铟基催化剂混合晶型调控对CO_(2)加氢制甲醇反应的影响  

Effect of Mixed Crystal Phase Control of Indium-Based Catalyst on the Reaction of CO_(2) Hydrogenation to Methanol

作　　者：王宇 李红伟 吴玉 胡志海 WANG Yu;LI Hongwei;WU Yu;HU Zhihai(SINOPEC Research Institute of Petroleum Processing Co.,Ltd.,Beijing 100083,China)

机构地区：[1]中石化石油化工科学研究院有限公司,北京100083

出　　处：《石油学报（石油加工）》2024年第4期983-992,共10页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家重点研发计划重点专项(2021YFE0191200)基金资助。

摘　　要：CO_(2)是主要的温室气体,其化工转化近年来成为研究热点。对于CO_(2)加氢制甲醇反应,六方晶型结构铟基催化剂(h-In_(2)O_(3))具有低CO_(2)转化率和高甲醇选择性,立方晶型结构铟基催化剂(c-In_(2)O_(3))具有高CO_(2)转化率和低甲醇选择性。为保持六方晶型铟基催化剂的高甲醇选择性且提高其CO_(2)转化率,采用水热法通过控制水热时间,在六方晶型结构的铟基催化剂上添加立方晶型结构,制备得到分别含质量分数33%和62%立方晶型结构的催化剂样品In-33c和In-62c,并评价其催化剂性能。采用XRD、XPS、H_(2)-TPR、CO_(2)-TPD、N_(2)物理吸附-脱附等分析方法对所制备的催化剂进行表征。结果表明:与h-In_(2)O_(3)相比,In-33c和In-62c样品的催化效果均有提升,2种晶型具有协同作用,且In-62c的催化效果优于In-33c;在反应温度300℃、反应压力3.0 MPa条件下,In-62c催化剂的CO_(2)转化率达到10.8%、甲醇选择性达到80.4%;与h-In_(2)O_(3)催化剂相比,CO_(2)转化率相对提高了63.4%,甲醇选择性相对提高了22.2%。The chemical conversion of CO_(2),the main greenhouse gas,has become a research hotspot in recent years.For the reaction of CO_(2) hydrogenation to methanol,the hexagonal indium-based catalyst(h-In_(2)O_(3))has low CO_(2) conversion and high methanol selectivity,and the cubic indium-based catalyst(c-In_(2)O_(3))has high CO_(2) conversion and low methanol selectivity.In order to maintain the high methanol selectivity of hexagonal indium-based catalyst and improve its CO_(2) conversion,the hydrothermal method was used to add the cubic crystalline phase structure to the hexagonal indium-based catalyst by controlling the hydrothermal time.Then the catalyst samples In-33c and In-62c with mass fraction of 33%and 62%cubic crystal structure were prepared,of which the catalytic performance was evaluated The catalyst samples were characterized by XRD,XPS,H_(2)-TPR,CO_(2)-TPD and N_(2) absorption-desorption.The performance evaluation results show that the catalytic effects of In-33c and In-62c are improved as compared with h-In_(2)O_(3),the two crystal forms have synergistic effect,and In-62c has better catalytic effect than In-33c.At the reaction temperature of 300℃and reaction pressure of 3.0 MPa,the CO_(2) conversion rate of In-62c catalyst can reach 10.8%and the methanol selectivity is 80.4%,which are respectively increased by 63.4%and 22.2%when compared with the pure phase h-In_(2)O_(3) catalyst.

关 键 词：氧化铟 晶型 立方晶型 六方晶型 二氧化碳加氢 甲醇 

分 类 号：TQ426.94[化学工程]