1. Oxygen vacancy-engineered titanium-based perovskite for boosting H2O activation and lower-temperature hydrolysis of organic sulfur.
- Author
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Zheng Wei, Mengfei Zhao, Zhenwen Yang, Xiaoxiao Duan, Guoxia Jiang, Ganggang Li, Fenglian Zhang, and Zhengping Hao
- Subjects
SULFUR ,HYDROLYSIS ,PEROVSKITE ,HETEROGENEOUS catalysis ,CHEMICAL reactions ,PHOTOVOLTAIC power systems - Abstract
Modulation of water activation is crucial to water-involved chemical reactions in heterogeneous catalysis. Organic sulfur (COS and CS
2 ) hydrolysis is such a typical reaction involving water (H2 O) molecule as a reactant. However, limited by the strong O-H bond in H2 O, satisfactory CS2 hydrolysis performance is attained at high temperature above 310 °C, which is at the sacrifice of the Claus conversion, strongly hindering sulfur recovery efficiency improvement and pollution emissions control of the Claus process. Herein, we report a facile oxygen vacancy (VO ) engineering on titanium-based perovskite to motivate H2 O activation for enhanced COS and CS2 hydrolysis at lower temperature. Increased amount of VO contributed to improved degree of H2 O dissociation to generate more active -OH, due to lower energy barrier for H2 O dissociation over surface rich in VO, particularly VO clusters. Besides, low-coordinated Ti ions adjacent to VO were active sites for H2 O activation. Consequently, complete conversion of COS and CS2 was achieved over SrTiO3 after H2 reduction treatment at 225 °C, a favorable temperature for the Claus conversion, at which both satisfying COS and CS2 hydrolysis performance and improved sulfur recovery efficiency can be obtained simultaneously. Additionally, the origin of enhanced hydrolysis activity from boosted H2 O activation by VO was revealed via in-depth mechanism study. This provides more explicit direction for further design of efficacious catalysts for H2 O-involved reactions. [ABSTRACT FROM AUTHOR]- Published
- 2023
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