Germanium-substituted Zn2TiO4 solid solution photocatalyst for conversion of CO2 into fuels

Autor: Jiaxue Lu, Jinni Shen, Deli Li, Jun Liang, Yao Chai, Yongfan Zhang, Xuxu Wang, Li Li
Rok vydání: 2019
Předmět:
Zdroj: Journal of Catalysis. 371:144-152
ISSN: 0021-9517
DOI: 10.1016/j.jcat.2019.01.017
Popis: Photocatalytic CO2 reduction conjugated with H2O oxidation is regarded as a promising artificial photosynthesis system because it can simultaneously solve energy and environment problems. Here, a novel solid solution, Zn2Ti1−xGexO4 (0 ≤ x ≤ 0.15), with high photocatalytic activity for the reaction was successfully synthesized via a facile molten salts route. The Zn-based solid solutions with size about 200 nm have a homogeneous inverted cubic spinel structure (Fd3m) and a continuously modulated band gap with the Ge content. For the CO2 reduction reaction with H2O under simulated solar irradiation, the Zn2Ti1−xGexO4 solid solutions display not only high activity for the conversion of CO2 into CH 4 and CO fuels, but also long-term stability (>60 h of catalytic reaction). Experimental results and theoretical calculations indicated that the conduction and the valence bands of the cubic spinel Zn2TiO4 are positively shifted by introducing Zn2GeO4 with a pseudocubic inverse spinel structure, but the band gaps of solid solutions are simultaneously modulated with the introduction of germanium. Nevertheless, the Zn2TiO4 affords a light-carrier effective mass and strong electron delocalization by forming a solid solution with Zn2GeO4, which is beneficial to improving migration of photogenerated electrons and holes. As a synergistic result of band gap narrowing and high carrier diffusion, good conversion efficiencies for production of solar fuels through the reactions of CO2 reduction with H2O are achieved.
Databáze: OpenAIRE