https://scholars.lib.ntu.edu.tw/handle/123456789/630146
標題: | Naphthalene Diimide-Based Donor-Acceptor-Donor Small Molecules as Metal-Free Organocatalysts for Photocatalytic CO2 Reaction | 作者: | Wang, Shih Hao Chen, Pin Zhen Chen, Yen Yu Khurshid, Farheen Cai, Cheng Wei YU-YING LAI Chung, Po Wen RU-JONG JENG Rwei, Syang Peng LEE-YIH WANG |
關鍵字: | CO photoreduction 2 | conjugated small molecules | organocatalysts | photocatalysts | photochemical reaction | 公開日期: | 28-九月-2022 | 出版社: | AMER CHEMICAL SOC | 卷: | 14 | 期: | 38 | 來源出版物: | ACS Applied Materials and Interfaces | 摘要: | The application of organic small molecules as metal-free photocatalysts for light-driven photoreduction of carbon dioxide (CO2) has seldom been explored. This work developed four naphthalene diimide (NDI)-derived donor-acceptor-donor small molecules with different numbers of thiophene units, namely, NDI-2T, NDI-TT, NDI-4T, and NDI-6T, as metal-free photocatalysts to catalyze the reduction of CO2 under irradiation with an air mass 1.5G solar simulator at one-sun intensity. The structure-property relationship was investigated by exploring the effects of the electron-donating ability of the donor units on the optical properties, redox potential, electron-hole distribution, and exciton lifetime. NDI-6T exhibited the most red-shifted absorption, longest exciton lifetime, and strongest electron-hole separation. However, the large upshift in oxidation potential because of the elevated electron-donating ability of the hexathiophene unit significantly reduced the driving force for catalyst regeneration, leading to poor catalytic performance. Alternatively, NDI-4T possessed proper redox potentials, reduced charge-transfer resistance, and excellent photocurrent intensity; therefore, it effectively converted CO2 to a single product of CO in the presence of water as an electron donor without a sacrificial reagent or cocatalyst with a product yield of 168.6 μmol gcat-1 24 h-1, which was considerably higher than those of NDI-TT (111.9 μmol gcat-1 24 h-1), NDI-2T (88.4 μmol gcat-1 24 h-1), and NDI-6T (40.5 μmol gcat-1 24 h-1). This study provides a practical guideline for the molecular design of conjugated organic molecules as promising photocatalysts for CO2 photoreduction. |
URI: | https://scholars.lib.ntu.edu.tw/handle/123456789/630146 | ISSN: | 19448244 | DOI: | 10.1021/acsami.2c08531 |
顯示於: | 高分子科學與工程學研究所 |
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