期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 245, 期 -, 页码 555-568出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2019.01.022
关键词
Platinum nanoclusters; Graphene; Zeolite-template; Electrocatalytic oxidations; Glycerol
资金
- core KRICT projects from the Korea Research Institute of Chemical Technology (KRICT) [SI1801-05, KK1806-G09]
- Technology Development Program to Solve Climate Changes of the National Research Foundation (NRF) - Ministry of Science, ICT AMP
- Future Planning [2017M1A2A2049168]
- Basic Science Research Program through the NRF [NRF-2017R1D1A1B04031539]
- development program of KIER [B8-2423]
- National Research Council of Science & Technology (NST), Republic of Korea [SI1801-05, KIER2-3] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
Preparing Pt nanostructure catalysts with better support materials is an efficient catalyst design strategy to develop high performance Pt-based electrocatalysts. Here we report for the first time a method to synthesize highly-dispersed Pt nanoclusters supported on microporous three-dimensional (3D) graphene-like carbon (3D-GLC) for use in the electrochemical oxidation reaction. The Pt nanoclusters loaded on 3D graphene-like carbon (Pt/3D-GLC) are synthesized by Ca2+-exchanged beta zeolite template based carbon synthesis and subsequent Pt impregnation methods. Highly-dispersed Pt nanoclusters (ca. 1.25 +/- 0.30 nm) loaded on the 3D-GLC having a large surface area (ca. 2910 m(2)/g) demonstrate superior electrocatalytic performance for electrochemical glycerol oxidation reaction (GOR) over that of a commercial Pt/C catalyst. We hypothesize in this work that the improved GOR performance of Pt/3D-GLC is related to the increase of Pt active sites by decreasing Pt cluster size and the change in the physicochemical properties of the Pt by interaction between the Pt cluster and 3D-GLC. In addition, first-principle density functional theory (DFT) and ab-initio molecular dynamics (MD) simulations are performed to demonstrate that the finely-dispersed Pt nanoclusters on 3D-GLC support can give rise to excellent GOR activity in accordance with the enhanced adsorption behavior of glycerol on its Pt crystal surfaces.
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