Elucidating the Reactivity and Mechanism of CO2 Electroreduction at Highly Dispersed Cobalt Phthalocyanine

Minghui Zhu, Ruquan Ye, Kyoungsuk Jin, Nikifar Lazouski, Karthish Manthiram

Research output: Contribution to journalArticlepeer-review

78 Citations (Scopus)

Abstract

Transforming carbon dioxide to carbon monoxide with electrochemical methods allows for small-scale, modular conversion of point sources of carbon dioxide. In this work, through the preparation of a well-dispersed cobalt phthalocyanine model catalyst immobilized on carbon paper, we revealed high turnover frequencies for reducing carbon dioxide at low catalyst loadings, which are obscured at higher loadings due to aggregation. The low catalyst loadings have also enabled mechanistic studies that provide a detailed understanding of the molecular-level picture of how cobalt phthalocyanine facilitates proton and electron transfers in the rate-limiting step. We are able to tune the rate-limiting step from electron transfer to concerted proton-electron transfer, enabling higher rates of carbon dioxide reduction. Our results highlight the significance of dispersion for understanding the intrinsic catalytic performance of metal phthalocyanines for electroreduction of CO2.

Original languageEnglish
Pages (from-to)1381-1386
Number of pages6
JournalACS Energy Letters
Volume3
Issue number6
DOIs
Publication statusPublished - 2018 Jun 8
Externally publishedYes

ASJC Scopus subject areas

  • Chemistry (miscellaneous)
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Materials Chemistry

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