Atomic hydrogen-mediated enhanced electrocatalytic hydrodehalogenation on Pd@MXene electrodes
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...
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Published in | Journal of hazardous materials Vol. 459; p. 132113 |
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Main Authors | , , , , , |
Format | Journal Article |
Language | English |
Published |
Netherlands
Elsevier B.V
05.10.2023
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Subjects | |
Online Access | Get full text |
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Summary: | 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 (kobs) 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.
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•MXene remarkably decreased Pd particle size and enhanced its dispersity.•Pd@MXene catalyst promoted the generation of high-activity species of H*.•The H* mediated dehalogenation was the dominant pathway for DCF conversion.•DFT calculations demonstrated MXene modulated the electronic structure of Pd.•The Pd@MX/CC electrode demonstrated efficacy across a broad range of substrate concentrations and halogen pollutants types. |
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Bibliography: | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
ISSN: | 0304-3894 1873-3336 |
DOI: | 10.1016/j.jhazmat.2023.132113 |