水滑石基NiAl复合氧化物催化剂的CO2甲烷化催化性能研究OA
Study on catalytic performances of hydrotalcite-derived NiAl composite oxide catalysts for CO2 methanation
CO2甲烷化技术能够将温室气体CO2转化为具有高附加值的CH4,是实现碳循环利用的重要路径,其中Ni基催化剂因具有成本低廉和催化活性良好的优点而成为CO2甲烷化的研究热点.然而,Ni基催化剂通常面临活性金属易烧结及CH4选择性低等问题.针对上述问题,采用水热-焙烧法制备了一系列不同Ni含量(10%、30%、50%和60%,质量分数)的水滑石基NiAl复合氧化物催化剂(NiAl-m),利用XRD、XPS和SEM等方法对催化剂进行了系统表征,调控了Ni物种的化学状态与催化剂表面碱性.结果表明,随着Ni含量升高,催化剂的比表面积减小,Ni物种由NiAl2O4尖晶石相逐渐转变为NiO相,同时表面碱性位点数量先增大后减小.其中,NiAl-50在400℃、0.1 MPa和空速6400 mL/(g·h)反应条件下表现出最优催化性能,CO2转化率达到约80%,CH4选择性为99.8%.活性Ni物种与碱性位点的协同作用是决定催化剂CO2甲烷化催化性能的关键,且NiAl-m催化下反应遵循甲酸盐路径.本研究可为设计高性能Ni基CO2甲烷化催化剂提供重要的理论依据.
CO2 methanation offers a crucial route for carbon recycling by transforming greenhouse gas CO2 into high-value CH4.Ni-based catalysts have attracted extensive research interest in CO2 methanation due to their low cost and favorable activity.However,Ni-based catalysts often suffer from issues such as sintering of active metal particles and low CH4 selectivity.To address these challenges,a series of hydrotalcite-derived NiAl composite oxide catalysts(NiAl-m)with different Ni contents(10%,30%,50%and 60%,mass fraction)were prepared via hydrothermal-calcination method,and characterized by XRD,XPS,SEM and so on,and the chemical state of Ni species and the surface basicity of the catalysts were controlled.The results show that with the Ni content increasing,the specific surface area of catalysts decreases,and the Ni species gradually transform NiAl2O4 spinel phase to NiO phase.At the same time,the number of surface basic sites first increases and then decreases.NiAl-50 exhibits the best performance under the conditions of 400℃,0.1 MPa and space velocity of 6400 mL/(g·h),with the CO2 conversion rate of about 80%and CH4 selectivity of 99.8%.The synergistic effect between active Ni species and basic sites is key to the catalytic performances of catalysts for CO2 methanation,and the reaction catalyzed by NiAl-m follows the formate pathway.This study can provide important theoretical basis for designing high-performance Ni-based catalysts for CO2 methanation.
曹振兴;齐国金;王硕;杨永琪;任美熹;赵永华
辽宁工业大学 化学与环境工程学院,辽宁 锦州 121001辽宁工业大学 化学与环境工程学院,辽宁 锦州 121001辽宁工业大学 化学与环境工程学院,辽宁 锦州 121001辽宁工业大学 化学与环境工程学院,辽宁 锦州 121001辽宁工业大学 化学与环境工程学院,辽宁 锦州 121001辽宁工业大学 化学与环境工程学院,辽宁 锦州 121001
化学化工
CO2CH4甲烷化NiAl复合氧化物碱性位点
CO2CH4methanationNiAl composite oxidebasic sites
《低碳化学与化工》 2026 (8)
14-21,8
国家级大学生创新创业训练计划(202510154006)辽宁省教育厅基本科研项目(LJ242510154001).
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