CO_(2)-assisted oxidation dehydrogenation of light alkanes over metal-based heterogeneous catalysts  

负载型多相金属催化剂用于二氧化碳辅助低碳烷烃氧化脱氢反应

作　　者：Yingbin Zheng Xinbao Zhang Junjie Li Jie An Longya Xu Xiujie Li Xiangxue Zhu 郑颖滨;张新宝;李俊杰;安杰;徐龙伢;李秀杰;朱向学(中国科学院大连化学物理研究所,能源催化转化全国重点实验室,辽宁大连116023;中国科学院大学,北京100049)

机构地区：[1]State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China [2]University of Chinese Academy of Sciences,Beijing 100049,China

出　　处：《Chinese Journal of Catalysis》2024年第10期40-69,共30页催化学报（英文）

基　　金：国家自然科学基金(22078312);大连市重点领域创新团队(2020RT06);中国科学院“西部之光-西部交叉团队”重点实验室专项(xbzg-zdsys-202318).

摘　　要：Light olefins are important platform feedstocks in the petrochemical industry,and the ongoing global economic development has driven sustained growth in demand for these compounds.The dehydrogenation of alkanes,derived from shale gas,serves as an alternative olefins production route.Concurrently,the target of realizing carbon neutrality promotes the comprehensive utilization of greenhouse gas.The integrated process of light alkanes dehydrogenation and carbon dioxide reduction(CO_(2)-ODH)can produce light olefins and realize resource utilization of CO_(2),which has gained wide popularity.With the introduction of CO_(2),coke deposition and metal reduction encountered in alkanes dehydrogenation reactions can be effectively suppressed.CO_(2)-assisted alkanes dehydrogenation can also reduce the risk of potential explosion hazard associated with O_(2)-oxidative dehydrogenation reactions.Recent investigations into various metal-based catalysts including mono-and bi-metallic alloys and oxides have displayed promising performances due to their unique properties.This paper provides the comprehensive review and critical analysis of advancements in the CO_(2)-assisted oxidative dehydrogenation of light alkanes(C2-C4)on metal-based catalysts developed in recent years.Moreover,it offers a comparative summary of the structural properties,catalytic activities,and reaction mechanisms over various active sites,providing valuable insights for the future design of dehydrogenation catalysts.低碳烯烃(C2-C4)是石油化工产业链中的重要原料,其需求量随着全球经济的稳步增长而持续攀升.近年来,页岩气革命在全球范围内兴起,促进了低碳烷烃脱氢技术的蓬勃发展,使之成为低碳烯烃供给的关键路线之一,同时,全球CO_(2)排放量与日俱增,引发的温室效应等环境问题威胁着人类社会的健康发展为有效利用CO_(2)中的碳氧资源,研究者们将CO_(2)引入低碳烷烃脱氢体系中,一方面可有效避免直接脱氢反应中活性金属组分易烧结的问题;另一方面,可解决强氧化剂易深度氧化低碳烯烃引起的目标产品选择性低和副产大量CO_(x)的难题,并减少反应体系易燃易爆的风险;同时,该过程还可副产CO,H^(2)等基础化工原料,对于优化能源结构和促进化学工业的可持续发展具有重要意义.近年来,用于CO_(2)辅助低碳烷烃氧化脱氢反应的催化技术取得显著进展.各类金属基催化剂因其独特性质展现出优异的催化性能,但不同催化剂也面临着各自的挑战。例如Pt基催化剂因高活性而受到广泛关注,但环境有害的氯化再生技术仍然是函待解决的难题;Cr基催化剂因潜在的环境毒性问题而面临挑战.此外,氧化还原型金属(如V,Fe等)和主族金属(如Ga,In等)催化剂也展现出了良好的脱氢能力,但其性能仍有待进一步提升.通过调控催化剂的组成、结构或反应条件,有望进一步提升这些催化剂的脱氢效率和选择性.为进一步促进低碳烷烃和CO_(2)资源的高值化利用,并为高效催化剂的开发设计提供指导,本文综述了各类金属基(包括贵金属、过渡金属、金属氧化物以及高熵合金体系)催化剂在CO_(2)辅助低碳烷烃(乙烷、丙烷、丁烷)氧化脱氢反应中的最新研究成果,旨在为相关领域的研究人员提供有益的参考和启示,推动CO_(2)辅助低碳烷烃氧化脱氢技术向更高效、更环保的方向发展.聚焦于活性金属的种类和�

关 键 词：Light alkanes dehydrogenation CO_(2)utilization Metal-based catalysts Light olefins Coupling reaction 

分 类 号：O62[理学—有机化学]