Efficient and Stable Catalytic Hydrogen Evolution of ZrO2/CdSe-DETA Nanocomposites under Visible Light

Abstract

Composite photocatalysts are crucial for photocatalytic hydrogen evolution. In this work, ZrO2/CdSe-diethylenetriamine (ZrO2/CdSe-DETA) heterojunction nanocomposites are synthesized, and efficiently and stably catalyzed hydrogen evolution under visible light. X-ray photoelectron spectroscopy (XPS) and high resolution transmission electron microscope (HRTEM) confirm the formation of heterojunctions between ZrO2 (ZO) and CdSe-DETA (CS). Ultraviolet–visible spectroscopy diffuse reflectance spectra (UV-vis DRS), Mott–Schottky, and theoretical calculations confirm that the mechanism at the heterojunction of the ZrO2/CdSe-DETA (ZO/CS) nanocomposites is Type-I. Among the ZO/CS nanocomposites (ZO/CS-0.4, ZO/CS-0.6, and ZO/CS-0.8; in the nanocomposites, the mass ratio of ZO to CS is 0.1:0.0765, 0.1:0.1148, and 0.1:0.1531, respectively). ZO/CS-0.6 nanocomposite has the best photocatalytic hydrogen evolution activity (4.27 mmol g−1 h−1), which is significantly higher than ZO (trace) and CS (1.75 mmol g−1 h−1). Within four cycles, the ZO/CS-0.6 nanocomposite maintains an efficient catalytic hydrogen evolution rate. Due to the existence of the heterojunction of the composites, the photogenerated electron-hole pairs can be effectively separated, which accelerates the photocatalytic hydrogen evolution reaction and reduces the progress of photocorrosion. This work reveals the feasibility of ZO/CS nanocomposite photocatalysts for hydrogen evolution.