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

Wang, Jiajun; Kattel, Shyam; Hawxhurst, Christopher J.; Lee, Ji Hoon; Tackett, Brian M.; Chang, Kuan; Rui, Ning; Liu, Chang ‐Jun; Chen, Jingguang G.

doi:10.1002/ange.201900781

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

Journal Article · Mon Mar 18 00:00:00 EDT 2019 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.201900781· OSTI ID:1542779

Wang, Jiajun ^[1]; Kattel, Shyam ^[2]; Hawxhurst, Christopher J. ^[3]; Lee, Ji Hoon ^[3]; Tackett, Brian M. ^[3]; Chang, Kuan ^[3]; Rui, Ning ^[4]; Liu, Chang ‐Jun ^[4]; ^[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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704

OSTI ID:: 1542779

Alternate ID(s):: OSTI ID: 1504298

Report Number(s):: BNL-211861-2019-JAAM

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 19 Vol. 131; ISSN 0044-8249

Publisher:: German Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (42)

TEM Studies of Platinum Nanowires Fabricated in Mesoporous Silica MCM-41 Liu, Zheng; Sakamoto, Yasuhiro; Ohsuna, Tetsu Angewandte Chemie, Vol. 112, Issue 17 https://doi.org/10.1002/1521-3757(20000901)112:17<3237::AID-ANGE3237>3.0.CO;2-7	journal	September 2000
TEM Studies of Platinum Nanowires Fabricated in Mesoporous Silica MCM-41 Liu, Zheng; Sakamoto, Yasuhiro; Ohsuna, Tetsu Angewandte Chemie, Vol. 39, Issue 17 https://doi.org/10.1002/1521-3773(20000901)39:17<3107::AID-ANIE3107>3.0.CO;2-J	journal	September 2000
Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles Lee, Ji Hoon; Kattel, Shyam; Xie, Zhenhua Advanced Functional Materials, Vol. 28, Issue 45 https://doi.org/10.1002/adfm.201804762	journal	September 2018
Achieving the Widest Range of Syngas Proportions at High Current Density over Cadmium Sulfoselenide Nanorods in CO ₂ Electroreduction He, Rong; Zhang, An; Ding, Yilun Advanced Materials, Vol. 30, Issue 7 https://doi.org/10.1002/adma.201705872	journal	January 2018
Shape-Controlled CO ₂ Electrochemical Reduction on Nanosized Pd Hydride Cubes and Octahedra Zhu, Wenlei; Kattel, Shyam; Jiao, Feng Advanced Energy Materials, Vol. 9, Issue 9 https://doi.org/10.1002/aenm.201802840	journal	January 2019
Multiple Phases of Molybdenum Carbide as Electrocatalysts for the Hydrogen Evolution Reaction Wan, Cheng; Regmi, Yagya N.; Leonard, Brian M. Angewandte Chemie, Vol. 126, Issue 25 https://doi.org/10.1002/ange.201402998	journal	May 2014
Understanding of Strain Effects in the Electrochemical Reduction of CO ₂ : Using Pd Nanostructures as an Ideal Platform Huang, Hongwen; Jia, Huanhuan; Liu, Zhao Angewandte Chemie, Vol. 129, Issue 13 https://doi.org/10.1002/ange.201612617	journal	February 2017
Carbon Dioxide Electroreduction into Syngas Boosted by a Partially Delocalized Charge in Molybdenum Sulfide Selenide Alloy Monolayers Xu, Jiaqi; Li, Xiaodong; Liu, Wei Angewandte Chemie, Vol. 129, Issue 31 https://doi.org/10.1002/ange.201704928	journal	June 2017
Exclusive Formation of Formic Acid from CO ₂ Electroreduction by a Tunable Pd-Sn Alloy Bai, Xiaofang; Chen, Wei; Zhao, Chengcheng Angewandte Chemie, Vol. 129, Issue 40 https://doi.org/10.1002/ange.201707098	journal	August 2017
Dynamic Changes in the Structure, Chemical State and Catalytic Selectivity of Cu Nanocubes during CO ₂ Electroreduction: Size and Support Effects Grosse, Philipp; Gao, Dunfeng; Scholten, Fabian Angewandte Chemie, Vol. 130, Issue 21 https://doi.org/10.1002/ange.201802083	journal	April 2018
Multiple Phases of Molybdenum Carbide as Electrocatalysts for the Hydrogen Evolution Reaction Wan, Cheng; Regmi, Yagya N.; Leonard, Brian M. Angewandte Chemie International Edition, Vol. 53, Issue 25 https://doi.org/10.1002/anie.201402998	journal	May 2014
Understanding of Strain Effects in the Electrochemical Reduction of CO ₂ : Using Pd Nanostructures as an Ideal Platform Huang, Hongwen; Jia, Huanhuan; Liu, Zhao Angewandte Chemie International Edition, Vol. 56, Issue 13 https://doi.org/10.1002/anie.201612617	journal	February 2017
Carbon Dioxide Electroreduction into Syngas Boosted by a Partially Delocalized Charge in Molybdenum Sulfide Selenide Alloy Monolayers Xu, Jiaqi; Li, Xiaodong; Liu, Wei Angewandte Chemie International Edition, Vol. 56, Issue 31 https://doi.org/10.1002/anie.201704928	journal	June 2017
Exclusive Formation of Formic Acid from CO ₂ Electroreduction by a Tunable Pd-Sn Alloy Bai, Xiaofang; Chen, Wei; Zhao, Chengcheng Angewandte Chemie International Edition, Vol. 56, Issue 40 https://doi.org/10.1002/anie.201707098	journal	August 2017
Dynamic Changes in the Structure, Chemical State and Catalytic Selectivity of Cu Nanocubes during CO ₂ Electroreduction: Size and Support Effects Grosse, Philipp; Gao, Dunfeng; Scholten, Fabian Angewandte Chemie International Edition, Vol. 57, Issue 21 https://doi.org/10.1002/anie.201802083	journal	April 2018
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 Ong, Wee-Jun; Putri, Lutfi Kurnianditia; Tan, Yoong-Chuen Nano Research, Vol. 10, Issue 5 https://doi.org/10.1007/s12274-016-1391-4	journal	February 2017
Reactions of synthesis gas Wender, Irving Fuel Processing Technology, Vol. 48, Issue 3 https://doi.org/10.1016/S0378-3820(96)01048-X	journal	September 1996
Surface and Heterointerface Engineering of 2D MXenes and Their Nanocomposites: Insights into Electro- and Photocatalysis Peng, Jiahe; Chen, Xingzhu; Ong, Wee-Jun Chem, Vol. 5, Issue 1 https://doi.org/10.1016/j.chempr.2018.08.037	journal	January 2019
Theoretical prediction and experimental verification of low loading of platinum on titanium carbide as low-cost and stable electrocatalysts Kimmel, Yannick C.; Yang, Leerang; Kelly, Thomas G. Journal of Catalysis, Vol. 312 https://doi.org/10.1016/j.jcat.2014.02.002	journal	April 2014
Opportunities and Challenges in Utilizing Metal-Modified Transition Metal Carbides as Low-Cost Electrocatalysts Tackett, Brian M.; Sheng, Wenchao; Chen, Jingguang G. Joule, Vol. 1, Issue 2 https://doi.org/10.1016/j.joule.2017.07.002	journal	October 2017
Active Sites of Au and Ag Nanoparticle Catalysts for CO ₂ Electroreduction to CO Back, Seoin; Yeom, Min Sun; Jung, Yousung ACS Catalysis, Vol. 5, Issue 9 https://doi.org/10.1021/acscatal.5b00462	journal	August 2015
Understanding the Low-Overpotential Production of CH ₄ from CO ₂ on Mo ₂ C Catalysts Kim, Seok Ki; Zhang, Yin-Jia; Bergstrom, Helen ACS Catalysis, Vol. 6, Issue 3 https://doi.org/10.1021/acscatal.5b02424	journal	February 2016
CO ₂ Electroreduction on Au/TiC: Enhanced Activity Due to Metal–Support Interaction Kim, Jun-Hyuk; Woo, Hyunje; Choi, Jihwan ACS Catalysis, Vol. 7, Issue 3 https://doi.org/10.1021/acscatal.6b03706	journal	February 2017
TiC- and TiN-Supported Single-Atom Catalysts for Dramatic Improvements in CO ₂ Electrochemical Reduction to CH ₄ Back, Seoin; Jung, Yousung ACS Energy Letters, Vol. 2, Issue 5 https://doi.org/10.1021/acsenergylett.7b00152	journal	April 2017
Understanding of Electrochemical Mechanisms for CO ₂ Capture and Conversion into Hydrocarbon Fuels in Transition-Metal Carbides (MXenes) Li, Neng; Chen, Xingzhu; Ong, Wee-Jun ACS Nano, Vol. 11, Issue 11 https://doi.org/10.1021/acsnano.7b03738	journal	September 2017
A New Class of Electrocatalysts for Hydrogen Production from Water Electrolysis: Metal Monolayers Supported on Low-Cost Transition Metal Carbides Esposito, Daniel V.; Hunt, Sean T.; Kimmel, Yannick C. Journal of the American Chemical Society, Vol. 134, Issue 6 https://doi.org/10.1021/ja208656v	journal	February 2012
Exceptional Size-Dependent Activity Enhancement in the Electroreduction of CO ₂ over Au Nanoparticles Mistry, Hemma; Reske, Rulle; Zeng, Zhenhua Journal of the American Chemical Society, Vol. 136, Issue 47 https://doi.org/10.1021/ja508879j	journal	November 2014
Grain-Boundary-Dependent CO ₂ Electroreduction Activity Feng, Xiaofeng; Jiang, Kaili; Fan, Shoushan Journal of the American Chemical Society, Vol. 137, Issue 14 https://doi.org/10.1021/ja5130513	journal	April 2015
Enhancing CO ₂ Electroreduction with the Metal–Oxide Interface Gao, Dunfeng; Zhang, Yi; Zhou, Zhiwen Journal of the American Chemical Society, Vol. 139, Issue 16 https://doi.org/10.1021/jacs.7b00102	journal	April 2017
Temperature- and Pressure-Dependent Hydrogen Concentration in Supported PdH _x Nanoparticles by Pd K-Edge X-ray Absorption Spectroscopy Bugaev, Aram L.; Guda, Alexander A.; Lomachenko, Kirill A. The Journal of Physical Chemistry C, Vol. 118, Issue 19 https://doi.org/10.1021/jp500734p	journal	May 2014
Departures from the Adsorption Energy Scaling Relations for Metal Carbide Catalysts Michalsky, Ronald; Zhang, Yin-Jia; Medford, Andrew J. The Journal of Physical Chemistry C, Vol. 118, Issue 24 https://doi.org/10.1021/jp503756g	journal	June 2014
A selective and efficient electrocatalyst for carbon dioxide reduction Lu, Qi; Rosen, Jonathan; Zhou, Yang Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4242	journal	January 2014
Combining CO2 reduction with propane oxidative dehydrogenation over bimetallic catalysts Gomez, Elaine; Kattel, Shyam; Yan, Binhang Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-03793-w	journal	April 2018
A review of catalysts for the electroreduction of carbon dioxide to produce low-carbon fuels Qiao, Jinli; Liu, Yuyu; Hong, Feng Chem. Soc. Rev., Vol. 43, Issue 2 https://doi.org/10.1039/C3CS60323G	journal	January 2014
Recycling of carbon dioxide to methanol and derived products – closing the loop Goeppert, Alain; Czaun, Miklos; Jones, John-Paul Chem. Soc. Rev., Vol. 43, Issue 23 https://doi.org/10.1039/C4CS00122B	journal	January 2014
Reactions of water and C1 molecules on carbide and metal-modified carbide surfaces Wan, Weiming; Tackett, Brian M.; Chen, Jingguang G. Chemical Society Reviews, Vol. 46, Issue 7 https://doi.org/10.1039/C6CS00862C	journal	January 2017
Electrochemical reduction of CO ₂ to synthesis gas with controlled CO/H ₂ ratios Sheng, Wenchao; Kattel, Shyam; Yao, Siyu Energy & Environmental Science, Vol. 10, Issue 5 https://doi.org/10.1039/C7EE00071E	journal	January 2017
Hydride phase formation in carbon supported palladium nanoparticle electrodes investigated using in situ EXAFS and XRD Rose, Abigail; Maniguet, Stephanie; Mathew, Rebecca J. Physical Chemistry Chemical Physics, Vol. 5, Issue 15 https://doi.org/10.1039/b302956e	journal	January 2003
Fuel production from CO2 using solar-thermal energy: system level analysis Kim, Jiyong; Johnson, Terry A.; Miller, James E. Energy & Environmental Science, Vol. 5, Issue 9 https://doi.org/10.1039/c2ee21798h	journal	January 2012
Role of Strain and Ligand Effects in the Modification of the Electronic and Chemical Properties of Bimetallic Surfaces Kitchin, J. R.; Nørskov, J. K.; Barteau, M. A. Physical Review Letters, Vol. 93, Issue 15 https://doi.org/10.1103/PhysRevLett.93.156801	journal	October 2004
Self-assembly of noble metal monolayers on transition metal carbide nanoparticle catalysts Hunt, S. T.; Milina, M.; Alba-Rubio, A. C. Science, Vol. 352, Issue 6288 https://doi.org/10.1126/science.aad8471	journal	May 2016
Selective increase in CO ₂ electroreduction activity at grain-boundary surface terminations Mariano, Ruperto G.; McKelvey, Kim; White, Henry S. Science, Vol. 358, Issue 6367 https://doi.org/10.1126/science.aao3691	journal	November 2017

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO2 electroreduction
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