Promote the activation and ring opening of intermediates for stable photocatalytic toluene degradation over Zn-Ti-LDH

Yongyi Liu; Si Chen; Kanglu Li; Jielin Wang; Peng Chen; Hong Wang; Jieyuan Li; Fan Dong

doi:10.1016/j.jcis.2021.08.146

Promote the activation and ring opening of intermediates for stable photocatalytic toluene degradation over Zn-Ti-LDH

J Colloid Interface Sci. 2022 Jan 15;606(Pt 2):1435-1444. doi: 10.1016/j.jcis.2021.08.146. Epub 2021 Aug 24.

Authors

Yongyi Liu¹, Si Chen², Kanglu Li³, Jielin Wang¹, Peng Chen⁴, Hong Wang¹, Jieyuan Li⁵, Fan Dong⁶

Affiliations

¹ Research Center for Environmental and Energy Catalysis, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China.
² Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313000, China.
³ Research Center for Environmental and Energy Catalysis, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China; College of Architecture and Environment, Sichuan University, Chengdu, Sichuan 610065, China.
⁴ Research Center for Environmental and Energy Catalysis, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China; School of New Energy and Materials, Southwest Petroleum University, Chengdu 610500, China.
⁵ Research Center for Environmental and Energy Catalysis, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China; Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313000, China.
⁶ Research Center for Environmental and Energy Catalysis, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China; Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313000, China. Electronic address: dfctbu@126.com.

PMID: 34492478
DOI: 10.1016/j.jcis.2021.08.146

Abstract

Improving the selectivity of photocatalysis and reducing the generation of toxic by-products are the two key challenges for the development of highly efficient and stable photocatalysts. In this work, it was revealed that Zn-Ti-layered double hydroxide (ZT-LDH) photocatalyst, which generated less intermediates, showed better toluene degradation efficiency (removal ratio, 75.2%) and stability, compared with P25 (removal ratio, 10.9%). During the photocatalytic toluene degradation, benzaldehyde and benzoic acid were the main intermediates existed in the gas phase and on the surface of the catalyst, respectively. By combining experiments with theoretical calculation, it was found that the hydrogen atoms on the hydroxyl groups in the LDH would selectively attract the oxygen atoms in the carbon-oxygen double bond of the two major intermediates, facilitating their adsorption and activation on ZT-LDH. Besides, the surface electronic structure of ZT-LDH was demonstrated to facilitate the ring-opening reaction of the two major intermediates, eventually maintaining high activity and stability. This work could provide new molecular perspectives for understanding the photocatalytic reactions in VOCs degradation and developing efficient and stable photocatalysts.

Keywords: Intermediate; LDH; Mechanism; Photocatalysis; Toluene.