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Efficient elimination of chlorinated organics on a phosphoric acid modified CeO2 catalyst: a hydrolytic destruction route

Dai, Xiaoxia, Wang, Xinwei, Long, Yunpeng, Pattisson, Samuel, Lu, Yunhao, Morgan, David John, Taylor, Stuart Hamilton, Carter, James H., Hutchings, Graham J., Wu, Zhongbiao and Weng, Xiaole 2019. Efficient elimination of chlorinated organics on a phosphoric acid modified CeO2 catalyst: a hydrolytic destruction route. Environmental Science and Technology 53 (21) , pp. 12697-12705. 10.1021/acs.est.9b05088
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Abstract

The development of efficient technologies to prevent the emission of hazardous chlorinated organics from industrial sources without forming harmful by-products, such as dioxins, is a major challenge in environmental chemistry. Herein, we developed a new hydrolytic destruction route for efficient chlorinated organics elimination and demonstrated that phosphoric acid modified CeO2 (HP-CeO2) can hydrolytically destruct chlorobenzene (CB) without forming polychlorinated congeners under the industry-relevant reaction conditions. The active site and origin of hydrolysis reactivity of HP-CeO2 were probed, which showed the surface phosphate groups can hydrolytically react with CB and water to form phenol and HCl, thus facilitating the chlorine desorption and ensuring a continual O2 activation. Subsequent density functional theory (DFT) calculations revealed a distinctly decreased formation energy of oxygen vacancy nearest (VO-1) and next-nearest (VO-2) to the bonded phosphate groups, which led to a significantly improved oxidizing ability of the catalyst. Significantly, no toxic dioxins were detected from the hydrolysis destruction of CB, which has been frequently cited as a significant challenge to avoid in the conventional oxidation route. This work not only reports an efficient route and corresponding phosphate active site for chlorinated organics elimination, but also illustrates that rational design of reaction route can solve some of the most important challenges in environmental catalysis.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: American Chemical Society
ISSN: 0013-936X
Date of First Compliant Deposit: 14 October 2019
Date of Acceptance: 2 October 2019
Last Modified: 30 Nov 2019 06:59
URI: http://orca-mwe.cf.ac.uk/id/eprint/126031

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