Elucidating the Role of Single-Atom Pd for Electrocatalytic Hydrodechlorination
- 21 September 2021
- journal article
- research article
- Published by American Chemical Society (ACS) in Environmental Science & Technology
- Vol. 55 (19), 13306-13316
- https://doi.org/10.1021/acs.est.1c04294
Abstract
In this study, we loaded Pd catalysts onto a reduced graphene oxide (rGO) support in an atomically dispersed fashion [i.e., Pd single-atom catalysts (SACs) on rGO or Pd1/rGO] via a facile and scalable synthesis based on anchor-site and photoreduction techniques. The as-synthesized Pd1/rGO significantly outperformed the Pd nanoparticle (Pdnano) counterparts in the electrocatalytic hydrodechlorination of chlorinated phenols. Downsizing Pdnano to Pd1 leads to a substantially higher Pd atomic efficiency (14 times that of Pdnano), remarkably reducing the cost for practical applications. The unique single-atom architecture of Pd1 additionally affects the desorption energy of the intermediate, suppressing the catalyst poisoning by Cl–, which is a prevalent challenge with Pdnano. Characterization and experimental results demonstrate that the superior performance of Pd1/rGO originates from (1) enhanced interfacial electron transfer through Pd–O bonds due to the electronic metal–support interaction and (2) increased atomic H (H*) utilization efficiency by inhibiting H2 evolution on Pd1. This work presents an important example of how the unique geometric and electronic structure of SACs can tune their catalytic performance toward beneficial use in environmental remediation applications.Funding Information
- Division of Engineering Education and Centers (EEC-1449500)
- Division of Chemical, Bioengineering, Environmental, and Transport Systems (1955793)
- National Natural Science Foundation of China (51625801, 51878169)
- Guangdong Province
- Guangdong Innovation Team Project for Colleges and Universities (2016KCXTD023)
This publication has 75 references indexed in Scilit:
- Toxicological Profile of Chlorophenols and Their Derivatives in the Environment: The Public Health PerspectiveThe Scientific World Journal, 2013
- Highly Conductive and Porous Activated Reduced Graphene Oxide Films for High-Power SupercapacitorsNano Letters, 2012
- Single-atom catalysis of CO oxidation using Pt1/FeOxNature Chemistry, 2011
- The electrochemical approach to concerted proton—electron transfers in the oxidation of phenols in waterProceedings of the National Academy of Sciences of the United States of America, 2009
- Deactivation resistance of Pd/Au nanoparticle catalysts for water-phase hydrodechlorinationJournal of Catalysis, 2009
- Evidence for Concerted Proton−Electron Transfer in the Electrochemical Oxidation of Phenols with Water As Proton Acceptor. Tri-tert-butylphenol.Journal of the American Chemical Society, 2008
- Pentachlorophenol and Cancer Risk: Focusing the Lens on Specific Chlorophenols and ContaminantsEnvironmental Health Perspectives, 2008
- Electronic Transport Properties of Individual Chemically Reduced Graphene Oxide SheetsNano Letters, 2007
- Performance of alumina-supported noble metal catalysts for the combustion of trichloroethene at dry and wet conditionsApplied Catalysis B: Environmental, 2006
- Catalytic behaviour of Cl-free and Cl-containing Pd/Al2O3 catalysts in the total oxidation of methane at low temperatureApplied Catalysis A: General, 2000