Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts
Abstract
Efficient, stable catalysts with high selectivity for a single product are essential if electroreduction of CO2 is to become a viable route to the synthesis of industrial feedstocks and fuels. A plasma oxidation pre-treatment of silver foil enhances the number of low-coordinated catalytically active sites, which dramatically lowers the overpotential and increases the activity of CO2 electroreduction to CO. At -0.6 V versus RHE more than 90 % Faradaic efficiency towards CO was achieved on a pre-oxidized silver foil. While transmission electron microscopy (TEM) and operando X-ray absorption spectroscopy showed that oxygen species can survive in the bulk of the catalyst during the reaction, quasi in situ X-ray photoelectron spectroscopy showed that the surface is metallic under reaction conditions. Finally, DFT calculations reveal that the defect-rich surface of the plasma-oxidized silver foils in the presence of local electric fields drastically decrease the overpotential of CO2 electroreduction.
- Authors:
-
- Ruhr Univ., Bochum (Germany). Dept. of Physics; Univ. of Central Florida, Orlando, FL (United States). Dept. of Physics
- Ruhr Univ., Bochum (Germany). Dept. of Physics
- Copenhagen Univ. (Denmark). Dept. of Chemistry
- Univ. of Pittsburgh, PA (United States). Chemical and Petroleum Engineering and Physics
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
- Univ. of Copenhagen (Denmark). Dept. of Chemistry
- Ruhr Univ., Bochum (Germany). Dept. of Physics; Fritz-Haber Inst. of the Max Planck Society, Berlin (Germany). Dept. of Interface Science
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE
- OSTI Identifier:
- 1433976
- Alternate Identifier(s):
- OSTI ID: 1374678
- Report Number(s):
- BNL-203511-2018-JAAM
Journal ID: ISSN 1433-7851
- Grant/Contract Number:
- SC0012704; AC02-06CH11357; FG02-03ER15476; CHEM 1213182; CHE-1534630; 03SF0523C; ERC-725915; CF15-0165
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 56; Journal Issue: 38; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Mistry, Hemma, Choi, Yong‐Wook, Bagger, Alexander, Scholten, Fabian, Bonifacio, Cecile S., Sinev, Ilya, Divins, Nuria J., Zegkinoglou, Ioannis, Jeon, Hyo Sang, Kisslinger, Kim, Stach, Eric A., Yang, Judith C., Rossmeisl, Jan, and Roldan Cuenya, Beatriz. Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts. United States: N. p., 2017.
Web. doi:10.1002/anie.201704613.
Mistry, Hemma, Choi, Yong‐Wook, Bagger, Alexander, Scholten, Fabian, Bonifacio, Cecile S., Sinev, Ilya, Divins, Nuria J., Zegkinoglou, Ioannis, Jeon, Hyo Sang, Kisslinger, Kim, Stach, Eric A., Yang, Judith C., Rossmeisl, Jan, & Roldan Cuenya, Beatriz. Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts. United States. https://doi.org/10.1002/anie.201704613
Mistry, Hemma, Choi, Yong‐Wook, Bagger, Alexander, Scholten, Fabian, Bonifacio, Cecile S., Sinev, Ilya, Divins, Nuria J., Zegkinoglou, Ioannis, Jeon, Hyo Sang, Kisslinger, Kim, Stach, Eric A., Yang, Judith C., Rossmeisl, Jan, and Roldan Cuenya, Beatriz. Thu .
"Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts". United States. https://doi.org/10.1002/anie.201704613. https://www.osti.gov/servlets/purl/1433976.
@article{osti_1433976,
title = {Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts},
author = {Mistry, Hemma and Choi, Yong‐Wook and Bagger, Alexander and Scholten, Fabian and Bonifacio, Cecile S. and Sinev, Ilya and Divins, Nuria J. and Zegkinoglou, Ioannis and Jeon, Hyo Sang and Kisslinger, Kim and Stach, Eric A. and Yang, Judith C. and Rossmeisl, Jan and Roldan Cuenya, Beatriz},
abstractNote = {Efficient, stable catalysts with high selectivity for a single product are essential if electroreduction of CO2 is to become a viable route to the synthesis of industrial feedstocks and fuels. A plasma oxidation pre-treatment of silver foil enhances the number of low-coordinated catalytically active sites, which dramatically lowers the overpotential and increases the activity of CO2 electroreduction to CO. At -0.6 V versus RHE more than 90 % Faradaic efficiency towards CO was achieved on a pre-oxidized silver foil. While transmission electron microscopy (TEM) and operando X-ray absorption spectroscopy showed that oxygen species can survive in the bulk of the catalyst during the reaction, quasi in situ X-ray photoelectron spectroscopy showed that the surface is metallic under reaction conditions. Finally, DFT calculations reveal that the defect-rich surface of the plasma-oxidized silver foils in the presence of local electric fields drastically decrease the overpotential of CO2 electroreduction.},
doi = {10.1002/anie.201704613},
journal = {Angewandte Chemie (International Edition)},
number = 38,
volume = 56,
place = {United States},
year = {Thu Aug 10 00:00:00 EDT 2017},
month = {Thu Aug 10 00:00:00 EDT 2017}
}
Web of Science
Works referenced in this record:
CO2 Reduction at Low Overpotential on Cu Electrodes Resulting from the Reduction of Thick Cu2O Films
journal, April 2012
- Li, Christina W.; Kanan, Matthew W.
- Journal of the American Chemical Society, Vol. 134, Issue 17, p. 7231-7234
Nanostructured Metallic Electrocatalysts for Carbon Dioxide Reduction
journal, October 2014
- Lu, Qi; Rosen, Jonathan; Jiao, Feng
- ChemCatChem, Vol. 7, Issue 1
Electrochemical reduction of carbon dioxides to carbon monoxide at a gold electrode in aqueous potassium hydrogen carbonate
journal, January 1987
- Hori, Yoshio; Murata, Akira; Kikuchi, Katsuhei
- Journal of the Chemical Society, Chemical Communications, Issue 10
Tuning of Silver Catalyst Mesostructure Promotes Selective Carbon Dioxide Conversion into Fuels
journal, November 2016
- Yoon, Youngmin; Hall, Anthony Shoji; Surendranath, Yogesh
- Angewandte Chemie, Vol. 128, Issue 49
Enhancement in carbon dioxide activity and stability on nanostructured silver electrode and the role of oxygen
journal, January 2016
- Jee, Michael Shincheon; Jeon, Hyo Sang; Kim, Cheonghee
- Applied Catalysis B: Environmental, Vol. 180
Insight into Electrochemical CO 2 Reduction on Surface-Molecule-Mediated Ag Nanoparticles
journal, December 2016
- Kim, Cheonghee; Eom, Taedaehyeong; Jee, Michael Shincheon
- ACS Catalysis, Vol. 7, Issue 1
Liquid-metal electrode to enable ultra-low temperature sodium–beta alumina batteries for renewable energy storage
journal, August 2014
- Lu, Xiaochuan; Li, Guosheng; Kim, Jin Y.
- Nature Communications, Vol. 5, Issue 1
Mechanistic Insights into the Electrochemical Reduction of CO 2 to CO on Nanostructured Ag Surfaces
journal, June 2015
- Rosen, Jonathan; Hutchings, Gregory S.; Lu, Qi
- ACS Catalysis, Vol. 5, Issue 7
Status and perspectives of CO2 conversion into fuels and chemicals by catalytic, photocatalytic and electrocatalytic processes
journal, January 2013
- Kondratenko, Evgenii V.; Mul, Guido; Baltrusaitis, Jonas
- Energy & Environmental Science, Vol. 6, Issue 11
Stable surface oxygen on nanostructured silver for efficient CO2 electroreduction
journal, June 2017
- Jee, Michael Shincheon; Kim, Haeri; Jeon, Hyo Sang
- Catalysis Today, Vol. 288
Tuning of Silver Catalyst Mesostructure Promotes Selective Carbon Dioxide Conversion into Fuels
journal, November 2016
- Yoon, Youngmin; Hall, Anthony Shoji; Surendranath, Yogesh
- Angewandte Chemie International Edition, Vol. 55, Issue 49
Nanoparticle Silver Catalysts That Show Enhanced Activity for Carbon Dioxide Electrolysis
journal, January 2013
- Salehi-Khojin, Amin; Jhong, Huei-Ru Molly; Rosen, Brian A.
- The Journal of Physical Chemistry C, Vol. 117, Issue 4
Thickness- and Particle-Size-Dependent Electrochemical Reduction of Carbon Dioxide on Thin-Layer Porous Silver Electrodes
journal, January 2016
- Zhang, Lin; Wang, Zhiyong; Mehio, Nada
- ChemSusChem, Vol. 9, Issue 5
Carbon Foam Decorated with Silver Nanoparticles for Electrochemical CO 2 Conversion
journal, January 2017
- Ma, Sichao; Liu, Jianfeng; Sasaki, Kazunari
- Energy Technology, Vol. 5, Issue 6
Selective and Efficient Reduction of Carbon Dioxide to Carbon Monoxide on Oxide-Derived Nanostructured Silver Electrocatalysts
journal, July 2016
- Ma, Ming; Trześniewski, Bartek J.; Xie, Jie
- Angewandte Chemie, Vol. 128, Issue 33
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
Enhanced CO selectivity and stability for electrocatalytic reduction of CO 2 on electrodeposited nanostructured porous Ag electrode
journal, September 2016
- Wang, Hua; Han, Zhenzhen; Zhang, Libo
- Journal of CO2 Utilization, Vol. 15
Selective CO 2 reduction on a polycrystalline Ag electrode enhanced by anodization treatment
journal, January 2015
- Zhou, Li Qin; Ling, Chen; Jones, Michael
- Chemical Communications, Vol. 51, Issue 100
Electric Field Effects in Electrochemical CO 2 Reduction
journal, September 2016
- Chen, Leanne D.; Urushihara, Makoto; Chan, Karen
- ACS Catalysis, Vol. 6, Issue 10
Insights into the electrocatalytic reduction of CO 2 on metallic silver surfaces
journal, January 2014
- Hatsukade, Toru; Kuhl, Kendra P.; Cave, Etosha R.
- Phys. Chem. Chem. Phys., Vol. 16, Issue 27
Effect of Chloride Anions on the Synthesis and Enhanced Catalytic Activity of Silver Nanocoral Electrodes for CO 2 Electroreduction
journal, August 2015
- Hsieh, Yu-Chi; Senanayake, Sanjaya D.; Zhang, Yu
- ACS Catalysis, Vol. 5, Issue 9
Monitoring the Chemical State of Catalysts for CO 2 Electroreduction: An In Operando Study
journal, November 2015
- Dutta, Abhijit; Kuzume, Akiyoshi; Rahaman, Motiar
- ACS Catalysis, Vol. 5, Issue 12
Selective and Efficient Reduction of Carbon Dioxide to Carbon Monoxide on Oxide-Derived Nanostructured Silver Electrocatalysts
journal, July 2016
- Ma, Ming; Trześniewski, Bartek J.; Xie, Jie
- Angewandte Chemie International Edition, Vol. 55, Issue 33
Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene
journal, June 2016
- Mistry, Hemma; Varela, Ana Sofia; Bonifacio, Cecile S.
- Nature Communications, Vol. 7, Issue 1
Insights into an autonomously formed oxygen-evacuated Cu 2 O electrode for the selective production of C 2 H 4 from CO 2
journal, January 2015
- Kim, Dahee; Lee, Seunghwa; Ocon, Joey D.
- Physical Chemistry Chemical Physics, Vol. 17, Issue 2
Calculated Phase Diagrams for the Electrochemical Oxidation and Reduction of Water over Pt(111)
journal, November 2006
- Rossmeisl, Jan; Nørskov, Jens K.; Taylor, Christopher D.
- The Journal of Physical Chemistry B, Vol. 110, Issue 43
Silver Supported on Titania as an Active Catalyst for Electrochemical Carbon Dioxide Reduction
journal, January 2014
- Ma , Sichao; Lan , Yangchun; Perez, Gaby M. J.
- ChemSusChem, Vol. 7, Issue 3
Prospects of CO2 Utilization via Direct Heterogeneous Electrochemical Reduction
journal, December 2010
- Whipple, Devin T.; Kenis, Paul J. A.
- The Journal of Physical Chemistry Letters, Vol. 1, Issue 24, p. 3451-3458
Tin Oxide Dependence of the CO 2 Reduction Efficiency on Tin Electrodes and Enhanced Activity for Tin/Tin Oxide Thin-Film Catalysts
journal, January 2012
- Chen, Yihong; Kanan, Matthew W.
- Journal of the American Chemical Society, Vol. 134, Issue 4
Aqueous CO 2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles
journal, November 2012
- Chen, Yihong; Li, Christina W.; Kanan, Matthew W.
- Journal of the American Chemical Society, Vol. 134, Issue 49
Achieving Selective and Efficient Electrocatalytic Activity for CO 2 Reduction Using Immobilized Silver Nanoparticles
journal, October 2015
- Kim, Cheonghee; Jeon, Hyo Sang; Eom, Taedaehyeong
- Journal of the American Chemical Society, Vol. 137, Issue 43
Subsurface Oxygen in Oxide-Derived Copper Electrocatalysts for Carbon Dioxide Reduction
journal, December 2016
- Eilert, André; Cavalca, Filippo; Roberts, F. Sloan
- The Journal of Physical Chemistry Letters, Vol. 8, Issue 1
Works referencing / citing this record:
An overview on the recent developments of Ag-based electrodes in the electrochemical reduction of CO 2 to CO
journal, January 2020
- Mahyoub, Samah A.; Qaraah, Fahim A.; Chen, Chengzhen
- Sustainable Energy & Fuels, Vol. 4, Issue 1
Metal-based heterogeneous electrocatalysts for reduction of carbon dioxide and nitrogen: mechanisms, recent advances and perspective
journal, January 2018
- Zhou, Jun-Hao; Zhang, Ya-Wen
- Reaction Chemistry & Engineering, Vol. 3, Issue 5
Hohe elektromagnetische Feldverstärkung in nanotubularen TiO 2 -Elektroden
journal, May 2018
- Öner, Ibrahim Halil; Querebillo, Christine Joy; David, Christin
- Angewandte Chemie, Vol. 130, Issue 24
A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO 2 to Value‐Added Chemicals and Fuel
journal, November 2019
- Daiyan, Rahman; Saputera, Wibawa Hendra; Masood, Hassan
- Advanced Energy Materials, Vol. 10, Issue 11
A Br − anion adsorbed porous Ag nanowire film: in situ electrochemical preparation and application toward efficient CO 2 electroreduction to CO with high selectivity
journal, January 2018
- Qiu, Weibin; Liang, Ruping; Luo, Yonglan
- Inorganic Chemistry Frontiers, Vol. 5, Issue 9
Progress in development of electrocatalyst for CO 2 conversion to selective CO production
journal, March 2020
- Nguyen, Dang Le Tri; Kim, Younghye; Hwang, Yun Jeong
- Carbon Energy, Vol. 2, Issue 1
Nitrogen-carbon layer coated nickel nanoparticles for efficient electrocatalytic reduction of carbon dioxide
journal, March 2019
- Tan, Dongxing; Cui, Chaonan; Shi, Jinbiao
- Nano Research, Vol. 12, Issue 5
Partially Oxidized Palladium Nanodots for Enhanced Electrocatalytic Carbon Dioxide Reduction
journal, August 2018
- Lu, Hui; Zhang, Le; Zhong, Ju Hua
- Chemistry - An Asian Journal, Vol. 13, Issue 19
Reordering d Orbital Energies of Single‐Site Catalysts for CO 2 Electroreduction
journal, September 2019
- Han, Jianyu; An, Pengfei; Liu, Shuhu
- Angewandte Chemie International Edition, Vol. 58, Issue 36
Boosting CO 2 electroreduction over silver nanowires modified by wet-chemical sulfidation and subsequent electrochemical de-sulfidation
journal, January 2019
- Hu, Liang; Zhang, Yicheng; Han, Weiqiang
- New Journal of Chemistry, Vol. 43, Issue 8
A Graphene‐Supported Single‐Atom FeN 5 Catalytic Site for Efficient Electrochemical CO 2 Reduction
journal, September 2019
- Zhang, Huinian; Li, Jing; Xi, Shibo
- Angewandte Chemie, Vol. 131, Issue 42
Iodide-derived nanostructured silver promotes selective and efficient carbon dioxide conversion into carbon monoxide
journal, January 2018
- Zhang, Ya; Ji, Lei; Qiu, Weibin
- Chemical Communications, Vol. 54, Issue 21
Cu x Ni y alloy nanoparticles embedded in a nitrogen–carbon network for efficient conversion of carbon dioxide
journal, January 2019
- Tan, Dongxing; Zhang, Jianling; Cheng, Xiuyan
- Chemical Science, Vol. 10, Issue 16
A Review of Recent Advances of Dielectric Barrier Discharge Plasma in Catalysis
journal, October 2019
- Li, Ju; Ma, Cunhua; Zhu, Shengjie
- Nanomaterials, Vol. 9, Issue 10
Facet Sensitivity of Capping Ligand-Free Ag Crystals in CO 2 Electrochemical Reduction to CO
journal, October 2018
- Yang, Min; Zhang, Jiazhou; Cao, Yongyong
- ChemCatChem, Vol. 10, Issue 22
Catalytic Hydrogen Production by Janus CuAg Nanostructures
journal, April 2018
- Zhang, Jin; Shao, Qi; Wang, Pengtang
- ChemNanoMat, Vol. 4, Issue 5
Rapid precipitation-reduction synthesis of carbon-supported silver for efficient oxygen reduction reaction in alkaline solution
journal, July 2019
- Cai, Shijin; Jin, Jutao; Qiao, Xiaochang
- Journal of Solid State Electrochemistry, Vol. 23, Issue 8
A Graphene‐Supported Single‐Atom FeN 5 Catalytic Site for Efficient Electrochemical CO 2 Reduction
journal, October 2019
- Zhang, Huinian; Li, Jing; Xi, Shibo
- Angewandte Chemie International Edition, Vol. 58, Issue 42
Dramatic differences in carbon dioxide adsorption and initial steps of reduction between silver and copper
journal, April 2019
- Ye, Yifan; Yang, Hao; Qian, Jin
- Nature Communications, Vol. 10, Issue 1
Understanding Selective Reduction of CO 2 to CO on Modified Carbon Electrocatalysts
journal, May 2018
- Jung, Hyejin; Lee, Si Young; Won, Da Hye
- ChemElectroChem, Vol. 5, Issue 12
Reordering d Orbital Energies of Single‐Site Catalysts for CO 2 Electroreduction
journal, July 2019
- Han, Jianyu; An, Pengfei; Liu, Shuhu
- Angewandte Chemie, Vol. 131, Issue 36
Plasma-Assisted Synthesis and Surface Modification of Electrode Materials for Renewable Energy
journal, February 2018
- Dou, Shuo; Tao, Li; Wang, Ruilun
- Advanced Materials, Vol. 30, Issue 21
Rational Design of Ag‐Based Catalysts for the Electrochemical CO 2 Reduction to CO: A Review
journal, December 2019
- Sun, Dalei; Xu, Xiaomin; Qin, Yanling
- ChemSusChem, Vol. 13, Issue 1
1D/2D nitrogen-doped carbon nanorod arrays/ultrathin carbon nanosheets: outstanding catalysts for the highly efficient electroreduction of CO 2 to CO
journal, January 2019
- Zhu, Ying; Lv, Kuilin; Wang, Xingpu
- Journal of Materials Chemistry A, Vol. 7, Issue 24
Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels
journal, September 2019
- Birdja, Yuvraj Y.; Pérez-Gallent, Elena; Figueiredo, Marta C.
- Nature Energy, Vol. 4, Issue 9
Operando EXAFS study reveals presence of oxygen in oxide-derived silver catalysts for electrochemical CO 2 reduction
journal, January 2019
- Firet, Nienke J.; Blommaert, Marijn A.; Burdyny, Thomas
- Journal of Materials Chemistry A, Vol. 7, Issue 6
Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products
journal, March 2019
- Gao, Dunfeng; Arán-Ais, Rosa M.; Jeon, Hyo Sang
- Nature Catalysis, Vol. 2, Issue 3
Recent Advances in Electrochemical CO 2 -to-CO Conversion on Heterogeneous Catalysts
journal, August 2018
- Zheng, Tingting; Jiang, Kun; Wang, Haotian
- Advanced Materials, Vol. 30, Issue 48
Understanding activity and selectivity of metal-nitrogen-doped carbon catalysts for electrochemical reduction of CO2
journal, October 2017
- Ju, Wen; Bagger, Alexander; Hao, Guang-Ping
- Nature Communications, Vol. 8, Issue 1
Colloidal silver diphosphide (AgP2) nanocrystals as low overpotential catalysts for CO2 reduction to tunable syngas
journal, December 2019
- Li, Hui; Wen, Peng; Itanze, Dominique S.
- Nature Communications, Vol. 10, Issue 1
High Electromagnetic Field Enhancement of TiO 2 Nanotube Electrodes
journal, May 2018
- Öner, Ibrahim Halil; Querebillo, Christine Joy; David, Christin
- Angewandte Chemie International Edition, Vol. 57, Issue 24
Operando Insight into the Correlation between the Structure and Composition of CuZn Nanoparticles and Their Selectivity for the Electrochemical CO 2 Reduction
journal, November 2019
- Jeon, Hyo Sang; Timoshenko, Janis; Scholten, Fabian
- Journal of the American Chemical Society, Vol. 141, Issue 50
Understanding activity and selectivity of metal-nitrogen-doped carbon catalysts for electrochemical reduction of CO2
journal, October 2017
- Ju, Wen; Bagger, Alexander; Hao, Guang-Ping
- Nature Communications, Vol. 8, Issue 1
Dramatic differences in carbon dioxide adsorption and initial steps of reduction between silver and copper
journal, April 2019
- Ye, Yifan; Yang, Hao; Qian, Jin
- Nature Communications, Vol. 10, Issue 1
A Review of Recent Advances of Dielectric Barrier Discharge Plasma in Catalysis
journal, October 2019
- Li, Ju; Ma, Cunhua; Zhu, Shengjie
- Nanomaterials, Vol. 9, Issue 10