| Autor: |
Gao, Fei, Wu, Ya-Pan, Wu, Xue-Qian, Li, Dong-Sheng, Yang, Guoping, Wang, Yao-Yu |
| Zdroj: |
Inorganic Chemistry; May 2024, Vol. 63 Issue: 19 p8948-8957, 10p |
| Abstrakt: |
Excellent electrocatalytic CO2reduction reaction activity has been demonstrated by transition metals and nitrogen-codoped carbon (M–N–C) catalysts, especially for transition-metal porphyrin (MTPP)-based catalysts. In this work, we propose to use one-step low-temperature pyrolysis of the isostructural MTPP-based metal–organic frameworks (MOFs) and electrochemical in situ reduction strategies to obtain a series of hybrid catalysts of Co nanoparticles (Co NPs) and MTPP, named Co NPs/MTPP (M = Fe, Co, and Ni). The in situ introduction of Co NPs can efficiently enhance the electrocatalytic ability of MTPP (M = Fe, Co, and Ni) to convert CO2to CO, particularly for FeTPP. Co NPs/FeTPP endowed a high CO faradaic efficiency (FECOmax= 95.5%) in the H cell, and the FECO> 90.0% is in the broad potential range of −0.72 to −1.22 VRHE. In addition, the Co NPs/FeTPP achieved 145.4 mA cm–2at a lower potential of −0.70 VRHEwith an FECOof 94.7%, and the CO partial currents increased quickly to reach 202.2 mA cm–2at −0.80 VRHEwith an FECOof 91.6% in the flow cell. It is confirmed that Co NPs are necessary for hybrid catalysts to get superior electrocatalytic activity; Co NPs also can accelerate H2O dissociation and boost the proton supply capacity to hasten the proton-coupled electron-transfer process, effectively adjusting the adsorption strength of the reaction intermediates. |
| Databáze: |
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