Journal
CHEMICAL ENGINEERING JOURNAL
Volume 441, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136084
Keywords
Perylene diimide; Photocatalysis; D; A; Built-in electric field; Nitrogen Fixation
Categories
Funding
- Guizhou Provincial Science and Technology Foundation [ZK2021069]
- Young Science and Technology Talents Development Project of Education Department in Guizhou Province [KY2022144]
- National Natural Science Foundation of China [21725602, 21975069]
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This study successfully improves the photoreactivity and stability of perylene-3,4,9,10tetracarboxylic acid diimide (PDI) composite by constructing polarity-bridged acceptor-donor units. The polarity bridging adjusts the band gaps and absorption characteristics, enhancing carrier separation and exciton dissociation efficiency.
Constructing acceptor-donor units (D/A) of polymer is an efficient method for promoting carrier separation to optimize photoreactivity. However, the carriers across the D/A interface of micromolecule was relatively hindered by the Coulomb potential. In this work, the polarity-bridged acceptor-donor units of perylene-3,4,9,10tetracarboxylic acid diimide (PDI) composite (BOPDI) has been constructed using a simple strategy. The improved BOPDI achieves excellent photocatalytic nitrogen fixation rate (74.0 mu mol g- 1h- 1) as well as stability without using any co-catalyst and sacrificial agent, which is 11 times that of the original PDI group. DFT calculations and experimental results show that the polarity-bridges reasonably adjusts the Highest Occupied Molecular Orbital (HOMO) and Lowest Unoccupied Molecular Orbital (LUMO) bands and absorption characteristics, ensuring the BOPDI absorbed near-infrared light and activated N2 molecules. In addition, the polarity bridged units strengthen the construction of the built-in electric field for overcoming the Coulomb potential, resulting in a higher carrier separation and exciton dissociation efficiency. This work not only provides a tactics for enhancing the electronic transmission of D/A units, but also expanding the application research of PDI composite materials in the photocatalytic reduction of nitrogen.
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