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Synthesis of Nickel-Doped Ceria Catalysts for Selective Acetylene Hydrogenation

机译:用于选择性乙炔氢化的镍掺杂的掺杂二氧化铈催化剂的合成

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Metallic nickel is known to be an active, but not a selective hydrogenation catalyst for conversion of alkynes to alkenes. On the other hand, nickel oxide is not active. Recently, we have demonstrated that nickel doped into ceria provides an inexpensive catalyst for selective hydrogenation of acetylene in the presence of ethylene. Here, we evaluate various synthesis methods to achieve optimal selective hydrogenation performance. We examined incipient wetness impregnation, coprecipitation, solution combustion, and sol-gel synthesis to study how the method of preparation affects catalytic structure and behavior. Sol-gel synthesis, coprecipitation, and solution combustion synthesis methods favor nickel incorporation into the ceria lattice, while incipient wetness impregnation creates segregated nickel species on the ceria surface. For hydrogenation of acetylene, these nickel surface species lead to poor ethylene selectivity due to ethane and oligomer formation. However, when nickel is incorporated into the ceria lattice, ethane formation is prevented even while achieving 100 % conversion of acetylene. Coke formation is also significantly reduced on these catalysts compared to conventional nanoparticle counterparts. We conclude that sol-gel synthesis provides the optimal method for creating a uniform dopant distribution within the high surface area ceria.
机译:已知金属镍是活性的,但不是选择性氢化催化剂,用于将炔烃转化为烯烃。另一方面,氧化镍不活跃。最近,我们已经证明掺杂进入Ceria的镍提供乙烯存在下乙炔的催化剂,用于选择性乙炔。在这里,我们评估各种合成方法以实现最佳选择性氢化性能。我们检查了初期的湿度浸渍,共沉淀,溶液燃烧和溶胶 - 凝胶合成,以研究制备方法如何影响催化结构和行为。溶胶 - 凝胶合成,共沉淀和溶液燃烧合成方法有利于镍掺入Ceria格子,而初期的湿润浸渍在二氧化铈表面上产生隔离的镍种。对于乙炔的氢化,由于乙烷和低聚物形成,这些镍表面物种导致乙烯选择性差。然而,当镍掺入Ceria格子中时,即使在实现100%转化乙炔的100%转化时,也能防止乙烷形成。与常规的纳米颗粒对应物相比,这些催化剂也显着降低了焦炭形成。我们得出结论,溶胶 - 凝胶合成提供了在高表面积内产生均匀掺杂剂分布的最佳方法。

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