Synthesis of Narrow-Band-Gap GaN:ZnO Solid Solution for Photocatalytic Overall Water Splitting
Synthesis of Narrow-Band-Gap GaN:ZnO Solid Solution for Photocatalytic Overall Water Splitting
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DOI：
10.1021/acscatal.2c04361
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发表时间：
2022-11
期刊：
影响因子：
12.9
通讯作者：
Kaiwei Liu;Boyang Zhang;Jifang Zhang;W. Lin;Jiaming Wang;Yao Xu;Y. Xiang;T. Hisatomi;K. Domen;Guijun Ma
中科院分区：
文献类型：
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作者：
Kaiwei Liu;Boyang Zhang;Jifang Zhang;W. Lin;Jiaming Wang;Yao Xu;Y. Xiang;T. Hisatomi;K. Domen;Guijun Ma
GaN和ZnO(GaN：ZnO)固溶体是一种很有前途的可见光驱动整体分解水的光催化剂。然而，在广泛应用的氨氮化过程中，由于氧化锌的损失，活性GaN：ZnO的带隙仍然很大，约为2.7 eV。在这种情况下，通过在密封真空管中焙烧Ga2O、Zn和NH4Cl的混合物，合成了禁带宽度为2.3 eV的颗粒状GaN：ZnO。该合成方法还具有氮气利用率高达87%的特点。制备的窄禁带GaN：ZnO在整个裂水反应中表现出较高的活性。在牺牲剂存在下，GaN：ZnO在420 nm处产生H_2和O_2的表观量子产率分别为5.1%和14.3%。以GaN：ZnO为析氧光催化剂，以SrTiO3：Rh为析氢光催化剂，构建了Z-方案整体分解水体系，获得了3.7×10-2%的光能转换效率和100h的光化学稳定性，为合成窄禁带GaN：ZnO固溶体提供了一条途径，展示了该材料在长波长可见光下由水制氢的潜力。
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 NH3nitridation 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 H2and O2generation 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 × 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 H2production from water under long-wavelength visible light.