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

Title: Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO2 by Supporting Palladium on Metal Carbides

Abstract

Abstract Electrochemical CO 2 reduction reaction (CO 2 RR) with renewable electricity is a potentially sustainable method to reduce CO 2 emissions. Palladium supported on cost‐effective transition‐metal carbides (TMCs) are studied to reduce the Pd usage and tune the activity and selectivity of the CO 2 RR to produce synthesis gas, using a combined approach of studying thin films and practical powder catalysts, in situ characterization, and density functional theory (DFT) calculations. Notably, Pd/TaC exhibits higher CO 2 RR activity, stability and CO Faradaic efficiency than those of commercial Pd/C while significantly reducing the Pd loading. In situ measurements confirm the transformation of Pd into hydride (PdH) under the CO 2 RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. This work suggests the prospect of using TMCs as low‐cost and stable substrates to support and modify Pd for enhanced CO 2 RR activity.

Authors:
 [1];  [2];  [3];  [3];  [3];  [3];  [4];  [4]; ORCiD logo [2]
+ Show Author Affiliations
  1. Tianjin Univ., Tianjin (People's Republic of China); Columbia Univ., New York, NY (United States)
  2. Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Columbia Univ., New York, NY (United States)
  4. Tianjin Univ., Tianjin (People's Republic of China)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1542779
Alternate Identifier(s):
OSTI ID: 1504298
Report Number(s):
BNL-211861-2019-JAAM
Journal ID: ISSN 0044-8249
Grant/Contract Number:  
SC0012704; FG02-13ER16381; SC0009476
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Angewandte Chemie
Additional Journal Information:
Journal Volume: 131; Journal Issue: 19; Journal ID: ISSN 0044-8249
Publisher:
German Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CO2 electroreduction; carbides; in-situ X-ray spectroscopy; computational chemistry; palladium hydride

Citation Formats

Wang, Jiajun, Kattel, Shyam, Hawxhurst, Christopher J., Lee, Ji Hoon, Tackett, Brian M., Chang, Kuan, Rui, Ning, Liu, Chang ‐Jun, and Chen, Jingguang G. Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO2 by Supporting Palladium on Metal Carbides. United States: N. p., 2019. Web. doi:10.1002/ange.201900781.
Copy to clipboard
Wang, Jiajun, Kattel, Shyam, Hawxhurst, Christopher J., Lee, Ji Hoon, Tackett, Brian M., Chang, Kuan, Rui, Ning, Liu, Chang ‐Jun, & Chen, Jingguang G. Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO2 by Supporting Palladium on Metal Carbides. United States. https://doi.org/10.1002/ange.201900781
Copy to clipboard
Wang, Jiajun, Kattel, Shyam, Hawxhurst, Christopher J., Lee, Ji Hoon, Tackett, Brian M., Chang, Kuan, Rui, Ning, Liu, Chang ‐Jun, and Chen, Jingguang G. 2019. "Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO2 by Supporting Palladium on Metal Carbides". United States. https://doi.org/10.1002/ange.201900781. https://www.osti.gov/servlets/purl/1542779.
Copy to clipboard
@article{osti_1542779,
title = {Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO2 by Supporting Palladium on Metal Carbides},
author = {Wang, Jiajun and Kattel, Shyam and Hawxhurst, Christopher J. and Lee, Ji Hoon and Tackett, Brian M. and Chang, Kuan and Rui, Ning and Liu, Chang ‐Jun and Chen, Jingguang G.},
abstractNote = {Abstract Electrochemical CO 2 reduction reaction (CO 2 RR) with renewable electricity is a potentially sustainable method to reduce CO 2 emissions. Palladium supported on cost‐effective transition‐metal carbides (TMCs) are studied to reduce the Pd usage and tune the activity and selectivity of the CO 2 RR to produce synthesis gas, using a combined approach of studying thin films and practical powder catalysts, in situ characterization, and density functional theory (DFT) calculations. Notably, Pd/TaC exhibits higher CO 2 RR activity, stability and CO Faradaic efficiency than those of commercial Pd/C while significantly reducing the Pd loading. In situ measurements confirm the transformation of Pd into hydride (PdH) under the CO 2 RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. This work suggests the prospect of using TMCs as low‐cost and stable substrates to support and modify Pd for enhanced CO 2 RR activity.},
doi = {10.1002/ange.201900781},
url = {https://www.osti.gov/biblio/1542779}, journal = {Angewandte Chemie},
issn = {0044-8249},
number = 19,
volume = 131,
place = {United States},
year = {Mon Mar 18 00:00:00 EDT 2019},
month = {Mon Mar 18 00:00:00 EDT 2019}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/ange.201900781
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Understanding of Strain Effects in the Electrochemical Reduction of CO 2 : Using Pd Nanostructures as an Ideal Platform
journal, February 2017

Selective increase in CO 2 electroreduction activity at grain-boundary surface terminations
journal, November 2017

Carbon Dioxide Electroreduction into Syngas Boosted by a Partially Delocalized Charge in Molybdenum Sulfide Selenide Alloy Monolayers
journal, June 2017

Fuel production from CO2 using solar-thermal energy: system level analysis
journal, January 2012

Exceptional Size-Dependent Activity Enhancement in the Electroreduction of CO 2 over Au Nanoparticles
journal, November 2014

Grain-Boundary-Dependent CO 2 Electroreduction Activity
journal, April 2015

Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles
journal, September 2018

Combining CO2 reduction with propane oxidative dehydrogenation over bimetallic catalysts
journal, April 2018

Multiple Phases of Molybdenum Carbide as Electrocatalysts for the Hydrogen Evolution Reaction
journal, May 2014

Dynamic Changes in the Structure, Chemical State and Catalytic Selectivity of Cu Nanocubes during CO 2 Electroreduction: Size and Support Effects
journal, April 2018

Temperature- and Pressure-Dependent Hydrogen Concentration in Supported PdH x Nanoparticles by Pd K-Edge X-ray Absorption Spectroscopy
journal, May 2014

Hydride phase formation in carbon supported palladium nanoparticle electrodes investigated using in situ EXAFS and XRD
journal, January 2003

Reactions of water and C1 molecules on carbide and metal-modified carbide surfaces
journal, January 2017

Understanding the Low-Overpotential Production of CH 4 from CO 2 on Mo 2 C Catalysts
journal, February 2016

A selective and efficient electrocatalyst for carbon dioxide reduction
journal, January 2014

Reactions of synthesis gas
journal, September 1996

Active Sites of Au and Ag Nanoparticle Catalysts for CO 2 Electroreduction to CO
journal, August 2015

Electrochemical reduction of CO 2 to synthesis gas with controlled CO/H 2 ratios
journal, January 2017

Exclusive Formation of Formic Acid from CO 2 Electroreduction by a Tunable Pd-Sn Alloy
journal, August 2017

Enhancing CO 2 Electroreduction with the Metal–Oxide Interface
journal, April 2017

Self-assembly of noble metal monolayers on transition metal carbide nanoparticle catalysts
journal, May 2016

Understanding of Strain Effects in the Electrochemical Reduction of CO 2 : Using Pd Nanostructures as an Ideal Platform
journal, February 2017

A New Class of Electrocatalysts for Hydrogen Production from Water Electrolysis: Metal Monolayers Supported on Low-Cost Transition Metal Carbides
journal, February 2012

Departures from the Adsorption Energy Scaling Relations for Metal Carbide Catalysts
journal, June 2014

TEM Studies of Platinum Nanowires Fabricated in Mesoporous Silica MCM-41
journal, September 2000

Role of Strain and Ligand Effects in the Modification of the Electronic and Chemical Properties of Bimetallic Surfaces
journal, October 2004

Recycling of carbon dioxide to methanol and derived products – closing the loop
journal, January 2014

CO 2 Electroreduction on Au/TiC: Enhanced Activity Due to Metal–Support Interaction
journal, February 2017

Multiple Phases of Molybdenum Carbide as Electrocatalysts for the Hydrogen Evolution Reaction
journal, May 2014

Shape-Controlled CO 2 Electrochemical Reduction on Nanosized Pd Hydride Cubes and Octahedra
journal, January 2019

Opportunities and Challenges in Utilizing Metal-Modified Transition Metal Carbides as Low-Cost Electrocatalysts
journal, October 2017

TEM Studies of Platinum Nanowires Fabricated in Mesoporous Silica MCM-41
journal, September 2000

Exclusive Formation of Formic Acid from CO 2 Electroreduction by a Tunable Pd-Sn Alloy
journal, August 2017

A review of catalysts for the electroreduction of carbon dioxide to produce low-carbon fuels
journal, January 2014

    Sort options
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Coupling of Solar Energy and Thermal Energy for Carbon Dioxide Reduction: Status and Prospects
    journal, February 2020

    Intensified Electrocatalytic CO 2 Conversion in Pressure‐Tunable CO 2 ‐Expanded Electrolytes
    journal, July 2019

    Kopplung von Solarenergie und Wärmeenergie zur Kohlendioxidreduktion: Aktueller Stand und Perspektiven
    journal, February 2020

      Sort options
      [ × clear filter / sort ]

      Similar records in OSTI.GOV collections: