Tailoring Copper Nanocrystals towards C 2 Products in Electrochemical CO 2 Reduction

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

doi:10.1002/ange.201601582

Title: Tailoring Copper Nanocrystals towards C ₂ Products in Electrochemical CO ₂ Reduction

Journal Article · Tue Apr 05 00:00:00 EDT 2016 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.201601582· OSTI ID:1401659

Loiudice, Anna ^[1]; Lobaccaro, Peter ^[2]; Kamali, Esmail A. ^[1]; Thao, Timothy ^[3]; Huang, Brandon H. ^[4]; Ager, Joel W. ^[5];

^[1]

Department of Chemical Sciences and Engineering École Polytechnique Fédérale de Lausanne 1950 Sion Switzerland
Joint Center for Artificial Photosynthesis Lawrence Berkeley National Laboratory Berkeley CA 94720 USA, Department of Chemical and Biomolecular Engineering University of California, Berkeley Berkeley CA 94720 USA
Department of Materials Science and Engineering University of California Berkeley CA 94720 USA
Department of Chemical and Biomolecular Engineering University of California, Berkeley Berkeley CA 94720 USA
Joint Center for Artificial Photosynthesis Lawrence Berkeley National Laboratory Berkeley CA 94720 USA, Department of Materials Science and Engineering University of California Berkeley CA 94720 USA

Abstract Favoring the CO ₂ 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 CO ₂ reduction. Here, we exploit the material tunability afforded by colloidal chemistry to establish unambiguous structure/property relations between Cu nanocrystals and their behavior as electrocatalysts for CO ₂ 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 %). Statistical analysis of the surface atom density suggests the key role played by edge sites in CO2RR.

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Sponsoring Organization:: USDOE

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

OSTI ID:: 1401659

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Vol. 128 Journal Issue: 19; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

References (29)

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
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
Face the Edges: Catalytic Active Sites of Nanomaterials Ni, Bing; Wang, Xun Advanced Science, Vol. 2, Issue 7 https://doi.org/10.1002/advs.201500085	journal	June 2015
Two Pathways for the Formation of Ethylene in CO Reduction on Single-Crystal Copper Electrodes Schouten, Klaas Jan P.; Qin, Zisheng; Pérez Gallent, Elena Journal of the American Chemical Society, Vol. 134, Issue 24 https://doi.org/10.1021/ja302668n	journal	June 2012
Engineering the surface structure of MoS₂ to preferentially expose active edge sites for electrocatalysis Kibsgaard, Jakob; Chen, Zhebo; Reinecke, Benjamin N. Nature Materials, Vol. 11, Issue 11, p. 963-969 https://doi.org/10.1038/nmat3439	journal	October 2012
Prospects of Nanoscience with Nanocrystals Kovalenko, Maksym V.; Manna, Liberato; Cabot, Andreu ACS Nano, Vol. 9, Issue 2 https://doi.org/10.1021/nn506223h	journal	January 2015
(Invited) Optimizing Electrocatalyst Selectivity for CO2 Reduction over H2 Evolution Peterson, A. A. ECS Transactions, Vol. 66, Issue 3 https://doi.org/10.1149/06603.0041ecst	journal	April 2015
Manipulating the Hydrocarbon Selectivity of Copper Nanoparticles in CO ₂ Electroreduction by Process Conditions Kas, Recep; Kortlever, Ruud; Yılmaz, Hasan ChemElectroChem, Vol. 2, Issue 3 https://doi.org/10.1002/celc.201402373	journal	December 2014
Catalytic Kinetics of Different Types of Surface Atoms on Shaped Pd Nanocrystals Chen, Tao; Chen, Sheng; Zhang, Yuwei Angewandte Chemie, Vol. 128, Issue 5 https://doi.org/10.1002/ange.201509165	journal	January 2016
The influence of pH on the reduction of CO and ${CO}_{2}$ to hydrocarbons on copper electrodes Schouten, Klaas Jan P.; Pérez Gallent, Elena; Koper, Marc T. M. Journal of Electroanalytical Chemistry, Vol. 716 https://doi.org/10.1016/j.jelechem.2013.08.033	journal	March 2014
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
High Selectivity for Ethylene from Carbon Dioxide Reduction over Copper Nanocube Electrocatalysts Roberts, F. Sloan; Kuhl, Kendra P.; Nilsson, Anders Angewandte Chemie, Vol. 127, Issue 17 https://doi.org/10.1002/ange.201412214	journal	February 2015
Enhanced Electrochemical Methanation of Carbon Dioxide with a Dispersible Nanoscale Copper Catalyst Manthiram, Karthish; Beberwyck, Brandon J.; Alivisatos, A. Paul Journal of the American Chemical Society, Vol. 136, Issue 38 https://doi.org/10.1021/ja5065284	journal	September 2014
Monodisperse Au Nanoparticles for Selective Electrocatalytic Reduction of CO ₂ to CO Zhu, Wenlei; Michalsky, Ronald; Metin, Önder Journal of the American Chemical Society, Vol. 135, Issue 45 https://doi.org/10.1021/ja409445p	journal	October 2013
Stable and selective electrochemical reduction of carbon dioxide to ethylene on copper mesocrystals Chen, Chung Shou; Handoko, Albertus D.; Wan, Jane Hui Catalysis Science & Technology, Vol. 5, Issue 1 https://doi.org/10.1039/C4CY00906A	journal	January 2015
Active and Selective Conversion of CO ₂ to CO on Ultrathin Au Nanowires Zhu, Wenlei; Zhang, Yin-Jia; Zhang, Hongyi Journal of the American Chemical Society, Vol. 136, Issue 46 https://doi.org/10.1021/ja5095099	journal	November 2014
Shape-Selective Formation of Monodisperse Copper Nanospheres and Nanocubes via Disproportionation Reaction Route and Their Optical Properties Guo, Huizhang; Chen, Yuanzhi; Cortie, Michael B. The Journal of Physical Chemistry C, Vol. 118, Issue 18 https://doi.org/10.1021/jp5014187	journal	April 2014
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
Structure effects on the energetics of the electrochemical reduction of CO2 by copper surfaces Durand, William J.; Peterson, Andrew A.; Studt, Felix Surface Science, Vol. 605, Issue 15-16 https://doi.org/10.1016/j.susc.2011.04.028	journal	August 2011
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
Catalytic Kinetics of Different Types of Surface Atoms on Shaped Pd Nanocrystals Chen, Tao; Chen, Sheng; Zhang, Yuwei Angewandte Chemie International Edition, Vol. 55, Issue 5 https://doi.org/10.1002/anie.201509165	journal	January 2016
How to make the most of carbon dioxide Lim, XiaoZhi Nature, Vol. 526, Issue 7575 https://doi.org/10.1038/526628a	journal	October 2015
Identification of Active Edge Sites for Electrochemical H₂ Evolution from MoS₂ Nanocatalysts Jaramillo, T. F.; Jorgensen, K. P.; Bonde, J. Science, Vol. 317, Issue 5834, p. 100-102 https://doi.org/10.1126/science.1141483	journal	July 2007
A new mechanism for the selectivity to C1 and C2 species in the electrochemical reduction of carbon dioxide on copper electrodes Schouten, K. J. P.; Kwon, Y.; van der Ham, C. J. M. Chemical Science, Vol. 2, Issue 10 https://doi.org/10.1039/c1sc00277e	journal	January 2011
Structure Sensitivity of Alkynol Hydrogenation on Shape- and Size-Controlled Palladium Nanocrystals: Which Sites Are Most Active and Selective? Crespo-Quesada, Micaela; Yarulin, Artur; Jin, Mingshang Journal of the American Chemical Society, Vol. 133, Issue 32 https://doi.org/10.1021/ja204557m	journal	August 2011
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
High Selectivity for Ethylene from Carbon Dioxide Reduction over Copper Nanocube Electrocatalysts Roberts, F. Sloan; Kuhl, Kendra P.; Nilsson, Anders Angewandte Chemie International Edition, Vol. 54, Issue 17 https://doi.org/10.1002/anie.201412214	journal	February 2015
Structure Sensitivity of the Electrochemical Reduction of Carbon Monoxide on Copper Single Crystals Schouten, Klaas Jan P.; Pérez Gallent, Elena; Koper, Marc T. M. ACS Catalysis, Vol. 3, Issue 6 https://doi.org/10.1021/cs4002404	journal	April 2013
Sustainable hydrocarbon fuels by recycling CO 2 and H 2 O with renewable or nuclear energy Graves, Christopher; Ebbesen, Sune D.; Mogensen, Mogens Renewable and Sustainable Energy Reviews, Vol. 15, Issue 1 https://doi.org/10.1016/j.rser.2010.07.014	journal	January 2011

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