| Autor: |
Yi−Rong Wang, Qiang Li, Long−Zhang Dong, Rui Wang, Qing Huang, Yu−Han Xia, Jin−Lan Wang, Jiang Liu, Ya-Qian Lan |
| Rok vydání: |
2019 |
| Předmět: |
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| Zdroj: |
Matter. 1:1656-1668 |
| ISSN: |
2590-2385 |
| DOI: |
10.1016/j.matt.2019.07.003 |
| Popis: |
Summary The activation of CO2 on the electrocatalyst surface is regarded as the rate-determining step in electrocatalytic CO2 reduction (ECR), and it is therefore highly important to find out its adsorption and activation mechanism. Herein, we develop the OH–-coordinated metal-organic framework (NNU-15) to simulate the surface state of catalyst in alkaline environment of ECR and then further explore its activation mechanism to CO2. NNU-15 shows high faradic efficiency for CO (FECO) reaching up to 99.2% at −0.6 V versus RHE along with long-term stability (110 h) and surpassing 96% over a wide potential range from −0.6 to −0.9 V. In the ECR process, single-crystal to single-crystal transformation between NNU-15 and NNU-15-CO2 demonstrates that coordinated OH– can activate the CO2 into HCO3–, which will chelate to the metal center. Theoretical calculations validate that both O-adsorbed and C-adsorbed initial geometries are inclined to result in the formation of HCO3– during the ECR process. |
| Databáze: |
OpenAIRE |
| Externí odkaz: |
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