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解决二氧化硅负载的单个银催化剂之间在组成和氢化性能方面的颗粒间异质性问题。

Resolving Interparticle Heterogeneities in Composition and Hydrogenation Performance between Individual Supported Silver on Silica Catalysts.

作者信息

Plessers Eva, Stassen Ivo, Sree Sreeprasanth Pulinthanathu, Janssen Kris P F, Yuan Haifeng, Martens Johan, Hofkens Johan, De Vos Dirk, Roeffaers Maarten B J

机构信息

Centre for Surface Chemistry and Catalysis, KU Leuven , Kasteelpark Arenberg 23, 3001 Heverlee, Belgium.

Department of Chemistry, KU Leuven , Celestijnenlaan 200 F, 3001 Heverlee, Belgium.

出版信息

ACS Catal. 2015 Nov 6;5(11):6690-6695. doi: 10.1021/acscatal.5b02119. Epub 2015 Sep 30.

Abstract

Supported metal nanoparticle catalysts are commonly obtained through deposition of metal precursors onto the support using incipient wetness impregnation. Typically, empirical relations between metal nanoparticle structure and catalytic performance are inferred from ensemble averaged data in combination with high-resolution electron microscopy. This approach clearly underestimates the importance of heterogeneities present in a supported metal catalyst batch. Here we show for the first time how incipient wetness impregnation leads to 10-fold variations in silver loading between individual submillimeter-sized silica support granules. This heterogeneity has a profound impact on the catalytic performance, with 100-fold variations in hydrogenation performance at the same level. In a straightforward fashion, optical microscopy interlinks single support particle level catalytic measurements to structural and compositional information. These detailed correlations reveal the optimal silver loading. A thorough consideration of catalyst heterogeneity and the impact thereof on the catalytic performance is indispensable in the development of catalysts.

摘要

负载型金属纳米颗粒催化剂通常通过初湿浸渍法将金属前驱体沉积在载体上获得。通常,金属纳米颗粒结构与催化性能之间的经验关系是通过结合高分辨率电子显微镜的系综平均数据推断出来的。这种方法明显低估了负载型金属催化剂批次中存在的不均匀性的重要性。在这里,我们首次展示了初湿浸渍法如何导致亚毫米级二氧化硅载体颗粒之间的银负载量出现10倍的差异。这种不均匀性对催化性能有深远影响,在相同水平下氢化性能会出现100倍的差异。通过一种直接的方式,光学显微镜将单个载体颗粒水平的催化测量与结构和组成信息联系起来。这些详细的相关性揭示了最佳的银负载量。在催化剂的开发中,全面考虑催化剂的不均匀性及其对催化性能的影响是必不可少的。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e816/4640703/11cbd1fdc9e5/cs-2015-02119s_0002.jpg

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