Biomimetic Phthalocyanine‐Based Covalent Organic Frameworks with Tunable Pendant Groups for Electrocatalytic CO2 Reduction

Author:

Xie Tao1,Chen Shuai1,Yue Yan1,Sheng Tian12,Huang Ning2,Xiong Yujie13ORCID

Affiliation:

1. anhui Engineering Research Center of Carbon Neutrality The Key Laboratory of Functional Molecular Solids Ministry of Education, Anhui Laboratory of Molecular-Based Materials, College of Chemistry and Materials Science Anhui Normal University Wuhu 241002 Anhui China

2. MOE Key Laboratory of Macromolecular Synthesis and Functionalization, State Key Laboratory of Silicon Materials, Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 Zhejiang China

3. School of Chemistry and Materials Science University of Science and Technology of China Hefei 230026 Anhui China

Abstract

AbstractElectrocatalytic carbon dioxide reduction reaction (CO2RR) is an effective way of converting CO2 into value‐added products using renewable energy, whose activity and selectivity can be in principle maneuvered by tuning the microenvironment near catalytic sites. Here, we demonstrate a strategy for tuning the microenvironment of CO2RR by learning from the natural chlorophyll and heme. Specifically, the conductive covalent organic frameworks (COFs) linked by piperazine serve as versatile supports for single‐atom catalysts (SACs), and the pendant groups modified on the COFs can be readily tailored to offer different push‐pull electronic effects for tunable microenvironment. As a result, while all the COFs exhibit high chemical structure stability under harsh conditions and good conductivity, the addition of −CH2NH2 can greatly enhance the activity and selectivity of CO2RR. As proven by experimental characterization and theoretical simulation, the electron‐donating group (−CH2NH2) not only reduces the surface work function of COF, but also improves the adsorption energy of the key intermediate *COOH, compared with the COFs with electron‐withdrawing groups (−CN, −COOH) near the active sites. This work provides insights into the microenvironment modulation of CO2RR electrocatalysts at the molecular level.

Funder

National Natural Science Foundation of China

Publisher

Wiley

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