材料科学
光电流
电子供体
光化学
催化作用
试剂
电子受体
氧化还原
光催化
二亚胺
接受者
分子
化学
物理化学
有机化学
光电子学
物理
冶金
凝聚态物理
苝
作者
Shih‐Hao Wang,Pin-Zhen Chen,Yen‐Yu Chen,Farheen Khurshid,Cheng-Wei Cai,Yu‐Ying Lai,Po‐Wen Chung,Ru‐Jong Jeng,Syang‐Peng Rwei,Leeyih Wang
标识
DOI:10.1021/acsami.2c08531
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.
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