期刊
ACS ENERGY LETTERS
卷 6, 期 9, 页码 3359-3366出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.1c01316
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资金
- National Natural Science Foundation of China [11875257, U1932212, U1932109]
- Postdoctoral Science Foundation of China [2020M682042]
Understanding the evolving dynamics of the catalytic active center is crucial for the development of efficient catalysts. Through synchrotron-based techniques, this study revealed the highly active Fe single-site catalyst structure and its excellent catalytic performance in the oxygen reduction reaction.
Understanding the nature of the catalytic active center and its evolving dynamics under operating conditions is critical for the development of efficient and highly selective catalysts. By combining synchrotron-based operando X-ray absorption and infrared spectroscopies, here we uncover at an atomic level a hydroxyl was coupled on the dynamically released coordination-unsaturated Fe-N-2 moieties to form a highly active OH-Fe-N-2 structure and then promotes the adsorption of O-2 during the catalytic oxygen reduction reaction (ORR), which greatly facilitates the fabrication of the key *OOH intermediate and simplifies the fracture of the O-O bond to accelerate the multielectron reaction kinetics. The resulting covalent organic framework-derived Fe single-site catalyst could efficiently deliver an excellent ORR catalytic activity with an extremely large kinetic current density (J(k)) of 81.3 mA cm(-2) and an extra high turnover frequency of 5804 h(-1), 20 times that of the Pt-C catalyst (288 h(-1), 7.7 mA cm(-2)).
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