Direct insights into the role of epoxy groups on cobalt sites for acidic H2O2 production
Open Access
- 21 August 2020
- journal article
- research article
- Published by Springer Science and Business Media LLC in Nature Communications
- Vol. 11 (1), 1-11
- https://doi.org/10.1038/s41467-020-17782-5
Abstract
Hydrogen peroxide produced by electrochemical oxygen reduction reaction provides a potentially cost effective and energy efficient alternative to the industrial anthraquinone process. In this study, we demonstrate that by modulating the oxygen functional groups near the atomically dispersed cobalt sites with proper electrochemical/chemical treatments, a highly active and selective oxygen reduction process for hydrogen peroxide production can be obtained in acidic electrolyte, showing a negligible amount of onset overpotential and nearly 100% selectivity within a wide range of applied potentials. Combined spectroscopic results reveal that the exceptionally enhanced performance of hydrogen peroxide generation originates from the presence of epoxy groups near the Co–N4 centers, which has resulted in the modification of the electronic structure of the cobalt atoms. Computational modeling demonstrates these electronically modified cobalt atoms will enhance the hydrogen peroxide productivity during oxygen reduction reaction in acid, providing insights into the design of electroactive materials for effective peroxide production.This publication has 60 references indexed in Scilit:
- Efficient Two-Electron Reduction of Dioxygen to Hydrogen Peroxide with One-Electron Reductants with a Small Overpotential Catalyzed by a Cobalt Chlorin ComplexJournal of the American Chemical Society, 2013
- Mesoporous Nitrogen-Doped Carbon for the Electrocatalytic Synthesis of Hydrogen PeroxideJournal of the American Chemical Society, 2012
- Probing the Thermal Deoxygenation of Graphene Oxide Using High-Resolution In Situ X-ray-Based SpectroscopiesThe Journal of Physical Chemistry C, 2011
- A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-PuThe Journal of Chemical Physics, 2010
- Electro-Fenton Process and Related Electrochemical Technologies Based on Fenton’s Reaction ChemistryChemical Reviews, 2009
- A Green Approach to the Synthesis of Graphene NanosheetsACS Nano, 2009
- From ultrasoft pseudopotentials to the projector augmented-wave methodPhysical Review B, 1999
- Generalized Gradient Approximation Made SimplePhysical Review Letters, 1996
- Efficient iterative schemes forab initiototal-energy calculations using a plane-wave basis setPhysical Review B, 1996
- Ab initiomolecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germaniumPhysical Review B, 1994