Highly dispersed, single-site copper catalysts for the electroreduction of CO2 to methane
Abstract
In this study, pyrolyzing Cu(II) precursors absorbed on carbon black gave an eletrocatalytic material for the electroreduction of CO2. Controlled potential electrolysis and GC analysis revealed an unexpected selectivity towards methane even in alkaline media, with a methane Faradaic efficiency as high as 42%, a partial current density of 100 mA/cm2 (at –1 V vs. RHE) and a methane/ethylene ratio of 4:1. XPS, EXAFS, and EDX mapping results indicate a single-site Cu(I) center as the catalytically active site. The limited size of the active sites is believed to be crucial for the preferential formation of methane over ethylene.
- Authors:
-
[2]
- Univ. of Illinois at Urbana-Champaign, IL (United States)
- Univ. of Illinois at Urbana-Champaign, IL (United States); Kyushu Univ., Fukuoka (Japan)
- Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE; National Science Foundation (NSF); Ministry of Education, Culture, Sports, Science, and Technology of Japan (MEXT)
- OSTI Identifier:
- 1831425
- Grant/Contract Number:
- AC02-06CH11357; CHE-1309731; WPI-I2CNER
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Electroanalytical Chemistry
- Additional Journal Information:
- Journal Volume: 875; Journal ID: ISSN 1572-6657
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 electroreduction; single-site catalysts; copper; methane
Citation Formats
Zhang, Teng, Verma, Sumit, Kim, Soojeong, Fister, Tim T., Kenis, Paul J.A., and Gewirth, Andrew A. Highly dispersed, single-site copper catalysts for the electroreduction of CO2 to methane. United States: N. p., 2020.
Web. doi:10.1016/j.jelechem.2020.113862.
Zhang, Teng, Verma, Sumit, Kim, Soojeong, Fister, Tim T., Kenis, Paul J.A., & Gewirth, Andrew A. Highly dispersed, single-site copper catalysts for the electroreduction of CO2 to methane. United States. https://doi.org/10.1016/j.jelechem.2020.113862
Zhang, Teng, Verma, Sumit, Kim, Soojeong, Fister, Tim T., Kenis, Paul J.A., and Gewirth, Andrew A. Thu .
"Highly dispersed, single-site copper catalysts for the electroreduction of CO2 to methane". United States. https://doi.org/10.1016/j.jelechem.2020.113862. https://www.osti.gov/servlets/purl/1831425.
@article{osti_1831425,
title = {Highly dispersed, single-site copper catalysts for the electroreduction of CO2 to methane},
author = {Zhang, Teng and Verma, Sumit and Kim, Soojeong and Fister, Tim T. and Kenis, Paul J.A. and Gewirth, Andrew A.},
abstractNote = {In this study, pyrolyzing Cu(II) precursors absorbed on carbon black gave an eletrocatalytic material for the electroreduction of CO2. Controlled potential electrolysis and GC analysis revealed an unexpected selectivity towards methane even in alkaline media, with a methane Faradaic efficiency as high as 42%, a partial current density of 100 mA/cm2 (at –1 V vs. RHE) and a methane/ethylene ratio of 4:1. XPS, EXAFS, and EDX mapping results indicate a single-site Cu(I) center as the catalytically active site. The limited size of the active sites is believed to be crucial for the preferential formation of methane over ethylene.},
doi = {10.1016/j.jelechem.2020.113862},
journal = {Journal of Electroanalytical Chemistry},
number = ,
volume = 875,
place = {United States},
year = {Thu Jan 16 00:00:00 EST 2020},
month = {Thu Jan 16 00:00:00 EST 2020}
}
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Works referenced in this record:
The importance of surface morphology in controlling the selectivity of polycrystalline copper for CO2 electroreduction
journal, January 2012
- Tang, Wei; Peterson, Andrew A.; Varela, Ana Sofia
- Phys. Chem. Chem. Phys., Vol. 14, Issue 1
A Highly Selective Copper-Indium Bimetallic Electrocatalyst for the Electrochemical Reduction of Aqueous CO 2 to CO
journal, December 2014
- Rasul, Shahid; Anjum, Dalaver H.; Jedidi, Abdesslem
- Angewandte Chemie International Edition, Vol. 54, Issue 7
Electrochemical CO 2 Reduction to Hydrocarbons on a Heterogeneous Molecular Cu Catalyst in Aqueous Solution
journal, June 2016
- Weng, Zhe; Jiang, Jianbing; Wu, Yueshen
- Journal of the American Chemical Society, Vol. 138, Issue 26
Electroreduction of Carbon Dioxide to Hydrocarbons Using Bimetallic Cu–Pd Catalysts with Different Mixing Patterns
journal, December 2016
- Ma, Sichao; Sadakiyo, Masaaki; Heima, Minako
- Journal of the American Chemical Society, Vol. 139, Issue 1
Electrochemical Reduction of Carbon Dioxide to Hydrocarbons with High Faradaic Efficiency in LiOH/Methanol
journal, August 1999
- Kaneco, Satoshi; Iiba, Kenji; Suzuki, Syo-ko
- The Journal of Physical Chemistry B, Vol. 103, Issue 35
XANES, EXAFS and photocatalytic investigations on copper oxide nanoparticles and nanocomposites
journal, January 2015
- Sharma, Aditya; Varshney, Mayora; Park, Jaehun
- RSC Advances, Vol. 5, Issue 28
Recent Advances in Inorganic Heterogeneous Electrocatalysts for Reduction of Carbon Dioxide
journal, March 2016
- Zhu, Dong Dong; Liu, Jin Long; Qiao, Shi Zhang
- Advanced Materials, Vol. 28, Issue 18
Selective electro- or photo-reduction of carbon dioxide to formic acid using a Cu–Zn alloy catalyst
journal, January 2017
- Yin, Ge; Abe, Hideki; Kodiyath, Rajesh
- Journal of Materials Chemistry A, Vol. 5, Issue 24
Particle Size Effects in the Catalytic Electroreduction of CO 2 on Cu Nanoparticles
journal, May 2014
- Reske, Rulle; Mistry, Hemma; Behafarid, Farzad
- Journal of the American Chemical Society, Vol. 136, Issue 19
Electrochemical reduction of CO2 at copper single crystal Cu(S)-[n(111)×(111)] and Cu(S)-[n(110)×(100)] electrodes
journal, September 2002
- Takahashi, Ichiro; Koga, Osamu; Hoshi, Nagahiro
- Journal of Electroanalytical Chemistry, Vol. 533, Issue 1-2, p. 135-143
Controllable Hydrocarbon Formation from the Electrochemical Reduction of CO 2 over Cu Nanowire Arrays
journal, April 2016
- Ma, Ming; Djanashvili, Kristina; Smith, Wilson A.
- Angewandte Chemie International Edition, Vol. 55, Issue 23
A Gross-Margin Model for Defining Technoeconomic Benchmarks in the Electroreduction of CO 2
journal, June 2016
- Verma, Sumit; Kim, Byoungsu; Jhong, Huei-Ru “Molly”
- ChemSusChem, Vol. 9, Issue 15
PRODUCTION OF CO AND CH 4 IN ELECTROCHEMICAL REDUCTION OF CO 2 AT METAL ELECTRODES IN AQUEOUS HYDROGENCARBONATE SOLUTION
journal, November 1985
- Hori, Yoshio; Kikuchi, Katsuhei; Suzuki, Shin
- Chemistry Letters, Vol. 14, Issue 11
Selective Formation of C2 Compounds from Electrochemical Reduction of CO 2 at a Series of Copper Single Crystal Electrodes
journal, January 2002
- Hori, Yoshio; Takahashi, Ichiro; Koga, Osamu
- The Journal of Physical Chemistry B, Vol. 106, Issue 1
Electrochemical reduction of carbon dioxide at various series of copper single crystal electrodes
journal, May 2003
- Hori, Y.; Takahashi, I.; Koga, O.
- Journal of Molecular Catalysis A: Chemical, Vol. 199, Issue 1-2, p. 39-47
Production of Methane and Ethylene in Electrochemical Reduction of Carbon Dioxide at Copper Electrode in Aqueous Hydrogencarbonate Solution
journal, June 1986
- Hori, Yoshio; Kikuchi, Katsuhei; Murata, Akira
- Chemistry Letters, Vol. 15, Issue 6
Electrochemical Reduction of CO2 to CH3OH at Copper Oxide Surfaces
journal, January 2011
- Le, M.; Ren, M.; Zhang, Z.
- Journal of The Electrochemical Society, Vol. 158, Issue 5
Formation of hydrocarbons in the electrochemical reduction of carbon dioxide at a copper electrode in aqueous solution
journal, January 1989
- Hori, Yoshio; Murata, Akira; Takahashi, Ryutaro
- Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 85, Issue 8
Metal–organic framework-mediated strategy for enhanced methane production on copper nanoparticles in electrochemical CO2 reduction
journal, May 2019
- Kim, Mun Kyoung; Kim, Hyeok Joo; Lim, Hyungseob
- Electrochimica Acta, Vol. 306
Polymer-supported CuPd nanoalloy as a synergistic catalyst for electrocatalytic reduction of carbon dioxide to methane
journal, December 2015
- Zhang, Sheng; Kang, Peng; Bakir, Mohammed
- Proceedings of the National Academy of Sciences, Vol. 112, Issue 52
Quantum Mechanical Screening of Single-Atom Bimetallic Alloys for the Selective Reduction of CO 2 to C 1 Hydrocarbons
journal, October 2016
- Cheng, Mu-Jeng; Clark, Ezra L.; Pham, Hieu H.
- ACS Catalysis, Vol. 6, Issue 11
High Selectivity for Ethylene from Carbon Dioxide Reduction over Copper Nanocube Electrocatalysts
journal, February 2015
- Roberts, F. Sloan; Kuhl, Kendra P.; Nilsson, Anders
- Angewandte Chemie International Edition, Vol. 54, Issue 17
Electrochemical CO 2 reduction on Cu 2 O-derived copper nanoparticles: controlling the catalytic selectivity of hydrocarbons
journal, January 2014
- Kas, Recep; Kortlever, Ruud; Milbrat, Alexander
- Phys. Chem. Chem. Phys., Vol. 16, Issue 24
Efficient High Rate Carbon Dioxide Reduction to Methane and Ethylene at in situ Electrodeposited Copper Electrode
journal, September 1987
- Cook, Ronald L.; MacDuff, Robert C.; Sammells, Anthony F.
- Journal of The Electrochemical Society, Vol. 134, Issue 9
Electrocatalytic CO2 Conversion to Oxalate by a Copper Complex
journal, January 2010
- Angamuthu, R.; Byers, P.; Lutz, M.
- Science, Vol. 327, Issue 5963
Cu–Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO 2 to CO
journal, April 2016
- Sarfraz, Saad; Garcia-Esparza, Angel T.; Jedidi, Abdesslem
- ACS Catalysis, Vol. 6, Issue 5
Single-Atom Catalysts: Synthetic Strategies and Electrochemical Applications
journal, July 2018
- Chen, Yuanjun; Ji, Shufang; Chen, Chen
- Joule, Vol. 2, Issue 7
Nanoporous Copper Films by Additive-Controlled Electrodeposition: CO 2 Reduction Catalysis
journal, April 2017
- Hoang, Thao T. H.; Ma, Sichao; Gold, Jake I.
- ACS Catalysis, Vol. 7, Issue 5
Design of Alloy Electrocatalysts for CO[sub 2] Reduction
journal, January 1991
- Watanabe, Masahiro
- Journal of The Electrochemical Society, Vol. 138, Issue 11
Electrocatalytic Reduction of Carbon Dioxide by the Binuclear Copper Complex [Cu2(6-(diphenylphosphino-2,2'-bipyridyl)2(MeCN)2][PF6]2
journal, October 1994
- Haines, Raymond J.; Wittrig, Rebecca E.; Kubiak, Clifford P.
- Inorganic Chemistry, Vol. 33, Issue 21
High-Selectivity Electrochemical Conversion of CO 2 to Ethanol using a Copper Nanoparticle/N-Doped Graphene Electrode
journal, September 2016
- Song, Yang; Peng, Rui; Hensley, Dale K.
- ChemistrySelect, Vol. 1, Issue 19
Pulsed Electroreduction of CO[sub 2] on Cu-Ag Alloy Electrodes
journal, January 2000
- Ishimaru, S.; Shiratsuchi, R.; Nogami, G.
- Journal of The Electrochemical Society, Vol. 147, Issue 5
Density functional theory calculations of XPS binding energy shift for nitrogen-containing graphene-like structures
journal, January 2013
- Artyushkova, K.; Kiefer, B.; Halevi, B.
- Chemical Communications, Vol. 49, Issue 25
Selective Electrochemical Reduction of Carbon Dioxide to Ethylene and Ethanol on Copper(I) Oxide Catalysts
journal, March 2015
- Ren, Dan; Deng, Yilin; Handoko, Albertus Denny
- ACS Catalysis, Vol. 5, Issue 5
Structure-Sensitive CO 2 Electroreduction to Hydrocarbons on Ultrathin 5-fold Twinned Copper Nanowires
journal, January 2017
- Li, Yifan; Cui, Fan; Ross, Michael B.
- Nano Letters, Vol. 17, Issue 2
Electrochemical Reduction of CO 2 at Intentionally Oxidized Copper Electrodes
journal, November 1991
- Frese, Karl W.
- Journal of The Electrochemical Society, Vol. 138, Issue 11
Tailoring Copper Nanocrystals towards C 2 Products in Electrochemical CO 2 Reduction
journal, April 2016
- Loiudice, Anna; Lobaccaro, Peter; Kamali, Esmail A.
- Angewandte Chemie International Edition, Vol. 55, Issue 19
CO 2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface
journal, May 2018
- Dinh, Cao-Thang; Burdyny, Thomas; Kibria, Md Golam
- Science, Vol. 360, Issue 6390
Enhanced Electrochemical Methanation of Carbon Dioxide with a Dispersible Nanoscale Copper Catalyst
journal, September 2014
- Manthiram, Karthish; Beberwyck, Brandon J.; Alivisatos, A. Paul
- Journal of the American Chemical Society, Vol. 136, Issue 38
Composition dependent activity of Cu–Pt nanocrystals for electrochemical reduction of CO 2
journal, January 2015
- Guo, Xin; Zhang, Yuxia; Deng, Chen
- Chemical Communications, Vol. 51, Issue 7
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
Electrochemical and Surface Studies of Carbon Dioxide Reduction to Methane and Ethylene at Copper Electrodes in Aqueous Solutions
journal, January 1989
- DeWulf, David W.
- Journal of The Electrochemical Society, Vol. 136, Issue 6, p. 1686-1691
Synergistic geometric and electronic effects for electrochemical reduction of carbon dioxide using gold–copper bimetallic nanoparticles
journal, September 2014
- Kim, Dohyung; Resasco, Joaquin; Yu, Yi
- Nature Communications, Vol. 5, Issue 1
Reduction of CO2 and CO to methane on Cu foil electrodes
journal, April 1988
- Kim, J. J.; Summers, D. P.; Frese, K. W.
- Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 245, Issue 1-2, p. 223-244
High Rate Gas Phase CO[sub 2] Reduction to Ethylene and Methane Using Gas Diffusion Electrodes
journal, January 1990
- Cook, Ronald L.
- Journal of The Electrochemical Society, Vol. 137, Issue 2
Greenhouse Gas Emissions, Energy Efficiency, and Cost of Synthetic Fuel Production Using Electrochemical CO 2 Conversion and the Fischer–Tropsch Process
journal, June 2016
- Li, Xuping; Anderson, Paul; Jhong, Huei-Ru Molly
- Energy & Fuels, Vol. 30, Issue 7
Metal organic frameworks derived single atom catalysts for electrocatalytic energy conversion
journal, March 2019
- Sun, Tingting; Xu, Lianbin; Wang, Dingsheng
- Nano Research, Vol. 12, Issue 9
Spectroscopic Observation of a Hydrogenated CO Dimer Intermediate During CO Reduction on Cu(100) Electrodes
journal, February 2017
- Pérez-Gallent, Elena; Figueiredo, Marta C.; Calle-Vallejo, Federico
- Angewandte Chemie International Edition, Vol. 56, Issue 13
Catalysts and Reaction Pathways for the Electrochemical Reduction of Carbon Dioxide
journal, September 2015
- Kortlever, Ruud; Shen, Jing; Schouten, Klaas Jan P.
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 20
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