摘要
二氧化碳甲烷化技术作为全球气候变化背景下碳捕集与利用(CCU)的关键路径,对实现碳中和目标具有重要意义。镍(Ni)基催化剂因兼具高活性、高甲烷选择性及成本优势已成为二氧化碳甲烷化技术领域的研究核心,但面临低温活性不足、高温易失活及积碳等挑战,因而有必要系统梳理镍基催化剂在二氧化碳甲烷化中的研究进展。对关于二氧化碳甲烷化反应机理的研究现状进行综述,并结合镍催化剂结构及载体性质的研究成果,重点分析活性位点调控及载体设计策略。最新研究成果表明,二氧化碳甲烷化主要遵循甲酸盐反应路径与CO反应路径,Ni的粒径、分散度及与载体的相互作用均显著影响催化性能。引入贵金属、过渡金属及稀土元素作为助剂,可通过优化电子结构、增强金属分散度及调控碱性位点等机制提升催化活性。在载体工程方面,氧化铈(CeO_(2))、氧化钇(Y_(2)O_(3))等氧化物通过调控SMSI效应、界面电子结构及氧空位密度可有效提升性能,而碳纳米管(CNT)、分子筛、金属有机框架(MOF)衍生物等新型载体则通过特殊结构增强Ni分散性与抗烧结能力;核壳结构、限域封装等设计可有效抑制Ni颗粒烧结,从而延长催化剂寿命。未来研究需结合原位表征与理论计算,深入解析多路径竞争机制和构效关系,开发精准可控的合成方法以优化助剂与载体的协同效应,推动镍基催化剂向高效、稳定、低成本方向发展,助力二氧化碳甲烷化技术的工业化应用。
In the context of global climate change,carbon dioxide methanation,as a key pathway for Carbon Capture and Utilization(CCU),plays a significant role in achieving carbon neutrality goals.Nickel(Ni)based catalysts have become the focus of research in this field due to their high activity,high methane selectivity,and cost advantages.However,they face challenges such as insufficient low-temperature activity,deactivation at high temperatures,and carbon deposition.Therefore,it is necessary to systematically summarize the research progress of Ni-based catalysts in CO 2 methanation.Accordingly,this paper reviews the research on the reaction mechanisms of CO_(2) methanation,and combined with research findings on catalyst structure and support properties,this paper focuses on analyzing strategies for active site modulation and support design.Extensive studies reveal that CO_(2) methanation primarily follows two pathways:the formate pathway and the CO dissociation pathway.Furthermore,the particle size,dispersion of Ni,and its interaction with the support significantly influence catalytic performance.Notably,introducing promoters such as noble metals,transition metals,and rare-earth elements can enhance catalytic activity through mechanisms including optimizing electronic structures,improving metal dispersion,and modulating basic sites.In terms of support engineering,oxides like cerium oxide(CeO_(2))and yttrium oxide(Y_(2)O_(3))effectively enhance performance by regulating the strong metal-support interaction(SMSI)effect,interfacial electronic structure,and oxygen vacancy density.Meanwhile,novel supports such as carbon nanotubes(CNTs),zeolites,and metal-organic framework(MOF)derivatives enhance Ni dispersion and sintering resistance through their unique structures.Specifically,designs like core-shell and embedded structures effectively inhibit Ni particle sintering and extend catalyst lifespan.In the future,it is necessary to combine in-situ characterization and theoretical calculations to deeply analyze the multi-path competition mechanism and structure-activity relationship.This will help develop precise and controllable synthesis methods to optimize the synergistic effects of promoters and supports,thereby promoting Ni-based catalysts development towards high efficiency,stability,and low cost,and ultimately facilitating the industrial application of CO_(2) methanation technology.
作者
陈一铭
CHEN Yiming(China Coal Research Institute Corporation Ltd.,Beijing 100013,China;National Energy Technology&Equipment Laboratory of Coal Utilization and Emission Control,Beijing 100013,China;CCTEG Low-carbon Technology Institute,Beijing 100013,China)
出处
《煤质技术》
2025年第4期19-32,52,共15页
Coal Quality Technology
基金
国家重点研发计划资助项目(2023YFB4103802、2024YFB4105301)
鄂尔多斯市国家可持续发展议程创新示范区建设科技支撑基金资助项目(KCX2024014)
煤炭科学技术研究院有限公司科技发展基金资助项目(MKYZX-001、2024ZD1-01)。
关键词
二氧化碳甲烷化
镍基催化剂
反应机理
活性位点
反应路径
载体性质
分散度
CO_(2) methanation
Nickel-based catalyst
reaction mechanism
active site
formate pathway
support property
dispersion
