Ultrafast and energy-saving microwave-assisted conversion of inert carbon nanomaterials to highly efficient Fenton-like metal-free catalysts for pollutants degradation

Qi Fu; Huajie Zhong; Yu Hou; Jiaxing Yu; Huangsheng Yang; Nan Li; Yuanjun Tong; Songbo Wei; Junhui Wang; Gangfeng Ouyang

doi:10.1016/j.scitotenv.2023.166121

Ultrafast and energy-saving microwave-assisted conversion of inert carbon nanomaterials to highly efficient Fenton-like metal-free catalysts for pollutants degradation

Sci Total Environ. 2023 Dec 1:902:166121. doi: 10.1016/j.scitotenv.2023.166121. Epub 2023 Aug 8.

Authors

Qi Fu¹, Huajie Zhong², Yu Hou¹, Jiaxing Yu¹, Huangsheng Yang¹, Nan Li¹, Yuanjun Tong¹, Songbo Wei³, Junhui Wang⁴, Gangfeng Ouyang⁵

Affiliations

¹ MOE Key Laboratory of Bioinorganic and Synthetic Chemistry/KLGHEI of Environment and Energy Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou, Guangdong 510275, China.
² School of Chemical Engineering and Technology, Sun Yat-Sen University, Zhuhai 519082, Guangdong, China.
³ Department of Chemistry, University of California, Riverside, CA 92521, USA.
⁴ School of Chemical Engineering and Technology, Sun Yat-Sen University, Zhuhai 519082, Guangdong, China. Electronic address: wangjh36@mail.sysu.edu.cn.
⁵ MOE Key Laboratory of Bioinorganic and Synthetic Chemistry/KLGHEI of Environment and Energy Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou, Guangdong 510275, China; College of Chemistry & Molecular Engineering, Center of Advanced Analysis and Computational Science, Zhengzhou University, Zhengzhou 450001, China; Guangdong Provincial Key Laboratory of Emergency Test for Dangerous Chemicals, Guangdong Institute of Analysis (China National Analytical Center Guangzhou), Guangdong Academy of Science, 100 Xianlie Middle Road, Guangzhou 510070, China.

PMID: 37562621
DOI: 10.1016/j.scitotenv.2023.166121

Abstract

Carbon-driven persulfate (PDS)-based Fenton-like reactions have been widely viewed as prospective strategies to cope with the water pollution. However, high cost, harsh condition and complex modification processes are usually required to boost the catalytic activities of carbocatalysts. Herein, we proposed an ultrafast, energy-efficient, and convenient approach to convert various low-performance carbon materials into highly efficient catalysts by microwave treatment in just 1 min without any other tedious treatment. This process only requires 57 kJ/g energy input, 5 orders of magnitude lower than the traditional calcination process. The catalytic performance of microwave-treated materials could increase by more than 380 times, which is even better than those of the single-atom catalysts. Moreover, DFT calculations and QSARs analyses reveal that the negatively charged carboxyl group is not conducive to the adsorption of PDS (S₂O₈^2-) due to electrostatic repulsion, and also increases the work function of the carbocatalysts, which hinders the electron transfer process.

Keywords: Carbon nanomaterials; Carboxyl group; Fenton-like reaction; Microwave treatment; Persulfate.