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

Abstract

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.

Authors:

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

Publication Date:: Tue Apr 05 00:00:00 EDT 2016

Sponsoring Org.:: USDOE

OSTI Identifier:: 1401659

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

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Angewandte Chemie

Additional Journal Information:: Journal Name: Angewandte Chemie Journal Volume: 128 Journal Issue: 19; Journal ID: ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Loiudice, Anna, Lobaccaro, Peter, Kamali, Esmail A., Thao, Timothy, Huang, Brandon H., Ager, Joel W., and Buonsanti, Raffaella. Tailoring Copper Nanocrystals towards C 2 Products in Electrochemical CO 2 Reduction.  Germany: N. p., 2016. 
Web.  doi:10.1002/ange.201601582.

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                    Loiudice, Anna, Lobaccaro, Peter, Kamali, Esmail A., Thao, Timothy, Huang, Brandon H., Ager, Joel W., & Buonsanti, Raffaella. Tailoring Copper Nanocrystals towards C 2 Products in Electrochemical CO 2 Reduction.  Germany.  https://doi.org/10.1002/ange.201601582

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                    Loiudice, Anna, Lobaccaro, Peter, Kamali, Esmail A., Thao, Timothy, Huang, Brandon H., Ager, Joel W., and Buonsanti, Raffaella. Tue .  
"Tailoring Copper Nanocrystals towards C 2 Products in Electrochemical CO 2 Reduction".  Germany.  https://doi.org/10.1002/ange.201601582.

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@article{osti_1401659,

  title        = {Tailoring Copper Nanocrystals towards C 2 Products in Electrochemical CO 2 Reduction},

  author       = {Loiudice, Anna and Lobaccaro, Peter and Kamali, Esmail A. and Thao, Timothy and Huang, Brandon H. and Ager, Joel W. and Buonsanti, Raffaella},

  abstractNote = {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.},

  doi          = {10.1002/ange.201601582},

  journal      = {Angewandte Chemie},

  number       = 19,

  volume       = 128,

  place        = {Germany},

  year         = {Tue Apr 05 00:00:00 EDT 2016},

  month        = {Tue Apr 05 00:00:00 EDT 2016}

}

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

Abstract

Citation Formats

The importance of surface morphology in controlling the selectivity of polycrystalline copper for CO2 electroreduction journal, January 2012

CO2 Reduction at Low Overpotential on Cu Electrodes Resulting from the Reduction of Thick Cu2O Films journal, April 2012

Face the Edges: Catalytic Active Sites of Nanomaterials journal, June 2015

Two Pathways for the Formation of Ethylene in CO Reduction on Single-Crystal Copper Electrodes journal, June 2012

Engineering the surface structure of MoS2 to preferentially expose active edge sites for electrocatalysis journal, October 2012

Prospects of Nanoscience with Nanocrystals journal, January 2015

(Invited) Optimizing Electrocatalyst Selectivity for CO2 Reduction over H2 Evolution journal, April 2015

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Catalytic Kinetics of Different Types of Surface Atoms on Shaped Pd Nanocrystals journal, January 2016

The influence of pH on the reduction of CO and CO 2 to hydrocarbons on copper electrodes journal, March 2014

Particle Size Effects in the Catalytic Electroreduction of CO 2 on Cu Nanoparticles journal, May 2014

High Selectivity for Ethylene from Carbon Dioxide Reduction over Copper Nanocube Electrocatalysts journal, February 2015

Enhanced Electrochemical Methanation of Carbon Dioxide with a Dispersible Nanoscale Copper Catalyst journal, September 2014

Monodisperse Au Nanoparticles for Selective Electrocatalytic Reduction of CO 2 to CO journal, October 2013

Stable and selective electrochemical reduction of carbon dioxide to ethylene on copper mesocrystals journal, January 2015

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How to make the most of carbon dioxide journal, October 2015

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

The importance of surface morphology in controlling the selectivity of polycrystalline copper for CO2 electroreduction
journal, January 2012

CO₂ Reduction at Low Overpotential on Cu Electrodes Resulting from the Reduction of Thick Cu₂O Films
journal, April 2012

Face the Edges: Catalytic Active Sites of Nanomaterials
journal, June 2015

Two Pathways for the Formation of Ethylene in CO Reduction on Single-Crystal Copper Electrodes
journal, June 2012

Engineering the surface structure of MoS₂ to preferentially expose active edge sites for electrocatalysis
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