Catalytic degradation of benzene at room temperature over FeN4O2 sites embedded in porous carbon

Hui Ding; Lingxiao Xue; Jiahao Cui; Yongqiang Wang; Dan Zhao; Xing Zhi; Rui Liu; Jianfeng Fu; Shejiang Liu; Bingfeng Fu; Jiahui Shi; Ximeng Xu; Gang Kevin Li

doi:10.1016/j.jhazmat.2023.132520

Catalytic degradation of benzene at room temperature over FeN₄O₂ sites embedded in porous carbon

J Hazard Mater. 2023 Oct 15:460:132520. doi: 10.1016/j.jhazmat.2023.132520. Epub 2023 Sep 9.

Authors

Hui Ding¹, Lingxiao Xue², Jiahao Cui³, Yongqiang Wang⁴, Dan Zhao³, Xing Zhi⁵, Rui Liu³, Jianfeng Fu³, Shejiang Liu³, Bingfeng Fu⁶, Jiahui Shi³, Ximeng Xu³, Gang Kevin Li⁷

Affiliations

¹ School of Environmental Science and Engineering, Tianjin University, Tianjin, China. Electronic address: dinghui@tju.edu.cn.
² School of Environmental Science and Engineering, Tianjin University, Tianjin, China; Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai, China.
³ School of Environmental Science and Engineering, Tianjin University, Tianjin, China.
⁴ School of Environmental Science and Engineering, Tianjin University, Tianjin, China; Department of Chemical Engineering, The University of Melbourne, Parkville, Victoria 3010, Australia. Electronic address: wangyongqiang@tju.edu.cn.
⁵ Department of Mechanical Engineering, The University of Melbourne, Parkville, Victoria 3010, Australia.
⁶ Shenzhen Yuanqi Environmental Energy Technology Co., Ltd., Futian District, Shenzhen, China.
⁷ Department of Chemical Engineering, The University of Melbourne, Parkville, Victoria 3010, Australia. Electronic address: li.g@unimelb.edu.au.

PMID: 37703730
DOI: 10.1016/j.jhazmat.2023.132520

Abstract

Benzene and its aromatic derivatives are typical volatile organic compounds for indoor and outdoor air pollution, harmful to human health and the environment. It has been considered extremely difficult to break down benzene rings at ambient conditions without external energy input, due to the extraordinary stability of the aromatic structure. Here, we show one such solution that can thoroughly degrade benzene to basically water and carbon dioxide at 25 °C in air using atomically dispersed Fe in N-doped porous carbon, with almost 100% benzene conversion. Further experimental studies combined with molecular simulations reveal the mechanism of this catalytic reaction. Hydroxyl radicals (·OH) evolved on the atomically dispersed FeN₄O₂ catalytic centers were found responsible for initiating and completing the oxidation of benzene. This work provides a new chemistry to degrade aromatics at ambient conditions and also a pathway to generate active ·OH oxidant for generic remediation of organic pollutants.

Keywords: Aromatic VOCs; Atomically dispersed Fe catalyst; Benzene oxidation mechanism; Catalytic oxidation; Hydroxyl radicals.