Highly active and stable pyridine N-anchored single-atom palladium catalyst for electrocatalytic hydrodechlorination of 2,4-dichlorophenol

Mengyin Chen, Yang Fan, Haining Sun, Bolian Xu, Yubing Liu, Rongwei Shi, Naizhang Xu, Lijun Yang, Shupeng Zhang, Lei Yu, Yining Fan

Abstract: Electrocatalytic hydrodechlorination (EHDC) is promising for the removal of chlorophenol pollutants from water due to its mild reaction conditions, high efffciency and facile continuous operation. The previously reported lowcoordinationN-anchored single-atom Pd catalysts show excellent initial activity but suffer from deactivation induced by structural degradation, limiting their industrial applications. To resolve this issue, we proposed a novel strategy to construct a highly active, selective and stable electrocatalyst by implanting single-atom Pd₁ sites into FeCl₃-catalyzed carbonized covalent triazine framework (CTF)-derived carbon with abundant pyridine N atoms and a large speciffc surface area. These structural features facilitate the formation of well-deffned Pd1-N₄ sites via Pd ← N coordination. The Pd1-N4 sites promote the reaction between adsorbed H* species and 2,4- dichlorophenol (2,4-DCP) through the Eley-Rideal mechanism and improve H* utilization, thereby improving the catalytic activity. Furthermore, the Pd1-N₄ structure with ultrahigh metal-ligand bond dissociation energy overcomes the structural degradation-induced deactivation issue of the reported single-atom Pd catalyst. This work offers a universal and feasible design paradigm for developing high-performance single-atom electrocatalyststoward sustainable abatement of chlorinated organic pollutants.

原文：https://www.sciencedirect.com/science/article/pii/S1383586626026821

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