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Breaking Scaling Relationships in CO₂ Reduction on Copper Alloys with Organic Additives

Lai, Yunchieh and Watkins, Nicholas and Rosas-Hernández, Alonso and Thevenon, Arnaud and Heim, Gavin P. and Zhou, Lan and Peters, Jonas C. and Gregoire, John M. and Agapie, Theodor (2021) Breaking Scaling Relationships in CO₂ Reduction on Copper Alloys with Organic Additives. . (Unpublished) https://resolver.caltech.edu/CaltechAUTHORS:20210610-080047277

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Abstract

Boundary conditions for catalyst performance in the conversion of common precursors such as N₂, O₂, H₂O, and CO₂ are governed by linear free energy and scaling relationships. Knowledge of these limits offers an impetus for designing strategies to alter reaction mechanisms to improve performance. Towards a more sustainable carbon economy, understanding the basis of catalytic selectivity for CO₂ conversion to chemical feedstocks/fuels is key. Herein, high-throughput experimentation on 14 bulk copper bimetallic alloys allowed for data-driven identification of a fundamental linear scaling relationship between methane and C₂₊ products that constrains the Faradaic efficiency for C–C coupling. We have furthermore demonstrated that coating the electrodes with a molecular film breaks the scaling relationship to promote C₂₊ product formation.


Item Type:Report or Paper (Discussion Paper)
Related URLs:
URLURL TypeDescription
https://doi.org/10.26434/chemrxiv.14751534.v1DOIDiscussion Paper
ORCID:
AuthorORCID
Rosas-Hernández, Alonso0000-0002-0812-5591
Thevenon, Arnaud0000-0002-5543-6595
Zhou, Lan0000-0002-7052-266X
Peters, Jonas C.0000-0002-6610-4414
Gregoire, John M.0000-0002-2863-5265
Agapie, Theodor0000-0002-9692-7614
Alternate Title:Breaking Scaling Relationships in CO2 Reduction on Copper Alloys with Organic Additives
Additional Information:Licence: CC BY-NC-ND 4.0. Submitted date: 08/06/2021; Posted date: 09/06/2021. This material is based on work performed by the Liquid Sunlight Alliance, which is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub under Award Number DE-SC0021266. A.T. acknowledges Marie Skłodowska-Curie Fellowship H2020-MSCA-IF-2017 (793471). J.C.P. also acknowledges general support from the Resnick Sustainability Institute at Caltech. Data and materials availability: All material preparation and characterization, synthetic and electrochemical procedures, and raw data is available within the supplementary materials. No conflict of interest.
Group:Resnick Sustainability Institute, JCAP
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0021266
Marie Curie Fellowship793471
Resnick Sustainability InstituteUNSPECIFIED
Subject Keywords:carbon dioxide reduction; scaling relationship; high throughput experimentation; Copper Alloys; Modified Electrodes; organic additives
Record Number:CaltechAUTHORS:20210610-080047277
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210610-080047277
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:109461
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:10 Jun 2021 16:29
Last Modified:12 Aug 2021 23:29

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