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用于N2O分解及H2还原的Ni-Pt/SiO2催化剂的表面性质

Surface properties of Ni-Pt/SiO2 catalysts for N2O decomposition and reduction by H2.

作者信息

Arenas-Alatorre Jesús, Gómez-Cortés Antonio, Avalos-Borja Miguel, Díaz Gabriela

机构信息

Instituto de Física-UNAM, Apdo. Postal 20-364, C.P. 01000, México.

出版信息

J Phys Chem B. 2005 Feb 17;109(6):2371-6. doi: 10.1021/jp048843q.

Abstract

The surface properties of bimetallic Ni-Pt/SiO2 catalysts with variable Ni/Ni + Pt atomic ratio (0.75, 0.50, and 0.25) were studied using N2O decomposition and N2O reduction by hydrogen reactions as probes. Catalysts were prepared by incipient wetness impregnation of the silica support with aqueous solutions of the metal precursors to a total metal loading of 2 wt %. For both model reactions, Pt/SiO2 catalyst was substantially more active than Ni/SiO2 catalyst. Mean particle size by TEM was about the same (in the range 6-8 nm) for all catalysts and truly bimetallic particles (more than 95%) were evidenced by EDS in the Ni-Pt/SiO2 catalysts. CO adsorption on the bimetallic catalysts showed differences in the linear CO absorption band as a function of the Ni/Pt atomic ratio. Bimetallic Ni-Pt/SiO2 catalysts showed, for the N2O decomposition, a catalytic behavior that points out an ensemble-size sensitive behavior for Ni-rich compositions. For the N2O + H2 reaction, the bimetallic catalysts were very active at low temperature. The following activity order at 300 K was observed: Ni75Pt25 > Ni25Pt75 approximately Ni50Pt50 > Pt. TOF values for these catalysts increased 2-5 times compared to the most active reference catalyst (Pt/SiO2). The enhancement of the activity in the Ni75Pt25 bimetallic catalysts is explained in terms of the presence of mixed Ni-Pt ensembles.

摘要

以N₂O分解反应和H₂还原N₂O反应为探针,研究了具有不同Ni/Ni + Pt原子比(0.75、0.50和0.25)的双金属Ni-Pt/SiO₂催化剂的表面性质。通过用金属前驱体的水溶液对二氧化硅载体进行初湿浸渍来制备催化剂,使总金属负载量达到2 wt%。对于这两个模型反应,Pt/SiO₂催化剂的活性明显高于Ni/SiO₂催化剂。所有催化剂通过透射电子显微镜测得的平均粒径大致相同(在6 - 8 nm范围内),并且能量散射谱证明Ni-Pt/SiO₂催化剂中存在真正的双金属颗粒(超过95%)。双金属催化剂上的CO吸附显示,线性CO吸收带随Ni/Pt原子比而变化。对于N₂O分解反应,双金属Ni-Pt/SiO₂催化剂表现出的催化行为表明,富Ni组成具有集合尺寸敏感行为。对于N₂O + H₂反应,双金属催化剂在低温下非常活跃。在300 K时观察到以下活性顺序:Ni₇₅Pt₂₅ > Ni₂₅Pt₇₅ ≈ Ni₅₀Pt₅₀ > Pt。与活性最高的参比催化剂(Pt/SiO₂)相比,这些催化剂的TOF值提高了2 - 5倍。Ni₇₅Pt₂₅双金属催化剂活性的增强是由混合的Ni-Pt集合体的存在来解释的。

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