IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-36530-z.html
   My bibliography  Save this article

Steering carbon dioxide reduction toward C–C coupling using copper electrodes modified with porous molecular films

Author

Listed:
  • Siqi Zhao

    (Interdisciplinary Nanoscience Center (iNANO)
    Aarhus University)

  • Oliver Christensen

    (University of Copenhagen)

  • Zhaozong Sun

    (Interdisciplinary Nanoscience Center (iNANO))

  • Hongqing Liang

    (Leibniz-Institut für Katalyse)

  • Alexander Bagger

    (University of Copenhagen)

  • Kristian Torbensen

    (Interdisciplinary Nanoscience Center (iNANO)
    Aarhus University)

  • Pegah Nazari

    (Aarhus University
    Aarhus University)

  • Jeppe Vang Lauritsen

    (Interdisciplinary Nanoscience Center (iNANO))

  • Steen Uttrup Pedersen

    (Interdisciplinary Nanoscience Center (iNANO)
    Aarhus University)

  • Jan Rossmeisl

    (University of Copenhagen)

  • Kim Daasbjerg

    (Interdisciplinary Nanoscience Center (iNANO)
    Aarhus University
    Aarhus University)

Abstract

Copper offers unique capability as catalyst for multicarbon compounds production in the electrochemical carbon dioxide reduction reaction. In lieu of conventional catalysis alloying with other elements, copper can be modified with organic molecules to regulate product distribution. Here, we systematically study to which extent the carbon dioxide reduction is affected by film thickness and porosity. On a polycrystalline copper electrode, immobilization of porous bipyridine-based films of varying thicknesses is shown to result in almost an order of magnitude enhancement of the intrinsic current density pertaining to ethylene formation while multicarbon products selectivity increases from 9.7 to 61.9%. In contrast, the total current density remains mostly unaffected by the modification once it is normalized with respect to the electrochemical active surface area. Supported by a microkinetic model, we propose that porous and thick films increase both local carbon monoxide partial pressure and the carbon monoxide surface coverage by retaining in situ generated carbon monoxide. This reroutes the reaction pathway toward multicarbon products by enhancing carbon–carbon coupling. Our study highlights the significance of customizing the molecular film structure to improve the selectivity of copper catalysts for carbon dioxide reduction reaction.

Suggested Citation

  • Siqi Zhao & Oliver Christensen & Zhaozong Sun & Hongqing Liang & Alexander Bagger & Kristian Torbensen & Pegah Nazari & Jeppe Vang Lauritsen & Steen Uttrup Pedersen & Jan Rossmeisl & Kim Daasbjerg, 2023. "Steering carbon dioxide reduction toward C–C coupling using copper electrodes modified with porous molecular films," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36530-z
    DOI: 10.1038/s41467-023-36530-z
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-36530-z
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-023-36530-z?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Karen Chan, 2020. "A few basic concepts in electrochemical carbon dioxide reduction," Nature Communications, Nature, vol. 11(1), pages 1-4, December.
    2. Chanyeon Kim & Justin C. Bui & Xiaoyan Luo & Jason K. Cooper & Ahmet Kusoglu & Adam Z. Weber & Alexis T. Bell, 2021. "Tailored catalyst microenvironments for CO2 electroreduction to multicarbon products on copper using bilayer ionomer coatings," Nature Energy, Nature, vol. 6(11), pages 1026-1034, November.
    3. Jing Li & Xiaoxia Chang & Haochen Zhang & Arnav S. Malkani & Mu-jeng Cheng & Bingjun Xu & Qi Lu, 2021. "Electrokinetic and in situ spectroscopic investigations of CO electrochemical reduction on copper," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    4. Fengwang Li & Arnaud Thevenon & Alonso Rosas-Hernández & Ziyun Wang & Yilin Li & Christine M. Gabardo & Adnan Ozden & Cao Thang Dinh & Jun Li & Yuhang Wang & Jonathan P. Edwards & Yi Xu & Christopher , 2020. "Molecular tuning of CO2-to-ethylene conversion," Nature, Nature, vol. 577(7791), pages 509-513, January.
    5. Christina W. Li & Jim Ciston & Matthew W. Kanan, 2014. "Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper," Nature, Nature, vol. 508(7497), pages 504-507, April.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Yan Lin & Tuo Wang & Lili Zhang & Gong Zhang & Lulu Li & Qingfeng Chang & Zifan Pang & Hui Gao & Kai Huang & Peng Zhang & Zhi-Jian Zhao & Chunlei Pei & Jinlong Gong, 2023. "Tunable CO2 electroreduction to ethanol and ethylene with controllable interfacial wettability," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Seung-Jae Shin & Hansol Choi & Stefan Ringe & Da Hye Won & Hyung-Suk Oh & Dong Hyun Kim & Taemin Lee & Dae-Hyun Nam & Hyungjun Kim & Chang Hyuck Choi, 2022. "A unifying mechanism for cation effect modulating C1 and C2 productions from CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    3. Jiajie Hou & Bingjun Xu & Qi Lu, 2024. "Influence of electric double layer rigidity on CO adsorption and electroreduction rate," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    4. Xinyi Ren & Jian Zhao & Xuning Li & Junming Shao & Binbin Pan & Aude Salamé & Etienne Boutin & Thomas Groizard & Shifu Wang & Jie Ding & Xiong Zhang & Wen-Yang Huang & Wen-Jing Zeng & Chengyu Liu & Ya, 2023. "In-situ spectroscopic probe of the intrinsic structure feature of single-atom center in electrochemical CO/CO2 reduction to methanol," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. Jongyoun Kim & Taemin Lee & Hyun Dong Jung & Minkyoung Kim & Jungsu Eo & Byeongjae Kang & Hyeonwoo Jung & Jaehyoung Park & Daewon Bae & Yujin Lee & Sojung Park & Wooyul Kim & Seoin Back & Youngu Lee &, 2024. "Vitamin C-induced CO2 capture enables high-rate ethylene production in CO2 electroreduction," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    6. Xiaoxia Chang & Sudarshan Vijay & Yaran Zhao & Nicholas J. Oliveira & Karen Chan & Bingjun Xu, 2022. "Understanding the complementarities of surface-enhanced infrared and Raman spectroscopies in CO adsorption and electrochemical reduction," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    7. 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).
    8. Jing Li & Haocheng Xiong & Xiaozhi Liu & Donghuan Wu & Dong Su & Bingjun Xu & Qi Lu, 2023. "Weak CO binding sites induced by Cu–Ag interfaces promote CO electroreduction to multi-carbon liquid products," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    9. Sung-Fu Hung & Aoni Xu & Xue Wang & Fengwang Li & Shao-Hui Hsu & Yuhang Li & Joshua Wicks & Eduardo González Cervantes & Armin Sedighian Rasouli & Yuguang C. Li & Mingchuan Luo & Dae-Hyun Nam & Ning W, 2022. "A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    10. Guifeng Ma & Olga A. Syzgantseva & Yan Huang & Dragos Stoian & Jie Zhang & Shuliang Yang & Wen Luo & Mengying Jiang & Shumu Li & Chunjun Chen & Maria A. Syzgantseva & Sen Yan & Ningyu Chen & Li Peng &, 2023. "A hydrophobic Cu/Cu2O sheet catalyst for selective electroreduction of CO to ethanol," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    11. Jie Ding & Fuhua Li & Xinyi Ren & Yuhang Liu & Yifan Li & Zheng Shen & Tian Wang & Weijue Wang & Yang-Gang Wang & Yi Cui & Hongbin Yang & Tianyu Zhang & Bin Liu, 2024. "Molecular tuning boosts asymmetric C-C coupling for CO conversion to acetate," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    12. Kang Yang & Ming Li & Tianqi Gao & Guoliang Xu & Di Li & Yao Zheng & Qiang Li & Jingjing Duan, 2024. "An acid-tolerant metal-organic framework for industrial CO2 electrolysis using a proton exchange membrane," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    13. Ruijuan Zhao & Lei Li & Qianbao Wu & Wei Luo & Qiu Zhang & Chunhua Cui, 2024. "Spontaneous formation of reactive redox radical species at the interface of gas diffusion electrode," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    14. Huali Wu & Ji Li & Kun Qi & Yang Zhang & Eddy Petit & Wensen Wang & Valérie Flaud & Nicolas Onofrio & Bertrand Rebiere & Lingqi Huang & Chrystelle Salameh & Luc Lajaunie & Philippe Miele & Damien Voir, 2021. "Improved electrochemical conversion of CO2 to multicarbon products by using molecular doping," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    15. Hongfei Wang & Zhipeng Yu & Jie Zhou & Chengming Li & Ananthanarasimhan Jayanarasimhan & Xiqiang Zhao & Hao Zhang, 2023. "A Scientometric Review of CO 2 Electroreduction Research from 2005 to 2022," Energies, MDPI, vol. 16(2), pages 1-21, January.
    16. Darband, Ghasem Barati & Aliofkhazraei, Mahmood & Shanmugam, Sangaraju, 2019. "Recent advances in methods and technologies for enhancing bubble detachment during electrochemical water splitting," Renewable and Sustainable Energy Reviews, Elsevier, vol. 114(C), pages 1-1.
    17. Wanyu Deng & Peng Zhang & Yu Qiao & Georg Kastlunger & Nitish Govindarajan & Aoni Xu & Ib Chorkendorff & Brian Seger & Jinlong Gong, 2024. "Unraveling the rate-determining step of C2+ products during electrochemical CO reduction," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    18. Kaili Yao & Jun Li & Adnan Ozden & Haibin Wang & Ning Sun & Pengyu Liu & Wen Zhong & Wei Zhou & Jieshu Zhou & Xi Wang & Hanqi Liu & Yongchang Liu & Songhua Chen & Yongfeng Hu & Ziyun Wang & David Sint, 2024. "In situ copper faceting enables efficient CO2/CO electrolysis," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    19. TsingHai Wang & Cheng-Di Dong & Jui-Yen Lin & Chiu-Wen Chen & Jo-Shu Chang & Hyunook Kim & Chin-Pao Huang & Chang-Mao Hung, 2021. "Recent Advances in Carbon Dioxide Conversion: A Circular Bioeconomy Perspective," Sustainability, MDPI, vol. 13(12), pages 1-31, June.
    20. Hefei Li & Pengfei Wei & Tianfu Liu & Mingrun Li & Chao Wang & Rongtan Li & Jinyu Ye & Zhi-You Zhou & Shi-Gang Sun & Qiang Fu & Dunfeng Gao & Guoxiong Wang & Xinhe Bao, 2024. "CO electrolysis to multicarbon products over grain boundary-rich Cu nanoparticles in membrane electrode assembly electrolyzers," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36530-z. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.