Mechanistic Insight on the Formation of GaN:ZnO Solid Solution from Zn-Ga Layered Double Hydroxide Using Urea as the Nitriding Agent

被引:23
作者
Katagiri, Kiyofumi [1 ]
Hayashi, Yuki [1 ]
Yoshiyuki, Risa [1 ]
Inumaru, Kei [1 ]
Uchiyama, Tomoki [2 ]
Nagata, Noriyuki [2 ]
Uchimoto, Yoshiharu [2 ]
Miyoshi, Akinobu [3 ]
Maeda, Kazuhiko [3 ]
机构
[1] Hiroshima Univ, Grad Sch Engn, Dept Appl Chem, 1-4-1 Kagamiyama, Hiroshima 7398527, Japan
[2] Kyoto Univ, Grad Sch Human & Environm Studies, Sakyo Ku, Yoshida Nihonmatsu Cho, Kyoto 6068501, Japan
[3] Tokyo Inst Technol, Sch Sci, Dept Chem, Meguro Ku, 2-12-1 NE 2 Ookayama, Tokyo 1528550, Japan
关键词
VISIBLE-LIGHT-DRIVEN; CRYSTAL-STRUCTURE; RECENT PROGRESS; WATER; PHOTOCATALYST; ABSORPTION; (GA1-XZNX)(N1-XOX); SEMICONDUCTORS; CARBODIIMIDE; IRRADIATION;
D O I
10.1021/acs.inorgchem.8b02498
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
A solid solution of GaN and ZnO (GaN:ZnO) is promising as a photocatalyst for visible-light-driven overall water splitting to produce H-2. However, several obstacles still exist in the conventional preparation procedure of GaN:ZnO. For example, the atomic distributions of Zn and Ga are nonuniform in GaN:ZnO when a mixture of the metal oxides, i.e. Ga2O3 and ZnO, is used as a precursor. In addition, GaN:ZnO is generally prepared under a harmful NH3 flow for long durations at high temperatures. Here, a facile synthesis of GaN:ZnO with homogeneous atomic composition via a simple and safe procedure is reported. A layered double hydroxide (LDH) containing Zn2+ and Ga3+ was used to increase the uniformity of the atomic distributions of Zn and Ga in GaN:ZnO. We employed urea as a nitriding agent instead of gaseous NH3 to increase the safety of the reaction. Through the optimization of reaction conditions such as heat treatment temperature and content of urea, single-phase GaN:ZnO was successfully obtained. In addition, the nitridation mechanism using urea was investigated in detail. NH3 released from the thermal decomposition of urea did not directly nitride the LDH precursor. X-ray absorption and infrared spectroscopies revealed that Zn(CN2)-like intermediate species were generated at the middle temperature range and Ga-N bonds formed at high temperature along with dissociation of CO and CO2.
引用
收藏
页码:13953 / 13962
页数:10
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