Effect of the Pd/MWCNTs anode catalysts preparation methods on their morphology and activity in a direct formic acid fuel cell

被引:37
|
作者
Lesiak, B. [1 ]
Mazurkiewicz, M. [2 ]
Malolepszy, A. [2 ]
Stobinski, L. [1 ,2 ]
Mierzwa, B. [1 ]
Mikolajczuk-Zychora, A. [1 ]
Juchniewicz, K. [1 ]
Borodzinski, A. [1 ]
Zemek, J. [3 ]
Jiricek, P. [3 ]
机构
[1] Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland
[2] Warsaw Univ Technol, Fac Chem & Proc Engn, Warynskiego 1, PL-00645 Warsaw, Poland
[3] Acad Sci Czech Republic, Inst Phys, Cukrovarnicka 10, Prague 16253 6, Czech Republic
关键词
Electro-oxidation; DFAFC; Pd/MWCNTs; Preparation conditions; Reducing agents; Microwave conditions; RAY PHOTOELECTRON-SPECTROSCOPY; WALLED CARBON NANOTUBES; PD NANOPARTICLES; PALLADIUM NANOCRYSTALS; PARTICLE-SIZE; ELECTROOXIDATION REACTION; SURFACE-TREATMENT; OXIDATION; OXYGEN; XPS;
D O I
10.1016/j.apsusc.2016.06.152
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
Impact of Pd/MWCNTs catalysts preparation method on the catalysts morphology and activity in a formic acid electrooxidation reaction was investigated. Three reduction methods of Pd precursor involving reduction in a high pressure microwave reactor (Pdl), reduction with NaBH4 (Pd2) and microwave assisted polyol method (Pd3) were used in this paper. Crystallites size and morphology were studied using the scanning transmission electron microscopy (STEM), X-ray diffraction (XRD), whereas elemental composition, Pd chemical state and functional groups content by the X-ray photoelectron spectroscopy (XPS). The prepared catalysts were tested in a direct formic acid fuel cell (DFAFC) as an anode material. The catalytic activity was correlated with a mean fraction of the total Pd atoms exposed at the surface (FE). The value of FE was calculated from the crystallites size distribution determined by the STEM measurements. Non-linear dependence of a current density versus FE, approaching the maximum at FE approximate to 0.25 suggests that the catalytic process proceeded at Pd nanocrystallites faces, with inactive edges and corners. Pd2 catalyst exhibited highest activity due to its smallest Pd crystallites (3.2 nm), however the absence of Pd crystallites aggregation and low content of carbon in PdCx phase, i.e. x = 4 at.% may also affect the observed. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:929 / 937
页数:9
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