IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-50522-7.html
   My bibliography  Save this article

High-purity ethylene production via indirect carbon dioxide electrochemical reduction

Author

Listed:
  • Wenpeng Ni

    (Hunan University)

  • Houjun Chen

    (Hunan University)

  • Naizhuo Tang

    (Hunan University)

  • Ting Hu

    (Hunan University)

  • Wei Zhang

    (Hunan University)

  • Yan Zhang

    (Hunan University)

  • Shiguo Zhang

    (Hunan University)

Abstract

High-purity ethylene production from CO2 electroreduction (CO2RR) is a coveted, yet arduous feat because the product stream comprises a blend of unreacted CO2, H2, and other off-target CO2 reduction products. Here we present an indirect reduction strategy for CO2-to-ethylene conversion, one that employs 2-bromoethanol (Br-EO) as a mediator. Br-EO is initially generated from CO2RR and subsequently undergoes reduction to ethylene without the need for energy-intensive separation steps. The optimized AC-Ag/C catalyst with Cl incorporation reduces the energy barrier of the debromination step during Br-EO reduction, and accelerates the mass-transfer process, delivering a 4-fold decrease of the relaxation time constant. Resultantly, AC-Ag/C achieved a FEethylene of over 95.0 ± 0.36% at a low potential of −0.08 V versus reversible hydrogen electrode (RHE) in an H-type cell with 0.5 M KCl electrolyte, alongside a near 100% selectivity within the range of −0.38 to −0.58 V versus RHE. Through this indirect strategy, the average ethylene purity within 6-hour electrolysis was 98.00 ± 1.45 wt%, at −0.48 V (vs RHE) from the neutralized electrolyte after CO2 reduction over the Cu/Cu2O catalyst in a flow-cell.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-50522-7
    DOI: 10.1038/s41467-024-50522-7
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-50522-7
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-024-50522-7?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. 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.
    2. Jiarui Yang & Wen-Hao Li & Hai-Tao Tang & Ying-Ming Pan & Dingsheng Wang & Yadong Li, 2023. "CO2-mediated organocatalytic chlorine evolution under industrial conditions," Nature, Nature, vol. 617(7961), pages 519-523, May.
    3. 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. "Correction: Corrigendum: Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene," Nature Communications, Nature, vol. 7(1), pages 1-1, December.
    4. Jun Li & Adnan Ozden & Mingyu Wan & Yongfeng Hu & Fengwang Li & Yuhang Wang & Reza R. Zamani & Dan Ren & Ziyun Wang & Yi Xu & Dae-Hyun Nam & Joshua Wicks & Bin Chen & Xue Wang & Mingchuan Luo & Michae, 2021. "Silica-copper catalyst interfaces enable carbon-carbon coupling towards ethylene electrosynthesis," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    5. Chuan Xia & Peng Zhu & Qiu Jiang & Ying Pan & Wentao Liang & Eli Stavitski & Husam N. Alshareef & Haotian Wang, 2019. "Continuous production of pure liquid fuel solutions via electrocatalytic CO2 reduction using solid-electrolyte devices," Nature Energy, Nature, vol. 4(9), pages 776-785, September.
    6. Hao Sun & Ling Chen & Likun Xiong & Kun Feng & Yufeng Chen & Xiang Zhang & Xuzhou Yuan & Baiyu Yang & Zhao Deng & Yu Liu & Mark H. Rümmeli & Jun Zhong & Yan Jiao & Yang Peng, 2021. "Promoting ethylene production over a wide potential window on Cu crystallites induced and stabilized via current shock and charge delocalization," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    7. 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.
    8. Wenzheng Li & Zhenglei Yin & Zeyu Gao & Gongwei Wang & Zhen Li & Fengyuan Wei & Xing Wei & Hanqing Peng & Xingtao Hu & Li Xiao & Juntao Lu & Lin Zhuang, 2022. "Bifunctional ionomers for efficient co-electrolysis of CO2 and pure water towards ethylene production at industrial-scale current densities," Nature Energy, Nature, vol. 7(9), pages 835-843, September.
    9. 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.
    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. 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).
    2. 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.
    3. 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.
    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. Yizhou Dai & Huan Li & Chuanhao Wang & Weiqing Xue & Menglu Zhang & Donghao Zhao & Jing Xue & Jiawei Li & Laihao Luo & Chunxiao Liu & Xu Li & Peixin Cui & Qiu Jiang & Tingting Zheng & Songqi Gu & Yao , 2023. "Manipulating local coordination of copper single atom catalyst enables efficient CO2-to-CH4 conversion," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    6. Xiaojie She & Lingling Zhai & Yifei Wang & Pei Xiong & Molly Meng-Jung Li & Tai-Sing Wu & Man Chung Wong & Xuyun Guo & Zhihang Xu & Huaming Li & Hui Xu & Ye Zhu & Shik Chi Edman Tsang & Shu Ping Lau, 2024. "Pure-water-fed, electrocatalytic CO2 reduction to ethylene beyond 1,000 h stability at 10 A," Nature Energy, Nature, vol. 9(1), pages 81-91, January.
    7. 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.
    8. Zhenyu Jin & Yingqing Guo & Chaozhi Qiu, 2022. "Electro-Conversion of Carbon Dioxide to Valuable Chemicals in a Membrane Electrode Assembly," Sustainability, MDPI, vol. 14(9), pages 1-24, May.
    9. Yufei Cao & Zhu Chen & Peihao Li & Adnan Ozden & Pengfei Ou & Weiyan Ni & Jehad Abed & Erfan Shirzadi & Jinqiang Zhang & David Sinton & Jun Ge & Edward H. Sargent, 2023. "Surface hydroxide promotes CO2 electrolysis to ethylene in acidic conditions," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    10. Weihua Guo & Siwei Zhang & Junjie Zhang & Haoran Wu & Yangbo Ma & Yun Song & Le Cheng & Liang Chang & Geng Li & Yong Liu & Guodan Wei & Lin Gan & Minghui Zhu & Shibo Xi & Xue Wang & Boris I. Yakobson , 2023. "Accelerating multielectron reduction at CuxO nanograins interfaces with controlled local electric field," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    11. 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.
    12. 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.
    13. 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.
    14. 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.
    15. 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.
    16. 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.
    17. 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.
    18. Leiming Hu & Jacob A. Wrubel & Carlos M. Baez-Cotto & Fry Intia & Jae Hyung Park & Arthur Jeremy Kropf & Nancy Kariuki & Zhe Huang & Ahmed Farghaly & Lynda Amichi & Prantik Saha & Ling Tao & David A. , 2023. "A scalable membrane electrode assembly architecture for efficient electrochemical conversion of CO2 to formic acid," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    19. 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.
    20. Yongxiang Liang & Jiankang Zhao & Yu Yang & Sung-Fu Hung & Jun Li & Shuzhen Zhang & Yong Zhao & An Zhang & Cheng Wang & Dominique Appadoo & Lei Zhang & Zhigang Geng & Fengwang Li & Jie Zeng, 2023. "Stabilizing copper sites in coordination polymers toward efficient electrochemical C-C coupling," Nature Communications, Nature, vol. 14(1), pages 1-10, 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:15:y:2024:i:1:d:10.1038_s41467-024-50522-7. 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.