Carbon nanotube (CNT)-supported Pt metal nanoparticles were covered with silica layers by utilizing the
successive hydrolysis of 3-aminopropyl-triethoxysilane and tetraethoxysilane on CNTs with Pt hydroxide.
The CNT-supported Pt metal particles covered with silica layers (denoted as SiO2/Pt/CNT) were used as the
electrocatalysts. SiO2/Pt/CNT electrocatalysts showed a high stability for the repeated potential cycling
experiment, whereas Pt/CNT electrocatalysts were deactivated seriously for the experiment because of the
growth of Pt metal particles in size. The silica layers in SiO2/Pt/CNT prevent the dissolution of Pt metal
particles as well as the migration and agglomeration of Pt metal particles on the supports, which results in the
improvement of the stability of Pt/CNT electrocatalysts.
Multiwalled carbon nanotube ͑CNT͒-supported Pt nanoparticles ͑Pt/CNT͒ were covered with silica layers by successive hydrolysis of 3-aminopropyl-triethoxysilane and tetraethoxysilane on CNTs with Pt metal precursors, followed by reduction with hydrogen. The Pt/CNT covered with silica layers ͑SiO 2 /Pt/CNT͒ was used as a cathode catalyst for a proton exchange membrane fuel cell ͑PEMFC͒. The activity of SiO 2 /Pt/CNT catalyst for the oxygen reduction reaction in a single-cell PEMFC was similar to that of Pt/CNT, in spite of the uniform coverage of Pt with silica layers, indicating that the coverage of Pt/CNT with silica layers did not appreciably decrease the catalytic activity. In addition, SiO 2 /Pt/CNT electrocatalyst showed high stability during potential cycling from 0.05 to 1.20 V vs reversible hydrogen electrode in an aqueous H 2 SO 4 electrolyte, whereas Pt/CNT significantly deactivated during the experiment. The structural change of Pt species in these electrocatalysts during potential cycling was investigated by transmission electron microscopy images and Pt L III -edge X-ray absorption fine structure. The crystallite size of Pt metal in SiO 2 /Pt/CNT did not change appreciably during the potential cycling, while Pt metal crystallites in Pt/CNT seriously aggregated. Silica layers enveloping Pt metal particles in SiO 2 /Pt/CNT prevent the dissolution and redeposition of Pt metal particles as well as the agglomeration of Pt metal particles on the supports.
Carbon nanotube (CNT)-supported Pt metal nanoparticles were covered with silica layers by hydrolysis of 3-aminopropyl-triethoxysilane (APTES) and/or tetraethoxysilane (TEOS). The hydrolysis of only APTES resulted in a uniform coverage of silica layers on Pt/CNT, but the thickness of the silica layers was very thin (\1 nm). Pt/CNT could also be coated with silica layers of a few nanometers in thickness by hydrolysis of TEOS, but exposed surfaces of CNTs in the sample were frequently observed. In contrast, the successive hydrolysis of APTES and TEOS brought about a uniform coverage of silica layers of a few nanometers in thickness on Pt/CNT. The silica-coated Pt/CNT showed high catalytic activity for electrochemical reactions in aqueous H 2 SO 4 electrolyte, in spite of a uniform coverage of Pt metal with silica layers. In addition, the coverage of Pt/CNT with silica layers improved its durability in electrochemical reactions.
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