journal article·2023-06-05

Modulating Electrochemical CO2 Reduction Performance via Sulfur-Containing Linkages Engineering in Metallophthalocyanine Based Covalent Organic Frameworks

Xiubei Yang, Xuewen Li, Minghao Liu, Shuai Yang, Qianyuan Niu, Lipeng Zhai, Zheng Jiang, Qing Xu, Gaofeng Zeng

ACS Materials Letters· Volume 5· Issue 6
Publisher page

Abstract

Covalent organic frameworks (COFs) with metallophthalocyanine (MPc) units provide new opportunities for the design of advanced materials with attractive electrical properties. However, the limited synthetic linkage chemistry hinders their further exploration. Herein, we demonstrated heterocycles strategy-based linkage engineering to fabricate two novel MPc-based COFs with thiomorpholine and dithiine linkages. More S atoms in dithiine-linked CoPc-DSDS-COF contributed to the higher conductivity (0.78 mS cm –1 ) and higher reductive ability than those of thiomorpholine-linked CoPc-DNDS-COF (0.62 mS cm –1 ) and, thus, result in higher activity with a partial current density for CO of 30.42 mA cm –2 at −1.0 V vs RHE and in selectivity toward CO 2 reduction with the Faradaic efficiency of 96.5% at −0.9 V. Additionally, the theoretical calculation revealed the dithiine linkages showed better suppressing ability of the competing hydrogen evolution reaction than the thiomorpholine linkages. This work gives us a new insight into catalytic COFs via strategic linkage engineering at the atomic level.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Covalent Organic Framework Applications · CO2 Reduction Techniques and Catalysts · Metal-Organic Frameworks: Synthesis and Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute (SARI), Chinese Academy of Sciences (CAS), Shanghai 201210, P. R. China

School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, P. R. China

Shanghai Synchrotron Radiation Facility, Zhangjiang Lab, Shanghai Advanced Research Institute, University of Chinese Academy of Sciences, Shanghai 201210, P. R. China

Henan Key Laboratory of Functional Salt Materials, Center for Advanced Materials Research, Zhongyuan University of Technology, Zhengzhou 450007, P. R. China

Funding

Natural Science Foundation of Shanghai · Science and Technology Department of Henan Province · Science and Technology Commission of Shanghai Municipality · National Natural Science Foundation of China

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