Enhancement of Electrocatalytic CO2 Reduction to Methane by CoTMPyP when Hosted in a 3D Covalent Graphene Framework

Yair Bochlin, Lior Ezuz, Yanir Kadosh, Daniel Benjamin, Yuval Mordekovitz, Shmuel Hayun, Eli Korin, Armand Bettelheim

Research output: Contribution to journalArticlepeer-review

9 Scopus citations

Abstract

Electrocatalytic reduction of carbon dioxide is a promising technique to convert CO2 into useful products and to aid environmental concerns. Here, we report on the preparation of a unique three-dimensional graphene-based structure, covalent graphene framework (CGF), which is obtained by the chemical attachment of a nitro-functionalized graphene derivative to a 3D aniline-based linker. CGF is then used to host cobalt [5,10,15,20-(tetra-N-methyl-4-pyridyl)porphyrin] (CoTMPyP) as a catalyst for electrochemical CO2 reduction. The porous structure of CGF with free amine functional groups enables strong irreversible adsorption of CO2 which promotes the formation and stabilization of a key carbamate intermediate. The combined CGF-CoTMPyP catalytic system shows enhanced performance for the 8e- CO2 reduction to CH4 (faradaic efficiency ∼20%) at −0.72 V versus RHE in aqueous solutions. This work emphasizes the importance of tuning the morphology and chemical composition of the catalyst surroundings in the design of efficient catalytic systems in the field of energy conversion.

Original languageEnglish
Pages (from-to)10033-10041
Number of pages9
JournalACS Applied Energy Materials
Volume4
Issue number9
DOIs
StatePublished - 27 Sep 2021

Keywords

  • CO
  • CO reduction
  • azo-bridges
  • carbamate
  • cobalt porphyrin
  • covalent graphene frameworks
  • electrocatalysis
  • methane

ASJC Scopus subject areas

  • Chemical Engineering (miscellaneous)
  • Energy Engineering and Power Technology
  • Materials Chemistry
  • Electrical and Electronic Engineering
  • Electrochemistry

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