首页|二氧化碳催化加氢金属有机框架负载型金属催化剂的研究进展

二氧化碳催化加氢金属有机框架负载型金属催化剂的研究进展

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自人类进入工业社会起,化石燃料的大量使用使二氧化碳等温室气体排放加剧,对生态环境造成了难以逆转的破坏.随着从可再生能源获得的绿氢逐步增加,二氧化碳催化加氢生成高附加值化学品如甲醇、甲酸和甲烷等逐渐成为二氧化碳转化最有应用前景的方法之一.载体材料性质对于二氧化碳催化加氢金属催化剂性能有着重要的调控作用.金属有机框架材料(MOFs)具有比表面积大、孔隙率高、结构可设计等特点,逐渐成为二氧化碳催化加氢金属催化剂的载体材料.在本文中,分别揭示了MOFs负载单金属和金属合金催化剂的催化性质和性能,着重于归纳总结载体和金属活性物质之间相互作用以及其对反应性能的影响.详细介绍了多种MOFs负载金属材料调控方法包括选择性锚定、限域封装、尺寸调节、配体优化等方法,以及它们在催化加氢反应中实际应用路径和效果.通过和传统均相、多相加氢催化剂进行比较,揭示了MOFs材料在加氢反应中的独特性质和优异性能.依据文献报道,提出了理性设计高性能MOFs基金属加氢催化剂的一般原则,给出了生成不同产物反应机理的理论描述.综上,本文为提高二氧化碳催化加氢反应性能提供了可行路径,为拓宽MOFs材料的应用前景提供了有力支持.
Recent developments of MOF-supported metal catalysts for CO2 hydrogenation
Since the industrial age,the massive use of fossil fuels has intensified the emission of greenhouse gases such as carbon dioxide,which has caused irreversible damage to the ecological environment.With rapid increase of green hydrogen obtained from renewable energy sources,catalytic hydrogenation of carbon dioxide to produce high value-added chemicals such as methanol,formic acid and methane has gradually become one of the most promising methods for carbon dioxide conversion.The properties of support materials play an important role in regulating the performance of metal catalysts for carbon dioxide-catalytic hydrogenation.On the other hand,metal-organic frameworks(MOFs)have the unique properties of large specific surface area,high porosity,and designable structure(both metal centers and organic ligands are easy to be functionalized),and have gradually become the rising support materials for catalytic carbon dioxide hydrogenation metal catalysts.In this paper,the catalytic properties and performance of MOF-supported mono-metal and metal-alloy catalysts are revealed through the reaction processes of different hydrogenation products(methanol,formic acid,methane),and the interaction between support and metal active substance and its influence on the reaction properties are summarized.A variety of regulatory methods for MOFs supported metal materials,including selective anchoring,encapsulation,size adjustment,ligand optimization,were discussed in detail,and the practical application and performance of these methods are revealed.The unique properties and superior activity of MOFs in hydrogenation reaction are disclosed through a comparison with the conventional homogeneous and heterogeneous hydrogenation catalysts.According to the literature reports,the general principles of rational design of high performance MOF-based metal catalysts are put forward,and the theoretical description of reaction mechanisms of different products is given.In summary,this paper provides a feasible path for improving the performance of carbon dioxide catalytic hydrogenation catalysts,and a strong support for further expanding the application scope of MOF-based materials.

metal-organic frameworksCO2 hydrogenationmetal catalystreaction mechanism

闫冰洁、曹佳慧、孙晓颖、李波

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沈阳师范大学化学化工学院,沈阳 110034

金属有机框架材料 二氧化碳加氢 金属催化剂 反应机理

2024

中国科学(化学)
中国科学院

中国科学(化学)

CSTPCD北大核心
影响因子:0.685
ISSN:1674-7224
年,卷(期):2024.54(12)