摘要
丙烯是石油化工产业的基础原材料,也是衡量化工产业的重要指标.催化丙烷直接和氧化脱氢是制备丙烯的重要途径,目前传统催化剂面临着反应温度高、易积碳以及环境不友好等问题,急需发展新型催化剂材料来推动进一步发展.在本文中系统总结了几类新型丙烷脱氢催化剂材料(金属氧化物、分子筛、碳基材料、金属-有机框架(MOFs)、高熵金属间化合物)的最新研究进展.首先介绍了各种新型材料的本征催化性质和活性,在此基础之上详细分析了各种性能优化方法的实现途径和作用机理.在分子水平上梳理了催化剂材料上活性中心催化性质,揭示了可能的反应机理.对于金属氧化物催化剂材料,突出了氧空位在反应中的重要作用以及调节氧空位的可行方法.对于分子筛材料,主要介绍了锚定活性金属物种的新策略和新方法,尤其是对于小尺寸金属团簇以及单原子催化剂.对于碳基材料,说明了非金属催化剂相对于传统金属催化剂的独特催化性质以及利用杂原子调控性能的方法.另一方面,针对新型MOFs和高熵合金催化材料研究进展也进行了简要介绍.最后,分别总结了每类新型催化剂材料的优势和面临的主要问题,围绕丙烯选择性和催化剂稳定性给出了进一步提高催化性能的可行方法.
The propene is the raw materials for petrochemical industry and the important metric for the developments of chemicals.The catalytic direct and oxidative dehydrogenation of propane is one of the main routes to produce propene.Currently,the conventional propane dehydrogenation catalysts confront several critical issues including high reaction temperature,coke deposition,and adverse environmental effects which spurred the urgent needs of alternative novel catalytic materials.In current work,the new developments of several novel propane dehydrogenation catalysts(metal oxide,zeolites,carbon based material,metal-organic framework(MOFs),and high-entropy intermetallics(HEI))are introduced.First of all,the intrinsic catalytic properties of each material are described together with the related optimization methods.The properties of active centers are carefully calibrated and the possible reaction mechanism is discussed.For the metal-based materials,the focus is put on the critical role of oxygen vacancy and the methods to adjust the number of vacancy sites.For zeolites,their main application is to anchor active metal materials,in particularly subnano size clusters or single atom catalysts.For carbon materials,their unique characters associated with metal-free catalysts are distinguished from conventional metal catalysts.A brief summary is also performed for novel MOFs and HEI materials.In the end,the advantage and disadvantage associated with each catalyst material are carefully summarized,and the methods for further improvements are presented regarding to high propene selectivity and catalyst stability.
作者
彭馨瑶
汤雨晴
孙晓颖
于湛
李波
Xin-Yao Peng;Yu-Qing Tang;Xiao-Ying Sun;Zhan Yu;Bo Li(College of Chemistry and Chemical Engineering,Shenyang Normal University,Shenyang 110034,China)
出处
《中国科学:化学》
北大核心
2025年第2期400-432,共33页
SCIENTIA SINICA Chimica
基金
国家自然科学基金(编号:22172100,22372105)
辽宁省教育厅基本科研项目(编号:JYTZD2023183)
辽宁省属本科高校基本科研业务费专项资金(编号:LJ212410166043)
沈阳师范大学(编号:BS202208)资助项目。
