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

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.

SUBMITTER: Zhu HJ 

PROVIDER: S-EPMC6981265 | biostudies-literature | 2020 Jan

REPOSITORIES: biostudies-literature