- 學位論文
二芳基乙烯衍生物：一個創新的光催化 CO2轉化為CO的還原反應
Diarylethene Derivatives: An Innovative Target for Photocatalytic CO2-to-CO Reduction
本文將於2028/09/05開放下載。若您希望在開放下載時收到通知，可將文章加入收藏。
摘要
光催化二氧化碳還原反應已經成為全球性議題，近年來，除了雙核超分子系統，利用氫鍵、動態配位結合等高效的光催化體系皆已被廣泛報導。值得注意的是，反應的可調控性是一個創新的目標，表明其為一個具有高自由度的開/關反應。本研究中選用二芳基乙烯衍生物作為光致變色材料，並於實驗中證明該材料的高度可逆性以及高響應。其中，透過核磁共振光譜儀及紫外線/可見光光譜儀進行滴定實驗，並成功確定了光催化劑與二芳基乙烯之間的配位關係。在光催化二氧化碳還原反應中，得知開放形式的轉換數 (TON) 為313；封閉形式的轉換數 (TON) 為27，並透過開放/封閉形式之間的光誘導相互轉換證明了二氧化碳還原反應的可控性。
並列摘要
There is a need to explore photocatalytic CO2 reduction worldwide. In recent years, high efficiency photocatalysis systems such as bi-nuclear supramolecular, hydrogen bonding, dynamic coordination, and others were reported extensively. It is noteworthy that the controllable element of the reaction is an innovative target, indicating that it is a switch-on/off reaction with a high degree of freedom. We have used diarylethene darivates as a photochromic material herein, and the material was demonstrated to be highly reversible and responsive. As a result of 1H nuclear magnetic resonance and UV titrations, we were able to determine the coordination between catalyst and diarylethene. A photocatalytic conversion of CO2 to CO gave a turnover number (TON) of 313 for the open form and 27 for the closed form, respectively, as a result of the photocatalytic CO2-to-CO conversion. The light-induced interconversion between open and closed forms demonstrated its controllability.
參考文獻
1. Gabrielli, P.; Gazzani, M.; Mazzotti, M. The Role of Carbon Capture and Utilization, Carbon Capture and Storage, and Biomass to Enable a Net-Zero-CO2 Emissions Chemical Industry. Ind. Eng. Chem. Res. 2020, 59, 7033-7045.
2. Michailos, S.; McCord, S.; Sick, V.; Stokes, G.; Styring, P. Dimethyl ether synthesis via captured CO2 hydrogenation within the power to liquids concept: A techno-economic assessment. Energy Convers. Manage. 2019, 184, 262-276.
3. Yao, B.; Xiao, T.; Makgae, O. A.; Jie, X.; Gonzalez-Cortes, S.; Guan, S.; Kirkland, A. I.; Dilworth, J. R.; Al-Megren, H. A.; Alshihri, S. M.; et al. Transforming carbon dioxide into jet fuel using an organic combustion-synthesized Fe-Mn-K catalyst. Nat. Commun. 2020, 11, 6395.
4. Peter, S. C. Reduction of CO2 to Chemicals and Fuels: A Solution to Global Warming and Energy Crisis. ACS Energy Lett. 2018, 3, 1557-1561.
5. Wang, W.; Wang, S.; Ma, X.; Gong, J. Recent advances in catalytic hydrogenation of carbon dioxide. Chem. Soc. Rev. 2011, 40, 3703-3727.