Tailoring Copper Nanocrystals towards C2 Products in Electrochemical CO2 Reduction

Loiudice, Anna; Lobaccaro, Peter; Kamali, Esmail A.; Thao, Timothy; Huang, Brandon H.; Ager, Joel W.; Buonsanti, Raffaella

doi:10.1002/anie.201601582

Tailoring Copper Nanocrystals towards C₂ Products in Electrochemical CO₂ Reduction

Journal Article · Tue Apr 05 00:00:00 EDT 2016 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201601582· OSTI ID:1530238

Loiudice, Anna ^[1]; Lobaccaro, Peter ^[2]; Kamali, Esmail A. ^[1]; Thao, Timothy ^[3]; Huang, Brandon H. ^[3]; Ager, Joel W. ^[2]; ^[1]

École Polytechnique Fédérale de Lausanne, Sion (Switzerland)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)

Favoring the CO₂ reduction reaction (CO₂RR) over the hydrogen evolution reaction and controlling the selectivity towards multicarbon products are currently major scientific challenges in sustainable energy research. It is known that the morphology of the catalyst can modulate catalytic activity and selectivity, yet this remains a relatively underexplored area in electrochemical CO₂ reduction. In this study, we exploit the material tunability afforded by colloidal chemistry to establish unambiguous structure/property relations between Cu nanocrystals and their behavior as electrocatalysts for CO₂ reduction. Our study reveals a non-monotonic size-dependence of the selectivity in cube-shaped copper nanocrystals. Among 24 nm, 44 nm and 63 nm cubes tested, the cubes with 44 nm edge length exhibited the highest selectivity towards CO₂RR (80 %) and faradaic efficiency for ethylene (41 %). Finally, statistical analysis of the surface atom density suggests the key role played by edge sites in CO₂RR.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

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

Grant/Contract Number:: AC02-05CH11231; SC0004993

OSTI ID:: 1530238

Alternate ID(s):: OSTI ID: 1401425

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 19 Vol. 55; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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The importance of grand-canonical quantum mechanical methods to describe the effect of electrode potential on the stability of intermediates involved in both electrochemical CO ₂ reduction and hydrogen evolution Zhang, Haochen; Goddard, William A.; Lu, Qi Physical Chemistry Chemical Physics, Vol. 20, Issue 4 https://doi.org/10.1039/c7cp08153g	journal	January 2018
Electrochemical processes on solid shaped nanoparticles with defined facets Strasser, Peter; Gliech, Manuel; Kuehl, Stefanie Chemical Society Reviews, Vol. 47, Issue 3 https://doi.org/10.1039/c7cs00759k	journal	January 2018
Joint tuning of nanostructured Cu-oxide morphology and local electrolyte programs high-rate CO ₂ reduction to C ₂ H ₄ Pang, Yuanjie; Burdyny, Thomas; Dinh, Cao-Thang Green Chemistry, Vol. 19, Issue 17 https://doi.org/10.1039/c7gc01677h	journal	January 2017
Recent advances in the nanoengineering of electrocatalysts for CO ₂ reduction Li, Fengwang; MacFarlane, Douglas R.; Zhang, Jie Nanoscale, Vol. 10, Issue 14 https://doi.org/10.1039/c7nr09620h	journal	January 2018
Efficient electrochemical transformation of CO ₂ to C ₂ /C ₃ chemicals on benzimidazole-functionalized copper surfaces Zhong, Shenghong; Yang, Xiulin; Cao, Zhen Chemical Communications, Vol. 54, Issue 80 https://doi.org/10.1039/c8cc04735a	journal	January 2018
Cu( ii )-nanoparticle-derived structures under CO ₂ reduction conditions: a matter of shape Basiratnia, Amir; Rempel, Jacob; Li, Feng Physical Chemistry Chemical Physics, Vol. 21, Issue 11 https://doi.org/10.1039/c8cp07891b	journal	January 2019
From CO ₂ methanation to ambitious long-chain hydrocarbons: alternative fuels paving the path to sustainability Marques Mota, Filipe; Kim, Dong Ha Chemical Society Reviews, Vol. 48, Issue 1 https://doi.org/10.1039/c8cs00527c	journal	January 2019
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
Sequential catalysis enables enhanced C–C coupling towards multi-carbon alkenes and alcohols in carbon dioxide reduction: a study on bifunctional Cu/Au electrocatalysts Gao, Jing; Ren, Dan; Guo, Xueyi Faraday Discussions, Vol. 215 https://doi.org/10.1039/c8fd00219c	journal	January 2019
Efficient electroreduction of CO ₂ to C2 products over B-doped oxide-derived copper Chen, Chunjun; Sun, Xiaofu; Lu, Lu Green Chemistry, Vol. 20, Issue 20 https://doi.org/10.1039/c8gc02389a	journal	January 2018
Facet- and structure-dependent catalytic activity of cuprous oxide/polypyrrole particles towards the efficient reduction of carbon dioxide to methanol Periasamy, Arun Prakash; Ravindranath, Rini; Senthil Kumar, Sakkarapalayam Murugesan Nanoscale, Vol. 10, Issue 25 https://doi.org/10.1039/c8nr02117a	journal	January 2018
3D hierarchical porous indium catalyst for highly efficient electroreduction of CO ₂ Luo, Wen; Xie, Wei; Li, Mo Journal of Materials Chemistry A, Vol. 7, Issue 9 https://doi.org/10.1039/c8ta11645h	journal	January 2019
Mild pyrolysis of ionic self-assembled cobalt porphyrins on carbon toward efficient electrochemical conversion of CO ₂ to CO Zhang, Xue; Liu, Huiyuan; Qin, Jiaqi Chemical Communications, Vol. 55, Issue 39 https://doi.org/10.1039/c9cc02156f	journal	January 2019
Size dependent selectivity of Cu nano-octahedra catalysts for the electrochemical reduction of CO ₂ to CH ₄ Iyengar, Pranit; Huang, Jianfeng; De Gregorio, Gian Luca Chemical Communications, Vol. 55, Issue 60 https://doi.org/10.1039/c9cc02522g	journal	January 2019
Selective electrochemical CO ₂ conversion to multicarbon alcohols on highly efficient N-doped porous carbon-supported Cu catalysts Han, Hyunsu; Noh, Yuseong; Kim, Yoongon Green Chemistry, Vol. 22, Issue 1 https://doi.org/10.1039/c9gc03088c	journal	January 2020
Organic–inorganic hybrids for CO ₂ sensing, separation and conversion Rebber, Matthias; Willa, Christoph; Koziej, Dorota Nanoscale Horizons, Vol. 5, Issue 3 https://doi.org/10.1039/c9nh00380k	journal	January 2020
Theoretical study of CO ₂ adsorption on Pt Matsuda, Shofu; Mukai, Tsuyoshi; Sakurada, Seishiro New Journal of Chemistry, Vol. 43, Issue 35 https://doi.org/10.1039/c9nj03092a	journal	January 2019
Regulating C–C coupling in thermocatalytic and electrocatalytic CO x conversion based on surface science Jiang, Yawen; Long, Ran; Xiong, Yujie Chemical Science, Vol. 10, Issue 31 https://doi.org/10.1039/c9sc02014d	journal	January 2019
Molecular tunability of surface-functionalized metal nanocrystals for selective electrochemical CO ₂ reduction Pankhurst, James R.; Guntern, Yannick T.; Mensi, Mounir Chemical Science, Vol. 10, Issue 44 https://doi.org/10.1039/c9sc04439f	journal	January 2019
Electrochemical CO ₂ reduction on nanostructured metal electrodes: fact or defect? Kas, Recep; Yang, Kailun; Bohra, Divya Chemical Science, Vol. 11, Issue 7 https://doi.org/10.1039/c9sc05375a	journal	January 2020
Advanced engineering of core/shell nanostructures for electrochemical carbon dioxide reduction Shao, Qi; Wang, Pengtang; Liu, Shangheng Journal of Materials Chemistry A, Vol. 7, Issue 36 https://doi.org/10.1039/c9ta07016h	journal	January 2019
Current progress in electrocatalytic carbon dioxide reduction to fuels on heterogeneous catalysts Liu, Anmin; Gao, Mengfan; Ren, Xuefeng Journal of Materials Chemistry A, Vol. 8, Issue 7 https://doi.org/10.1039/c9ta11966c	journal	January 2020
Self-assembling of formic acid on the partially oxidized p (2 × 1) Cu(110) surface reconstruction at low coverages Chen, Zhu; Martirez, John Mark P.; Zahl, Percy The Journal of Chemical Physics, Vol. 150, Issue 4 https://doi.org/10.1063/1.5046697	journal	January 2019
Cu metal embedded in oxidized matrix catalyst to promote CO ₂ activation and CO dimerization for electrochemical reduction of CO ₂ Xiao, Hai; Goddard, William A.; Cheng, Tao Proceedings of the National Academy of Sciences https://doi.org/10.1073/pnas.1702405114	journal	June 2017
Copper nanoparticle ensembles for selective electroreduction of CO ₂ to C ₂ –C ₃ products Kim, Dohyung; Kley, Christopher S.; Li, Yifan Proceedings of the National Academy of Sciences, Vol. 114, Issue 40 https://doi.org/10.1073/pnas.1711493114	journal	September 2017
Hydrogen bonding steers the product selectivity of electrocatalytic CO reduction Li, Jingyi; Li, Xiang; Gunathunge, Charuni M. Proceedings of the National Academy of Sciences, Vol. 116, Issue 19 https://doi.org/10.1073/pnas.1900761116	journal	April 2019
Tailoring gas-phase CO ₂ electroreduction selectivity to hydrocarbons at Cu nanoparticles Merino-Garcia, I.; Albo, J.; Irabien, A. Nanotechnology, Vol. 29, Issue 1 https://doi.org/10.1088/1361-6528/aa994e	journal	November 2017
A spongy nickel-organic CO ₂ reduction photocatalyst for nearly 100% selective CO production Niu, Kaiyang; Xu, You; Wang, Haicheng Science Advances, Vol. 3, Issue 7 https://doi.org/10.1126/sciadv.1700921	journal	July 2017
Ultrastable atomic copper nanosheets for selective electrochemical reduction of carbon dioxide Dai, Lei; Qin, Qing; Wang, Pei Science Advances, Vol. 3, Issue 9 https://doi.org/10.1126/sciadv.1701069	journal	September 2017
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
Zn(II) porphyrin-based photocatalytic synthesis of Cu nanoparticles for electrochemical reduction of CO 2 Zhang, Siyu; Zhang, Xue; Liu, Huiyuan Journal of Porphyrins and Phthalocyanines, Vol. 22, Issue 05 https://doi.org/10.1142/s1088424618500293	journal	April 2018
Heterogeneous catalysts for catalytic CO2 conversion into value-added chemicals Whang, Ho Seok; Lim, Jinkyu; Choi, Min Suk BMC Chemical Engineering, Vol. 1, Issue 1 https://doi.org/10.1186/s42480-019-0007-7	journal	March 2019
Electrochemical Reduction of CO2 to Formate on Easily Prepared Carbon-Supported Bi Nanoparticles Ávila-Bolívar, Beatriz; García-Cruz, Leticia; Montiel, Vicente Molecules, Vol. 24, Issue 11 https://doi.org/10.3390/molecules24112032	journal	May 2019

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Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
colloidal chemistry
electrochemical CO2 reduction
nanocrystals
nanocubes
selectivity