Spaced Double Hydrogen Bonding in an Imidazole Poly Ionic Liquid Composite for Highly Efficient and Selective Photocatalytic Air Reductive H 2 O 2 Synthesis

• Published in: Angewandte Chemie International Edition Vol. 63; no. 15; p. e202400857
• Main Authors: Cheng, Yu, Jin, Jie, Yan, Huan, Zhou, Guosheng, Xu, Yangrui, Tang, Liguang, Liu, Xinlin, Li, Hongping, Zhang, Kan, Lu, Ziyang
• Format: Journal Article
• Language: English
• Published: Germany 08-04-2024
• Subjects: Exposed electron-riched active site; Air efficient utilization; H2O2 photosynthesis; O2 selective adsorption; Spaced double hydrogen bond
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202400857

Photocatalytic oxygen reductive H
O
production is a promising approach to alternative industrial anthraquinone processes while suffering from the requirement of pure O
feedstock for practical application. Herein, we report a spaced double hydrogen bond (IC-H-bond) through multi-component Radziszewski reaction in an imidazole poly-ionic-liquid composite (SI-PIL-TiO
) and levofloxacin hydrochloride (LEV) electron donor for highly efficient and selective photocatalytic air reductive H
O
production. It is found that the IC-H-bond formed by spaced imino (-NH-) group of SI-PIL-TiO
and carbonyl (-C=O) group of LEV can switch the imidazole active sites characteristic from a covered state to a fully exposed one to shield the strong adsorption of electron donor and N
in the air, and propel an intenser positive potential and more efficient orbitals binding patterns of SI-PIL-TiO
surface to establish competitive active sites for selectivity O
chemisorption. Moreover, the high electron enrichment of imidazole as an active site for the 2e
oxygen reduction ensures the rapid reduction of O
. Therefore, the IC-H-bond enables a total O
utilization and conversion efficiency of 94.8 % from direct photocatalytic air reduction, achieving a H
O
production rate of 1518 μmol/g/h that is 16 and 23 times compared to poly-ionic-liquid composite without spaced imino groups (PIL-TiO
) and TiO
, respectively.