4.7 Article

A comparative study of the dichloromethane catalytic combustion over ruthenium-based catalysts: Unveiling the roles of acid types in dissociative adsorption and by-products formation

期刊

JOURNAL OF COLLOID AND INTERFACE SCIENCE
卷 605, 期 -, 页码 537-546

出版社

ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2021.07.095

关键词

Dichloromethane; Catalytic oxidation; Acid sites; By-products; Ru

资金

  1. National Natural Science Foundation of China [22076164]
  2. Funda-mental Research Funds for the Central Universities [2021XZZX025]
  3. Program for the Zhejiang Leading Team of ST Innovation [2013TD07]

向作者/读者索取更多资源

A comparative investigation of Ru-based catalysts on different supports for catalytic combustion of dichloromethane was conducted, revealing that Lewis acid sites were more active than Brønsted acid sites. The presence of Cl species on TiO2 and Al2O3 supports interacted strongly with Lewis acid sites, leading to the formation of more polychlorinated toxic by-products. The study provides valuable insights into the development of catalytic combustion catalysts for chlorinated volatile organic compounds.
Herein, a comparative investigation of the Ru-based catalysts with different kinds of supports (TiO2, Al2O3, HZSM-5 SiO2/Al2O3 = 27 and 130, respectively) for catalytic combustion of dichloromethane (DCM) has been performed. The characterization results showed that the C-Cl bond of DCM was cleaved on both the Bronsted and Lewis acid sites of the catalysts. However, the Lewis acid sites were more active than the Bronsted acid sites. The relatively strong Lewis acidity of Ru/TiO2 improved the dissociative adsorption of DCM, accounting for its superior activity. The yield of toxic by-products was strongly associated with the acid types of the catalysts. The Cl species deposited on TiO2 and Al2O3 supports interacted strongly with the Lewis acid sites, thereby promoting the electrophilic chlorination reactions and yielding more polychlorinated by-products, especially highly toxic dibenzo-p-dioxins and dibenzofurans (PCDD/Fs). However, the Cl deposits on Ru/HZSM-5 (SiO2/Al2O3 = 27) with abundant Bronsted acid sites, mainly existed as hydrogen-bonded Cl species, with good mobility and less propensity for chlorinating carbonaceous matter. Moreover, Ru/HZSM-5 (SiO2/Al2O3 = 130) yielded the highest polychlorinated by-products and PCDD/Fs because of its poor redox ability and high surface area. Overall, this study provides valuable insights into the CVOCs catalytic combustion catalysts development. (C) 2021 Elsevier Inc. All rights reserved.

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