Rh-Mn-LiSiO2催化剂上CO加氢制C2含氧化合物：载体硅烷化程度的影响.pdfVIP

文章编号: 0253-2409(2015)11-1380-07 Received: 2015-05-12; Revised: 2015-07-18. *Corresponding author. Tel / Fax: 0411 E-mail: dyj@ dicp. ac. cn. Rh-Mn-Li / SiO2 催化剂上 CO加氢制 C2 含氧化合物: 载体硅烷化程度的影响 胡宗贵1, 李经伟2, 陈维苗2, 邵守言1, 朱桂生1, 丁云杰2,* (1.江苏索普(集团)有限公司, 江苏 镇江 212006; 2.中国科学院大连化学物理研究所 洁净能源国家实验室, 辽宁 大连 116023) 摘 要: 以三甲基氯硅烷为硅烷化试剂,对硅胶进行不同程度硅烷化预处理,采用浸渍法制备了其负载的 Rh-Mn-Li 催化剂, 用于 CO加氢制 C2 含氧化合物的反应,并运用红外光谱、N2 吸附-脱附法、C含量测定、透射电镜、H2 程序升温还原和程序升 温表面反应等手段对载体和催化剂进行了表征。 结果表明,制得的不同硅烷化程度硅胶织构性质变化不大,它们负载的催化 剂上 Rh平均粒径均在 3 nm左右,硅烷化对催化剂吸附 CO的形态和 Rh的还原性能的影响均很小,但随着载体硅烷化程度的 提高,催化剂上 Rh解离 CO的能力增加,因而其活性逐渐增加,且不影响 C2 含氧化合物的选择性。 关键词: CO加氢; C2 含氧化合物; 硅烷化; 硅胶; 铑基催化剂; 三甲基氯硅烷 中图分类号: TQ245. 23 文献标识码: A Rh-Mn-Li / SiO2 catalyst for CO hydrogenation to C2 oxygenates: Effect of support silanization degree on its catalytic performance HU Zong-gui1, LI Jing-wei2, CHEN Wei-miao2, SHAO Shou-yan1, ZHU Gui-sheng1, DING Yun-jie2,* (1. Jiangsu SOPO (Group) Co. , Ltd. , Zhenjiang 212006, China; 2. Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China) Abstract: Silica was treated with trimethylchlorosilane before using as the supports for Rh-Mn-Li catalysts in CO hydrogenation to C2 oxygenates. The catalysts were characterized by infrared spectroscopy, N2 adsorption- desorption, C content measurements, transmission electron microscopy, H2 temperature programmed reduction, and temperature programmed surface reaction. The results showed that the silanization degree has little effect on the textural properties of silica. The mean Rh particle size ( about 3 nm), CO adsorption state on Rh and reducibility of Rh supported on silica remain unchanged by the silanization of silica support. However, with an increase of the silanization degree of silica, the ability of Rh to dissociate CO is improved, which can enhance the catalytic activity of Rh-Mn-Li / SiO2 in CO hydrogenation but has little influence on the selectivity towards C2 oxygenates.