0102900]
- Jilin Province Science and Technology Development Program [20190201270JC, 20180101030JC]
- Gusu talent program
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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.
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