La, Al-dominated stabilization of Cr3+in crystal-remolded SrTiO3 for efficient visible-light-driven overall water splitting

被引:9
作者
Qin, Yalei [1 ]
Xu, Ruize [1 ]
Ding, Lingling [1 ]
Wang, Tao [1 ]
Guo, Donglei [2 ]
Fang, Fan [1 ]
Chang, Kun [1 ]
机构
[1] Nanjing Univ Aeronaut & Astronaut, Coll Mat Sci & Technol, Ctr Hydrogenergy, Nanjing 210016, Peoples R China
[2] Luoyang Normal Univ, Coll Chem & Chem Engn, Key Lab Funct oriented Porous Mat, Luoyang 471934, Peoples R China
基金
中国国家自然科学基金;
关键词
Visible light; Overall water splitting; Crystal remolding; La; Al -cooperated mechanism; SrTiO3; TOTAL-ENERGY CALCULATIONS; DOPED SRTIO3; TRANSITION-METAL; PHOTOCATALYTIC ACTIVITIES; HYDROGEN EVOLUTION; CODOPED SRTIO3; H-2; EVOLUTION; CR; NANOPARTICLES; TIO2;
D O I
10.1016/j.jcat.2024.115317
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
Achieving efficient solar-to-hydrogen conversion through visible-light-driven overall water splitting poses a significant challenge for particulate photocatalysts. Although bandgap engineering can be realized by ion doping, the introduced defects simultaneously enhance the recombination of electron-hole pairs. Herein, La/(Cr, Al) codoped SrTiO3 was remolded via the ion implantation flux method. The La, Cr and Al achieve valence state equilibrium upon stabilizing the crystal lattice, resulting in visible-light absorption. The optimized La/(Cr, Al)SrTiO3 photocatalyst exhibits an overall water-splitting reaction under visible light, yielding 73.2 mu mol & sdot;h- 1 for H2 and 35.0 mu mol & sdot;h- 1 for O2 with an apparent quantum yield of 1.44 % at 420 nm. Based on theoretical calculation, we proposed a La, Al-cooperated mechanism that a little Cr3+ was fixed by the surrounding Al3+, and the valence state was stabilized by La3+ during the crystal remolding, thereby giving the guidance for designing visible-light materials applied in overall water splitting.
引用
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页数:11
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