Reorganization of Interfacial Water by an Amphiphilic Cationic Surfactant Promotes CO2 Reduction
- 16 July 2020
- journal article
- research article
- Published by American Chemical Society (ACS) in The Journal of Physical Chemistry Letters
- Vol. 11 (14), 5457-5463
- https://doi.org/10.1021/acs.jpclett.0c01334
Abstract
The presence of cetyltrimethylammonium bromide (CTAB) near the surface of a Cu electrode promotes the electrochemical reduction of CO2 to fuels. CTAB increases the CO2 reduction rate by as much as 10x and decreased the HER rate by 4x, leading to similar to 75% selectivity toward the reduction of CO2. Surface enhanced infrared absorption spectroscopy (SEIRAS) was used to probe the effects of CTAB adsorption on the structure of interfacial water and CO2 reduction intermediates. HER suppression was found to arise from the displacement of interfacial water molecules from CTAB adsorption within the double layer. The enhanced CO2 reduction rate can be correlated to an increased population of atop-bound CO and the emergence of a low frequency atop-CO band. These results unravel the role of additives in improving CO2-to-fuels electrocatalysis and establishing this as a powerful methodology for directing product selectivity.Funding Information
- Division of Chemistry (CHE-1764310)
- Johns Hopkins University
This publication has 56 references indexed in Scilit:
- Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface areaNature Catalysis, 2019
- CO 2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interfaceScience, 2018
- Mechanism of CO2 Reduction at Copper Surfaces: Pathways to C2 ProductsACS Catalysis, 2018
- Selective increase in CO 2 electroreduction activity at grain-boundary surface terminationsScience, 2017
- Engineering Cu surfaces for the electrocatalytic conversion of CO 2 : Controlling selectivity toward oxygenates and hydrocarbonsProceedings of the National Academy of Sciences of the United States of America, 2017
- Tuning of Silver Catalyst Mesostructure Promotes Selective Carbon Dioxide Conversion into FuelsAngewandte Chemie, 2016
- Polymer coordination promotes selective CO2reduction by cobalt phthalocyanineChemical Science, 2016
- Mesostructure-Induced Selectivity in CO2 Reduction CatalysisJournal of the American Chemical Society, 2015
- Selectivity of CO2 Reduction on Copper Electrodes: The Role of the Kinetics of Elementary StepsAngewandte Chemie, 2013
- Selective Formation of C2 Compounds from Electrochemical Reduction of CO2 at a Series of Copper Single Crystal ElectrodesThe Journal of Physical Chemistry B, 2001