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载体对Fe基催化剂CO2催化加氢制低碳烯烃性能的影响

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选择适宜载体对于合理设计高效CO2催化加氢制低碳烯烃(乙烯、丙烯和丁烯)的新型Fe基催化剂十分重要.采用水热法合成不同载体并浸渍K和Fe制备了一系列Fe基催化剂(K-Fe/ZrO2、K-Fe/ZnO、K-Fe/TiO2和K-Fe/Al2O3),考察了载体对催化剂CO2催化加氢性能的影响.采用XRD、N2吸/脱附、Raman、CO-TPD、CO2-TPD、原位Raman和水接触角测试等表征方法,研究了载体对Fe活性物种生成的诱导作用.结果表明,在温度320℃、压力2.0 MPa、原料气V(CO2):V(H2):V(Ar)=1:3:3和气时空速10000 mL/(g·h)的反应条件下,K-Fe/ZrO2表现出较高低碳烯烃选择性(42.4%)和CO2转化率(36.2%).与其他催化剂相比,K-Fe/ZrO2对CO和CO2具有适宜强度的吸附性能,有利于CO2活化和碳沉积,在获得更多FexCy活性物种的同时,抑制了烯烃二次加氢.此外,K-Fe/ZrO2在反应过程中因碳沉积而具有较强疏水性,进一步减轻了FexCy被水氧化的程度,提高了低碳烯烃选择性.
Effects of supports on catalytic performances of Fe-based catalysts for CO2 hydrogenation to light olefins
The selection of suitable support is crucial for the rational design of novel and efficient Fe-based catalysts for CO2 hydrogenation to light olefins(ethylene,propylene and butene).Supports were synthesized by hydrothermal method,and impregnated with K and Fe to prepare a series of Fe-based catalysts(K-Fe/ZrO2,K-Fe/ZnO,K-Fe/TiO2 and K-Fe/Al2O3).The effects of these supports on the catalytic performance of CO2 hydrogenation were investigated.The catalysts were characterized by XRD,N2 absorption/desorption,Raman,CO-TPD,CO2-TPD,in suit Raman and water droplet contact angle tests,and the induction effects of supports on the generation of Fe active species were studied.The results show that under reaction conditions of temperature of 320℃,pressure of 2.0 MPa,feed gas V(CO2):V(H2):V(Ar)=1:3:3 and gas hourly space velocity of 10000 mL/(g·h),K-Fe/ZrO2 exhibites superior selectivity of light olefins(42.4%)and CO2 conversion rate(36.2%).Compared to other catalysts,K-Fe/ZrO2 has a suitable adsorption capacity for CO and CO2,which is beneficial for CO2 activation and carbon deposition.It also inhibits the secondary hydrogenation of olefins while obtaining more FexCy active species.Additionally,K-Fe/ZrO2 exhibites strong hydrophobicity due to carbon deposition during the reaction process,further reducing the degree of water oxidation of FexCy and improving the selectivity of light olefins.

CO2 hydrogenationlight olefinssupportdynamic evolutionFe-based catalysts

李广辉、张艳艳、王萌、高健、张振洲、孙绍晖

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郑州大学 炼焦煤资源绿色开发国家重点实验室,河南 郑州 450001

郑州大学 化工学院 先进功能材料制造教育部工程研究中心,河南 郑州 450001

CO2加氢 低碳烯烃 载体 动态演变 Fe基催化剂

2024

天然气化工—C1化学与化工
西南化工研究设计院有限公司 全国天然气化工与碳一化工信息中心

天然气化工—C1化学与化工

CSTPCD北大核心
影响因子:0.814
ISSN:1001-9219
年,卷(期):2024.49(12)