Journal
JOURNAL OF POWER SOURCES
Volume 347, Issue -, Pages 69-78Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.jpowsour.2017.02.044
Keywords
Graphene cellular monolith; Porous architecture; Multimetallic nanoparticle; Electrocatalyst; Oxygen reduction reaction
Funding
- National Natural Science Foundation of China [51572114, 51672112]
- Laboratory Directed Research and Development Program as part of the Chemical Imaging Initiative at PNNL
- DOE's Office of Biological and Environmental Research and located at PNNL
- DOE [DE-AC05-76RLO1830]
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Graphene cellular monolith (GCM) can be used as an excellent support for nanoparticles in widespread applications. However, it's still a great challenge to deposit the desirable nanoparticles in GCM that have small size, controllable structure, composition, and high dispersion using the current methods. Here we demonstrate a green, efficient and large-scale method to address this challenge using supercritical fluid (SCF). By this superior method, graphene hydrogel can be transferred into GCM while being deposited with ultrafine and highly dispersive nanoparticles. Specifically, the bimetallic PtFe/GCM and the trimetallic PtFeCo/GCM catalysts are successfully synthesized, and their electrocatalytic performances toward oxygen reduction reaction (ORR) are also studied. The resultant PtFe/GCM shows the significant enhancement in ORR activity, including a factor of 8.47 enhancement in mass activity (0.72 A mg(pt)(-1)),and a factor of 7.67 enhancement in specific activity (0.92 mA cm(-2)), comparing with those of the commercial Pt/C catalyst (0.085 A mg(pt)(-1), 0.12 mA cm(-2)). Importantly, by introducing the Co, the trimetallic PtFeCo/GCM exhibits the further improved ORR activities (1.28 A mg(pt)(-1), 1.80 mA cm(-2)). The high ORR activity is probably attributed to the alloying structure, ultrafine size, highly dispersive, well-defined, and a better interface with 3D porous graphene support. (C) 2017 Elsevier B.V. All rights reserved.
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