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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
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    References listed on IDEAS

    as
    1. 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.
    2. 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.
    3. 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.
    4. 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.
    5. 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.
    6. 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.
    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. 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.
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