School of Chemical Engineering and Technology, Sun Yat-sen University

在煤炭开采的过程中,低浓度瓦斯的涌出会造成大量温室气体的排放。通过催化氧化反应将瓦斯转化为二氧化碳,可以有效减少温室效应。然而,目前所报道催化剂的活性与稳定性大多难以满足实际应用的需求。简要论述了煤矿瓦斯催化氧化的反应机理,总结了近期低浓度煤矿瓦斯氧化催化剂的研究进展,并探讨了未来高效稳定煤矿瓦斯氧化催化剂的设计思路。甲烷C—H键活化是煤矿瓦斯催化氧化反应的决速步骤。高活性的贵金属催化剂和热稳定性好的非贵金属氧化物催化剂是两类常用的瓦斯氧化催化剂。对于贵金属催化剂,活性金属的类型与分散性对C—H活化性能至关重要,可以通过改性载体与掺杂助剂来调控金属的分散度。对于非贵金属氧化物催化剂,可以通过调变催化剂的结构或掺杂助剂来调控比表面积、氧空位浓度、化学键等性质,从而改善催化剂的活性。此外,煤矿瓦斯氧化催化剂还需要具备优异的耐水和耐硫性能。通过构筑包覆结构或构筑特殊金属结构,可以促进水的解吸;通过掺杂助剂调控活性金属的电子结构与催化剂表面基团,也可以提高催化剂的耐水稳定性。构筑包覆结构可以阻止含硫组分在活性位点的吸附,而添加牺牲剂可以优先吸附含硫组分,是常用的提升催化剂耐硫稳定性的策略之一。

During the coal extraction process, the emission of low-concentration coal mine gas signifi-cantly contributes to greenhouse gas emissions. Catalytic oxidation is an effective strategy for convertingthe coal mine gas to carbon dioxide, thereby alleviating the greenhouse effect. However, the activityand stability of most reported catalysts remain inadequate for widespread application. The reactionmechanisms of coal mine gas oxidation are summarized, and the recent progress and future perspectivesfor catalyst design are presented. C—H activation is the rate-determining step in coal mine gas oxida-tion reactions. Noble-metal catalysts with high activity for C—H activation and metal oxide catalystswith high thermal stability are widely used for coal mine gas oxidation. Regarding the noble-metal cata-lysts, the type of active metals significantly influences C—H activation. Modification of the supportsand the addition of additives can adjust the distribution of active metals. For metal oxide catalysts,modification of catalyst structure and composition can regulate the surface areas, oxygen vacancy con-centrations, and chemical bonds, thereby improving catalytic activity. In addition, the water resistanceand sulfur resistance of catalysts are vital for the stable oxidation of coal mine gas. The construction ofan encapsulated structure and a specific active metal structure are conducive to water desorption. Fur-thermore, the addition of dopants can adjust electronic structure of active metals, thus enhancing thewater resistance of catalysts. With regard to sulfur resistance, the construction of an encapsulated struc-ture to weaken sulfur adsorption and the addition of a sacrificial component to delay sulfur deactivationare two commonly-used strategies.

广东省自然科学基金杰出青年基金资助项目(2022B1515020098);广东省重点领域研发计划资助项目(2020B1111360004)

武金玮,张明康,叶城荫,等.低浓度煤矿瓦斯氧化催化剂研究进展[J].能源环境保护,2024,38(3):74-82.

WU Jinwei, ZHANG Mingkang, YE Chengyin, et al. Recent progress on catalysts for low-concentration coal minegas oxidation[J]. Energy Environmental Protection, 2024, 38(3): 74-82.