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

机译:Ni-Cu双金属催化剂上的纯乙炔半氢化反应:Cu / Ni比对催化性能的影响

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摘要

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(C H ) = 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.
机译:乙烯是重要的化工原料,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,通过共浸渍法制备了一系列具有不同Cu / Ni摩尔比的双金属催化剂,用于将电石乙炔氢化为乙烯。引入适量的Cu不仅有效地抑制了乙烷和生油的形成,从而提高了乙烯的选择性,而且还抑制了碳沉积物的形成,从而改善了催化剂的稳定性。 Ni-Cu双金属催化剂的乙烯选择性比Ni单金属对应物的乙烯选择性从45%提高到63%,并且在250°C,8000 mL·g·h和V( H)/ V(CH)=3。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-温度程序化还原证明镍之间存在相互作用。与Cu结合,结合X射线光电子能谱和密度泛函理论计算结果,Cu将电子转移到Ni上改变了NiCu催化剂中Ni电子云的密度,从而减少了乙炔和乙烯的吸附,有利于乙烯的选择性。

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