H*ads dynamics engineering via bimetallic Pd-Cu@MXene catalyst for enhanced electrocatalytic hydrodechlorination

Lan-Ying Liu; Min-Hua Cui; John Justo Ambuchi; Shi-Ming Niu; Xin-Hui Li; Wo-Long Wang; He Liu; Guo-Shuai Liu; Ai-Jie Wang

doi:10.1016/j.envres.2024.118859

H*_ads dynamics engineering via bimetallic Pd-Cu@MXene catalyst for enhanced electrocatalytic hydrodechlorination

Environ Res. 2024 Apr 3;252(Pt 1):118859. doi: 10.1016/j.envres.2024.118859. Online ahead of print.

Authors

Lan-Ying Liu¹, Min-Hua Cui², John Justo Ambuchi³, Shi-Ming Niu¹, Xin-Hui Li¹, Wo-Long Wang¹, He Liu⁴, Guo-Shuai Liu¹, Ai-Jie Wang⁵

Affiliations

¹ Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environment & Ecology, Jiangnan University, Wuxi, 214122, PR China.
² Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environment & Ecology, 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.
³ Department of Agriculture and Environmental Studies, Rongo University, Rongo, Kenya.
⁴ Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environment & Ecology, 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.
⁵ 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: 38574986
DOI: 10.1016/j.envres.2024.118859

Abstract

Electrocatalytic hydrodechlorination (EHDC) is a promising approach to safely remove halogenated emerging contaminants (HECs) pollutants. However, sluggish production dynamics of adsorbed atomic H (H*_ads) limit the applicability of this green process. In this study, bimetallic Pd-Cu@MXene catalysts were synthesized to achieve highly efficient removal of HECs. The alloy electrode (Pd-Cu@MX/CC) exhibited better EHDC performance in comparison to Pd@MX/CC electrode, resulting in diclofenac degradation efficiency of 93.3 ± 0.1%. The characterization analysis revealed that the Pd⁰/Pd^II ratio decreased by forming bimetallic Pd-Cu alloy. Density functional theory calculations further demonstrated the electronic configuration modulation of the Pd-Cu@MXene catalysts, optimizing binging energies for H* and thereby facilitating H*_ads production and tuning the reduction capability of H*_ads. Noteably, the amounts and reduction potential of H*_ads for Pd-Cu@MXene catalysts were 1.5 times higher and 0.37 eV lower than those observed for the mono Pd electrode. Hence, the introduction of Cu into the Pd catalyst optimized the dynamics of H*_ads production, thereby conferring significant advantages to EHDC reactions. This augmentation was underscored by the successful application of the alloy catalysts supported by MXene in EHDC experiments involving other HECs, which represented a new paradigm for EHDC for efficient recalcitrant pollutant removal by H*_ads.

Keywords: Adsorbed atomic H (H*(ads)); Bimetallic Pd–Cu nanoparticles; Density functional theory (DFT) calculation; Electrocatalytic hydrodehalogenation (EHDC); MXene.