Research Article


2020, 13(8): 2079–2084


Synergy of Fe-N4 and non-coordinated boron atoms for highly selective oxidation of amine into nitrile

Hong-Hui Wang1, Li-Bing Lv1, Shi-Nan Zhang1, Hui Su1, Guang-Yao Zhai1, Wei-Wei Lei2, Xin-Hao Li1 (✉), and Jie-Sheng Chen1

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1 School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
2 Institute for Frontier Materials, Deakin University, Victoria 3216, Australia

Keywords: atomically dispersed catalyst, Fe-N4, non-coordinated boron, selective oxidation, nitrile
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The rational design of highly active and stable atomically dispersed M-X4 (M = Fe, Co, Ni, etc., X = C, N) -based catalysts holds promises for wide application in almost all realms of catalysis. Despite great effort in the construction of specific M-X4 centers, the possible effect of non-coordinated heteroatoms on the catalytic activity of metal centers has been rarely explored. Herein, we develop a new type of M-X4 catalyst composed of Fe-N4 centers and non-coordinated B heteroatoms (FeNC+B) and find the key role of non-coordinated B adjacent to Fe-N4 centers in tailoring their electron density and final catalytic selectivity. The experimental and theoretical results demonstrated that non-coordinated boron atoms could decrease the electron density of Fe-N4 centers to a suitable level and thus boost the selective production of nitriles from amine oxidation by depressing the formation of imines due to the flattened energy barrier of the reversible conversion of imines back to amines. As a reusable heterocatalyst, the state-of-the-art FeNC+B catalyst provides a turn-over frequency (TOF) value of 21.6 molbenzonitrile·molFe−1·h−1 (100 °C), outpacing that of bench-marked nonnoble-metal-based homogeneous catalyst by a factor of 3.4.
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Synergy of Fe-N4 and non-coordinated boron atoms for highly selective oxidation of amine into nitrile. Nano Res. 2020, 13(8): 2079–2084

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