二氧化碳加氢制高级醇Fe基催化剂研究进展  

Research progress on Fe-based catalysts for CO_(2)hydrogenation to higher alcohols

作　　者：秦婷婷 牛强 QIN Tingting;NIU Qiang(Inner Mongolia Erdos Electric Power and Metallurgy Group Co.,Ltd.,Ordos 016064,Inner Mongolia,China)

机构地区：[1]内蒙古鄂尔多斯电力冶金集团股份有限公司,内蒙古鄂尔多斯016064

出　　处：《化工进展》2025年第1期253-265,共13页Chemical Industry and Engineering Progress

基　　金：内蒙古自治区科技重大专项(2021ZD0042);内蒙古自治区科技计划(2023YFHH0043)。

摘　　要：高级醇(HA)可作为重要的能源化工基础原料。CO_(2)加氢制备高级醇(CO_(2)-HAS)具有流程短、效率高、操作简便等特点,该技术兼具碳减排和高附加值利用的双重意义。Fe基催化剂的低成本和高活性优势使其具备工业应用潜力,但仍存在反应网络复杂、C—C键生成难控制、高级醇收率不理想等问题。本文从热力学角度分析了CO_(2)-HAS的固有限制和适宜的工艺条件,简述了高级醇生成的转化路径和Fe物种演变。进一步阐述了反应条件、助剂、制备方法和载体等因素对Fe基催化剂反应性能的影响,并揭示了Fe基多功能催化反应偶联的构建策略以及对性能的促进机制。基于此,指出中间物种的定向转化和C—C偶联的精准调控是Fe基催化剂设计的关键考量。预测3D打印自催化技术将助力Fe基催化剂的大规模制备,多元化的技术整合可能是CO_(2)-HAS产业化开发的可行方式之一。廉价的绿氢制备技术与CO_(2)捕集技术的突破与耦合将推动CO_(2)-HAS的高质量发展并成为主流趋势。Higher alcohols(HA)are important basic raw materials of energy and chemical industry.Higher alcohols synthesis via CO_(2)hydrogenation(CO_(2)-HAS)possesses the characteristics of short process,high efficiency,and easy operation,which exhibits the great significance for both emission reduction and high value-added utilization of CO_(2).Fe-based catalysts show great potential for industrial application due to their low cost and high activity,but they still faces some problems such as complex reaction network,difficult control of C—C bond formation and unsatisfactory yield of HA.Herein,the inherent limitation and suitable process conditions of CO_(2)-HAS were analyzed from the thermodynamic point of view,and the transformation path of HA and the evolution of Fe species were described.The effects of reaction conditions,promoters,preparation methods and supports on the performance of Fe-based catalysts were further discussed.The construction strategy of Fe-based multifunction catalytic reaction-coupling and its promoting mechanism were also revealed.The directed conversion of intermediate species and the precise regulation of C—C coupling are the key considerations in the design of Fe-based catalysts.3D printing self-catalytic technology is expected to accelerate the large-scale preparation of Fe-based catalysts.Integration of various technologies may be one of the feasible ways for the industrial exploration of CO_(2)-HAS.The breakthrough of cheap green hydrogen production technology and its coupling with CO_(2)capture technology will promote high quality development of CO_(2)-HAS and will be the mainstream trend in the future.

关 键 词：二氧化碳加氢 高级醇 Fe基催化剂 C—C耦合 

分 类 号：TQ426[化学工程] O643.36[理学—物理化学]