Multi-metallic aerogels have emerged as a promising unsupported, high surface area-based metal material for different applications in heterogeneous catalysis and electrochemistry. The fabrication of these multi-metallic aerogels is based on a complex gelation process which is characterized by controlled aggregation of metallic nanoparticles to form a macroscopic network structure in aqueous solution. However, achieving structural homogeneity of the multi-metallic aerogels in terms of diameter of the nanochains and chemical composition at the nano- as well as at the macro-scale is still a great challenge.
In this paper, we show the characterization of two Pd-Pt aerogels prepared by the two-step gelation method. The structural homogeneity and chemical distribution of both metals (Pd and Pt) inside the aerogels were analyzed using high-resolution (scanning) transmission microscopy (HR(S)TEM), energy-dispersive X-ray spectroscopy (EDX), extended X-ray absorption fine structure (EXAFS) spectroscopy, and cyclic voltammetry. Based on the microscopic and spectroscopic results, the Pd-Pt aerogels show the presence of Pd/Pt-rich domains inside the long-range framework. It is evident that the initial monometallic features dominate over alloying during the gelation process. Although the same synthetic approach for Pd-Pt aerogels with different atomic ratios was used, we observed that the sizes of these monometallic domains strongly varied between the Pd-rich and Pt-rich aerogels. For instance, the Pd-rich aerogels showed larger clusters with a size range from few nanometers up to several tens of nanometers, while the dimension of the clusters of the Pt-rich aerogels varies from the sub-nanometers to a few nanometers. The presence of the metal clusters strongly influenced the electrochemical robustness of these Pd-Pt aerogels. Electrochemical durability investigations revealed that the aerogels with a high content of Pd are less stable due to the gradual dissolution of the less noble metal in particular inside the Pd-rich domains. A better chemical and structural homogeneity might improve the life-time of the Pd-Pt aerogels under electrochemical conditions.
In this work, we provide a better understanding about the structure and chemical distribution of the bimetallic aerogel framework prepared by the two step gelation process.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa:de:qucosa:31073 |
| Date | 19 July 2018 |
| Creators | Oezaslan, Mehtap, Herrmann, Anne-Kristin, Werheid, Matthias, Frenkel, Anatoly, Nachtegaal, Maarten, Dosche, Carsten, Laugier Bonnaud, Celine, Ceren Yilmaz, Hale, Kühn, Laura, Rhiel, Erhard, Gaponik, Nikolai, Eychmüller, Alexander, Schmidt, Thomas Justus |
| Publisher | Wiley VCH Verlag |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | doc-type:article, info:eu-repo/semantics/article, doc-type:Text |
| Source | ChemCatChem (2017), 9(5), S. 798-808. E-ISSN 1867-3899. DOI: 10.1002/cctc.201600667 |
| Rights | info:eu-repo/semantics/openAccess |
| Relation | 10.1002/cctc.201600667 |
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