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通过树枝状大分子模板化的铂铜纳米颗粒调节负载型催化剂的反应活性。

Tuning supported catalyst reactivity with dendrimer-templated Pt-Cu nanoparticles.

作者信息

Hoover Natalie N, Auten Bethany J, Chandler Bert D

机构信息

Department of Chemistry, Trinity University, One Trinity Place, San Antonio, Texas 78212-7200, USA.

出版信息

J Phys Chem B. 2006 May 4;110(17):8606-12. doi: 10.1021/jp060833x.

Abstract

The effects of particle composition on heterogeneous catalysis were studied using dendrimer-encapsulated nanoparticles (DENs) as precursors to supported Pt-Cu catalysts. Bimetallic Pt-Cu DENs with varying Pt/Cu ratios were prepared in an anaerobic aqueous solution and deposited onto a high-purity commercial alumina support. The dendrimer template was then thermally removed to yield supported nanoparticle catalysts, which were studied with toluene hydrogenation and CO oxidation catalysis as well as infrared spectroscopy of adsorbed CO. Incorporating Cu into Pt nanoparticles had opposite effects on the two test reactions. Cu acted as a mild promoter for CO oxidation catalysis, and the promoting effect was independent of the amount of Cu present. Conversely, Cu acted as a strong poison for toluene hydrogenation catalysis, and the normalized rate tracked inversely with Cu content. Infrared spectroscopy of the supported nanoparticles indicated that electronic effects (electron donation from Cu to Pt) were minimal for these materials. Consequently, the catalysis results are interpreted in terms of potential structural differences as a function of Cu incorporation and reaction conditions.

摘要

使用树枝状聚合物包裹的纳米颗粒(DENs)作为负载型Pt-Cu催化剂的前驱体,研究了颗粒组成对多相催化的影响。在厌氧水溶液中制备了具有不同Pt/Cu比的双金属Pt-Cu DENs,并将其沉积在高纯度商业氧化铝载体上。然后热去除树枝状聚合物模板,得到负载型纳米颗粒催化剂,并用甲苯加氢和CO氧化催化以及吸附CO的红外光谱对其进行了研究。将Cu掺入Pt纳米颗粒对这两个测试反应有相反的影响。Cu作为CO氧化催化的温和促进剂,促进作用与Cu的含量无关。相反,Cu作为甲苯加氢催化的强毒物,归一化速率与Cu含量成反比。负载型纳米颗粒的红外光谱表明,这些材料的电子效应(从Cu到Pt的电子给予)很小。因此,根据Cu掺入和反应条件的潜在结构差异来解释催化结果。

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