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In-situ Nanostructuring and Stabilization of Polycrystalline Copper by an Organic Salt Additive Promotes Electrocatalytic CO₂ Reduction to Ethylene

Thevenon, Arnaud and Rosas-Hernández, Alonso and Peters, Jonas C. and Agapie, Theodor (2019) In-situ Nanostructuring and Stabilization of Polycrystalline Copper by an Organic Salt Additive Promotes Electrocatalytic CO₂ Reduction to Ethylene. Angewandte Chemie International Edition, 58 (47). pp. 16952-16958. ISSN 1433-7851. https://resolver.caltech.edu/CaltechAUTHORS:20190923-102748967

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Abstract

Bridging homogeneous molecular systems with heterogeneous catalysts is a promising approach for the development of new electrodes, combining the advantages of both approaches. In the context of CO₂ electroreduction, molecular enhancement of planar copper electrodes has enabled promising advancement towards high Faradaic efficiencies for multicarbon products. Besides, nanostructured copper electrodes have also demonstrated enhanced performance at comparatively low overpotentials. Herein, we report a novel and convenient method for nanostructuring copper electrodes using N,N’‐ethylene‐phenanthrolinium dibromide as molecular additive. Selectivities up to 70% for C≥₂ products are observed for more than 40 h without significant change in the surface morphology. Mechanistic studies reveal several roles for the organic additive, including: the formation of cube‐like nanostructures by corrosion of the copper surface, the stabilization of these nanostructures during electrocatalysis by formation of a protective organic layer, and the promotion of C≥₂ products.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1002/anie.201907935DOIArticle
ORCID:
AuthorORCID
Thevenon, Arnaud0000-0002-5543-6595
Rosas-Hernández, Alonso0000-0002-0812-5591
Peters, Jonas C.0000-0002-6610-4414
Agapie, Theodor0000-0002-9692-7614
Alternate Title:In-situ Nanostructuring and Stabilization of Polycrystalline Copper by an Organic Salt Additive Promotes Electrocatalytic CO2 Reduction to Ethylene
Additional Information:© 2019 Wiley-‐VCH Verlag GmbH & Co. KGaA, Weinheim. Accepted manuscript online: 19 September 2019; Manuscript accepted: 19 September 2019; Manuscript revised: 13 August 2019; Manuscript received: 25 June 2019. NMR, AFM and XPS, SEM and EDX measurements were collected at the NMR Facility (Division of CCE), the Molecular Materials Research Center (Beckman Institute) and the Analytic Facilities (Division of Geological and Planetary Sciences) of the California Institute of Technology, respectively. This material is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993 and Marie Curie Fellowship H2020-MSCA-IF-2017 (793471) (A.T.). J.C.P. acknowledges additional support from the Resnick Sustainability Institute at Caltech. The authors declare no conflict of interest.
Group:JCAP, Resnick Sustainability Institute
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Marie Curie FellowshipH2020-MSCA-IF-2017
Resnick Sustainability InstituteUNSPECIFIED
Subject Keywords:Carbon Dioxide; electrocatalysis; ethylene; nanocubes; Stability
Issue or Number:47
Record Number:CaltechAUTHORS:20190923-102748967
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20190923-102748967
Official Citation:A. Thevenon, A. Rosas-Hernández, J. C. Peters, T. Agapie, Angew. Chem. Int. Ed. 2019, 58, 16952. https://doi.org/10.1002/anie.201907935
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:98794
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:23 Sep 2019 21:16
Last Modified:15 Nov 2019 18:08

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