4.8 Article

Synthesis of Narrow-Band-Gap GaN:ZnO Solid Solution for Photocatalytic Overall Water Splitting

Journal

ACS CATALYSIS
Volume 12, Issue 23, Pages 14637-14646

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c0436114637

Keywords

photocatalysis; overall water splitting; Z-scheme system; GaN; ZnO solid solution; oxynitrides

Funding

  1. Starting Foundation of Shanghai Tech University
  2. National Natural Science Foundation of China [21972092]
  3. JST, PRESTO, Japan [JPMJPR20T9]
  4. SPST of Shanghai-Tech University [AIC10112914, EM02161943]

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This study presents a novel synthesis method to prepare narrow-band-gap GaN:ZnO solid solution and demonstrates its potential in visible-light-driven overall water splitting.
The solid solution of GaN and ZnO (GaN:ZnO) is a promising photocatalyst applicable to visible-light-driven overall water splitting. However, the band gap of active GaN:ZnO remains as large as ca. 2.7 eV because of the loss of ZnO during the widely applied NH3 nitridation process. Herein, particulate GaN:ZnO exhibiting a band gap of 2.3 eV was synthesized via calcination of a mixture of Ga2O3, Zn, and NH4Cl in a sealed evacuated tube. The synthesis method was also featured with a high nitrogen utilization rate of 87%. The prepared narrow-band-gap GaN:ZnO was active in the overall water-splitting reaction. In the presence of sacrificial reagents, the apparent quantum yields of GaN:ZnO at 420 nm for H2 and O2 generation were 5.1 and 14.3%, respectively. GaN:ZnO was applied as an oxygen evolution photocatalyst to construct a Z-scheme overall water-splitting system with SrTiO3:Rh as a hydrogen evolution photocatalyst, which achieved a solar-to-hydrogen energy conversion efficiency of 3.7 x 10-2% and a remarkable photochemical stability up to 100 h. This work provides an approach to the synthesis of narrow-band-gap GaN:ZnO solid solution and shows the potential of this material in H2 production from water under long-wavelength visible light.

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