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

Hong-Jing Zhu, Meng Lu, Yi-Rong Wang, Su-Juan Yao, Mi Zhang, Yu-He Kan, Jiang Liu, Yifa Chen, Shun-Li Li and Ya-Qian Lan ()
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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

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-019-14237-4

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