Deformed One-Dimensional Covalent Organic Polymers for Enhanced CO Electroreduction to Methanol
Year: 2025
Type: article
Abstract: Spatially arranged molecular catalysts in polymeric frameworks, typically in a layered structure, are emerging strategies to mitigate the molecular aggregation and improve the catalytic performance. However, the effect of local coordination induced by polymerization remains underexplored. Here, we develop one-dimensional cobalt-tetra-amino-phthalocyanine-based covalent organic polymers (1D-COP) for the electrochemical CO reduction reaction (CORR). We use carbon nanotubes as ideal templates to induce local curvature of the 1D-COP. The COP on single-walled CNT (1D-COP/SWCNT) catalyst exhibits a maximum methanol Faradaic efficiency of 70% in an H-cell, which exceeds those on wider-diameter multiwalled carbon nanotubes (22% for 4-6 nm and 14% for 10-20 nm). Using X-ray and vibronic spectroscopies, we have observed distinct local geometries and electronic structures induced by the strong interactions between the COP layer and CNT substrates. Density functional theory calculations further support that increased curvature of the COP-SWCNT catalyst enhances the *CO binding species, leading to improved subsequent reduction reactions. Our results highlight the critical role of the local structure in polymeric frameworks for improved electrocatalytic performance.
Source: ACS Nano
Authors: Yong Liu, Honglei Wang, Honglei Wang, Yun Song, Charles B. Musgrave III, Pei Xiong, Jiangtong Li, Geng Li, Libei Huang, Jianjun Su, Yinger Xin, Qiang Zhang, Weihua Guo, Mingming He, Tanglue Feng, Xing Li, Molly Meng-Jung Li, Peter A. van Aken, Hongguang Wang, Hongguang Wang, William A. Goddard III, Ruquan Ye
Language: English
Field: Energy
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $4,500
Funders: California Institute of Technology, City University of Hong Kong, State Key Laboratory in Marine Pollution, Science and Technology Foundation of Shenzhen City, European Commission, Research Grants Council, University Grants Committee, Hong Kong Polytechnic University, Technische Universität Ilmenau, Basic and Applied Basic Research Foundation of Guangdong Province
Awards: G2152291004, Designing effective molecule/electrode interfaces for universal molecular CO2 reduction in strong acids, G2986027338, Enabling Science and Technology through European Electron Microscopy, G5597625300, G5633541800, G6326200580, G7239583613, Steering the Local Environment of Ultrathin Covalent Organic Polymers for Efficient Electroreduction of CO2 to Methanol
OpenAlex ID: W4411418864