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Research Article | Open Access

A single-atom Fe–N2 embedded in nitrogen-doped porous carbon as a bifunctional photocatalyst for efficient removal of marine petroleum pollutants

Xin LiaYuwen ChenaZhiyue ZhaoaYizhe HuangaKe ZhuaSitong FengbShaojuan Luob( )Lei Wangc( )Kai Yana( )
Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou, 510275, PR China
School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, 510006, PR China
School of Materials and Environmental Engineering, Institute of Urban Ecology and Environment Technology, Shenzhen Polytechnic, Shenzhen, PR China
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HIGHLIGHTS

● A Fe–N2 single-atom embedded in Ndoped porous carbon (FC) was fabricated.

● The FC achieved a synergistic effect of BPA oxidation and Cr(Ⅵ) reduction.

● ·OH and e were the main ROS used for photo-oxidation and reduction, respectively.

● Possible pathways for BPA degradation and decreased biotoxicity are proposed.

● The FC-BPA-Cr(Ⅵ) system has the potential to remove pollutants from seawater.

Abstract

Petroleum and its refined products enter the marine environment during the extraction process, causing serious pollution. Herein, a bifunctional Fe–N2 single-atom embedded in nitrogen-doped porous carbon photocatalyst (FC) was fabricated for the efficient removal of marine petroleum pollutants. The combination of highly dispersed Fe–N2 active sites, large surface area, high porosity, and good conductivity results in excellent photocatalytic activities. The FC catalyst exhibited a 96.7% degradation rate in the oxidative removal of bisphenol A (BPA) and a 63.4% reduction of Cr(Ⅵ) within 1 ​h, whereas the reaction equilibrium rate constants of 0.0132 ​min−1 and 0.0505 ​min−1 were reached, respectively. FC with good stability and reusability could reach 88.3% and 53.5% removal rate of BPA and Cr(Ⅵ) after 5 cycles. Radical quenching experiments and electron spin resonance (ESR) confirmed that ·OH and e were the most driving active species for photo-oxidation and reduction, respectively. Besides, the FC catalyst was applied to an actual seawater system and the simulation results showed a good removal rate (82.7% of BPA and 50.9% of Cr(Ⅵ) within 1 ​h). The BPA oxidation pathway in the system was proposed and the toxicity of each intermediate was accessed. This work offers a new way to construct single-atom functionalized carbon-based catalysts for marine pollution control.

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References

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Environmental Functional Materials
Pages 48-57

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Cite this article:
Li X, Chen Y, Zhao Z, et al. A single-atom Fe–N2 embedded in nitrogen-doped porous carbon as a bifunctional photocatalyst for efficient removal of marine petroleum pollutants. Environmental Functional Materials, 2023, 2(1): 48-57. https://doi.org/10.1016/j.efmat.2023.04.001

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Received: 07 March 2023
Revised: 17 April 2023
Accepted: 27 April 2023
Published: 12 May 2023
© 2023 The Authors.

This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).