以理論計算方法探討CO在Cu(711)表面上的電化學還原

Computational Electrochemical Reduction of CO on Cu(711) surface

辜敏韶(KU Min-Shao)

指導教授 ： 蔡明剛

國立臺灣師範大學/理學院/化學系/碩士(2019年)

https://doi.org/10.6345/NTNU201900830

摘要

在現今社會中，使用銅做為電催化電極是現今將二氧化碳電還原成許多有用的燃料的其中一項主要方法。透過製備不同的銅電極材料表面來區分各種催化途徑成為CO2電還原化學最關注的主題之一；而催化體系設計的成功與否，取決於是否提高還原CO2的選擇性。利用理論計算，我們研究Cu(711)表面，以了解早期實驗觀察所顯示的C-C耦合的有趣選擇性。通過分析沿著CO2還原機理的各種關鍵中間體的電子結構，可以為設計用於Cn（n≥2）烴合成的Cu電極材料的新形態提供進一步的見解。

關鍵字

理論計算 ； Cu(711) ； CO2

並列摘要

Carbon dioxide can be electrochemically reduced to many useful fuels using copper electrocatalysts. The differentiation of the various catalytic pathways by the preparation of Cu electrode materials becomes one of the most concerned topics for the CO2 electroreduction chemistry. The enhancement in the CO2 reduction selectivity determines the success of catalytic system design. Through theoretical calculations, we investigate Cu(711) surface in order to understand the intriguing selectivity for the C-C coupling shown by the early experimental observation. By analyzing the electronic structure of the various critical intermediates along the CO2 reduction mechanism, it will be possible to provide further insights for designing the new morphology of Cu electrode materials for Cn (n ≥ 2) hydrocarbon synthesis.

並列關鍵字

Theoretical calculation ； Cu(711) ； CO2

參考文獻

1. Garza, A. J.; Bell, A. T.; Head-Gordon, M., Mechanism of CO2 Reduction at Copper Surfaces: Pathways to C2 Products. ACS Catalysis 2018, 8 (2), 1490-1499.

2. Yang, K. D.; Lee, C. W.; Jin, K.; Im, S. W.; Nam, K. T., Current Status and Bioinspired Perspective of Electrochemical Conversion of CO2 to a Long-Chain Hydrocarbon. J Phys Chem Lett 2017, 8 (2), 538-545.

3. Schouten, K. J.; Qin, Z.; Perez Gallent, E.; Koper, M. T., Two pathways for the formation of ethylene in CO reduction on single-crystal copper electrodes. J Am Chem Soc 2012, 134 (24), 9864-7.

4. Dutta, A.; Rahaman, M.; Luedi, N. C.; Mohos, M.; Broekmann, P., Morphology Matters: Tuning the Product Distribution of CO2 Electroreduction on Oxide-Derived Cu Foam Catalysts. ACS Catalysis 2016, 6 (6), 3804-3814.

5. Yang, K. D.; Ko, W. R.; Lee, J. H.; Kim, S. J.; Lee, H.; Lee, M. H.; Nam, K. T., Morphology-Directed Selective Production of Ethylene or Ethane from CO2 on a Cu Mesopore Electrode. Angew Chem Int Ed Engl 2017, 56 (3), 796-800.