Electrochemical CO2 Reduction Reaction over Cu Nanoparticles with Tunable Activity and Selectivity Mediated by Functional Groups in Polymeric Binder

Chang, Qiaowan; Lee, Ji Hoon; Liu, Yumeng; Xie, Zhenhua; Hwang, Sooyeon; Marinkovic, Nebojsa S.; Park, Ah-Hyung Alissa; Kattel, Shyam; Chen, Jingguang G.

doi:10.1021/jacsau.1c00487

Title: Electrochemical CO₂ Reduction Reaction over Cu Nanoparticles with Tunable Activity and Selectivity Mediated by Functional Groups in Polymeric Binder

Abstract

Electrochemical carbon dioxide reduction reaction (CO₂RR) using copper (Cu)-based catalysts has received significant attention mainly because Cu is an element capable of producing hydrocarbons and oxygenates. One possible way to control the CO₂RR performance at the electrode interface is by modifying catalysts with specific functional groups of different polymeric binders, which are necessary components in the process of electrode fabrication. However, the modification effect of the key functional groups on the CO₂RR activity and selectivity is poorly understood over Cu-based catalysts. In this work, the role of functional groups (e.g., -COOH and -CF₂ groups) in hydrophilic and hydrophobic polymeric binders on the CO₂RR of Cu-based catalysts is investigated using a combination of electrochemical measurements, in-situ characterization and density functional theory (DFT) calculations. DFT results reveal that functional groups influence the binding energies of key intermediates involved in both CO₂RR and the competing hydrogen evolution reaction, consistent with experimental observation of binder-dependent product distributions among formic acid, CO, CH₄, and H₂. This study provides a fundamental understanding that the selection of desired polymeric binders is a useful strategy for tuning the CO₂RR activity and selectivity.

Authors:

Chang, Qiaowan ^[1];

^[2]; Liu, Yumeng ^[1]; Xie, Zhenhua ^[3];

^[3]; Marinkovic, Nebojsa S. ^[1];

^[1]; Kattel, Shyam ^[4];

^[5]

Columbia Univ., New York, NY (United States)
Columbia Univ., New York, NY (United States); Kyungpook National Univ., Daegu (Korea, Republic of)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Florida A & M University, Tallahassee, FL (United States)
Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

Publication Date:: Thu Dec 09 00:00:00 EST 2021

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

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Research Foundation of Korea (NRF); China Scholarship Council

OSTI Identifier:: 1837207

Report Number(s):: BNL-222517-2021-JAAM
Journal ID: ISSN 2691-3704

Grant/Contract Number:: SC0012704; 1927336; ACI-1548562; NRF-2021R1G1A1092280; 201806010243

Resource Type:: Accepted Manuscript

Journal Name:: JACS Au

Additional Journal Information:: Journal Volume: 2; Journal Issue: 1; Journal ID: ISSN 2691-3704

Publisher:: ACS Publications

Country of Publication:: United States

Language:: English

Subject:: 25 ENERGY STORAGE; polymeric binders; functional groups; copper; carbon dioxide reduction; density functional theory

Citation Formats


                    Chang, Qiaowan, Lee, Ji Hoon, Liu, Yumeng, Xie, Zhenhua, Hwang, Sooyeon, Marinkovic, Nebojsa S., Park, Ah-Hyung Alissa, Kattel, Shyam, and Chen, Jingguang G. Electrochemical CO2 Reduction Reaction over Cu Nanoparticles with Tunable Activity and Selectivity Mediated by Functional Groups in Polymeric Binder.  United States: N. p., 2021. 
Web.  doi:10.1021/jacsau.1c00487.

Copy to clipboard


                    Chang, Qiaowan, Lee, Ji Hoon, Liu, Yumeng, Xie, Zhenhua, Hwang, Sooyeon, Marinkovic, Nebojsa S., Park, Ah-Hyung Alissa, Kattel, Shyam, & Chen, Jingguang G. Electrochemical CO2 Reduction Reaction over Cu Nanoparticles with Tunable Activity and Selectivity Mediated by Functional Groups in Polymeric Binder.  United States.  https://doi.org/10.1021/jacsau.1c00487

Copy to clipboard


                    Chang, Qiaowan, Lee, Ji Hoon, Liu, Yumeng, Xie, Zhenhua, Hwang, Sooyeon, Marinkovic, Nebojsa S., Park, Ah-Hyung Alissa, Kattel, Shyam, and Chen, Jingguang G. Thu .  
"Electrochemical CO2 Reduction Reaction over Cu Nanoparticles with Tunable Activity and Selectivity Mediated by Functional Groups in Polymeric Binder".  United States.  https://doi.org/10.1021/jacsau.1c00487.  https://www.osti.gov/servlets/purl/1837207.

Copy to clipboard


                    
@article{osti_1837207,

  title        = {Electrochemical CO2 Reduction Reaction over Cu Nanoparticles with Tunable Activity and Selectivity Mediated by Functional Groups in Polymeric Binder},

  author       = {Chang, Qiaowan and Lee, Ji Hoon and Liu, Yumeng and Xie, Zhenhua and Hwang, Sooyeon and Marinkovic, Nebojsa S. and Park, Ah-Hyung Alissa and Kattel, Shyam and Chen, Jingguang G.},

  abstractNote = {Electrochemical carbon dioxide reduction reaction (CO2RR) using copper (Cu)-based catalysts has received significant attention mainly because Cu is an element capable of producing hydrocarbons and oxygenates. One possible way to control the CO2RR performance at the electrode interface is by modifying catalysts with specific functional groups of different polymeric binders, which are necessary components in the process of electrode fabrication. However, the modification effect of the key functional groups on the CO2RR activity and selectivity is poorly understood over Cu-based catalysts. In this work, the role of functional groups (e.g., -COOH and -CF2 groups) in hydrophilic and hydrophobic polymeric binders on the CO2RR of Cu-based catalysts is investigated using a combination of electrochemical measurements, in-situ characterization and density functional theory (DFT) calculations. DFT results reveal that functional groups influence the binding energies of key intermediates involved in both CO2RR and the competing hydrogen evolution reaction, consistent with experimental observation of binder-dependent product distributions among formic acid, CO, CH4, and H2. This study provides a fundamental understanding that the selection of desired polymeric binders is a useful strategy for tuning the CO2RR activity and selectivity.},

  doi          = {10.1021/jacsau.1c00487},

  journal      = {JACS Au},

  number       = 1,

  volume       = 2,

  place        = {United States},

  year         = {Thu Dec 09 00:00:00 EST 2021},

  month        = {Thu Dec 09 00:00:00 EST 2021}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1021/jacsau.1c00487

Other availability

Search WorldCat to find libraries that may hold this journal

Save / Share:

Export Metadata

Save to My Library

Works referenced in this record:

Electrochemical CO₂ Reduction on Metal Electrodes
book, January 2008

Hori, Y.; Vayenas, Constantinos G.; White, Ralph E.
Modern Aspects of Electrochemistry, p. 89-189
DOI: 10.1007/978-0-387-49489-0_3

Electrochemical CO2 reduction: Electrocatalyst, reaction mechanism, and process engineering
journal, November 2016

Lu, Qi; Jiao, Feng
Nano Energy, Vol. 29
DOI: 10.1016/j.nanoen.2016.04.009

Electrocatalytic process of CO selectivity in electrochemical reduction of CO₂ at metal electrodes in aqueous media
journal, August 1994

Hori, Yoshio; Wakebe, Hidetoshi; Tsukamoto, Toshio
Electrochimica Acta, Vol. 39, Issue 11-12, p. 1833-1839
DOI: 10.1016/0013-4686(94)85172-7

A review of the aqueous electrochemical reduction of CO₂ to hydrocarbons at copper
journal, August 2006

Gattrell, M.; Gupta, N.; Co, A.
Journal of Electroanalytical Chemistry, Vol. 594, Issue 1, p. 1-19
DOI: 10.1016/j.jelechem.2006.05.013

New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces
journal, January 2012

Kuhl, Kendra P.; Cave, Etosha R.; Abram, David N.
Energy & Environmental Science, Vol. 5, Issue 5
DOI: 10.1039/c2ee21234j

Electrochemical Conversion of CO ₂ to Syngas with Palladium-Based Electrocatalysts
journal, July 2020

Tackett, Brian M.; Lee, Ji Hoon; Chen, Jingguang G.
Accounts of Chemical Research, Vol. 53, Issue 8
DOI: 10.1021/acs.accounts.0c00277

Nanostructured Materials for Heterogeneous Electrocatalytic CO ₂ Reduction and their Related Reaction Mechanisms
journal, July 2017

Zhang, Lei; Zhao, Zhi-Jian; Gong, Jinlong
Angewandte Chemie International Edition, Vol. 56, Issue 38
DOI: 10.1002/anie.201612214

How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels
journal, January 2010

Peterson, Andrew A.; Abild-Pedersen, Frank; Studt, Felix
Energy & Environmental Science, Vol. 3, Issue 9
DOI: 10.1039/c0ee00071j

Selectivity of CO 2 Reduction on Copper Electrodes: The Role of the Kinetics of Elementary Steps
journal, January 2013

Nie, Xiaowa; Esopi, Monica R.; Janik, Michael J.
Angewandte Chemie, Vol. 125, Issue 9
DOI: 10.1002/ange.201208320

Facet Dependence of CO ₂ Reduction Paths on Cu Electrodes
journal, December 2015

Luo, Wenjia; Nie, Xiaowa; Janik, Michael J.
ACS Catalysis, Vol. 6, Issue 1
DOI: 10.1021/acscatal.5b01967

Engineering Cu surfaces for the electrocatalytic conversion of CO ₂ : Controlling selectivity toward oxygenates and hydrocarbons
journal, May 2017

Hahn, Christopher; Hatsukade, Toru; Kim, Youn-Geun
Proceedings of the National Academy of Sciences, Vol. 114, Issue 23
DOI: 10.1073/pnas.1618935114

Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons
journal, July 2018

Zhou, Yansong; Che, Fanglin; Liu, Min
Nature Chemistry, Vol. 10, Issue 9
DOI: 10.1038/s41557-018-0092-x

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

Effect of mass transfer and kinetics in ordered Cu-mesostructures for electrochemical CO2 reduction
journal, September 2018

Song, Hakhyeon; Im, Mintaek; Song, Jun Tae
Applied Catalysis B: Environmental, Vol. 232
DOI: 10.1016/j.apcatb.2018.03.071

Scalable Production of Efficient Single-Atom Copper Decorated Carbon Membranes for CO ₂ Electroreduction to Methanol
journal, July 2019

Yang, Hengpan; Wu, Yu; Li, Guodong
Journal of the American Chemical Society, Vol. 141, Issue 32
DOI: 10.1021/jacs.9b04907

Highly selective palladium-copper bimetallic electrocatalysts for the electrochemical reduction of CO2 to CO
journal, September 2016

Yin, Zhen; Gao, Dunfeng; Yao, Siyu
Nano Energy, Vol. 27
DOI: 10.1016/j.nanoen.2016.06.035

Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts
journal, August 2019

Lee, Ji Hoon; Kattel, Shyam; Jiang, Zhao
Nature Communications, Vol. 10, Issue 1
DOI: 10.1038/s41467-019-11352-0

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
DOI: 10.1038/ncomms5948

Tunable Cu Enrichment Enables Designer Syngas Electrosynthesis from CO ₂
journal, June 2017

Ross, Michael B.; Dinh, Cao Thang; Li, Yifan
Journal of the American Chemical Society, Vol. 139, Issue 27
DOI: 10.1021/jacs.7b04892

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
DOI: 10.1021/jacs.6b10740

Catalyst–electrolyte interface chemistry for electrochemical CO ₂ reduction
journal, January 2020

Sa, Young Jin; Lee, Chan Woo; Lee, Si Young
Chemical Society Reviews, Vol. 49, Issue 18
DOI: 10.1039/D0CS00030B

Tuning the Catalytic Activity and Selectivity of Cu for CO ₂ Electroreduction in the Presence of Halides
journal, February 2016

Varela, Ana Sofia; Ju, Wen; Reier, Tobias
ACS Catalysis, Vol. 6, Issue 4
DOI: 10.1021/acscatal.5b02550

Hydrolysis of Electrolyte Cations Enhances the Electrochemical Reduction of CO ₂ over Ag and Cu
journal, September 2016

Singh, Meenesh R.; Kwon, Youngkook; Lum, Yanwei
Journal of the American Chemical Society, Vol. 138, Issue 39
DOI: 10.1021/jacs.6b07612

Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide
journal, August 2017

Resasco, Joaquin; Chen, Leanne D.; Clark, Ezra
Journal of the American Chemical Society, Vol. 139, Issue 32
DOI: 10.1021/jacs.7b06765

Activation of C2H4 reaction pathways in electrochemical CO2 reduction under low CO2 partial pressure
journal, September 2020

Song, Hakhyeon; Song, Jun Tae; Kim, Beomil
Applied Catalysis B: Environmental, Vol. 272
DOI: 10.1016/j.apcatb.2020.119049

Modulating Local CO2 Concentration as a General Strategy for Enhancing C−C Coupling in CO2 Electroreduction
journal, May 2020

Tan, Ying Chuan; Lee, Kelvin Berm; Song, Hakhyeon
Joule, Vol. 4, Issue 5
DOI: 10.1016/j.joule.2020.03.013

CO ₂ electrolysis to multicarbon products at activities greater than 1 A cm ⁻²
journal, February 2020

García de Arquer, F. Pelayo; Dinh, Cao-Thang; Ozden, Adnan
Science, Vol. 367, Issue 6478
DOI: 10.1126/science.aay4217

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
DOI: 10.1126/science.aas9100

Scalable strategy to fabricate single Cu atoms coordinated carbons for efficient electroreduction of CO2 to CO
journal, October 2020

Yang, Fangqi; Mao, Xinyu; Ma, Mingfeng
Carbon, Vol. 168
DOI: 10.1016/j.carbon.2020.06.088

Single-atom catalysis for electrochemical CO2 reduction
journal, April 2019

Jia, Mingwen; Fan, Qun; Liu, Shizhen
Current Opinion in Green and Sustainable Chemistry, Vol. 16
DOI: 10.1016/j.cogsc.2018.11.002

Cu-Pd alloy nanoparticles as highly selective catalysts for efficient electrochemical reduction of CO2 to CO
journal, June 2019

Mun, Yeongdong; Lee, Seunghyun; Cho, Ara
Applied Catalysis B: Environmental, Vol. 246
DOI: 10.1016/j.apcatb.2019.01.021

Direct Evidence of Local pH Change and the Role of Alkali Cation during CO ₂ Electroreduction in Aqueous Media
journal, January 2020

Zhang, Fen; Co, Anne C.
Angewandte Chemie International Edition, Vol. 59, Issue 4
DOI: 10.1002/anie.201912637

Electrochemical Conversion of CO ₂ to Syngas with Controllable CO/H ₂ Ratios over Co and Ni Single-Atom Catalysts
journal, January 2020

He, Qun; Liu, Daobin; Lee, Ji Hoon
Angewandte Chemie International Edition, Vol. 59, Issue 8
DOI: 10.1002/anie.201912719

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

Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO ₂ by Supporting Palladium on Metal Carbides
journal, April 2019

Wang, Jiajun; Kattel, Shyam; Hawxhurst, Christopher J.
Angewandte Chemie International Edition, Vol. 58, Issue 19
DOI: 10.1002/anie.201900781

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

Analysis of Soils and Minerals Using X-ray Absorption Spectroscopy
book, April 2015

Kelly, S. D.; Hesterberg, D.; Ravel, B.
Methods of Soil Analysis Part 5-Mineralogical Methods
DOI: 10.2136/sssabookser5.5.c14

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005

Ravel, B.; Newville, M.
Journal of Synchrotron Radiation, Vol. 12, Issue 4
DOI: 10.1107/S0909049505012719

Inhomogeneous Electron Gas
journal, November 1964

Hohenberg, P.; Kohn, W.
Physical Review, Vol. 136, Issue 3B, p. B864-B871
DOI: 10.1103/PhysRev.136.B864

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965

Kohn, W.; Sham, L. J.
Physical Review, Vol. 140, Issue 4A, p. A1133-A1138
DOI: 10.1103/PhysRev.140.A1133

Generalized Gradient Approximation Made Simple
journal, October 1996

Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
DOI: 10.1103/PhysRevLett.77.3865

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Kresse, G.; Furthmüller, J.
Computational Materials Science, Vol. 6, Issue 1, p. 15-50
DOI: 10.1016/0927-0256(96)00008-0

Ab initio molecular dynamics for open-shell transition metals
journal, November 1993

Kresse, G.; Hafner, J.
Physical Review B, Vol. 48, Issue 17
DOI: 10.1103/PhysRevB.48.13115

Projector augmented-wave method
journal, December 1994

Blöchl, P. E.
Physical Review B, Vol. 50, Issue 24, p. 17953-17979
DOI: 10.1103/PhysRevB.50.17953

A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010

Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
The Journal of Chemical Physics, Vol. 132, Issue 15
DOI: 10.1063/1.3382344

Erratum: Accurate and simple analytic representation of the electron-gas correlation energy [Phys. Rev. B 45, 13244 (1992)]
journal, August 2018

Perdew, John P.; Wang, Yue
Physical Review B, Vol. 98, Issue 7
DOI: 10.1103/PhysRevB.98.079904

Electrochemical CO ₂ Reduction: Classifying Cu Facets
journal, July 2019

Bagger, Alexander; Ju, Wen; Varela, Ana Sofia
ACS Catalysis, Vol. 9, Issue 9
DOI: 10.1021/acscatal.9b01899

Imaging heterogeneity and transport of degraded Nafion membranes
journal, January 2015

Shi, Wenqing; Baker, Lane A.
RSC Advances, Vol. 5, Issue 120
DOI: 10.1039/C5RA20291D

Enhancing performance of PEM fuel cells: Using the Au nanoplatelet/Nafion interface to enable CO oxidation under ambient conditions
journal, July 2016

Li, Hongfei; Pan, Cheng; Zhao, Sijia
Journal of Catalysis, Vol. 339
DOI: 10.1016/j.jcat.2016.03.031

Single-Atomic Cu with Multiple Oxygen Vacancies on Ceria for Electrocatalytic CO ₂ Reduction to CH ₄
journal, June 2018

Wang, Yifei; Chen, Zheng; Han, Peng
ACS Catalysis, Vol. 8, Issue 8
DOI: 10.1021/acscatal.8b01014

Recent Advances in CO ₂ Reduction Electrocatalysis on Copper
journal, June 2018

Raciti, David; Wang, Chao
ACS Energy Letters, Vol. 3, Issue 7
DOI: 10.1021/acsenergylett.8b00553

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
DOI: 10.1021/acs.jpclett.5b01559

Synthesis and Characterization of (Cu, S) Co-doped SnO ₂ for Electrocatalytic Reduction of CO ₂ to Formate at Low Overpotential
journal, March 2018

Hu, Xueyan; Yang, Huimin; Guo, Minmin
ChemElectroChem, Vol. 5, Issue 9
DOI: 10.1002/celc.201800104

Lattice-Hydride Mechanism in Electrocatalytic CO ₂ Reduction by Structurally Precise Copper-Hydride Nanoclusters
journal, July 2017

Tang, Qing; Lee, Yongjin; Li, Dai-Ying
Journal of the American Chemical Society, Vol. 139, Issue 28
DOI: 10.1021/jacs.7b05591

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

Insight into the Role of Surface Wettability in Electrocatalytic Hydrogen Evolution Reactions Using Light-Sensitive Nanotubular TiO2 Supported Pt Electrodes
journal, February 2017

Meng, Chenhui; Wang, Bing; Gao, Ziyue
Scientific Reports, Vol. 7, Issue 1
DOI: 10.1038/srep41825

Nitrogen and fluorine dual-doped porous graphene-nanosheets as efficient metal-free electrocatalysts for hydrogen-evolution in acidic media
journal, January 2017

Yue, Xin; Huang, Shangli; Jin, Yanshuo
Catalysis Science & Technology, Vol. 7, Issue 11
DOI: 10.1039/C7CY00384F

Bio-inspired hydrophobicity promotes CO2 reduction on a Cu surface
journal, August 2019

Wakerley, David; Lamaison, Sarah; Ozanam, François
Nature Materials, Vol. 18, Issue 11
DOI: 10.1038/s41563-019-0445-x

Electrocatalysis at Organic–Metal Interfaces: Identification of Structure–Reactivity Relationships for CO ₂ Reduction at Modified Cu Surfaces
journal, March 2019

Buckley, Aya K.; Lee, Michelle; Cheng, Tao
Journal of the American Chemical Society, Vol. 141, Issue 18
DOI: 10.1021/jacs.8b13655

Hydrophobic Copper Interfaces Boost Electroreduction of Carbon Dioxide to Ethylene in Water
journal, January 2021

Liang, Hong-Qing; Zhao, Siqi; Hu, Xin-Ming
ACS Catalysis, Vol. 11, Issue 2
DOI: 10.1021/acscatal.0c03766

Triple-phase electrocatalysis for the enhanced CO2 reduction to HCOOH on a hydrophobic surface
journal, February 2021

Yue, Pengtao; Fu, Qian; Li, Jun
Chemical Engineering Journal, Vol. 405
DOI: 10.1016/j.cej.2020.126975

Similar Records in DOE PAGES and OSTI.GOV collections:

Metal-Coordinated Phthalocyanines as Platform Molecules for Understanding Isolated Metal Sites in the Electrochemical Reduction of CO₂

Journal Article Chang, Qiaowan ; Liu, Yumeng ; Lee, Ju-Hyeon ; ... - Journal of the American Chemical Society

Single-atom catalysts (SACs) of non-precious transition metals (TMs) often show unique electrochemical performance, including the electrochemical carbon dioxide reduction reaction (CO₂RR). However, the inhomogeneity in their structures makes it difficult to directly compare SACs of different TM for their CO₂RR activity, selectivity, and reaction mechanisms. Here, the comparison of isolated TMs (Fe, Co, Ni, Cu, and Zn) is systematically investigated using a series of crystalline molecular catalysts, namely TM-coordinated phthalocyanines (TMPcs), to directly compare the intrinsic role of the TMs with identical local coordination environments on the CO₂RR performance. The combined experimental measurements, in situ characterization, and density functional theorymore »« less
https://doi.org/10.1021/jacs.2c06953

Full Text Available
Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles

Journal Article Lee, Ji Hoon ; Kattel, Shyam ; Xie, Zhenhua ; ... - Advanced Functional Materials

Electrochemical CO₂ reduction reaction (CO₂RR) is one of the promising strategies for converting CO₂ to value-added chemicals. Gold (Au) catalysts are considered to be the best benchmarking materials for CO₂RR to produce CO. In this work, the role of different functional groups of polymeric binders on CO₂RR over Au catalysts is systematically investigated by combined experimental measurements and density functional theory (DFT) calculations. Especially, it is revealed that the functional groups can play a role in suppressing the undesired hydrogen evolution reaction, the main competing reaction against CO₂RR, thus enabling more catalytic active sites to be available for CO₂RR andmore »« less
Cited by 61
https://doi.org/10.1002/adfm.201804762

Full Text Available
Promotional effect of surface hydroxyls on electrochemical reduction of CO₂ over SnO_x/Sn electrode

Journal Article Cui, Chaonan ; Han, Jinyu ; Zhu, Xinli ; ... - Journal of Catalysis

In this study, tin oxide (SnO_x) formation on tin-based electrode surfaces during CO₂ electrochemical reduction can have a significant impact on the activity and selectivity of the reaction. In the present study, density functional theory (DFT) calculations have been performed to understand the role of SnO_x in CO₂ reduction using a SnO monolayer on the Sn(112) surface as a model for SnO_x. Water molecules have been treated explicitly and considered actively participating in the reaction. The results showed that H₂O dissociates on the perfect SnO monolayer into two hydroxyl groups symmetrically on the surface. CO₂ energetically prefers to react withmore »« less
Cited by 89
https://doi.org/10.1016/j.jcat.2015.12.001

Full Text Available
Selective Electrocatalytic Reduction of CO₂ into CO at Small, Thiol-Capped Au/Cu Nanoparticles

Journal Article Kauffman, Douglas R. ; Alfonso, Dominic R. ; Tafen, De Nyago ; ... - Journal of Physical Chemistry. C

The electrochemical CO₂ reduction reaction (CO₂RR) is a promising approach for converting fossil fuel emissions into environmentally sustainable chemicals and fuels. The ability to control the surface structure of CO₂RR nanocatalysts provides an opportunity to tune product selectivity. Bimetallic gold–copper catalysts have been identified as emerging electrocatalyst candidates, but Cu incorporation typically lowers product selectivity compared with pure Au. Here we show sustained CO selectivity and activity up to 49% Cu content in small (<2 nm), thiol-capped Au/Cu nanoparticles (NPs). Bimetallic NPs containing 49% Cu selectivity converted CO₂ into CO with 100 ± 6% CO Faradaic efficiency and average massmore »« less
Cited by 37
https://doi.org/10.1021/acs.jpcc.8b06234

Full Text Available
Understanding Selectivity for the Electrochemical Reduction of Carbon Dioxide to Formic Acid and Carbon Monoxide on Metal Electrodes

Journal Article Feaster, Jeremy T. ; Shi, Chuan ; Cave, Etosha R. ; ... - ACS Catalysis

Increases in energy demand and in chemical production, together with the rise in CO₂ levels in the atmosphere, motivate the development of renewable energy sources. Electrochemical CO₂ reduction to fuels and chemicals is an appealing alternative to traditional pathways to fuels and chemicals due to its intrinsic ability to couple to solar and wind energy sources. Formate (HCOO^–) is a key chemical for many industries; however, greater understanding is needed regarding the mechanism and key intermediates for HCOO^– production. This work reports a joint experimental and theoretical investigation of the electrochemical reduction of CO₂ to HCOO^– on polycrystalline Sn surfaces,more »« less
Cited by 539
https://doi.org/10.1021/acscatal.7b00687

Full Text Available

Similar Records

Title: Electrochemical CO2 Reduction Reaction over Cu Nanoparticles with Tunable Activity and Selectivity Mediated by Functional Groups in Polymeric Binder

Abstract

Citation Formats

Electrochemical CO2 Reduction on Metal Electrodes book, January 2008

Electrochemical CO2 reduction: Electrocatalyst, reaction mechanism, and process engineering journal, November 2016

Electrocatalytic process of CO selectivity in electrochemical reduction of CO2 at metal electrodes in aqueous media journal, August 1994

A review of the aqueous electrochemical reduction of CO2 to hydrocarbons at copper journal, August 2006

New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces journal, January 2012

Electrochemical Conversion of CO 2 to Syngas with Palladium-Based Electrocatalysts journal, July 2020

Nanostructured Materials for Heterogeneous Electrocatalytic CO 2 Reduction and their Related Reaction Mechanisms journal, July 2017

How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels journal, January 2010

Selectivity of CO 2 Reduction on Copper Electrodes: The Role of the Kinetics of Elementary Steps journal, January 2013

Facet Dependence of CO 2 Reduction Paths on Cu Electrodes journal, December 2015

Engineering Cu surfaces for the electrocatalytic conversion of CO 2 : Controlling selectivity toward oxygenates and hydrocarbons journal, May 2017

Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons journal, July 2018

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

Effect of mass transfer and kinetics in ordered Cu-mesostructures for electrochemical CO2 reduction journal, September 2018

Scalable Production of Efficient Single-Atom Copper Decorated Carbon Membranes for CO 2 Electroreduction to Methanol journal, July 2019

Highly selective palladium-copper bimetallic electrocatalysts for the electrochemical reduction of CO2 to CO journal, September 2016

Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts journal, August 2019

Synergistic geometric and electronic effects for electrochemical reduction of carbon dioxide using gold–copper bimetallic nanoparticles journal, September 2014

Tunable Cu Enrichment Enables Designer Syngas Electrosynthesis from CO 2 journal, June 2017

Electroreduction of Carbon Dioxide to Hydrocarbons Using Bimetallic Cu–Pd Catalysts with Different Mixing Patterns journal, December 2016

Catalyst–electrolyte interface chemistry for electrochemical CO 2 reduction journal, January 2020

Tuning the Catalytic Activity and Selectivity of Cu for CO 2 Electroreduction in the Presence of Halides journal, February 2016

Hydrolysis of Electrolyte Cations Enhances the Electrochemical Reduction of CO 2 over Ag and Cu journal, September 2016

Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide journal, August 2017

Activation of C2H4 reaction pathways in electrochemical CO2 reduction under low CO2 partial pressure journal, September 2020

Modulating Local CO2 Concentration as a General Strategy for Enhancing C−C Coupling in CO2 Electroreduction journal, May 2020

CO 2 electrolysis to multicarbon products at activities greater than 1 A cm −2 journal, February 2020

CO 2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface journal, May 2018

Scalable strategy to fabricate single Cu atoms coordinated carbons for efficient electroreduction of CO2 to CO journal, October 2020

Single-atom catalysis for electrochemical CO2 reduction journal, April 2019

Cu-Pd alloy nanoparticles as highly selective catalysts for efficient electrochemical reduction of CO2 to CO journal, June 2019

Direct Evidence of Local pH Change and the Role of Alkali Cation during CO 2 Electroreduction in Aqueous Media journal, January 2020

Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single-Atom Catalysts journal, January 2020

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

Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO 2 by Supporting Palladium on Metal Carbides journal, April 2019

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

Analysis of Soils and Minerals Using X-ray Absorption Spectroscopy book, April 2015

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT journal, June 2005

Inhomogeneous Electron Gas journal, November 1964

Self-Consistent Equations Including Exchange and Correlation Effects journal, November 1965

Generalized Gradient Approximation Made Simple journal, October 1996

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal, July 1996

Ab initio molecular dynamics for open-shell transition metals journal, November 1993

Projector augmented-wave method journal, December 1994

A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu journal, April 2010

Erratum: Accurate and simple analytic representation of the electron-gas correlation energy [Phys. Rev. B 45, 13244 (1992)] journal, August 2018

Electrochemical CO 2 Reduction: Classifying Cu Facets journal, July 2019

Imaging heterogeneity and transport of degraded Nafion membranes journal, January 2015

Enhancing performance of PEM fuel cells: Using the Au nanoplatelet/Nafion interface to enable CO oxidation under ambient conditions journal, July 2016

Single-Atomic Cu with Multiple Oxygen Vacancies on Ceria for Electrocatalytic CO 2 Reduction to CH 4 journal, June 2018

Recent Advances in CO 2 Reduction Electrocatalysis on Copper journal, June 2018

Catalysts and Reaction Pathways for the Electrochemical Reduction of Carbon Dioxide journal, September 2015

Synthesis and Characterization of (Cu, S) Co-doped SnO 2 for Electrocatalytic Reduction of CO 2 to Formate at Low Overpotential journal, March 2018

Lattice-Hydride Mechanism in Electrocatalytic CO 2 Reduction by Structurally Precise Copper-Hydride Nanoclusters journal, July 2017

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

Insight into the Role of Surface Wettability in Electrocatalytic Hydrogen Evolution Reactions Using Light-Sensitive Nanotubular TiO2 Supported Pt Electrodes journal, February 2017

Nitrogen and fluorine dual-doped porous graphene-nanosheets as efficient metal-free electrocatalysts for hydrogen-evolution in acidic media journal, January 2017

Bio-inspired hydrophobicity promotes CO2 reduction on a Cu surface journal, August 2019

Electrocatalysis at Organic–Metal Interfaces: Identification of Structure–Reactivity Relationships for CO 2 Reduction at Modified Cu Surfaces journal, March 2019

Hydrophobic Copper Interfaces Boost Electroreduction of Carbon Dioxide to Ethylene in Water journal, January 2021

Triple-phase electrocatalysis for the enhanced CO2 reduction to HCOOH on a hydrophobic surface journal, February 2021

Title: Electrochemical CO₂ Reduction Reaction over Cu Nanoparticles with Tunable Activity and Selectivity Mediated by Functional Groups in Polymeric Binder

Electrochemical CO₂ Reduction on Metal Electrodes
book, January 2008

Electrochemical CO2 reduction: Electrocatalyst, reaction mechanism, and process engineering
journal, November 2016

Electrocatalytic process of CO selectivity in electrochemical reduction of CO₂ at metal electrodes in aqueous media
journal, August 1994

A review of the aqueous electrochemical reduction of CO₂ to hydrocarbons at copper
journal, August 2006

New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces
journal, January 2012

Electrochemical Conversion of CO ₂ to Syngas with Palladium-Based Electrocatalysts
journal, July 2020

Nanostructured Materials for Heterogeneous Electrocatalytic CO ₂ Reduction and their Related Reaction Mechanisms
journal, July 2017

How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels
journal, January 2010

Selectivity of CO 2 Reduction on Copper Electrodes: The Role of the Kinetics of Elementary Steps
journal, January 2013

Facet Dependence of CO ₂ Reduction Paths on Cu Electrodes
journal, December 2015

Engineering Cu surfaces for the electrocatalytic conversion of CO ₂ : Controlling selectivity toward oxygenates and hydrocarbons
journal, May 2017

Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons
journal, July 2018

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

Effect of mass transfer and kinetics in ordered Cu-mesostructures for electrochemical CO2 reduction
journal, September 2018

Scalable Production of Efficient Single-Atom Copper Decorated Carbon Membranes for CO ₂ Electroreduction to Methanol
journal, July 2019

Highly selective palladium-copper bimetallic electrocatalysts for the electrochemical reduction of CO2 to CO
journal, September 2016

Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts
journal, August 2019

Synergistic geometric and electronic effects for electrochemical reduction of carbon dioxide using gold–copper bimetallic nanoparticles
journal, September 2014

Tunable Cu Enrichment Enables Designer Syngas Electrosynthesis from CO ₂
journal, June 2017

Electroreduction of Carbon Dioxide to Hydrocarbons Using Bimetallic Cu–Pd Catalysts with Different Mixing Patterns
journal, December 2016

Catalyst–electrolyte interface chemistry for electrochemical CO ₂ reduction
journal, January 2020

Tuning the Catalytic Activity and Selectivity of Cu for CO ₂ Electroreduction in the Presence of Halides
journal, February 2016

Hydrolysis of Electrolyte Cations Enhances the Electrochemical Reduction of CO ₂ over Ag and Cu
journal, September 2016

Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide
journal, August 2017

Activation of C2H4 reaction pathways in electrochemical CO2 reduction under low CO2 partial pressure
journal, September 2020

Modulating Local CO2 Concentration as a General Strategy for Enhancing C−C Coupling in CO2 Electroreduction
journal, May 2020

CO ₂ electrolysis to multicarbon products at activities greater than 1 A cm ⁻²
journal, February 2020

CO ₂ electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface
journal, May 2018

Scalable strategy to fabricate single Cu atoms coordinated carbons for efficient electroreduction of CO2 to CO
journal, October 2020

Single-atom catalysis for electrochemical CO2 reduction
journal, April 2019

Cu-Pd alloy nanoparticles as highly selective catalysts for efficient electrochemical reduction of CO2 to CO
journal, June 2019

Direct Evidence of Local pH Change and the Role of Alkali Cation during CO ₂ Electroreduction in Aqueous Media
journal, January 2020

Electrochemical Conversion of CO ₂ to Syngas with Controllable CO/H ₂ Ratios over Co and Ni Single-Atom Catalysts
journal, January 2020

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

Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO ₂ by Supporting Palladium on Metal Carbides
journal, April 2019

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

Analysis of Soils and Minerals Using X-ray Absorption Spectroscopy
book, April 2015

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005

Inhomogeneous Electron Gas
journal, November 1964

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965

Generalized Gradient Approximation Made Simple
journal, October 1996

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Ab initio molecular dynamics for open-shell transition metals
journal, November 1993

Projector augmented-wave method
journal, December 1994

A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010

Erratum: Accurate and simple analytic representation of the electron-gas correlation energy [Phys. Rev. B 45, 13244 (1992)]
journal, August 2018

Electrochemical CO ₂ Reduction: Classifying Cu Facets
journal, July 2019

Imaging heterogeneity and transport of degraded Nafion membranes
journal, January 2015

Enhancing performance of PEM fuel cells: Using the Au nanoplatelet/Nafion interface to enable CO oxidation under ambient conditions
journal, July 2016

Single-Atomic Cu with Multiple Oxygen Vacancies on Ceria for Electrocatalytic CO ₂ Reduction to CH ₄
journal, June 2018

Recent Advances in CO ₂ Reduction Electrocatalysis on Copper
journal, June 2018

Catalysts and Reaction Pathways for the Electrochemical Reduction of Carbon Dioxide
journal, September 2015

Synthesis and Characterization of (Cu, S) Co-doped SnO ₂ for Electrocatalytic Reduction of CO ₂ to Formate at Low Overpotential
journal, March 2018

Lattice-Hydride Mechanism in Electrocatalytic CO ₂ Reduction by Structurally Precise Copper-Hydride Nanoclusters
journal, July 2017

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

Insight into the Role of Surface Wettability in Electrocatalytic Hydrogen Evolution Reactions Using Light-Sensitive Nanotubular TiO2 Supported Pt Electrodes
journal, February 2017

Nitrogen and fluorine dual-doped porous graphene-nanosheets as efficient metal-free electrocatalysts for hydrogen-evolution in acidic media
journal, January 2017

Bio-inspired hydrophobicity promotes CO2 reduction on a Cu surface
journal, August 2019

Electrocatalysis at Organic–Metal Interfaces: Identification of Structure–Reactivity Relationships for CO ₂ Reduction at Modified Cu Surfaces
journal, March 2019

Hydrophobic Copper Interfaces Boost Electroreduction of Carbon Dioxide to Ethylene in Water
journal, January 2021

Triple-phase electrocatalysis for the enhanced CO2 reduction to HCOOH on a hydrophobic surface
journal, February 2021