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Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene

Author

Listed:
  • Hemma Mistry

    (University of Central Florida
    Ruhr-University Bochum)

  • Ana Sofia Varela

    (Technical University Berlin)

  • Cecile S. Bonifacio

    (Chemical and Petroleum Engineering and Physics, University of Pittsburgh)

  • Ioannis Zegkinoglou

    (Ruhr-University Bochum)

  • Ilya Sinev

    (Ruhr-University Bochum)

  • Yong-Wook Choi

    (Ruhr-University Bochum)

  • Kim Kisslinger

    (Center for Functional Nanomaterials, Brookhaven National Laboratory)

  • Eric A. Stach

    (Center for Functional Nanomaterials, Brookhaven National Laboratory)

  • Judith C. Yang

    (Chemical and Petroleum Engineering and Physics, University of Pittsburgh)

  • Peter Strasser

    (Technical University Berlin)

  • Beatriz Roldan Cuenya

    (Ruhr-University Bochum)

Abstract

There is an urgent need to develop technologies that use renewable energy to convert waste products such as carbon dioxide into hydrocarbon fuels. Carbon dioxide can be electrochemically reduced to hydrocarbons over copper catalysts, although higher efficiency is required. We have developed oxidized copper catalysts displaying lower overpotentials for carbon dioxide electroreduction and record selectivity towards ethylene (60%) through facile and tunable plasma treatments. Herein we provide insight into the improved performance of these catalysts by combining electrochemical measurements with microscopic and spectroscopic characterization techniques. Operando X-ray absorption spectroscopy and cross-sectional scanning transmission electron microscopy show that copper oxides are surprisingly resistant to reduction and copper+ species remain on the surface during the reaction. Our results demonstrate that the roughness of oxide-derived copper catalysts plays only a partial role in determining the catalytic performance, while the presence of copper+ is key for lowering the onset potential and enhancing ethylene selectivity.

Suggested Citation

  • Hemma Mistry & Ana Sofia Varela & Cecile S. Bonifacio & Ioannis Zegkinoglou & Ilya Sinev & Yong-Wook Choi & Kim Kisslinger & Eric A. Stach & Judith C. Yang & Peter Strasser & Beatriz Roldan Cuenya, 2016. "Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene," Nature Communications, Nature, vol. 7(1), pages 1-9, November.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms12123
    DOI: 10.1038/ncomms12123
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    Cited by:

    1. Antonia Herzog & Mauricio Lopez Luna & Hyo Sang Jeon & Clara Rettenmaier & Philipp Grosse & Arno Bergmann & Beatriz Roldan Cuenya, 2024. "Operando Raman spectroscopy uncovers hydroxide and CO species enhance ethanol selectivity during pulsed CO2 electroreduction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Zhiwen Jiang & Carine Clavaguéra & Changjiang Hu & Sergey A. Denisov & Shuning Shen & Feng Hu & Jun Ma & Mehran Mostafavi, 2023. "Direct time-resolved observation of surface-bound carbon dioxide radical anions on metallic nanocatalysts," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    3. Xiaozhi Su & Zhuoli Jiang & Jing Zhou & Hengjie Liu & Danni Zhou & Huishan Shang & Xingming Ni & Zheng Peng & Fan Yang & Wenxing Chen & Zeming Qi & Dingsheng Wang & Yu Wang, 2022. "Complementary Operando Spectroscopy identification of in-situ generated metastable charge-asymmetry Cu2-CuN3 clusters for CO2 reduction to ethanol," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    4. Wei Liu & Pengbo Zhai & Aowen Li & Bo Wei & Kunpeng Si & Yi Wei & Xingguo Wang & Guangda Zhu & Qian Chen & Xiaokang Gu & Ruifeng Zhang & Wu Zhou & Yongji Gong, 2022. "Electrochemical CO2 reduction to ethylene by ultrathin CuO nanoplate arrays," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    5. Shijia Mu & Honglei Lu & Qianbao Wu & Lei Li & Ruijuan Zhao & Chang Long & Chunhua Cui, 2022. "Hydroxyl radicals dominate reoxidation of oxide-derived Cu in electrochemical CO2 reduction," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    6. Chia-Shuo Hsu & Jiali Wang & You-Chiuan Chu & Jui-Hsien Chen & Chia-Ying Chien & Kuo-Hsin Lin & Li Duan Tsai & Hsiao-Chien Chen & Yen-Fa Liao & Nozomu Hiraoka & Yuan-Chung Cheng & Hao Ming Chen, 2023. "Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    7. Ahmad, Naveed & Chen, Ying & Wang, Xiaoxiao & Sun, Peixu & Bao, Yuting & Xu, Xia, 2022. "Highly efficient electrochemical upgrade of CO2 to CO using AMP capture solution as electrolyte," Renewable Energy, Elsevier, vol. 189(C), pages 444-453.
    8. Yong Yin & Bingcheng Luo & Kezhi Li & Benjamin M. Moskowitz & Bar Mosevitzky Lis & Israel E. Wachs & Minghui Zhu & Ye Sun & Tianle Zhu & Xiang Li, 2024. "Plasma-assisted manipulation of vanadia nanoclusters for efficient selective catalytic reduction of NOx," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    9. Qiong Lei & Liang Huang & Jun Yin & Bambar Davaasuren & Youyou Yuan & Xinglong Dong & Zhi-Peng Wu & Xiaoqian Wang & Ke Xin Yao & Xu Lu & Yu Han, 2022. "Structural evolution and strain generation of derived-Cu catalysts during CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    10. Yajun Zheng & Hedan Yao & Ruinan Di & Zhicheng Xiang & Qiang Wang & Fangfang Lu & Yu Li & Guangxing Yang & Qiang Ma & Zhiping Zhang, 2022. "Water coordinated on Cu(I)-based catalysts is the oxygen source in CO2 reduction to CO," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    11. Lei Wang & Zhiwen Chen & Yi Xiao & Linke Huang & Xiyang Wang & Holly Fruehwald & Dmitry Akhmetzyanov & Mathew Hanson & Zuolong Chen & Ning Chen & Brant Billinghurst & Rodney D. L. Smith & Chandra Veer, 2024. "Stabilized Cuδ+-OH species on in situ reconstructed Cu nanoparticles for CO2-to-C2H4 conversion in neutral media," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    12. Wenpeng Ni & Houjun Chen & Naizhuo Tang & Ting Hu & Wei Zhang & Yan Zhang & Shiguo Zhang, 2024. "High-purity ethylene production via indirect carbon dioxide electrochemical reduction," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    13. Ruiz-López, Estela & Gandara-Loe, Jesús & Baena-Moreno, Francisco & Reina, Tomas Ramirez & Odriozola, José Antonio, 2022. "Electrocatalytic CO2 conversion to C2 products: Catalysts design, market perspectives and techno-economic aspects," Renewable and Sustainable Energy Reviews, Elsevier, vol. 161(C).

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