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

Abstract

Electrochemical CO2 reduction reaction (CO2RR) with renewable electricity is a potentially sustainable method to reduce CO2 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 CO2RR 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 CO2RR 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 CO2RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. As a result, this work suggests the prospect of using TMCs as low-cost and stable substrates to support and modify Pd for enhanced CO2RR activity.

Authors:
 [1];  [2];  [3];  [3];  [3];  [3];  [4];  [4]; ORCiD logo [2]
  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 Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
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:
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.
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. doi:10.1002/ange.201900781.
Wang, Jiajun, Kattel, Shyam, Hawxhurst, Christopher J., Lee, Ji Hoon, Tackett, Brian M., Chang, Kuan, Rui, Ning, Liu, Chang ‐Jun, and Chen, Jingguang G. Mon . "Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO2 by Supporting Palladium on Metal Carbides". United States. doi:10.1002/ange.201900781. https://www.osti.gov/servlets/purl/1542779.
@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 = {Electrochemical CO2 reduction reaction (CO2RR) with renewable electricity is a potentially sustainable method to reduce CO2 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 CO2RR 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 CO2RR 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 CO2RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. As a result, this work suggests the prospect of using TMCs as low-cost and stable substrates to support and modify Pd for enhanced CO2RR activity.},
doi = {10.1002/ange.201900781},
journal = {Angewandte Chemie},
number = 19,
volume = 131,
place = {United States},
year = {2019},
month = {3}
}

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Works referenced in this record:

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

  • Lu, Qi; Rosen, Jonathan; Zhou, Yang
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4242

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

  • Kim, Jiyong; Johnson, Terry A.; Miller, James E.
  • Energy & Environmental Science, Vol. 5, Issue 9
  • DOI: 10.1039/c2ee21798h

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

  • Goeppert, Alain; Czaun, Miklos; Jones, John-Paul
  • Chem. Soc. Rev., Vol. 43, Issue 23
  • DOI: 10.1039/C4CS00122B

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

  • Grosse, Philipp; Gao, Dunfeng; Scholten, Fabian
  • Angewandte Chemie International Edition, Vol. 57, Issue 21
  • DOI: 10.1002/anie.201802083

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

  • Grosse, Philipp; Gao, Dunfeng; Scholten, Fabian
  • Angewandte Chemie, Vol. 130, Issue 21
  • DOI: 10.1002/ange.201802083

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


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


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

  • Gao, Dunfeng; Zhang, Yi; Zhou, Zhiwen
  • Journal of the American Chemical Society, Vol. 139, Issue 16
  • DOI: 10.1021/jacs.7b00102

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

  • Qiao, Jinli; Liu, Yuyu; Hong, Feng
  • Chem. Soc. Rev., Vol. 43, Issue 2
  • DOI: 10.1039/C3CS60323G

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

  • Feng, Xiaofeng; Jiang, Kaili; Fan, Shoushan
  • Journal of the American Chemical Society, Vol. 137, Issue 14
  • DOI: 10.1021/ja5130513

Reactions of synthesis gas
journal, September 1996


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

  • Sheng, Wenchao; Kattel, Shyam; Yao, Siyu
  • Energy & Environmental Science, Vol. 10, Issue 5
  • DOI: 10.1039/C7EE00071E

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

  • Xu, Jiaqi; Li, Xiaodong; Liu, Wei
  • Angewandte Chemie International Edition, Vol. 56, Issue 31
  • DOI: 10.1002/anie.201704928

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


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

  • Bai, Xiaofang; Chen, Wei; Zhao, Chengcheng
  • Angewandte Chemie International Edition, Vol. 56, Issue 40
  • DOI: 10.1002/anie.201707098

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

  • Bai, Xiaofang; Chen, Wei; Zhao, Chengcheng
  • Angewandte Chemie, Vol. 129, Issue 40
  • DOI: 10.1002/ange.201707098

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

  • Lee, Ji Hoon; Kattel, Shyam; Xie, Zhenhua
  • Advanced Functional Materials, Vol. 28, Issue 45
  • DOI: 10.1002/adfm.201804762

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

  • Zhu, Wenlei; Kattel, Shyam; Jiao, Feng
  • Advanced Energy Materials, Vol. 9, Issue 9
  • DOI: 10.1002/aenm.201802840

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

  • Huang, Hongwen; Jia, Huanhuan; Liu, Zhao
  • Angewandte Chemie International Edition, Vol. 56, Issue 13
  • DOI: 10.1002/anie.201612617

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


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


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


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

  • Esposito, Daniel V.; Hunt, Sean T.; Kimmel, Yannick C.
  • Journal of the American Chemical Society, Vol. 134, Issue 6
  • DOI: 10.1021/ja208656v

Theoretical prediction and experimental verification of low loading of platinum on titanium carbide as low-cost and stable electrocatalysts
journal, April 2014


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

  • Michalsky, Ronald; Zhang, Yin-Jia; Medford, Andrew J.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 24
  • DOI: 10.1021/jp503756g

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


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


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

  • Wan, Cheng; Regmi, Yagya N.; Leonard, Brian M.
  • Angewandte Chemie International Edition, Vol. 53, Issue 25
  • DOI: 10.1002/anie.201402998

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

  • Wan, Cheng; Regmi, Yagya N.; Leonard, Brian M.
  • Angewandte Chemie, Vol. 126, Issue 25
  • DOI: 10.1002/ange.201402998

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

  • Wan, Weiming; Tackett, Brian M.; Chen, Jingguang G.
  • Chemical Society Reviews, Vol. 46, Issue 7
  • DOI: 10.1039/C6CS00862C

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


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


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

  • Bugaev, Aram L.; Guda, Alexander A.; Lomachenko, Kirill A.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 19
  • DOI: 10.1021/jp500734p

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

  • Rose, Abigail; Maniguet, Stephanie; Mathew, Rebecca J.
  • Physical Chemistry Chemical Physics, Vol. 5, Issue 15
  • DOI: 10.1039/b302956e

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

  • Mistry, Hemma; Reske, Rulle; Zeng, Zhenhua
  • Journal of the American Chemical Society, Vol. 136, Issue 47
  • DOI: 10.1021/ja508879j

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