Nanoconfined Molecular Catalysts in Integrated Gas Diffusion Electrodes for High-Current-Density CO2 Electroreduction |
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| Authors: | Xiangzhou Lv Qian Liu Hao Yang Jianghao Wang Xiuju Wu Xiaotong Li Zhifu Qi Jianhua Yan Angjian Wu Tao Cheng Hao Bin Wu |
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| Affiliation: | 1. Institute for Composites Science Innovation (InCSI), State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027 China;2. Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou, 215123 China;3. Institute of Zhejiang University – Quzhou, 78 Jiuhua Boulevard North, Quzhou, 324000 China;4. Baima Lake Laboratory, Hangzhou, 310053 China;5. State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou, 310027 China |
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| Abstract: | Molecular catalysts are promising catalysts to electrochemically convert CO2 into CO with high selectivity. However, achieving industrial-level current density remains challenging due to the limitation of charge- and mass-transport in gas diffusion electrode. Herein, a novel gas diffusion electrode architecture by confining highly dispersed cobalt(II) phthalocyanine (CoPc) molecules into -graphene oxide (GO) nanosheets (denoted as CoPc@GO) is designed. Benefiting from the accelerated CO2 diffusion and charge transport in the nanoconfined structure, the designed electrode achieves a high CO partial current density of 481.65 ± 12.50 mA cm?2 and a cathode energy efficiency over 64% for CO. The experimentally measured CO2 transport dynamics and molecular dynamics simulation confirm the accelerated CO2 diffusion, while theoretical calculations reveal the decreased energy barrier of the CO2 activation in the confined space. This study paves a new way for electrode architecture design that would accelerate the implementation of CO2 electrolysis technology. |
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| Keywords: | accelerated CO
2 diffusion CO
2 reduction reaction gas diffusion electrodes molecular catalysts nanoconfinement |
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