IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-023-44586-0.html
   My bibliography  Save this article

Vitamin C-induced CO2 capture enables high-rate ethylene production in CO2 electroreduction

Author

Listed:
  • Jongyoun Kim

    (Daegu Gyeongbuk Institute of Science and Technology (DGIST))

  • Taemin Lee

    (Daegu Gyeongbuk Institute of Science and Technology (DGIST))

  • Hyun Dong Jung

    (Sogang University)

  • Minkyoung Kim

    (Daegu Gyeongbuk Institute of Science and Technology (DGIST))

  • Jungsu Eo

    (Daegu Gyeongbuk Institute of Science and Technology (DGIST))

  • Byeongjae Kang

    (Daegu Gyeongbuk Institute of Science and Technology (DGIST))

  • Hyeonwoo Jung

    (Daegu Gyeongbuk Institute of Science and Technology (DGIST))

  • Jaehyoung Park

    (Daegu Gyeongbuk Institute of Science and Technology (DGIST))

  • Daewon Bae

    (Daegu Gyeongbuk Institute of Science and Technology (DGIST))

  • Yujin Lee

    (Daegu Gyeongbuk Institute of Science and Technology (DGIST))

  • Sojung Park

    (Korea Institute of Energy Technology (KENTECH))

  • Wooyul Kim

    (Korea Institute of Energy Technology (KENTECH))

  • Seoin Back

    (Sogang University)

  • Youngu Lee

    (Daegu Gyeongbuk Institute of Science and Technology (DGIST))

  • Dae-Hyun Nam

    (Daegu Gyeongbuk Institute of Science and Technology (DGIST))

Abstract

High-rate production of multicarbon chemicals via the electrochemical CO2 reduction can be achieved by efficient CO2 mass transport. A key challenge for C−C coupling in high-current-density CO2 reduction is how to promote *CO formation and dimerization. Here, we report molecularly enhanced CO2-to-*CO conversion and *CO dimerization for high-rate ethylene production. Nanoconfinement of ascorbic acid by graphene quantum dots enables immobilization and redox reversibility of ascorbic acid in heterogeneous electrocatalysts. Cu nanowire with ascorbic acid nanoconfined by graphene quantum dots (cAA-CuNW) demonstrates high-rate ethylene production with a Faradaic efficiency of 60.7% and a partial current density of 539 mA/cm2, a 2.9-fold improvement over that of pristine CuNW. Furthermore, under low CO2 ratio of 33%, cAA-CuNW still exhibits efficient ethylene production with a Faradaic efficiency of 41.8%. We find that cAA-CuNW increases *CO coverage and optimizes the *CO binding mode ensemble between atop and bridge for efficient C−C coupling. A mechanistic study reveals that ascorbic acid can facilitate *CO formation and dimerization by favorable electron and proton transfer with strong hydrogen bonding.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-023-44586-0
    DOI: 10.1038/s41467-023-44586-0
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-44586-0
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-023-44586-0?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. 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. 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. 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.
    4. Changhyeok Choi & Geun Ho Gu & Juhwan Noh & Hyun S. Park & Yousung Jung, 2021. "Understanding potential-dependent competition between electrocatalytic dinitrogen and proton reduction reactions," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    5. Yifan Ye & Hao Yang & Jin Qian & Hongyang Su & Kyung-Jae Lee & Tao Cheng & Hai Xiao & Junko Yano & William A. Goddard & Ethan J. Crumlin, 2019. "Dramatic differences in carbon dioxide adsorption and initial steps of reduction between silver and copper," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    6. 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.
    7. Sheng-Chih Lin & Chun-Chih Chang & Shih-Yun Chiu & Hsiao-Tien Pai & Tzu-Yu Liao & Chia-Shuo Hsu & Wei-Hung Chiang & Ming-Kang Tsai & Hao Ming Chen, 2020. "Operando time-resolved X-ray absorption spectroscopy reveals the chemical nature enabling highly selective CO2 reduction," Nature Communications, Nature, vol. 11(1), pages 1-12, December.
    8. Tianyu Zhang & Weitao Li & Kai Huang & Huazhang Guo & Zhengyuan Li & Yanbo Fang & Ram Manohar Yadav & Vesselin Shanov & Pulickel M. Ajayan & Liang Wang & Cheng Lian & Jingjie Wu, 2021. "Regulation of functional groups on graphene quantum dots directs selective CO2 to CH4 conversion," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    Full references (including those not matched with items on IDEAS)

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. Kaihang Yue & Yanyang Qin & Honghao Huang & Zhuoran Lv & Mingzhi Cai & Yaqiong Su & Fuqiang Huang & Ya Yan, 2024. "Stabilized Cu0 -Cu1+ dual sites in a cyanamide framework for selective CO2 electroreduction to ethylene," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

    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. Stefan Ringe, 2023. "The importance of a charge transfer descriptor for screening potential CO2 reduction electrocatalysts," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    3. 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.
    4. 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.
    5. 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.
    6. 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.
    7. Shengdong Xiao & Caroline Akinyi & Jimmy Longun & Jude O. Iroh, 2022. "Polyimide Copolymers and Nanocomposites: A Review of the Synergistic Effects of the Constituents on the Fire-Retardancy Behavior," Energies, MDPI, vol. 15(11), pages 1-29, May.
    8. 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.
    9. 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.
    10. Khandelwal, Akshat & Maarisetty, Dileep & Baral, Saroj Sundar, 2022. "Fundamentals and application of single-atom photocatalyst in sustainable energy and environmental applications," Renewable and Sustainable Energy Reviews, Elsevier, vol. 167(C).
    11. 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.
    12. Tuğçe Beyazay & Kendra S. Belthle & Christophe Farès & Martina Preiner & Joseph Moran & William F. Martin & Harun Tüysüz, 2023. "Ambient temperature CO2 fixation to pyruvate and subsequently to citramalate over iron and nickel nanoparticles," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    13. Hai-Gang Qin & Yun-Fan Du & Yi-Yang Bai & Fu-Zhi Li & Xian Yue & Hao Wang & Jian-Zhao Peng & Jun Gu, 2023. "Surface-immobilized cross-linked cationic polyelectrolyte enables CO2 reduction with metal cation-free acidic electrolyte," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    14. Kaihang Yue & Yanyang Qin & Honghao Huang & Zhuoran Lv & Mingzhi Cai & Yaqiong Su & Fuqiang Huang & Ya Yan, 2024. "Stabilized Cu0 -Cu1+ dual sites in a cyanamide framework for selective CO2 electroreduction to ethylene," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    15. Wei Chen & Liang Zhang & Leitao Xu & Yuanqing He & Huan Pang & Shuangyin Wang & Yuqin Zou, 2024. "Pulse potential mediated selectivity for the electrocatalytic oxidation of glycerol to glyceric acid," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    16. 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.
    17. Xueping Qin & Heine A. Hansen & Karoliina Honkala & Marko M. Melander, 2023. "Cation-induced changes in the inner- and outer-sphere mechanisms of electrocatalytic CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    18. Huazhang Guo & Yuhao Lu & Zhendong Lei & Hong Bao & Mingwan Zhang & Zeming Wang & Cuntai Guan & Bijun Tang & Zheng Liu & Liang Wang, 2024. "Machine learning-guided realization of full-color high-quantum-yield carbon quantum dots," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    19. Jiali Wang & Chia-Shuo Hsu & Tai-Sing Wu & Ting-Shan Chan & Nian-Tzu Suen & Jyh-Fu Lee & Hao Ming Chen, 2023. "In situ X-ray spectroscopies beyond conventional X-ray absorption spectroscopy on deciphering dynamic configuration of electrocatalysts," Nature Communications, Nature, vol. 14(1), pages 1-23, December.
    20. Mengyang Fan & Rui Kai Miao & Pengfei Ou & Yi Xu & Zih-Yi Lin & Tsung-Ju Lee & Sung-Fu Hung & Ke Xie & Jianan Erick Huang & Weiyan Ni & Jun Li & Yong Zhao & Adnan Ozden & Colin P. O’Brien & Yuanjun Ch, 2023. "Single-site decorated copper enables energy- and carbon-efficient CO2 methanation in acidic conditions," Nature Communications, Nature, vol. 14(1), pages 1-8, 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_s41467-023-44586-0. 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.