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Title: Synthesis of an excellent electrocatalyst for oxygen reduction reaction with supercritical fluid: Graphene cellular monolith with ultrafine and highly dispersive multimetallic nanoparticles

Authors:
; ; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1397413
Grant/Contract Number:
AC05-76RLO1830
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Journal of Power Sources
Additional Journal Information:
Journal Volume: 347; Journal Issue: C; Related Information: CHORUS Timestamp: 2018-01-04 18:04:53; Journal ID: ISSN 0378-7753
Publisher:
Elsevier
Country of Publication:
Netherlands
Language:
English

Citation Formats

Zhou, Yazhou, Cheng, Xiaonong, Yen, Clive H., Wai, Chien M., Wang, Chongmin, Yang, Juan, and Lin, Yuehe. Synthesis of an excellent electrocatalyst for oxygen reduction reaction with supercritical fluid: Graphene cellular monolith with ultrafine and highly dispersive multimetallic nanoparticles. Netherlands: N. p., 2017. Web. doi:10.1016/j.jpowsour.2017.02.044.
Zhou, Yazhou, Cheng, Xiaonong, Yen, Clive H., Wai, Chien M., Wang, Chongmin, Yang, Juan, & Lin, Yuehe. Synthesis of an excellent electrocatalyst for oxygen reduction reaction with supercritical fluid: Graphene cellular monolith with ultrafine and highly dispersive multimetallic nanoparticles. Netherlands. doi:10.1016/j.jpowsour.2017.02.044.
Zhou, Yazhou, Cheng, Xiaonong, Yen, Clive H., Wai, Chien M., Wang, Chongmin, Yang, Juan, and Lin, Yuehe. Sat . "Synthesis of an excellent electrocatalyst for oxygen reduction reaction with supercritical fluid: Graphene cellular monolith with ultrafine and highly dispersive multimetallic nanoparticles". Netherlands. doi:10.1016/j.jpowsour.2017.02.044.
@article{osti_1397413,
title = {Synthesis of an excellent electrocatalyst for oxygen reduction reaction with supercritical fluid: Graphene cellular monolith with ultrafine and highly dispersive multimetallic nanoparticles},
author = {Zhou, Yazhou and Cheng, Xiaonong and Yen, Clive H. and Wai, Chien M. and Wang, Chongmin and Yang, Juan and Lin, Yuehe},
abstractNote = {},
doi = {10.1016/j.jpowsour.2017.02.044},
journal = {Journal of Power Sources},
number = C,
volume = 347,
place = {Netherlands},
year = {Sat Apr 01 00:00:00 EDT 2017},
month = {Sat Apr 01 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1016/j.jpowsour.2017.02.044

Citation Metrics:
Cited by: 1work
Citation information provided by
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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 reactionmore » (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 mgPt-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 mgPt-1, 0.12 mA cm-2). Importantly, by introducing the Co, the trimetallic PtFeCo/GCM exhibits the further improved ORR activities (1.28 A mgPt-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.« less
  • Three-dimensional (3D) graphene showed an advanced support for designing porous electrode materials due to its high specific surface area, large pore volume, and excellent electronic property. However, the electrochemical properties of reported porous electrode materials still need to be improved further. The current challenge is how to deposit desirable nanoparticles (NPs) with controllable structure, loading and composition in 3D graphene while maintaining the high dispersion. Herein, we demonstrate a modified supercritical fluid (SCF) technique to address this issue by controlling the SCF system. Using this superior method, a series of Pt-based/3D graphene materials with the ultrafine-sized, highly dispersive and controllablemore » composition multimetallic NPs were successfully synthesized. Specifically, the resultant Pt40Fe60/3D graphene showed a significant enhancement in electrocatalytic performance for the oxygen reduction reaction (ORR), including a factor of 14.2 enhancement in mass activity (1.70 A mgPt 1), a factor of 11.9 enhancement in specific activity (1.55 mA cm 2), and higher durability compared with that of Pt/C catalyst. After careful comparison, the Pt40Fe60/3D graphene catalyst shows the higher ORR activity than most of the reported similar 3D graphene-based catalysts. The successful synthesis of such attractive materials by this method also paves the way to develop 3D graphene in widespread applications.« less
  • A novel method for the synthesis of high-performance Pt electrocatalysts on graphitized carbon nanotubes (GCNTs) is reported. GCNTs are first noncovalently functionalized with a polyelectrolyte, poly(diallyldimethylammonium chloride) (PDDA). Pt precursors are uniformly distributed on the surface of PDDA-functionalized GCNTs via the electrostatic self-assembly between negatively charged PtCl62- and positively charged functional groups of PDDA and then Pt nanoparticles are in-situ prepared with the ethylene glycol reduction method. X-ray photoelectron spectroscopy measurement confirms the successful functionalization of PDDA on GCNTs. X-ray diffraction and transmission electron microscope images reveal that Pt nanoparticles with an average size of ~ 2.7 nm are uniformlymore » dispersed on the PDDA-functionalzied GCNTs. Pt/GCNTs electrocatalyst exhibits two times higher activity towards oxygen reduction reaction than Pt/CNTs because of the higher Pt electrochemical surface area and the higher electrical conductivity of GCNTs. Also, Pt/GCNTs exhibit a higher stability than Pt/CNTs. This enhanced durability can be attributed to the structural integrity and higher graphitization degree of GCNTs.« less
  • Carbon nanotubes (CNTs) are noncovalently functionalized with poly(allylamine hydrochloride) (PAH) and then employed as the support of Pt nanoparticles. X-Ray photoelectron spectroscopy confirms the successful functionalization of CNTs with PAH. The negatively charged Pt precursors are adsorbed on positively charged PAH-wrapping CNTs surface via electrostatic self-assembly and then in situ reduced in ethylene glycol. X-Ray diffraction and transmission electron microscope images reveal that Pt nanoparticles with an average size of 2.6 nm are uniformly dispersed on CNT surface. Pt/PAH-CNTs exhibit unexpectedly high activity towards oxygen reduction reaction, which can be attributed to the large electrochemical surface area of Pt nanoparticles.more » It also shows enhanced electrochemical stability due to the structural integrity of PAH-CNTs. This provides a facile approach to synthesize CNTs-based nanoelectrocatalysts.« less
  • We report the design and synthesis of multimetallic Au/Pt-bimetallic nanoparticles as a highly durable electrocatalyst for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. This system was first studied on well-defined Pt and FePt thin films deposited on a Au(111) surface, which has guided the development of novel synthetic routes toward shape-controlled Au nanoparticles coated with a Pt-bimetallic alloy. It has been demonstrated that these multimetallic Au/FePt{sub 3} nanoparticles possess both the high catalytic activity of Pt-bimetallic alloys and the superior durability of the tailored morphology and composition profile, with mass-activity enhancement of more than 1 ordermore » of magnitude over Pt catalysts. The reported synergy between well-defined surfaces and nanoparticle synthesis offers a persuasive approach toward advanced functional nanomaterials.« less