1. Pauling-type adsorption of O2 induced by S-scheme electric field for boosted photocatalytic H2O2 production.
- Author
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Zhou, Shuang, Wen, Da, Zhong, Wei, Zhang, Jianjun, Su, Yaorong, and Meng, Aiyun
- Subjects
X-ray photoelectron spectroscopy ,DENSITY functional theory ,FERMI level ,ELECTRIC fields ,OXYGEN reduction - Abstract
• Mesoporous oxygen-vacancy-rich TiO 2- x /g-C 3 N 4 S-scheme heterojunction was constructed. • S-scheme electric field induced Pauling-type O 2 adsorption configuration. • Pauling-type O 2 adsorption can promote 2e
− ORR selectivity. • TiO 2- x /g-C 3 N 4 exhibits efficient photocatalytic H 2 O 2 production activity. The effective adsorption of oxygen (O 2) molecules over photocatalysts is a critical step in promoting the performance of photocatalytic H 2 O 2 production. However, g-C 3 N 4 usually features a Yeager-type (side-on) adsorption configuration of O 2 molecules, which causes the breaking of O–O bonds and severely hinders the H 2 O 2 production activity. Herein, we synthesized an oxygen-vacancy-rich TiO 2– x /g-C 3 N 4 step-scheme (S-scheme) heterojunction to regulate the oxygen adsorption configuration and improve the 2e– ORR selectivity of H 2 O 2 production. In-situ X-ray photoelectron spectroscopy (in-situ XPS) and density functional theory (DFT) calculations reveal that the S-scheme heterojunction is formed between TiO 2– x and g-C 3 N 4. The difference between their Fermi levels leads to the electron flow from g-C 3 N 4 to TiO 2– x , which increases the electron-deficient sites in g-C 3 N 4. As a result, the cleavage of O–O bonds on the surface of g-C 3 N 4 is avoided and the oxygen adsorption configuration is tuned from Yeager-type to Pauling-type (end-on). Consequently, the photocatalytic H 2 O 2 production rate is dramatically improved to 1780.3 μmol h–1 , which is about 5 times higher than that of pristine g-C 3 N 4. This work paves a new way to tailor the oxygen adsorption configuration by rationally designing S-scheme heterojunction photocatalysts. [Display omitted] [ABSTRACT FROM AUTHOR]- Published
- 2024
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