不同前驱体对Rh@ZSM-5催化甲烷部分氧化反应性能的影响OA
Effects of different precursors on catalytic performances of Rh@ZSM-5 for partial oxidation of methane reaction
甲烷(CH4)是兼具高热值与强温室效应的"双刃剑"能源,开发CH4催化转化技术对能源利用与环境保护至关重要.贵金属催化剂虽在甲烷部分氧化(POM)反应中展现出高CH4转化率与产物选择性,却面临成本高昂的问题,利用分子筛的限域效应增大活性金属分散度来提高贵金属利用率是目前可行的降本方法.为了进一步提高催化剂催化POM反应性能,通过水热合成法,分别以氯化铑和硝酸铑为前驱体制备了Rh@ZSM-5(Cl)和Rh@ZSM-5催化剂,并利用XRD、TEM和N2吸/脱附等技术对催化剂和ZSM-5载体进行了表征,系统探究了前驱体引入对催化剂催化性能的调控作用,测试了催化剂催化性能差异.结果表明,氯化铑前驱体诱导了O—Rh—Cl活性物种生成,该物种显著增强了活性金属与载体的相互作用.Rh@ZSM-5(Cl)在POM反应中展现出优异的催化性能,在900℃时,CH4转化率达到90.7%,H2选择性达到94.5%,归因于O—Rh—Cl活性物种促进了水煤气变换反应(WGSR)与POM反应的动态耦合.
Methane(CH4)is a"double-edged sword"energy source with high calorific value and strong greenhouse effect,so the development of catalytic conversion technology for CH4 is crucial for energy utilization and environmental protection.Although noble metal catalysts show high CH4 conversion rates and product selectivities in partial oxidation of methane(POM)reaction,they face the problem of high cost.It is a feasible cost reduction method to improve the utilization rate of noble metals by increasing the dispersion of active metals through the domain-limiting effect of molecular sieves.In order to further improve the catalytic performances of catalysts for POM reaction,a hydrothermal synthesis method was used to prepare Rh@ZSM-5(Cl)and Rh@ZSM-5 catalysts with rhodium chloride and rhodium nitrate as precursors,respectively.The catalysts and ZSM-5 support were characterized by XRD,TEM,N2 adsorption/desorption and so on.The regulatory effect of precursor introduction on the catalytic performances of catalysts were explored,and the differences of catalytic performances were tested.The results show that rhodium chloride precursor induces the generation of O—Rh—Cl active species,significantly enhancing the interaction between active metals and the carriers.Rh@ZSM-5(Cl)exhibits excellent catalytic performance for POM reaction,with CH4 conversion rate of 90.7%and H2 selectivity of 94.5%at 900℃,attributed to the dynamic coupling of water-gas shift reaction(WGSR)and POM reaction promoted by O—Rh—Cl active species.
朱浩楠;刘梦涛;吕岩;孟园园;郭延文;丁传敏
太原理工大学 化学与化工学院,山西 太原 030024太原理工大学 化学与化工学院,山西 太原 030024太原理工大学 化学与化工学院,山西 太原 030024太原理工大学 化学与化工学院,山西 太原 030024太原理工大学 化学与化工学院,山西 太原 030024太原理工大学 化学与化工学院,山西 太原 030024
化学化工
甲烷部分氧化反应RhZSM-5沸石合成气
partial oxidation of methane reactionRhZSM-5 zeolitesyngas
《低碳化学与化工》 2026 (1)
24-31,8
山西省自然科学基金(202203021221091).
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