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:
-
[2]
- Tianjin Univ., Tianjin (People's Republic of China); Columbia Univ., New York, NY (United States)
- Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Columbia Univ., New York, NY (United States)
- 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:
- 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. https://doi.org/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. https://doi.org/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 = {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},
journal = {Angewandte Chemie},
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}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
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:
Achieving the Widest Range of Syngas Proportions at High Current Density over Cadmium Sulfoselenide Nanorods in CO 2 Electroreduction
journal, January 2018
- He, Rong; Zhang, An; Ding, Yilun
- Advanced Materials, Vol. 30, Issue 7
Unravelling charge carrier dynamics in protonated g-C3N4 interfaced with carbon nanodots as co-catalysts toward enhanced photocatalytic CO2 reduction: A combined experimental and first-principles DFT study
journal, February 2017
- Ong, Wee-Jun; Putri, Lutfi Kurnianditia; Tan, Yoong-Chuen
- Nano Research, Vol. 10, Issue 5
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, Vol. 129, Issue 13
TiC- and TiN-Supported Single-Atom Catalysts for Dramatic Improvements in CO 2 Electrochemical Reduction to CH 4
journal, April 2017
- Back, Seoin; Jung, Yousung
- ACS Energy Letters, Vol. 2, Issue 5
Selective increase in CO 2 electroreduction activity at grain-boundary surface terminations
journal, November 2017
- Mariano, Ruperto G.; McKelvey, Kim; White, Henry S.
- Science, Vol. 358, Issue 6367
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
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
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
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
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
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
Combining CO2 reduction with propane oxidative dehydrogenation over bimetallic catalysts
journal, April 2018
- Gomez, Elaine; Kattel, Shyam; Yan, Binhang
- Nature Communications, Vol. 9, Issue 1
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
Theoretical prediction and experimental verification of low loading of platinum on titanium carbide as low-cost and stable electrocatalysts
journal, April 2014
- Kimmel, Yannick C.; Yang, Leerang; Kelly, Thomas G.
- Journal of Catalysis, Vol. 312
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
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
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
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
Understanding the Low-Overpotential Production of CH 4 from CO 2 on Mo 2 C Catalysts
journal, February 2016
- Kim, Seok Ki; Zhang, Yin-Jia; Bergstrom, Helen
- ACS Catalysis, Vol. 6, Issue 3
A selective and efficient electrocatalyst for carbon dioxide reduction
journal, January 2014
- Lu, Qi; Rosen, Jonathan; Zhou, Yang
- Nature Communications, Vol. 5, Issue 1
Reactions of synthesis gas
journal, September 1996
- Wender, Irving
- Fuel Processing Technology, Vol. 48, Issue 3
Active Sites of Au and Ag Nanoparticle Catalysts for CO 2 Electroreduction to CO
journal, August 2015
- Back, Seoin; Yeom, Min Sun; Jung, Yousung
- ACS Catalysis, Vol. 5, Issue 9
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
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
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
Self-assembly of noble metal monolayers on transition metal carbide nanoparticle catalysts
journal, May 2016
- Hunt, S. T.; Milina, M.; Alba-Rubio, A. C.
- Science, Vol. 352, Issue 6288
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
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
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
TEM Studies of Platinum Nanowires Fabricated in Mesoporous Silica MCM-41
journal, September 2000
- Liu, Zheng; Sakamoto, Yasuhiro; Ohsuna, Tetsu
- Angewandte Chemie, Vol. 39, Issue 17
Role of Strain and Ligand Effects in the Modification of the Electronic and Chemical Properties of Bimetallic Surfaces
journal, October 2004
- Kitchin, J. R.; Nørskov, J. K.; Barteau, M. A.
- Physical Review Letters, Vol. 93, Issue 15
Surface and Heterointerface Engineering of 2D MXenes and Their Nanocomposites: Insights into Electro- and Photocatalysis
journal, January 2019
- Peng, Jiahe; Chen, Xingzhu; Ong, Wee-Jun
- Chem, Vol. 5, Issue 1
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
CO 2 Electroreduction on Au/TiC: Enhanced Activity Due to Metal–Support Interaction
journal, February 2017
- Kim, Jun-Hyuk; Woo, Hyunje; Choi, Jihwan
- ACS Catalysis, Vol. 7, Issue 3
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
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, Vol. 129, Issue 31
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
Opportunities and Challenges in Utilizing Metal-Modified Transition Metal Carbides as Low-Cost Electrocatalysts
journal, October 2017
- Tackett, Brian M.; Sheng, Wenchao; Chen, Jingguang G.
- Joule, Vol. 1, Issue 2
TEM Studies of Platinum Nanowires Fabricated in Mesoporous Silica MCM-41
journal, September 2000
- Liu, Zheng; Sakamoto, Yasuhiro; Ohsuna, Tetsu
- Angewandte Chemie, Vol. 112, Issue 17
Understanding of Electrochemical Mechanisms for CO 2 Capture and Conversion into Hydrocarbon Fuels in Transition-Metal Carbides (MXenes)
journal, September 2017
- Li, Neng; Chen, Xingzhu; Ong, Wee-Jun
- ACS Nano, Vol. 11, Issue 11
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
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
Works referencing / citing this record:
Coupling of Solar Energy and Thermal Energy for Carbon Dioxide Reduction: Status and Prospects
journal, February 2020
- Wang, Zhou-jun; Song, Hui; Liu, Huimin
- Angewandte Chemie International Edition
Intensified Electrocatalytic CO 2 Conversion in Pressure‐Tunable CO 2 ‐Expanded Electrolytes
journal, July 2019
- Shaughnessy, Charles I.; Sconyers, David J.; Kerr, Tyler A.
- ChemSusChem, Vol. 12, Issue 16
Kopplung von Solarenergie und Wärmeenergie zur Kohlendioxidreduktion: Aktueller Stand und Perspektiven
journal, February 2020
- Wang, Zhou‐jun; Song, Hui; Liu, Huimin
- Angewandte Chemie, Vol. 132, Issue 21