La,Al-Codoped SrTiO3 as a Photocatalyst in Overall Water Splitting: Significant Surface Engineering Effects on Defect Engineering

被引:133
作者
Qin, Yalei [1 ]
Fang, Fan [1 ]
Xie, Zhengzheng [1 ]
Lin, Huiwen [1 ]
Zhang, Kai [2 ]
Yu, Xu [3 ]
Chang, Kun [1 ]
机构
[1] Nanjing Univ Aeronaut & Astronaut, Jiangsu Key Lab Electrochem Energy Storage Techno, Coll Mat Sci & Technol, Nanjing 210016, Peoples R China
[2] Nanjing Univ Aeronaut & Astronaut, Coll Energy & Power Engn, Nanjing 210016, Peoples R China
[3] Yangzhou Univ, Sch Chem & Chem Engn, Yangzhou 225002, Jiangsu, Peoples R China
基金
中国国家自然科学基金;
关键词
photocatalysis; overall water splitting; La; Al-codoped SrTiO3; surficial Sr2+; defect engineering; HIGHLY EFFICIENT; DOPED SRTIO3; HYDROGEN EVOLUTION; H2O; NANOPARTICLES; CONVERSION; OXIDE; NANOCLUSTERS; PEROVSKITES; CATALYST;
D O I
10.1021/acscatal.1c02874
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Suppressing the formation of defects such as oxygen vacancies and Ti3+ in SrTiO3 perovskite lattice has been regarded as an effective way to improve photocatalytic performance in overall water-splitting reaction. In this work, a series of La,Al-codoped SrTiO3 catalysts are synthesized by a flux treatment method after grounding. An appropriate doping amount of La3+ and Al3+ ions into perovskite will lead to fewer defects, responsible for enhancing photocatalytic performance. Al3+ ion doping will introduce the oxygen vacancies into the perovskite, resulting in a decreasing number of Ti3+ ions. During the defect engineering, more Sr2+ will precipitate onto the perovskite surface caused by the introduction of Al3+. Hence, surface engineering is applied through appropriate La3+ ion doping contributing to the lattice distortion, allowing surficial Sr2+ to re-enter the perovskite lattice, leading to the promoted conversion of Ti3+ to Ti4+. Simultaneously, the La3+ ion doping is also beneficial to the decrease in oxygen vacancies. As a result, the essential relationship between the La3+ doping amount and photocatalytic performance in overall water splitting is revealed. The optimized 0.6% La and 1% Al codoped SrTiO3 sample loading Rh (0.1 wt %)/Cr2O3 (0.05 wt %)/CoOOH (0.05 wt %) gives the highest activity and good stability, with gas evolution rates of 1.79 mmol.h(-1) (H-2) and 0.91 mmol.h(-1) (O-2). In comparison, the apparent quantum efficiency is 78.43% under 365 nm irradiation.
引用
收藏
页码:11429 / 11439
页数:11
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