Highly efficient atomic hydrogen-mediated electrochemical hydrodehalogenation of trichloroacetic acid on 3D hierarchical multi-transition metal selenides

Sukai Hu; Daiqi Wang; Maohong Fan; Bo Yang; Huihuang Chen

doi:10.1016/j.jhazmat.2023.132282

Highly efficient atomic hydrogen-mediated electrochemical hydrodehalogenation of trichloroacetic acid on 3D hierarchical multi-transition metal selenides

J Hazard Mater. 2023 Oct 5:459:132282. doi: 10.1016/j.jhazmat.2023.132282. Epub 2023 Aug 13.

Authors

Sukai Hu¹, Daiqi Wang¹, Maohong Fan², Bo Yang¹, Huihuang Chen³

Affiliations

¹ College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, PR China.
² College of Engineering and Physical Sciences, University of Wyoming, Laramie, WY 82071, USA; College of Engineering, Georgia Institute of Technology, Atlanta, GA 30332, USA.
³ College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, PR China. Electronic address: hhchen@ustc.edu.cn.

PMID: 37591175
DOI: 10.1016/j.jhazmat.2023.132282

Abstract

Halogenated organic compounds as highly focused emerging contaminants pose a long-lasting threat to human health and the aquatic environment due to their high toxicities and strong anti-biodegradation characteristics. Electrochemical hydrodehalogenation (ECHD) is a promising technology with a low-carbon footprint to remove halogenated organic compounds while suffering from a lack of efficient and robust earth-abundant electrocatalysts. Herein, by integrating two kinds of transition metal dichalcogenides (i.e., MoSe₂ nanosheet and Ni₃Se₂ nanowire) into a conductive 3D porous network nickel foam, we obtained a hierarchical architecture (MoSe₂/Ni₃Se₂@NF) that promises high surface area, fast charge transfer and efficient mass transfer. The interface-confined epitaxial growth of Ni₃Se₂ nanowires on nickel foam provides abundant sites for the vertical growth of MoSe₂ nanosheets, which endows MoSe₂ with maximal accessible active edge sites to participate in the ECHD process. Benefiting from such a hierarchical 3D porous configuration, trichloroacetic acid (5 mg/L) was removed over 95% by MoSe₂/Ni₃Se₂@NF at - 1.2 V vs. SCE after 1 h, which dramatically outperformed that for NF (20%) and Ni₃Se₂@NF (53.2%). The major contributor to such boosted performance is the adsorbed atomic hydrogen (*H) generated during water splitting via suppressing hydrogen-hydrogen dimerization, as evidenced by radical quenching experiments and electron paramagnetic resonance spectroscopy. This study offers appealing opportunities for tailoring the catalytic performance of noble-metal-free heterogeneous catalysts for various applications that require noble-metal catalysts.

Keywords: Atomic hydrogen (*H); Electrochemical hydrodehalogenation; Halogenated organic pollutants; Non-noble metal catalysis; Transition metal dichalcogenides.