Pd nanoparticles on defective polymer carbon nitride: Enhanced activity and origin for electrocatalytic hydrodechlorination reaction

Here we report a facile defect-engineering strategy on the support to optimize the metal-support interaction and enhance the metal's electrocatalytic hydrodechlorination performance in converting 2,4-dichlorophenol (2,4-DCP) to phenol. The specific activity of the Pd nanoparticles (Pd NPs) on defective polymer carbon nitride (Pd/PCN-x) reaches 0.09 min(-1) m(-2) Pd, which is 1.5 times that of the Pd NPs supported on the perfect PCN (Pd/PCN-0). The combined experimental and theoretical results demonstrate that the strong adsorption of phenol on Pd/PCN-0 passivates the active sites, limiting the dechlorination progress. The PCN-x containing-C=N defects can effectively mediate the spatial configuration and electronic structure of Pd NPs, and promote the preferential adsorption of 2,4-DCP rather than phenol, resulting in an enhanced dechlorination efficiency. (C) 2020 Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences. Published by Elsevier B.V. All rights reserved.