Elucidation of high activity and reaction mechanism for 1,2-dichloroethane catalytic oxidation over CoMnOx/HZSM-5 catalyst

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2025-03-15 Epub Date: 2025-01-10 DOI:10.1016/j.micromeso.2025.113505

Peng Wang, Shilin Wu, Shuyun Ding, Ying Wang, Ningjie Fang, Yinghao Chu

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Abstract

The preparation of catalysts with excellent catalytic activity and stability in the catalytic oxidation of CVOCs by a simple and economical method with suitable support remained a challenge. For this reason, the MnCoO_x/HZ-x catalysts prepared by impregnation method with different Si/Al ratios of HZSM-5 as the support, and applied to the catalytic combustion of 1,2-dichloroethane (1,2-DCE). The results confirmed that the Si/Al ratio of the carrier affected the physicochemical properties of the surface active species, which improved the catalytic activity. The excellent catalytic activity (T₉₀ = 193 °C) and stability of MnCoO_x/HZ-25 were attributed to the abundance of Mn⁴⁺, Co²⁺, and surface adsorbed oxygen, the good redox capacity, and the suitable acidic strength stimulated by the lower Si/Al ratio of the carrier. In situ DRIFTS verified that at high temperatures and in the presence of oxygen, the production of vinyl alcohol or vinyl chloride species was not favored, and oxygenated intermediates such as carboxylates were mainly produced on MnCoO_x/HZ-25.

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1,2-二氯乙烷在CoMnOx/HZSM-5催化剂上催化氧化的高活性和反应机理的阐明

在合适的载体条件下，用简单经济的方法制备出具有良好催化活性和稳定性的CVOCs催化剂一直是一个挑战。为此，以不同Si/Al比的HZSM-5为载体，采用浸渍法制备了MnCoOx/HZ-x催化剂，并将其应用于1,2-二氯乙烷（1,2- dce）的催化燃烧。结果证实，载体的Si/Al比影响了表面活性物质的理化性质，从而提高了催化活性。MnCoOx/HZ-25具有优异的催化活性（T90 = 193℃）和稳定性，主要归功于其丰富的Mn4+、Co2+和表面吸附氧，良好的氧化还原能力，以及载体较低的Si/Al比所激发的适宜的酸性强度。原位漂移证实，在高温和有氧存在的情况下，乙烯醇或氯乙烯物种的生产不受欢迎，羧酸盐等含氧中间体主要在MnCoOx/HZ-25上生产。

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来源期刊

Microporous and Mesoporous Materials 化学-材料科学：综合

CiteScore

10.70

自引率

5.80%

发文量

649

审稿时长

26 days

期刊介绍： Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.