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Revealing Isolated M−N 3 C 1 Active Sites for Efficient Collaborative Oxygen Reduction Catalysis
Author(s) -
Li Feng,
Han GaoFeng,
Bu Yunfei,
Noh HyukJun,
Jeon JongPil,
Shin Tae Joo,
Kim SeokJin,
Wu Yuen,
Jeong Hu Young,
Fu Zhengping,
Lu Yalin,
Baek JongBeom
Publication year - 2020
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202008325
Subject(s) - catalysis , oxygen , chemistry , active site , oxygen reduction , oxygen atom , transition metal , atom (system on chip) , crystallography , carbon fibers , oxygen reduction reaction , inorganic chemistry , materials science , molecule , organic chemistry , electrochemistry , electrode , composite material , composite number , computer science , embedded system
Single atom catalysts (SACs) are of great importance for oxygen reduction, a critical process in renewable energy technologies. The catalytic performance of SACs largely depends on the structure of their active sites, but explorations of highly active structures for SAC active sites are still limited. Herein, we demonstrate a combined experimental and theoretical study of oxygen reduction catalysis on SACs, which incorporate M−N 3 C 1 site structure, composed of atomically dispersed transition metals (e.g., Fe, Co, and Cu) in nitrogenated carbon nanosheets. The resulting SACs with M−N 3 C 1 sites exhibited prominent oxygen reduction catalytic activities in both acidic and alkaline media, following the trend Fe−N 3 C 1 > Co−N 3 C 1 > Cu−N 3 C 1 . Theoretical calculations suggest the C atoms in these structures behave as collaborative adsorption sites to M atoms, thanks to interactions between the d / p orbitals of the M/C atoms in the M−N 3 C 1 sites, enabling dual site oxygen reduction.