| 张亚柳,杨双,师勉,梅毅,罗永明,何德东.Cr/MCM-41催化剂的制备及其用于丙烷非氧化脱氢反应[J].分子催化,2018,32(5):425-433 |
| Cr/MCM-41催化剂的制备及其用于丙烷非氧化脱氢反应 |
| Preparation of Cr/MCM-41 Catalyst and Its Application for Nonoxidative Dehydrogenation of Propane |
| 投稿时间：2018-06-03 修订日期：2018-08-21 |
| DOI： |
| 中文关键词: 丙烷 丙烯 非氧化脱氢 Cr/MCM-41 |
| 英文关键词:propane propylene non-oxidative dehydrogenation Cr/MCM-41 |
| 基金项目:国家自然科学基金（U1402233，21667016） |
| 作者 | 单位 | E-mail | | 张亚柳 | 昆明理工大学 化学工程学院, 云南 昆明 650500
云南省高校磷化工重点实验室, 云南 昆明 650500 | | | 杨双 | 昆明理工大学 环境科学与工程学院, 云南 昆明 650500 | | | 师勉 | 昆明理工大学 化学工程学院, 云南 昆明 650500
云南省高校磷化工重点实验室, 云南 昆明 650500 | | | 梅毅 | 昆明理工大学 化学工程学院, 云南 昆明 650500
云南省高校磷化工重点实验室, 云南 昆明 650500 | | | 罗永明 | 昆明理工大学 环境科学与工程学院, 云南 昆明 650500 | | | 何德东 | 昆明理工大学 化学工程学院, 云南 昆明 650500
昆明理工大学 环境科学与工程学院, 云南 昆明 650500
云南省高校磷化工重点实验室, 云南 昆明 650500 | dedong.he@qq.com |
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| 中文摘要: |
| 实验分别采用连续吸附法和传统浸渍法制备Cr/MCM-41催化剂（分别记为Cr/MCM-41-ad和Cr/MCM-41-imp），将制备的Cr/MCM-41催化剂用于丙烷非氧化脱氢制丙烯反应，并对反应过程中的温度、压力、空速等反应条件进行优化，在合适的条件即反应温度为630℃、压力为0.1 MPa、空速为4500 mL·h-1·g-1下比较两种方法制备的催化剂在丙烷脱氢制丙烯反应的催化性能.我们采用XRD、SEM-mapping、XPS、UV-vis、H2-TPR等表征手段对催化剂上α-Cr2O3晶体粒径、活性组分及分布等进行表征分析，结果表明Cr/MCM-41-ad和Cr/MCM-41-imp中同时均存在Cr（VI）、Cr（Ⅲ）和α-Cr2O3.其中XRD和SEM-Mapping结果可知，Cr/MCM-41-ad上获得的α-Cr2O3晶体粒径较小且分散性好；通过UV-vis、XPS和TPR结果证明Cr/MCM-41-imp催化剂存在非活性孤立态Cr（VI），较难还原，影响其反应活性.相比之下，吸附法制备的催化剂使Cr高分散，可避免形成非活性孤立态Cr（VI），进而提高丙烷脱氢催化活性.因此，吸附法制备的铬基催化剂用于丙烷脱氢制丙烯有一定的借鉴作用. |
| 英文摘要: |
| In this work, Cr/MCM-41 catalysts (named as Cr/MCM-41-adsorbed and Cr/MCM-41-impregnated) were prepared by column adsorption method and traditional impregnation method, respectively, and they were applied for the non-oxidative dehydrogenation of propane. The reaction conditions such as temperature, space velocity, and pressure were optimized. Moreover, catalytic activity of the catalysts prepared by the two methods was compared under the optimal conditions, with reaction temperature of 630℃, space velocity of 4500 mL·h-1·g-1, and pressure of 0.1 MPa. Furthermore, XRD, SEM-mapping, XPS, UV-Vis, H2-TPR were used to characterize and analyze the physicochemical property of the catalyst.The results show that Cr(VI), Cr(Ⅲ) and α-Cr2O3 were detected in both Cr/MCM-41-ad and Cr/MCM-41-imp. Among them, XRD and SEM-mapping results showed that the Cr crystal obtained on Cr/MCM-41-ad has a small particle size and good dispersibility; It is indicated by UV-vis, XPS and TPR that Cr/MCM-41-imp catalyst has inactive isolated Cr(VI), which was difficult to reduce and affect its reactivity. In contrast, the catalyst prepared by the adsorption method allows Cr to be highly dispersed, avoided the formation of inactive isolated Cr(VI), thereby improving the catalytic activity of propane dehydrogenation. Therefore, the chromium-based catalyst prepared by the adsorption method has a certain reference for the dehydrogenation of propane to propylene. 1 |
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