Scalable Gas Diffusion Electrode Fabrication for Electrochemical CO2 Reduction Using Physical Vapor Deposition Methods

Jeng, Emily; Qi, Zhen; Kashi, Ajay R.; Hunegnaw, Sara; Huo, Ziyang; Miller, John S.; Bayu Aji, Leonardus B.; Ko, Byung Hee; Shin, Haeun; Ma, Sichao; Kuhl, Kendra P.; Jiao, Feng; Biener, Juergen

doi:10.1021/acsami.1c17860

Scalable Gas Diffusion Electrode Fabrication for Electrochemical CO₂ Reduction Using Physical Vapor Deposition Methods

Journal Article · Sun Feb 06 23:00:00 EST 2022 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.1c17860· OSTI ID:1860768

Jeng, Emily ^[1]; ^[2]; Kashi, Ajay R. ^[3]; Hunegnaw, Sara ^[3]; Huo, Ziyang ^[3]; Miller, John S. ^[2]; Bayu Aji, Leonardus B. ^[2]; Ko, Byung Hee ^[1]; Shin, Haeun ^[1]; Ma, Sichao ^[3]; Kuhl, Kendra P. ^[3]; ^[1]; ^[2]

Univ. of Delaware, Newark, DE (United States). Center for Catalytic Science and Technology
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Twelve Incorporated, Berkeley, CA (United States)

Electrochemical CO₂ reduction (ECR) promises the replacement of fossil fuels as the source of feedstock chemicals and seasonal storage of renewable energy. While much progress has been made in catalyst development and electrochemical reactor design, few studies have addressed the effect of catalyst integration on device performance. Using a microfluidic gas diffusion electrolyzer, we systematically studied the effect of thickness and the morphology of electron beam (EB) and magnetron-sputtered (MS) Cu catalyst coatings on ECR performance. We observed that EB-Cu outperforms MS-Cu in current density, selectivity, and energy efficiency, with 400 nm thick catalyst coatings performing the best. Additionally, the superior performance of EB-Cu catalysts is assigned to their faceted surface morphology and sharper Cu/gas diffusion layer interface, which increases their hydrophobicity. Tests in a large-scale zero-gap electrolyzer yielded similar product selectivity distributions with an ethylene Faradaic efficiency of 39% at 200 mA/cm², demonstrating the scalability for industrial ECR applications.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Manufacturing Office; Total American Services, Inc.

Grant/Contract Number:: AC52-07NA27344; AC02-05CH11231

OSTI ID:: 1860768

Report Number(s):: LLNL-JRNL-821645; 1033655

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 6 Vol. 14; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (47)

A Highly Porous Copper Electrocatalyst for Carbon Dioxide Reduction Lv, Jing-Jing; Jouny, Matthew; Luc, Wesley Advanced Materials, Vol. 30, Issue 49 https://doi.org/10.1002/adma.201803111	journal	October 2018
The Effects of Catalyst Layer Deposition Methodology on Electrode Performance Jhong, Huei-Ru “Molly”; Brushett, Fikile R.; Kenis, Paul J. A. Advanced Energy Materials, Vol. 3, Issue 5 https://doi.org/10.1002/aenm.201200759	journal	February 2013
Tailoring Copper Nanocrystals towards C ₂ Products in Electrochemical CO ₂ Reduction Loiudice, Anna; Lobaccaro, Peter; Kamali, Esmail A. Angewandte Chemie International Edition, Vol. 55, Issue 19 https://doi.org/10.1002/anie.201601582	journal	April 2016
Nanostructured Metallic Electrocatalysts for Carbon Dioxide Reduction Lu, Qi; Rosen, Jonathan; Jiao, Feng ChemCatChem, Vol. 7, Issue 1 https://doi.org/10.1002/cctc.201402669	journal	October 2014
Electrocatalytic process of CO selectivity in electrochemical reduction of CO₂ at metal electrodes in aqueous media Hori, Yoshio; Wakebe, Hidetoshi; Tsukamoto, Toshio Electrochimica Acta, Vol. 39, Issue 11-12, p. 1833-1839 https://doi.org/10.1016/0013-4686(94)85172-7	journal	August 1994
Algorithms for the rapid simulation of Rutherford backscattering spectra Doolittle, Lawrence R. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 9, Issue 3 https://doi.org/10.1016/0168-583X(85)90762-1	journal	June 1985
The use of magnetron arrays for depositing large-area oxide coatings Jankowski, A.; McKernan, M.; Chesser, J. Surface and Coatings Technology, Vol. 133-134 https://doi.org/10.1016/S0257-8972(00)00903-8	journal	November 2000
Magnetron sputtering on large scale substrates: an overview on the state of the art Kukla, Reiner Surface and Coatings Technology, Vol. 93, Issue 1 https://doi.org/10.1016/S0257-8972(97)00018-2	journal	August 1997
Selective electrochemical CO2 reduction on Cu-Pd heterostructure Xie, Jia-Fang; Chen, Jie-Jie; Huang, Yu-Xi Applied Catalysis B: Environmental, Vol. 270 https://doi.org/10.1016/j.apcatb.2020.118864	journal	August 2020
Native oxidation of ultra high purity Cu bulk and thin films Iijima, J.; Lim, J. -W.; Hong, S. -H. Applied Surface Science, Vol. 253, Issue 5 https://doi.org/10.1016/j.apsusc.2006.05.063	journal	December 2006
Electrochemical conversion of CO2 to useful chemicals: current status, remaining challenges, and future opportunities Jhong, Huei-Ru “Molly”; Ma, Sichao; Kenis, Paul JA Current Opinion in Chemical Engineering, Vol. 2, Issue 2 https://doi.org/10.1016/j.coche.2013.03.005	journal	May 2013
Effects of Nafion impregnation using inkjet printing for membrane electrode assemblies in polymer electrolyte membrane fuel cells Wang, Zhuqing; Nagao, Yuki Electrochimica Acta, Vol. 129 https://doi.org/10.1016/j.electacta.2014.02.133	journal	May 2014
What Should We Make with CO2 and How Can We Make It? Bushuyev, Oleksandr S.; De Luna, Phil; Dinh, Cao Thang Joule, Vol. 2, Issue 5 https://doi.org/10.1016/j.joule.2017.09.003	journal	May 2018
Inkjet printing of carbon supported platinum 3-D catalyst layers for use in fuel cells Taylor, André D.; Kim, Edward Y.; Humes, Virgil P. Journal of Power Sources, Vol. 171, Issue 1 https://doi.org/10.1016/j.jpowsour.2007.01.024	journal	September 2007
Electrochemical CO2 reduction: Electrocatalyst, reaction mechanism, and process engineering Lu, Qi; Jiao, Feng Nano Energy, Vol. 29 https://doi.org/10.1016/j.nanoen.2016.04.009	journal	November 2016
Selectivity roadmap for electrochemical CO2 reduction on copper-based alloy catalysts Zhi, Xing; Jiao, Yan; Zheng, Yao Nano Energy, Vol. 71 https://doi.org/10.1016/j.nanoen.2020.104601	journal	May 2020
Recent progress on hybrid electrocatalysts for efficient electrochemical CO2 reduction Zhang, Baohua; Jiang, Yinzhu; Gao, Mingxia Nano Energy, Vol. 80 https://doi.org/10.1016/j.nanoen.2020.105504	journal	February 2021
Perspectives on oblique angle deposition of thin films: From fundamentals to devices Barranco, Angel; Borras, Ana; Gonzalez-Elipe, Agustin R. Progress in Materials Science, Vol. 76 https://doi.org/10.1016/j.pmatsci.2015.06.003	journal	March 2016
Electrochemical reduction of carbon dioxide at various series of copper single crystal electrodes Hori, Y.; Takahashi, I.; Koga, O. Journal of Molecular Catalysis A: Chemical, Vol. 199, Issue 1-2, p. 39-47 https://doi.org/10.1016/s1381-1169(03)00016-5	journal	May 2003
Electrolytic CO ₂ Reduction in a Flow Cell Weekes, David M.; Salvatore, Danielle A.; Reyes, Angelica Accounts of Chemical Research, Vol. 51, Issue 4 https://doi.org/10.1021/acs.accounts.8b00010	journal	March 2018
Progress and Perspectives of Electrochemical CO ₂ Reduction on Copper in Aqueous Electrolyte Nitopi, Stephanie; Bertheussen, Erlend; Scott, Soren B. Chemical Reviews, Vol. 119, Issue 12 https://doi.org/10.1021/acs.chemrev.8b00705	journal	April 2019
Catalysts and Reaction Pathways for the Electrochemical Reduction of Carbon Dioxide Kortlever, Ruud; Shen, Jing; Schouten, Klaas Jan P. The Journal of Physical Chemistry Letters, Vol. 6, Issue 20 https://doi.org/10.1021/acs.jpclett.5b01559	journal	September 2015
Sputtered Ga-Doped SnO _x Electron Transport Layer for Large-Area All-Inorganic Perovskite Solar Cells Zhao, Yan; Deng, Quanrong; Guo, Ruxin ACS Applied Materials & Interfaces, Vol. 12, Issue 49 https://doi.org/10.1021/acsami.0c19540	journal	November 2020
CO₂ Reduction at Low Overpotential on Cu Electrodes Resulting from the Reduction of Thick Cu₂O Films Li, Christina W.; Kanan, Matthew W. Journal of the American Chemical Society, Vol. 134, Issue 17, p. 7231-7234 https://doi.org/10.1021/ja3010978	journal	April 2012
Particle Size Effects in the Catalytic Electroreduction of CO ₂ on Cu Nanoparticles Reske, Rulle; Mistry, Hemma; Behafarid, Farzad Journal of the American Chemical Society, Vol. 136, Issue 19 https://doi.org/10.1021/ja500328k	journal	May 2014
Electroreduction of Carbon Dioxide to Hydrocarbons Using Bimetallic Cu–Pd Catalysts with Different Mixing Patterns Ma, Sichao; Sadakiyo, Masaaki; Heima, Minako Journal of the American Chemical Society, Vol. 139, Issue 1 https://doi.org/10.1021/jacs.6b10740	journal	December 2016
Large Area, Molecularly Smooth (0.2 nm rms) Gold Films for Surface Forces and Other Studies Chai, Liraz; Klein, Jacob Langmuir, Vol. 23, Issue 14 https://doi.org/10.1021/la063738o	journal	July 2007
Switchable imbibition in nanoporous gold Xue, Yahui; Markmann, Jürgen; Duan, Huiling Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5237	journal	July 2014
Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons Zhou, Yansong; Che, Fanglin; Liu, Min Nature Chemistry, Vol. 10, Issue 9 https://doi.org/10.1038/s41557-018-0092-x	journal	July 2018
Accelerated discovery of CO2 electrocatalysts using active machine learning Zhong, Miao; Tran, Kevin; Min, Yimeng Nature, Vol. 581, Issue 7807 https://doi.org/10.1038/s41586-020-2242-8	journal	May 2020
Metal ion cycling of Cu foil for selective C–C coupling in electrochemical CO2 reduction Jiang, Kun; Sandberg, Robert B.; Akey, Austin J. Nature Catalysis, Vol. 1, Issue 2 https://doi.org/10.1038/s41929-017-0009-x	journal	January 2018
Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area Wang, Lei; Nitopi, Stephanie; Wong, Andrew B. Nature Catalysis, Vol. 2, Issue 8 https://doi.org/10.1038/s41929-019-0301-z	journal	June 2019
The importance of surface morphology in controlling the selectivity of polycrystalline copper for CO2 electroreduction Tang, Wei; Peterson, Andrew A.; Varela, Ana Sofia Phys. Chem. Chem. Phys., Vol. 14, Issue 1 https://doi.org/10.1039/C1CP22700A	journal	January 2012
Towards sustainable fuels and chemicals through the electrochemical reduction of CO ₂ : lessons from water electrolysis Martín, Antonio J.; Larrazábal, Gastón O.; Pérez-Ramírez, Javier Green Chemistry, Vol. 17, Issue 12 https://doi.org/10.1039/C5GC01893E	journal	January 2015
Ultra-low voltage electrowetting using graphite surfaces Lomax, Deborah J.; Kant, Pallav; Williams, Aled T. Soft Matter, Vol. 12, Issue 42 https://doi.org/10.1039/C6SM01565D	journal	January 2016
Towards membrane-electrode assembly systems for CO ₂ reduction: a modeling study Weng, Lien-Chun; Bell, Alexis T.; Weber, Adam Z. Energy & Environmental Science, Vol. 12, Issue 6 https://doi.org/10.1039/C9EE00909D	journal	January 2019
New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces Kuhl, Kendra P.; Cave, Etosha R.; Abram, David N. Energy & Environmental Science, Vol. 5, Issue 5 https://doi.org/10.1039/c2ee21234j	journal	January 2012
CO ₂ reduction on gas-diffusion electrodes and why catalytic performance must be assessed at commercially-relevant conditions Burdyny, Thomas; Smith, Wilson A. Energy & Environmental Science, Vol. 12, Issue 5 https://doi.org/10.1039/c8ee03134g	journal	January 2019
Advanced manufacturing for electrosynthesis of fuels and chemicals from CO ₂ Corral, Daniel; Feaster, Jeremy T.; Sobhani, Sadaf Energy & Environmental Science, Vol. 14, Issue 5 https://doi.org/10.1039/d0ee03679j	journal	January 2021
Electrowetting on gold electrodes with microscopic three-dimensional structures for microfluidic devices Yokomaku, Hiroomi; Satoh, Wataru; Fukuda, Junji Journal of Applied Physics, Vol. 104, Issue 6 https://doi.org/10.1063/1.2976358	journal	September 2008
Engineering Cu surfaces for the electrocatalytic conversion of CO ₂ : Controlling selectivity toward oxygenates and hydrocarbons Hahn, Christopher; Hatsukade, Toru; Kim, Youn-Geun Proceedings of the National Academy of Sciences, Vol. 114, Issue 23 https://doi.org/10.1073/pnas.1618935114	journal	May 2017
The effect of oblique-angle sputtering on large area deposition: a unidirectional ultrathin Au plasmonic film growth design Bakkali, H.; Blanco, E.; Dominguez, M. Nanotechnology, Vol. 31, Issue 44 https://doi.org/10.1088/1361-6528/aba65b	journal	August 2020
CO ₂ electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface Dinh, Cao-Thang; Burdyny, Thomas; Kibria, Md Golam Science, Vol. 360, Issue 6390 https://doi.org/10.1126/science.aas9100	journal	May 2018
What would it take for renewably powered electrosynthesis to displace petrochemical processes? De Luna, Phil; Hahn, Christopher; Higgins, Drew Science, Vol. 364, Issue 6438 https://doi.org/10.1126/science.aav3506	journal	April 2019
Terawatt-scale photovoltaics: Transform global energy Haegel, Nancy M.; Atwater, Harry; Barnes, Teresa Science, Vol. 364, Issue 6443 https://doi.org/10.1126/science.aaw1845	journal	May 2019
Microfluidic Reactor for the Electrochemical Reduction of Carbon Dioxide: The Effect of pH Whipple, Devin T.; Finke, Eryn C.; Kenis, Paul J. A. Electrochemical and Solid-State Letters, Vol. 13, Issue 9 https://doi.org/10.1149/1.3456590	journal	January 2010
Magnetron Sputtering vs. Electrodeposition for Hard Chrome Coatings: A Comparison of Environmental and Economic Performances Merlo, Antoine; Léonard, Grégoire Materials, Vol. 14, Issue 14 https://doi.org/10.3390/ma14143823	journal	July 2021

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