Atomic Layer Deposition on Spray-Dried Supraparticles to Rationally Design Catalysts with Ultralow Noble Metal Loadings

IF 7 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Chemistry of Materials Pub Date : 2025-04-03 DOI:10.1021/acs.chemmater.4c03429
Philipp Groppe, Valentin Müller, Johannes Will, Xin Zhou, Kailun Zhang, Michael S. Moritz, Christian Papp, Jörg Libuda, Tanja Retzer, Erdmann Spiecker, Julien Bachmann, Karl Mandel, Susanne Wintzheimer
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Abstract

The controlled assembly of supraparticles by using spray-drying enables the synthesis of nanoporous materials. Changing the size of the constituent nanoparticles or their agglomeration states provides access to a diverse range of pore frameworks. This turns supraparticles into ideal scaffolds in heterogeneous catalysis. The combination of supraparticles with atomic layer deposition (ALD) as a surface functionalization technique offers excellent control over the deposition of a functional material and its distribution over the scaffold on the nanoscale. This work reports the combination of SiO2 supraparticles as tunable scaffolds and their loading with a platinum-based ALD catalyst. The deliberate adjustment of the scaffold pore framework via spray-drying and its effect on the catalyst deposition are highlighted. Furthermore, varying numbers of Pt ALD cycles are applied to explore the capability of the combination approach with respect to catalyst loading and Pt efficiency. High-resolution electron microscopy reveals ultrasmall Pt clusters deposited on the supraparticles after the very first ALD cycle. Using the hydrogenation of 4-nitrophenol as a demonstration, the impact of the pore framework and the Pt deposition variation in ALD on the catalytic functionality is investigated.

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喷雾干燥超颗粒原子层沉积,合理设计超低贵金属负载催化剂
利用喷雾干燥技术控制超微粒的组装,可以合成纳米多孔材料。改变组成纳米粒子的尺寸或其聚结状态,可获得各种孔隙框架。这使得超微粒成为异相催化的理想支架。将超微粒与原子层沉积(ALD)相结合作为一种表面功能化技术,可以很好地控制功能材料的沉积及其在纳米尺度支架上的分布。这项研究报告了二氧化硅超微粒作为可调支架与铂基 ALD 催化剂负载的结合。重点介绍了通过喷雾干燥有意调整支架孔隙框架及其对催化剂沉积的影响。此外,还应用了不同数量的铂 ALD 循环,以探索组合方法在催化剂负载和铂效率方面的能力。高分辨率电子显微镜显示,在第一个 ALD 循环后,超小型铂团簇沉积在超微粒上。以 4-硝基苯酚的氢化为例,研究了 ALD 中孔隙框架和铂沉积变化对催化功能的影响。
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来源期刊
Chemistry of Materials
Chemistry of Materials 工程技术-材料科学:综合
CiteScore
14.10
自引率
5.80%
发文量
929
审稿时长
1.5 months
期刊介绍: The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.
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