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Title: Carbon nanotube supported PdAg nanoparticles for electrocatalytic oxidation of glycerol in anion exchange membrane fuel cells

Journal Article · · Applied Catalysis B: Environmental
 [1];  [1];  [1];  [2]
  1. Iowa State Univ., Ames, IA (United States)
  2. Ames Lab. and Iowa State Univ., Ames, IA (United States)

Electro-oxidation of alcohol is the key reaction occurring at the anode of a direct alcohol fuel cell (DAFC), in which both reaction kinetics (rate) and selectivity (to deep oxidation products) need improvement to obtain higher power density and fuel utilization for a more efficient DAFC. We recently found that a PdAg bimetallic nanoparticle catalyst is more efficient than Pd for alcohol oxidation: Pd can facilitate deprotonation of alcohol in a base electrolyte, while Ag can promote intermediate aldehyde oxidation and cleavage of C-single bondC bond of C3 species to C2 species. Furthermore, a combination of the two active sites (Pd and Ag) with two different functions, can simultaneously improve the reaction rates and deeper oxidation products of alcohols. In this continuing work, Pd, Ag mono, and bimetallic nanoparticles supported on carbon nanotubes (Ag/CNT, Pd/CNT, Pd1Ag1/CNT, and Pd1Ag3/CNT) were prepared using an aqueous-phase reduction method; they served as working catalysts for studying electrocatalytic oxidation of glycerol in an anion-exchange membrane-based direct glycerol fuel cell. Combined XRD, TEM, and HAADF-STEM analyses performed to fully characterize as-prepared catalysts suggested that they have small particle sizes: 2.0 nm for Pd/CNT, 2.3 nm for PdAg/CNT, 2.4 nm for PdAg3/CNT, and 13.9 nm for Ag/CNT. XPS further shows that alloying with Ag results in more metal state Pd presented on the surface, and this may be related to their higher direct glycerol fuel cell (DGFC) performances. Single DGFC performance and product analysis results show that PdAg bimetallic nanoparticles can not only improve the glycerol reaction rate so that higher power output can be achieved, but also facilitate deep oxidation of glycerol so that a higher faradaic efficiency and fuel utilization can be achieved along with optimal reaction conditions (increased base-to-fuel ratio). Half-cell electrocatalytic activity measurement and single fuel cell product analysis of different glycerol oxidation intermediates, including C3: glycerate, tartronate, mesoxalate, and lactate; C2: glycolate and oxalate, over PdAg/CNT catalyst was further conducted and produced deeper insight into the synergistic effects and reaction pathways of bimetallic PdAg catalysts in glycerol electrocatalytic oxidation.

Research Organization:
Ames Lab., Ames, IA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
CBET-1501124 and 1159448; AC02-07CH11358
OSTI ID:
1350050
Alternate ID(s):
OSTI ID: 1414784
Report Number(s):
IS-J-9254; PII: S0926337317301947
Journal Information:
Applied Catalysis B: Environmental, Vol. 210, Issue C; ISSN 0926-3373
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 85 works
Citation information provided by
Web of Science

References (51)

The future of fossil fuels—is it the end? journal January 2016
Renewable Chemical Commodity Feedstocks from Integrated Catalytic Processing of Pyrolysis Oils journal November 2010
How America can look within to achieve energy security and reduce global warming journal December 2008
Direct glycerol fuel cell with polytetrafluoroethylene (PTFE) thin film separator journal May 2017
Biodiesel processing and production journal June 2005
Chemoselective catalytic conversion of glycerol as a biorenewable source to valuable commodity chemicals journal January 2008
Selective oxidation of glycerol with oxygen using mono and bimetallic catalysts based on Au, Pd and Pt metals journal May 2005
Selective catalytic oxidation of glycerol: perspectives for high value chemicals journal January 2011
From Glycerol to Value-Added Products journal June 2007
Copper-Modified Gold Nanoparticles as Highly Selective Catalysts for Glycerol Electro-Oxidation in Alkaline Solution journal September 2016
Oxidation of glycerol using supported Pt, Pd and Au catalysts journal February 2003
Development of a Transient Segregated Mathematical Model of the Semicontinuous Microbial Production Process of Dihydroxyacetone journal February 2006
Fuel cells for portable applications journal March 2002
Overview on the application of direct methanol fuel cell (DMFC) for portable electronic devices journal August 2009
What Are Batteries, Fuel Cells, and Supercapacitors? journal October 2004
Principles and Materials Aspects of Direct Alkaline Alcohol Fuel Cells journal August 2010
Alkaline direct alcohol fuel cells journal June 2010
Simultaneous Generation of Mesoxalic Acid and Electricity from Glycerol on a Gold Anode Catalyst in Anion-Exchange Membrane Fuel Cells journal May 2012
Pd–Ni electrocatalysts for efficient ethanol oxidation reaction in alkaline electrolyte journal October 2011
Development of glycerol/O2 biofuel cell journal November 2007
Electrocatalysis of oxygen reduction and small alcohol oxidation in alkaline media journal January 2007
Electrochemistry and the Future of the Automobile journal June 2010
Surface dealloyed PtCo nanoparticles supported on carbon nanotube: facile synthesis and promising application for anion exchange membrane direct crude glycerol fuel cell journal January 2013
Glycerol oxidation in solid oxide fuel cells based on a Ni-perovskite electrocatalyst journal March 2011
Study of operating conditions and cell design on the performance of alkaline anion exchange membrane based direct methanol fuel cells journal October 2011
Investigation of direct methanol fuel cells based on unsupported Pt–Ru anode catalysts with different chemical properties journal August 2000
Synthesis and characterization of the Au-modified Pd cathode catalyst for alkaline direct ethanol fuel cells journal September 2010
Structure and chemical composition of supported Pt–Sn electrocatalysts for ethanol oxidation journal September 2005
Recent progress in direct ethanol proton exchange membrane fuel cells (DE-PEMFCs) journal March 2006
Strong Impact of Platinum Surface Structure on Primary and Secondary Alcohol Oxidation during Electro-Oxidation of Glycerol journal June 2016
Comparison of ethanol electro-oxidation on Pt/C and Pd/C catalysts in alkaline media journal August 2012
Pd/Pt core–shell nanowire arrays as highly effective electrocatalysts for methanol electrooxidation in direct methanol fuel cells journal October 2008
Bi- and tri-metallic Pt-based anode catalysts for direct ethanol fuel cells journal May 2004
Pt-based anode catalysts for direct ethanol fuel cells journal November 2004
Oxidation of Glycerol to Glycolate by using Supported Gold and Palladium Nanoparticles journal December 2009
Au, Pd (mono and bimetallic) catalysts supported on graphite using the immobilisation method journal September 2005
Selective oxidation with air on metal catalysts journal September 1997
Chemoselective catalytic oxidation of glycerol with air on platinum metals journal June 1995
The effect of ZnS segregation on Zn-rich CZTS thin film solar cells journal May 2015
Reduction free room temperature synthesis of a durable and efficient Pd/ordered mesoporous carbon composite electrocatalyst for alkaline direct alcohols fuel cell journal January 2014
A hierarchical heterostructure based on Pd nanoparticles/layered double hydroxide nanowalls for enhanced ethanol electrooxidation journal January 2013
One-step synthesis of palladium-gold-silver ternary nanoparticles supported on reduced graphene oxide for the electrooxidation of methanol and ethanol journal August 2015
Investigation on ethanol electrooxidation via electrodeposited Pd–Co nanostructures supported on graphene oxide journal September 2015
Binary PdM catalysts (M = Ru, Sn, or Ir) over a reduced graphene oxide support for electro-oxidation of primary alcohols (methanol, ethanol, 1-propanol) under alkaline conditions journal January 2015
A green method to prepare Pd–Ag nanoparticles supported on reduced graphene oxide and their electrochemical catalysis of methanol and ethanol oxidation journal October 2014
Facile synthesis of PdSb x /C nanocatalyst with high performance for ethanol electro-oxidation in alkaline medium journal October 2014
Ultrafine nanoporous Cu–Pd alloys with superior catalytic activities towards electro-oxidation of methanol and ethanol in alkaline media journal January 2012
PdAg/CNT catalyzed alcohol oxidation reaction for high-performance anion exchange membrane direct alcohol fuel cell (alcohol = methanol, ethanol, ethylene glycol and glycerol) journal December 2016
Direct fast pyrolysis bio-oil fuel cell journal December 2016
Electrocatalytic selective oxidation of glycerol to tartronate on Au/C anode catalysts in anion exchange membrane fuel cells with electricity cogeneration journal July 2014
Platinum nanopaticles supported on stacked-cup carbon nanofibers as electrocatalysts for proton exchange membrane fuel cell journal April 2010

Cited By (11)

Glycerol Electro-Oxidation in Alkaline Media and Alkaline Direct Glycerol Fuel Cells journal November 2019
Electrocatalytic Oxidation of Small Molecule Alcohols over Pt, Pd, and Au Catalysts: The Effect of Alcohol’s Hydrogen Bond Donation Ability and Molecular Structure Properties journal April 2019
Sodium Alginate-Assisted Synthesis of PdAg Bimetallic Nanoparticles and their Enhanced Activity for Electrooxidation of Ethanol journal September 2019
Facile construction of fascinating trimetallic PdAuAg nanocages with exceptional ethylene glycol and glycerol oxidation activity journal January 2017
Advanced Catalytic Materials for Ethanol Oxidation in Direct Ethanol Fuel Cells journal February 2020
Glycerol oxidation assisted electrocatalytic nitrogen reduction: ammonia and glyceraldehyde co-production on bimetallic RhCu ultrathin nanoflake nanoaggregates journal January 2019
A review of recent progress on electrocatalysts toward efficient glycerol electrooxidation journal January 2020
Sustainable Conversion of Glycerol into Value-Added Chemicals by Selective Electro-Oxidation on Pt-Based Catalysts journal May 2018
Surfactant‐Assisted Electrodeposition of Nickel Nanostructures and Their Electrocatalytic Activities Toward Oxidation of Sodium Borohydride, Ethanol, and Methanol journal April 2019
Electro-oxidation of waste glycerol to tartronic acid over Pt/CNT nanocatalyst: study of effect of reaction time on product distribution journal November 2019
Sustainable Conversion of Glycerol into Value-Added Chemicals by Selective Electro-Oxidation on Pt-Based Catalysts journal June 2018