Atomic hydrogen-mediated enhanced electrocatalytic hydrodehalogenation on Pd@MXene electrodes

Lan-Ying Liu; Guo-Shuai Liu; Shi-Ming Niu; He Liu; Min-Hua Cui; Ai-Jie Wang

doi:10.1016/j.jhazmat.2023.132113

Atomic hydrogen-mediated enhanced electrocatalytic hydrodehalogenation on Pd@MXene electrodes

J Hazard Mater. 2023 Oct 5:459:132113. doi: 10.1016/j.jhazmat.2023.132113. Epub 2023 Jul 22.

Authors

Lan-Ying Liu¹, Guo-Shuai Liu¹, Shi-Ming Niu¹, He Liu², Min-Hua Cui³, Ai-Jie Wang⁴

Affiliations

¹ Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environmental and Civil Engineering, Jiangnan University, Wuxi 214122, PR China.
² Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environmental and Civil Engineering, Jiangnan University, Wuxi 214122, PR China; Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Suzhou University of Science and Technology, Suzhou 215009, PR China.
³ Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environmental and Civil Engineering, Jiangnan University, Wuxi 214122, PR China; Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Suzhou University of Science and Technology, Suzhou 215009, PR China. Electronic address: cuiminhua@jiangnan.edu.cn.
⁴ Key Laboratory of Environmental Biotechnology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, PR China; School of Civil & Environmental Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, PR China.

PMID: 37487329
DOI: 10.1016/j.jhazmat.2023.132113

Abstract

In this study, a Pd@MXene catalyst was synthesized to enhance the electrocatalytic hydrodehalogenation (ECH) of emerging halogenated organic pollutants (HOPs) by improving the dispersibility, catalytic activity, and stability of palladium (Pd). The average size of Pd nanoparticles (NPs) was reduced to 3.62 ± 0.34 nm with a more intensive peak of Pd (111), which facilitated atomic hydrogen (H*) production. The Pd@MX/CC electrode demonstrated superior ECH activity for diclofenac (DCF) degradation, with a reaction rate constant (k_obs) 2.48 times higher than that of Pd/CC (without MXene). The satisfactory ECH performance of Pd@MX/CC remained consistent within a wide range of initial DCF concentrations (5-100 mg/L), and no significant ECH attenuation was observed even after up to 10 batches. Furthermore, the high activity of Pd@MX/CC was also observed in the ECH of other halogenated organic pollutants (levofloxacin, tetrabromobisphenol A, and diatrizoate). Density functional theory (DFT) calculations revealed that electronic configuration modulation of the Pd@MXene catalyst optimized binging energies to H* , DCF, and dechlorinated products, thereby enhancing the ECH efficiency of DCF.

Keywords: Atomic hydrogen (H*); Density functional theory (DFT) calculation; Electrocatalytic hydrodehalogenation (ECH); MXene; Palladium (Pd).