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Ni/MCM-41催化剂在纯乙炔加氢制乙烯反应中的催化性能及失活研究

Catalytic performance and deactivation of Ni/MCM-41 catalyst in the hydrogenation of pure acetylene to ethylene.

作者信息

Zhou Shuzhen, Kang Lihua, Xu Zhu, Zhu Mingyuan

机构信息

School of Chemistry and Chemical Engineering of Shihezi University Shihezi Xinjiang 832003 P. R. China

Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan Shihezi Xinjiang 832003 P. R. China.

出版信息

RSC Adv. 2020 Jan 9;10(4):1937-1945. doi: 10.1039/c9ra09878j. eCollection 2020 Jan 8.

Abstract

Ni/MCM-41 catalysts were prepared by an impregnation method for acetylene hydrogenation to ethylene based on the calcium carbide acetylene route. X-ray diffraction and transmission electron microscopy indicated that Ni was uniformly dispersed on the support. Temperature-programmed reduction and X-ray photoelectron spectroscopy demonstrated a strong interaction between Ni and MCM-41, and Ni(0) and Ni(ii) coexisted in the catalyst. We optimized the catalytic activity by optimizing the Ni loading and reaction conditions including temperature, space velocity, and hydrogen/acetylene ratio. The acetylene conversion reached 100%, the ethylene selectivity reached 47%. Additionally, we tested the catalyst stability; the acetylene conversion was maintained at 100% for 25.73 h and was then rapidly reduced. ICP, TEM, FT-IR, thermogravimetric analysis and BET were used to investigate the reasons for catalyst deactivation; it was found that green oil deposition on the catalyst surface was the main reason for the catalyst deactivation.

摘要

基于电石乙炔路线,采用浸渍法制备了用于乙炔加氢制乙烯的Ni/MCM-41催化剂。X射线衍射和透射电子显微镜表明,Ni均匀分散在载体上。程序升温还原和X射线光电子能谱表明Ni与MCM-41之间存在强相互作用,且催化剂中Ni(0)和Ni(ii)共存。我们通过优化Ni负载量以及温度、空速和氢/乙炔比等反应条件来优化催化活性。乙炔转化率达到100%,乙烯选择性达到47%。此外,我们测试了催化剂的稳定性;乙炔转化率在25.73 h内保持在100%,然后迅速下降。采用电感耦合等离子体质谱、透射电子显微镜、傅里叶变换红外光谱、热重分析和比表面积分析等方法研究了催化剂失活的原因;发现催化剂表面的绿油沉积是催化剂失活的主要原因。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/dd82/9047415/dac77fccef40/c9ra09878j-s1.jpg

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