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Continuous production of pure liquid fuel solutions via electrocatalytic CO2 reduction using solid-electrolyte devices

Author

Listed:
  • Chuan Xia

    (Rice University
    Harvard University)

  • Peng Zhu

    (Rice University)

  • Qiu Jiang

    (King Abdullah University of Science and Technology (KAUST))

  • Ying Pan

    (Harvard University)

  • Wentao Liang

    (Northeastern University, Innovation Campus at Burlington, MA (ICBM))

  • Eli Stavitski

    (Brookhaven National Laboratory)

  • Husam N. Alshareef

    (King Abdullah University of Science and Technology (KAUST))

  • Haotian Wang

    (Rice University)

Abstract

Electrocatalytic CO2 reduction is often carried out in a solution electrolyte such as KHCO3(aq), which allows for ion conduction between electrodes. Therefore, liquid products that form are in a mixture with the dissolved salts, requiring energy-intensive downstream separation. Here, we report continuous electrocatalytic conversion of CO2 to pure liquid fuel solutions in cells that utilize solid electrolytes, where electrochemically generated cations (such as H+) and anions (such as HCOO−) are combined to form pure product solutions without mixing with other ions. Using a HCOOH-selective (Faradaic efficiencies > 90%) and easily scaled Bi catalyst at the cathode, we demonstrate production of pure HCOOH solutions with concentrations up to 12 M. We also show 100 h continuous and stable generation of 0.1 M HCOOH with negligible degradation in selectivity and activity. Production of other electrolyte-free C2+ liquid oxygenate solutions, including acetic acid, ethanol and n-propanol, are also demonstrated using a Cu catalyst. Finally, we show that our CO2 reduction cell with solid electrolytes can be modified to suit other, more complex practical applications.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natene:v:4:y:2019:i:9:d:10.1038_s41560-019-0451-x
    DOI: 10.1038/s41560-019-0451-x
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    Cited by:

    1. 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.
    2. 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.
    3. Bohua Ren & Guobin Wen & Rui Gao & Dan Luo & Zhen Zhang & Weibin Qiu & Qianyi Ma & Xin Wang & Yi Cui & Luis Ricardez–Sandoval & Aiping Yu & Zhongwei Chen, 2022. "Nano-crumples induced Sn-Bi bimetallic interface pattern with moderate electron bank for highly efficient CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    4. 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.
    5. Tufa, Ramato Ashu & Chanda, Debabrata & Ma, Ming & Aili, David & Demissie, Taye Beyene & Vaes, Jan & Li, Qingfeng & Liu, Shanhu & Pant, Deepak, 2020. "Towards highly efficient electrochemical CO2 reduction: Cell designs, membranes and electrocatalysts," Applied Energy, Elsevier, vol. 277(C).
    6. Pribyl-Kranewitter, B. & Beard, A. & Gîjiu, C.L. & Dinculescu, D. & Schmidt, T.J., 2022. "Influence of low-temperature electrolyser design on economic and environmental potential of CO and HCOOH production: A techno-economic assessment," Renewable and Sustainable Energy Reviews, Elsevier, vol. 154(C).
    7. 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.
    8. Xiaohan Yu & Yuting Xu & Le Li & Mingzhe Zhang & Wenhao Qin & Fanglin Che & Miao Zhong, 2024. "Coverage enhancement accelerates acidic CO2 electrolysis at ampere-level current with high energy and carbon efficiencies," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    9. Juncai Dong & Yangyang Liu & Jiajing Pei & Haijing Li & Shufang Ji & Lei Shi & Yaning Zhang & Can Li & Cheng Tang & Jiangwen Liao & Shiqing Xu & Huabin Zhang & Qi Li & Shenlong Zhao, 2023. "Continuous electroproduction of formate via CO2 reduction on local symmetry-broken single-atom catalysts," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    10. Jiexin Zhu & Jiantao Li & Ruihu Lu & Ruohan Yu & Shiyong Zhao & Chengbo Li & Lei Lv & Lixue Xia & Xingbao Chen & Wenwei Cai & Jiashen Meng & Wei Zhang & Xuelei Pan & Xufeng Hong & Yuhang Dai & Yu Mao , 2023. "Surface passivation for highly active, selective, stable, and scalable CO2 electroreduction," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    11. 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.
    12. 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.
    13. Xiao Zhang & Xunhua Zhao & Peng Zhu & Zachary Adler & Zhen-Yu Wu & Yuanyue Liu & Haotian Wang, 2022. "Electrochemical oxygen reduction to hydrogen peroxide at practical rates in strong acidic media," Nature Communications, Nature, vol. 13(1), pages 1-11, December.

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