Interfacial molecular regulation of TiO2 for enhanced and stable cocatalyst-free photocatalytic hydrogen production

Wenwei Lei; Hongji Wang; Sovann Khan; Norihiro Suzuki; Kai Takagi; Ken-Ichi Katsumata; Katsuya Teshima; Chiaki Terashima; Akira Fujishima

doi:10.1016/j.jcis.2023.04.118

Interfacial molecular regulation of TiO₂ for enhanced and stable cocatalyst-free photocatalytic hydrogen production

J Colloid Interface Sci. 2023 Sep:645:219-226. doi: 10.1016/j.jcis.2023.04.118. Epub 2023 Apr 28.

Authors

Wenwei Lei¹, Hongji Wang², Sovann Khan³, Norihiro Suzuki², Kai Takagi⁴, Ken-Ichi Katsumata⁵, Katsuya Teshima⁶, Chiaki Terashima⁷, Akira Fujishima⁴

Affiliations

¹ Hebei Key Laboratory of Nano-Biotechnology, School of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao 066004, Hebei, China. Electronic address: leiww@ysu.edu.cn.
² Hebei Key Laboratory of Nano-Biotechnology, School of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao 066004, Hebei, China.
³ International Institute for Carbon Neutral Energy Research (WPI-I2CNER), Kyushu University, Motooka 744, Nishi-ku, Fukuoka 819-0395, Japan.
⁴ Research Center for Space System Innovation, Tokyo University of Science, 2641 Yamazaki, Noda, Chiba 278-8510, Japan.
⁵ Department of Materials Science and Technology, Faculty of Advanced Engineering Industrial Science and Technology, Tokyo University of Science, 6-3-1 Niijuku, Katsushika-ku, Tokyo 125-8585, Japan.
⁶ Research Initiative for Supra-Materials, Shinshu University, 4-17-1 Wakasato, Nagano 380-8553, Japan.
⁷ Research Center for Space System Innovation, Tokyo University of Science, 2641 Yamazaki, Noda, Chiba 278-8510, Japan; Research Initiative for Supra-Materials, Shinshu University, 4-17-1 Wakasato, Nagano 380-8553, Japan. Electronic address: terashima@rs.tus.ac.jp.

PMID: 37149996
DOI: 10.1016/j.jcis.2023.04.118

Abstract

On the basis of the inherent property limitations of commercial P25-TiO₂, many surface interface modification methods have attracted substantial attention for further improving the photocatalytic properties. However, current strategies for designing and modifying efficient photocatalysts (which exhibit complicated manufacturing processes and harsh conditions) are not efficient for production that is low cost, is nontoxic, and exhibits good stability; and therefore restrict practical applications. Herein, a facile and reliable method is reported for in situ amine-containing silane coupling agent functionalization of commercial P25-TiO₂ by covalent surface modification for constructing a highly efficient photocatalyst. As a consequence, a high efficiency of H₂ evolution was achieved for TiO₂-SDA with 0.95 mmol h^-1 g^-1 (AQE ∼45.6 % at 365 nm) under solar light irradiation without a co-catalyst. The amination modification broadens the light absorption range of the photocatalyst, inhibits the binding of photogenerated carriers, and improves the photocatalytic efficiency; which was verified by photochemical properties and DFT theoretical calculations. This covalent modification method ensures the stability of the photocatalytic reaction. This work provides an approach for molecularly modified photocatalysts to improve photocatalytic performance by covalently modifying small molecules containing amine groups on the photocatalyst surface.

Keywords: Amine functionalization; DFT calculation; H(2) evolution; Molecular regulation; TiO(2).