摘要
C_(2)—C_(4)烯烃(C_(2)^(=)—C_(4)^(=))是国民经济发展的重要化工原料,我国C_(2)^(=)—C_(4)^(=)需求量逐年攀升,而其生产工艺主要依赖石脑油裂解。将煤炭、天然气、生物质等非石油基碳资源先转化为合成气(CO/H_(2))再转化为C_(2)^(=)—C_(4)^(=),对维护我国能源安全至关重要。同时,将工业烟气中的CO_(2)作为碳资源转化为C_(2)^(=)—C_(4)^(=),对实现人工碳循环、解决温室气体带来的全球气候问题具有重要战略意义。相比于传统费托合成技术,通过金属氧化物–分子筛(Oxide-Zeolite,OX-ZEO)路线将CO_(x)(包括CO和CO_(2))直接高选择性转化为C_(2)^(=)—C_(4)^(=)被认为是一个突破性的发展,但目前仍然存在CO_(x)转化效率与C_(2)^(=)—C_(4)^(=)产率的制衡关系。笔者概述了近年来OX-ZEO催化在CO_(x)加氢制低碳烯烃中的研究进展,重点讨论了影响催化性能的关键因素如金属氧化物的种类和元素组成以及分子筛酸性与拓扑结构等,详细解析了氧空位作用和抑制副反应策略对CO_(x)加氢反应调控机制,同时总结了OX-ZEO的催化反应机理,对OX-ZEO双功能催化路径在CO_(x)加氢转化制低碳烯烃应用中目前存在的挑战和未来的发展进行了展望。
C_(2)-C_(4)olefin(C_(2)^(=)—C_(4)^(=))is a major chemical raw material and in a flourishing demand in China.Currently,its manufacturing technique is mostly based on naphtha cracking,which is not in line with the national energy endowment of"rich coal but lean oil".Coal gasification,typically produces syngas(CO/H_(2))first,and subsequently to olefin(STO)is considered as a promising technology.Meanwhile,converting CO_(2)from industrial flue gas into C_(2)^(=)—C_(4)^(=)is critical for realizing the"Carbon Neutrality".The direct and highly selective conversion of CO_(x)(both CO and CO_(2))to C_(2)^(=)—C_(4)^(=)via the metal Oxide-Zeolite(OX-ZEO)route breaks through the limitation of the Anderson-Schulz-Flory distribution of the traditional Fischer-Tropsch synthesis technology,but still suffers from the trade-off between CO_(x)conversion efficiency and C_(2)^(=)—C_(4)^(=)yield.Recent development of OX-ZEO bifunctional catalysis strategy for CO_(x)hydrogenation to light olefins was reviewed,with emphasis on the effects of the type and elemental composition of metal oxides,the acidity and topological structure of zeolite on the catalytic performance.The role of oxygen vacancy and side reaction inhibition strategies on CO_(x)hydrogenation was clarified.In addition,the reaction mechanism over Ox-ZEO was reviewed in detail.With this,insights into significant promising tendencies and confronting challenges in the strategy of OX-ZEO for CO_(x)to light olefin was suggested.
作者
杨庆伟
孙哲毅
邵斌
胡军
YANG Qingwei;SUN Zheyi;SHAO Bin;HU Jun(Sinopec Maoming Petrochemical Company,Maoming 525000,China;School of Chemistry and Molecular Engineering,East China University of Science and Technology,Shanghai 200237,China)
出处
《洁净煤技术》
CAS
CSCD
北大核心
2024年第11期1-12,共12页
Clean Coal Technology
基金
国家自然科学基金资助项目(22278126,22250005,22408095)
中国博士后科学基金资助项目(2023M741170)
中央高校基本科研业务费专项资金资助项目(JKB01231715)。
关键词
低碳烯烃
合成气
二氧化碳
双功能催化剂
反应机理
light olefins
syngas
carbon dioxide
bifunctional catalyst
reaction mechanism
