skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Making ultrafine and highly-dispersive multimetallic nanoparticles in three-dimensional graphene with supercritical fluid as excellent electrocatalyst for oxygen reduction reaction

Journal Article · · Journal of Materials Chemistry. A
DOI:https://doi.org/10.1039/c6ta08508c· OSTI ID:1373018

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 controllable 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 cm2), 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.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1373018
Report Number(s):
PNNL-SA-127667; JMCAET; 48877; KP1704020
Journal Information:
Journal of Materials Chemistry. A, Vol. 4, Issue 47; ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English

References (35)

3D Honeycomb-Like Structured Graphene and Its High Efficiency as a Counter-Electrode Catalyst for Dye-Sensitized Solar Cells journal July 2013
Highly Sensitive Glucose Sensor Based on Pt Nanoparticle/Polyaniline Hydrogel Heterostructures journal March 2013
Improving Electrocatalysts for O 2 Reduction by Fine-Tuning the Pt−Support Interaction: Pt Monolayer on the Surfaces of a Pd 3 Fe(111) Single-Crystal Alloy journal September 2009
Mesoporous Silicates Prepared Using Preorganized Templates in Supercritical Fluids journal January 2004
Porous Materials and Supercritical Fluids journal July 2003
Preparation of Au/Pt Bimetallic Nanoparticles in Water-in-Oil Microemulsions journal January 2001
Activity Descriptor Identification for Oxygen Reduction on Platinum-Based Bimetallic Nanoparticles: In Situ Observation of the Linear Composition–Strain–Activity Relationship journal January 2015
Highly Compression-Tolerant Supercapacitor Based on Polypyrrole-mediated Graphene Foam Electrodes journal October 2012
MATERIALS SCIENCE: Enhanced: Making Nanoscale Materials with Supercritical Fluids journal January 2004
Platinum/Carbon Nanotube Nanocomposite Synthesized in Supercritical Fluid as Electrocatalysts for Low-Temperature Fuel Cells journal August 2005
Seed-Mediated Synthesis of Core/Shell FePtM/FePt (M = Pd, Au) Nanowires and Their Electrocatalysis for Oxygen Reduction Reaction journal September 2013
A Highly Efficient Chemical Sensor Material for H2S: α-Fe2O3 Nanotubes Fabricated Using Carbon Nanotube Templates journal December 2005
Noble-Metal-Promoted Three-Dimensional Macroassembly of Single-Layered Graphene Oxide journal May 2010
3D heterostructured architectures of Co3O4 nanoparticles deposited on porous graphene surfaces for high performance of lithium ion batteries journal January 2012
Electrocatalyst approaches and challenges for automotive fuel cells journal June 2012
Electrochemical Stability of Nanometer-Scale Pt Particles in Acidic Environments journal January 2010
A powerful approach to functional graphene hybrids for high performance energy-related applications journal January 2014
FePt Nanoparticles Assembled on Graphene as Enhanced Catalyst for Oxygen Reduction Reaction journal January 2012
Deposition of Conformal Copper and Nickel Films from Supercritical Carbon Dioxide journal September 2001
Diffusion driven layer-by-layer assembly of graphene oxide nanosheets into porous three-dimensional macrostructures journal October 2014
PtRu/Carbon Nanotube Nanocomposite Synthesized in Supercritical Fluid:  A Novel Electrocatalyst for Direct Methanol Fuel Cells journal October 2005
Lattice-strain control of the activity in dealloyed core–shell fuel cell catalysts journal April 2010
Evolution of nanoporosity in dealloying journal March 2001
Record activity and stability of dealloyed bimetallic catalysts for proton exchange membrane fuel cells journal January 2015
Architecture of PtFe/C catalyst with high activity and durability for oxygen reduction reaction journal August 2014
Macroscopic Multifunctional Graphene-Based Hydrogels and Aerogels by a Metal Ion Induced Self-Assembly Process journal February 2012
3D graphene-based hybrid materials: synthesis and applications in energy storage and conversion journal January 2016
Highly efficient nonprecious metal catalysts towards oxygen reduction reaction based on three-dimensional porous carbon nanostructures journal January 2016
Activated Graphene-Based Carbons as Supercapacitor Electrodes with Macro- and Mesopores journal July 2013
Understanding the electrocatalysis of oxygen reduction on platinum and its alloys journal January 2012
Trends in electrocatalysis on extended and nanoscale Pt-bimetallic alloy surfaces journal February 2007
Newly Designed Graphene Cellular Monolith Functionalized with Hollow Pt-M (M = Ni, Co) Nanoparticles as the Electrocatalyst for Oxygen Reduction Reaction journal September 2016
Beaded Cobalt Oxide Nanoparticles along Carbon Nanotubes: Towards More Highly Integrated Electronic Devices journal January 2005
Three-Dimensional Self-Assembly of Graphene Oxide and DNA into Multifunctional Hydrogels journal November 2010
Supercritical fluid synthesis and characterization of catalytic metal nanoparticles on carbon nanotubes journal January 2004