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A metal-free electrocatalyst for carbon dioxide reduction to multi-carbon hydrocarbons and oxygenates

Author

Listed:
  • Jingjie Wu

    (Rice University)

  • Sichao Ma

    (School of Chemical Sciences, University of Illinois at Urbana-Champaign
    International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Kyushu University)

  • Jing Sun

    (State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences)

  • Jake I. Gold

    (School of Chemical Sciences, University of Illinois at Urbana-Champaign)

  • ChandraSekhar Tiwary

    (Rice University)

  • Byoungsu Kim

    (School of Chemical Sciences, University of Illinois at Urbana-Champaign
    International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Kyushu University)

  • Lingyang Zhu

    (School of Chemical Sciences, University of Illinois at Urbana-Champaign)

  • Nitin Chopra

    (Saudi Basic Industries Corporation (SABIC))

  • Ihab N. Odeh

    (Saudi Basic Industries Corporation (SABIC))

  • Robert Vajtai

    (Rice University)

  • Aaron Z. Yu

    (School of Chemical Sciences, University of Illinois at Urbana-Champaign)

  • Raymond Luo

    (School of Chemical Sciences, University of Illinois at Urbana-Champaign)

  • Jun Lou

    (Rice University)

  • Guqiao Ding

    (State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences)

  • Paul J. A. Kenis

    (School of Chemical Sciences, University of Illinois at Urbana-Champaign
    International Institute for Carbon-Neutral Energy Research (WPI-I2CNER), Kyushu University)

  • Pulickel M. Ajayan

    (Rice University)

Abstract

Electroreduction of carbon dioxide into higher-energy liquid fuels and chemicals is a promising but challenging renewable energy conversion technology. Among the electrocatalysts screened so far for carbon dioxide reduction, which includes metals, alloys, organometallics, layered materials and carbon nanostructures, only copper exhibits selectivity towards formation of hydrocarbons and multi-carbon oxygenates at fairly high efficiencies, whereas most others favour production of carbon monoxide or formate. Here we report that nanometre-size N-doped graphene quantum dots (NGQDs) catalyse the electrochemical reduction of carbon dioxide into multi-carbon hydrocarbons and oxygenates at high Faradaic efficiencies, high current densities and low overpotentials. The NGQDs show a high total Faradaic efficiency of carbon dioxide reduction of up to 90%, with selectivity for ethylene and ethanol conversions reaching 45%. The C2 and C3 product distribution and production rate for NGQD-catalysed carbon dioxide reduction is comparable to those obtained with copper nanoparticle-based electrocatalysts.

Suggested Citation

  • Jingjie Wu & Sichao Ma & Jing Sun & Jake I. Gold & ChandraSekhar Tiwary & Byoungsu Kim & Lingyang Zhu & Nitin Chopra & Ihab N. Odeh & Robert Vajtai & Aaron Z. Yu & Raymond Luo & Jun Lou & Guqiao Ding , 2016. "A metal-free electrocatalyst for carbon dioxide reduction to multi-carbon hydrocarbons and oxygenates," Nature Communications, Nature, vol. 7(1), pages 1-6, December.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms13869
    DOI: 10.1038/ncomms13869
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    Cited by:

    1. Pribyl-Kranewitter, B. & Beard, A. & Gîjiu, C.L. & Dinculescu, D. & Schmidt, T.J., 2022. "Influence of low-temperature electrolyser design on economic and environmental potential of CO and HCOOH production: A techno-economic assessment," Renewable and Sustainable Energy Reviews, Elsevier, vol. 154(C).
    2. Giulia Tuci & Jonathan Filippi & Andrea Rossin & Lapo Luconi & Cuong Pham-Huu & Dmitry Yakhvarov & Francesco Vizza & Giuliano Giambastiani, 2020. "CO 2 Electrochemical Reduction by Exohedral N-Pyridine Decorated Metal-Free Carbon Nanotubes," Energies, MDPI, vol. 13(11), pages 1-15, May.
    3. Baiyu Yang & Ling Chen & Songlin Xue & Hao Sun & Kun Feng & Yufeng Chen & Xiang Zhang & Long Xiao & Yongze Qin & Jun Zhong & Zhao Deng & Yan Jiao & Yang Peng, 2022. "Electrocatalytic CO2 reduction to alcohols by modulating the molecular geometry and Cu coordination in bicentric copper complexes," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    4. Han, Juan & Deng, Ximing & Chen, Keyu & Imhanria, Sarah & Sun, Yan & Wang, Wei, 2021. "Electrochemical conversion of CO2 into tunable syngas on a B, P, N tri-doped carbon," Renewable Energy, Elsevier, vol. 177(C), pages 636-642.
    5. Cong Liu & Bingbao Mei & Zhaoping Shi & Zheng Jiang & Junjie Ge & Wei Xing & Ping Song & Weilin Xu, 2024. "Operando formation of highly efficient electrocatalysts induced by heteroatom leaching," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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