Boosting Benzene Oxidation with a Spin-State-Controlled Nuclearity Effect on Iron Sub-Nanocatalysts

Fanle Bu, Chaoqiu Chen, Yu Yu, Wentao Hao, Shichao Zhao, Yongfeng Hu, Yong Qin

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摘要

A fundamental understanding of the nature of nuclearity effects is important for the rational design of superior sub-nanocatalysts with low nuclearity, but remains a long-standing challenge. Using atomic layer deposition, we precisely synthesized Fe sub-nanocatalysts with tunable nuclearity (Fe1–Fe4) anchored on N,O-co-doped carbon nanorods (NOC). The electronic properties and spin configuration of the Fe sub-nanocatalysts were nuclearity dependent and dominated the H2O2 activation modes and adsorption strength of active O species on Fe sites toward C−H oxidation. The Fe1-NOC single atom catalyst exhibits state-of-the-art activity for benzene oxidation to phenol, which is ascribed to its unique coordination environment (Fe1N2O3) and medium spin state (t2g4eg1); turnover frequencies of 407 h−1 at 25 °C and 1869 h−1 at 60 °C were obtained, which is 3.4, 5.7, and 13.6 times higher than those of Fe dimer, trimer, and tetramer catalysts, respectively.

源语言英语
文章编号e202216062
期刊Angewandte Chemie - International Edition
62
3
DOI
出版状态已出版 - 16 1月 2023
已对外发布

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