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镍铜双金属催化剂上纯乙炔的半加氢反应:铜镍比对催化性能的影响。

Pure Acetylene Semihydrogenation over Ni-Cu Bimetallic Catalysts: Effect of the Cu/Ni Ratio on Catalytic Performance.

作者信息

Zhou Shuzhen, Kang Lihua, Zhou Xuening, Xu Zhu, Zhu Mingyuan

机构信息

College of Chemistry and Chemical Engineering, Yantai University, Yantai 264004, China.

School of Chemistry and Chemical Engineering, Shihezi University, Shihezi 832003, China.

出版信息

Nanomaterials (Basel). 2020 Mar 11;10(3):509. doi: 10.3390/nano10030509.

Abstract

Ethylene is an important chemical raw material and with the increasing consumption of petroleum resources, the production of ethylene through the calcium carbide acetylene route has important research significance. In this work, a series of bimetallic catalysts with different Cu/Ni molar ratios are prepared by co-impregnation method for the hydrogenation of calcium carbide acetylene to ethylene. The introduction of an appropriate amount of Cu effectively inhibits not only the formation of ethane and green oil, thus increasing the selectivity of ethylene, but also the formation of carbon deposits, which improves the stability of the catalyst. The ethylene selectivity of the Ni-Cu bimetallic catalyst increases from 45% to 63% compared with the Ni monometallic counterpart and the acetylene conversion still can reach 100% at the optimal conditions of 250 °C, 8000 mL·g·h and V(H)/V(CH) = 3. X-ray diffraction and transmission electron microscopy confirmed that the metal particles were highly dispersed on the support, High-resolution transmission electron microscopy and H-Temperature programmed reduction proved that there was an interaction between Ni and Cu, combined with X-ray photoelectron spectroscopy and density functional theory calculations results, Cu transferred electrons to Ni changed the Ni electron cloud density in NiCu catalysts, thus reducing the adsorption of acetylene and ethylene, which is favorable to ethylene selectivity.

摘要

乙烯是一种重要的化学原料,随着石油资源消耗的增加,通过电石乙炔路线生产乙烯具有重要的研究意义。在这项工作中,采用共浸渍法制备了一系列不同铜/镍摩尔比的双金属催化剂,用于电石乙炔加氢制乙烯。适量铜的引入不仅有效抑制了乙烷和绿油的生成,从而提高了乙烯的选择性,还抑制了积炭的形成,提高了催化剂的稳定性。与单金属镍催化剂相比,镍-铜双金属催化剂的乙烯选择性从45%提高到了63%,在250℃、8000 mL·g·h和V(H)/V(CH)=3的最佳条件下,乙炔转化率仍可达到100%。X射线衍射和透射电子显微镜证实金属颗粒高度分散在载体上,高分辨率透射电子显微镜和H-程序升温还原证明镍和铜之间存在相互作用,结合X射线光电子能谱和密度泛函理论计算结果,铜向镍转移电子改变了NiCu催化剂中镍的电子云密度,从而降低了乙炔和乙烯的吸附,有利于乙烯选择性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b4d1/7153591/63d9f442a7e7/nanomaterials-10-00509-sch001.jpg

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