Electrochemical CO2 Reduction to Hydrocarbons on a Heterogeneous Molecular Cu Catalyst in Aqueous Solution

Zhe Weng, Jianbing Jiang, Yueshen Wu, Zishan Wu, Xiaoting Guo, Kelly L. Materna, Wen Liu, Victor S. Batista, Gary W Brudvig, Hailiang Wang

Research output: Contribution to journalArticle

123 Citations (Scopus)

Abstract

Exploration of heterogeneous molecular catalysts combining the atomic-level tunability of molecular structures and the practical handling advantages of heterogeneous catalysts represents an attractive approach to developing high-performance catalysts for important and challenging chemical reactions such as electrochemical carbon dioxide reduction which holds the promise for converting emissions back to fuels utilizing renewable energy. Thus, far, efficient and selective electroreduction of CO2 to deeply reduced products such as hydrocarbons remains a big challenge. Here, we report a molecular copper-porphyrin complex (copper(II)-5,10,15,20-tetrakis(2,6-dihydroxyphenyl)porphyrin) that can be used as a heterogeneous electrocatalyst with high activity and selectivity for reducing CO2 to hydrocarbons in aqueous media. At -0.976 V vs the reversible hydrogen electrode, the catalyst is able to drive partial current densities of 13.2 and 8.4 mA cm-2 for methane and ethylene production from CO2 reduction, corresponding to turnover frequencies of 4.3 and 1.8 molecules·site-1·s-1 for methane and ethylene, respectively. This represents the highest catalytic activity to date for hydrocarbon production over a molecular CO2 reduction electrocatalyst. The unprecedented catalytic performance is attributed to the built-in hydroxyl groups in the porphyrin structure and the reactivity of the copper(I) metal center.

Original languageEnglish
Pages (from-to)8076-8079
Number of pages4
JournalJournal of the American Chemical Society
Volume138
Issue number26
DOIs
Publication statusPublished - Jul 6 2016

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Porphyrins
Hydrocarbons
Copper
Methane
Catalysts
Electrocatalysts
Renewable Energy
Catalyst activity
Ethylene
Molecular Structure
Carbon Dioxide
Hydroxyl Radical
Catalyst selectivity
Hydrogen
Electrodes
Metals
Molecular structure
Chemical reactions
Carbon dioxide
Current density

ASJC Scopus subject areas

  • Catalysis
  • Biochemistry
  • Chemistry(all)
  • Colloid and Surface Chemistry

Cite this

Electrochemical CO2 Reduction to Hydrocarbons on a Heterogeneous Molecular Cu Catalyst in Aqueous Solution. / Weng, Zhe; Jiang, Jianbing; Wu, Yueshen; Wu, Zishan; Guo, Xiaoting; Materna, Kelly L.; Liu, Wen; Batista, Victor S.; Brudvig, Gary W; Wang, Hailiang.

In: Journal of the American Chemical Society, Vol. 138, No. 26, 06.07.2016, p. 8076-8079.

Research output: Contribution to journalArticle

Weng, Zhe ; Jiang, Jianbing ; Wu, Yueshen ; Wu, Zishan ; Guo, Xiaoting ; Materna, Kelly L. ; Liu, Wen ; Batista, Victor S. ; Brudvig, Gary W ; Wang, Hailiang. / Electrochemical CO2 Reduction to Hydrocarbons on a Heterogeneous Molecular Cu Catalyst in Aqueous Solution. In: Journal of the American Chemical Society. 2016 ; Vol. 138, No. 26. pp. 8076-8079.
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