Controllable synthesis of palladium nanocubes/reduced graphene
oxide composites and their enhanced electrocatalytic performance
Yuting Zhang
a
, Qiwei Huang
a
, Gang Chang
a
,
*
, Zaoli Zhang
a
,
b
, Tiantian Xia
a
,
Honghui Shu
a
, Yunbin He
a
,
*
a
Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Ministry-of-Education Key Laboratory for the Green Preparation and
Application of Functional Materials, Faculty of Materials Science and Engineering, Hubei University, No.368 Youyi Avenue, Wuchang, Wuhan 430062, China
b
Erich Schmid Institute of Materials Science, Austrian Academy of Sciences, A-8700 Leoben, Austria
highlights
Pd nanocubes/reduced graphene oxide was synthesized within one-step process.
Environment friendly ascorbic acid was chosen as the reductant.
Experimental factors have been systematically studied for the formation mechanism.
The PdNCs/G exhibits superior activity and stability towards ethanol oxidation.
article info
Article history:
Received 24 October 2014
Received in revised form
15 January 2015
Accepted 20 January 2015
Available online 21 January 2015
Keywords:
Pd nanocubes
Graphene
One-step method
Ethanol oxidation
abstract
Homogeneous distribution of cube-shaped Pd nanocrystals on the surface of reduced graphene oxide is
obtained via a facile one-step method by employing AA and KBr as the reductant and capping agent,
respectively. The experimental factors affecting the morphology and structure of Pd nanoparticles have
been systematically investigated to explore the formation mechanism of Pd nanocubes (PdNCs). It is
revealed that PdNCs enclosed by active {100} facets with an average side length of 15 nm were suc-
cessfully synthesized on the surface of reduced graphene oxide. KBr plays the role for facet selection by
surface passivation and AA controls the reduction speed of Pd precursors, both of which govern the
morphology changes of palladium nanoparticles. In the further electrochemical evaluations, the Pd
nanocubes/reduced graphene oxide composites show better electrocatalytic activity and stability to-
wards the electro-oxidation of ethanol than both reduced graphene oxide supported Pd nanoparticles
and free-standing PdNCs. It could be attributed to the high electrocatalytic activity of the dominated
active {100} crystal facets of Pd nanocubes and the enhanced electron transfer of graphene. The
developed approach provide a versatile way for shape-controlled preparation of noble metal nano-
particles, which can work as novel electrocatalysts in the application of direct alcohols fuel cells.
© 2015 Elsevier B.V. All rights reserved.
1. Introduction
Novel electronic, thermal, optical, magnetic and catalytical
properties of nanocrystals are proved to be much dependent on
their shape and structure. Therefore, extensive interest in past
decades have been devoted to controllable synthesis of metal
nanocrystals with different shapes and facet orientations, which is
a powerful means to tune the properties of nanomaterials for
various applications [1e3]. As an extremely important nano-
material in catalysis, Pd nanocrystals exhibit efficient electro-
catalytic activities in fuel cell applications [4e7]. In this regard,
controlling the shape and facets of Pd nanocrystals is an effective
way to enhance the performance in catalytic reactions. Among the
Pd nanomaterials, Pd nanocubes have gained exceptional attention
for their superior catalytic ability resulting from the relatively high
surface energy of the surrounding {100} facets among low index
facets. Notably, Zhang et al. applied a one-pot method to fabricate
the cubic Pd nanocrystals with {100} facets showing a higher ac-
tivity than the {110}-facet-enclosed Pd rhombic dodecahedral in
* Corresponding authors.
E-mail addresses: gchanghubei@gmail.com (G. Chang), ybhe@hubu.edu.cn
(Y. He).
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Journal of Power Sources
journal homepage: www.elsevier.com/locate/jpowsour
http://dx.doi.org/10.1016/j.jpowsour.2015.01.127
0378-7753/© 2015 Elsevier B.V. All rights reserved.
Journal of Power Sources 280 (2015) 422e429