Molecule Confined Isolated Metal Sites Enable the Electrocatalytic Synthesis of Hydrogen Peroxide

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

45 Scopus Citations
View graph of relations

Author(s)

  • Xiaogang Li
  • Shasha Tang
  • Shuo Dou
  • Hong Jin Fan
  • Tej S. Choksi

Detail(s)

Original languageEnglish
Article number2104891
Journal / PublicationAdvanced Materials
Volume34
Issue number25
Online published19 Sept 2021
Publication statusPublished - 23 Jun 2022
Externally publishedYes

Abstract

The direct synthesis of hydrogen peroxide (H2O2) through the two-electron oxygen reduction reaction is a promising alternative to the industrial anthraquinone oxidation process. Selectivity to H2O2 is however limited by the four-electron pathway during oxygen reduction. Herein, it is reported that aminoanthraquinone confined isolated metal sites on carbon supports selectively steer oxygen reduction to H2O2 through the two-electron pathway. Confining isolated NiNx sites under aminoanthraquinone increases the selectivity to H2O2 from below 55% to above 80% over a wide potential range. Spectroscopy characterization and density functional theory calculations indicate that isolated NiNx sites are confined within a nanochannel formed between the molecule and the carbon support. The confinement reduces the thermodynamic barrier for OOH* desorption versus further dissociation, thus increasing the selectivity to H2O2. It is revealed how tailoring noncovalent interactions beyond the binding site can empower electrocatalysts for the direct synthesis of H2O2 through oxygen reduction. © 2021 Wiley-VCH GmbH.

Research Area(s)

  • electrocatalysis, hydrogen peroxide, isolated metal sites, molecular confinement, oxygen reduction

Citation Format(s)

Molecule Confined Isolated Metal Sites Enable the Electrocatalytic Synthesis of Hydrogen Peroxide. / Li, Xiaogang; Tang, Shasha; Dou, Shuo et al.
In: Advanced Materials, Vol. 34, No. 25, 2104891, 23.06.2022.

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review