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Efficient electron transmission in covalent organic framework nanosheets for highly active electrocatalytic carbon dioxide reduction

Author

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  • Hong-Jing Zhu

    (Nanjing Normal University)

  • Meng Lu

    (Nanjing Normal University)

  • Yi-Rong Wang

    (Nanjing Normal University)

  • Su-Juan Yao

    (Nanjing Normal University)

  • Mi Zhang

    (Nanjing Normal University)

  • Yu-He Kan

    (Huaiyin Normal University)

  • Jiang Liu

    (Nanjing Normal University)

  • Yifa Chen

    (Nanjing Normal University)

  • Shun-Li Li

    (Nanjing Normal University)

  • Ya-Qian Lan

    (Nanjing Normal University)

Abstract

Efficient conversion of carbon dioxide (CO2) into value-added products is essential for clean energy research. Design of stable, selective, and powerful electrocatalysts for CO2 reduction reaction (CO2RR) is highly desirable yet largely unmet. In this work, a series of metalloporphyrin-tetrathiafulvalene based covalent organic frameworks (M-TTCOFs) are designed. Tetrathiafulvalene, serving as electron donator or carrier, can construct an oriented electron transmission pathway with metalloporphyrin. Thus-obtained M-TTCOFs can serve as electrocatalysts with high FECO (91.3%, −0.7 V) and possess high cycling stability (>40 h). In addition, after exfoliation, the FECO value of Co-TTCOF nanosheets (~5 nm) is higher than 90% in a wide potential range from −0.6 to −0.9 V and the maximum FECO can reach up to almost 100% (99.7%, −0.8 V). The electrocatalytic CO2RR mechanisms are discussed and revealed by density functional theory calculations. This work paves a new way in exploring porous crystalline materials in electrocatalytic CO2RR.

Suggested Citation

  • Hong-Jing Zhu & Meng Lu & Yi-Rong Wang & Su-Juan Yao & Mi Zhang & Yu-He Kan & Jiang Liu & Yifa Chen & Shun-Li Li & Ya-Qian Lan, 2020. "Efficient electron transmission in covalent organic framework nanosheets for highly active electrocatalytic carbon dioxide reduction," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-019-14237-4
    DOI: 10.1038/s41467-019-14237-4
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    Cited by:

    1. Rengan Luo & Haifeng Lv & Qiaobo Liao & Ningning Wang & Jiarui Yang & Yang Li & Kai Xi & Xiaojun Wu & Huangxian Ju & Jianping Lei, 2021. "Intrareticular charge transfer regulated electrochemiluminescence of donor–acceptor covalent organic frameworks," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    2. Huihui Zhang & Chang Xu & Xiaowen Zhan & Yu Yu & Kaifu Zhang & Qiquan Luo & Shan Gao & Jinlong Yang & Yi Xie, 2022. "Mechanistic insights into CO2 conversion chemistry of copper bis-(terpyridine) molecular electrocatalyst using accessible operando spectrochemistry," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    3. Ji Wei Sun & Xuefeng Wu & Peng Fei Liu & Jiacheng Chen & Yuanwei Liu & Zhen Xin Lou & Jia Yue Zhao & Hai Yang Yuan & Aiping Chen & Xue Lu Wang & Minghui Zhu & Sheng Dai & Hua Gui Yang, 2023. "Scalable synthesis of coordinatively unsaturated metal-nitrogen sites for large-scale CO2 electrolysis," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    4. Minghao Liu & Shuai Yang & Xiubei Yang & Cheng-Xing Cui & Guojuan Liu & Xuewen Li & Jun He & George Zheng Chen & Qing Xu & Gaofeng Zeng, 2023. "Post-synthetic modification of covalent organic frameworks for CO2 electroreduction," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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