Boosting the electrocatalytic glycerol oxidation performance with highly-dispersed Pt nanoclusters loaded on 3D graphene-like microporous carbon

被引:50
|
作者
Lee, Daewon [1 ]
Kim, Youngmin [1 ]
Kwon, Yonghyun [2 ]
Lee, Jongmin [3 ]
Kim, Tae-Wan [4 ]
Noh, Yuseong [5 ]
Kim, Won Bae [5 ]
Seo, Min Ho [3 ]
Kim, Kyoungsoo [6 ]
Kim, Hyung Ju [1 ,7 ]
机构
[1] Korea Res Inst Chem Technol, Carbon Resources Inst, 141 Gajeong Ro, Daejeon 34114, South Korea
[2] Inst for Basic Sci Korea, Ctr Nanomat & Chem React, Daejeon 34141, South Korea
[3] Korea Inst Energy Res, New & Renewable Energy Res Inst, Hydrogen & Fuel Cell Ctr, 20-41 Sinjaesaengeneogi Ro, Haseo Myeon 56332, Jellabuk Do, South Korea
[4] Korea Res Inst Chem Technol, Ctr Convergent Chem Proc, 141 Gajeong Ro, Daejeon 34114, South Korea
[5] Pohang Univ Sci & Technol POSTECH, Dept Chem Engn, 77 Cheongam Ro, Pohang, South Korea
[6] Chonbuk Natl Univ CBNU, Dept Chem, 567 Baekje Daero, Jeonju Si 54896, Jeollabuk Do, South Korea
[7] Univ Sci & Technol, Adv Mat & Chem Engn, 113 Gwahangno, Yuseong 34113, Daejeon, South Korea
基金
新加坡国家研究基金会;
关键词
Platinum nanoclusters; Graphene; Zeolite-template; Electrocatalytic oxidations; Glycerol; MEMBRANE FUEL-CELLS; SUPPORTED PTRU CATALYSTS; OXYGEN REDUCTION; PLATINUM CLUSTERS; ANODE CATALYSTS; CRUDE GLYCEROL; ELECTROOXIDATION; NANOPARTICLES; EFFICIENT; BIOMASS;
D O I
10.1016/j.apcatb.2019.01.022
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:555 / 568
页数:14
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