An Artificial Electrode/Electrolyte Interface for CO₂ Electroreduction by Cation Surfactant Self‐Assembly

Abstract

In this work, an artificial electrode/electrolyte (E/E) interface,made by coating the electrode surface with aquaternary ammonium cation (R 4 N +)s urfactant, was successfully developed, leading to ac hange in the CO 2 reduction reaction (CO 2 RR) pathway.This artificial E/E interface,with high CO 2 permeability,p romotes CO 2 transportation and hydrogenation, as well as suppresses the hydrogen evolution reaction (HER). Linear and branched surfactants facilitated formic acid and CO production, respectively.M olecular dynamics simulations show that the artificial interface provided af acile CO 2 diffusion pathway.M oreover,d ensity-functional theory (DFT) calculations revealed the stabilization of the key intermediate,O CHO*, through interactions with R 4 N + .T his strategy might also be applicable to other electrocatalytic reactions where gas consumption is involved.

Selectivity and Intrinsic Activity of Functionalized Cu Surfaces: Can the CO2 Reduction Reaction be Improved on Cu?

“…The products affected by this are usually the less favorable ones, such as methane and CO, along with H 2 from the competing HER. In fact, Figure 4a,c shows that both selectivities and intrinsic activities are diminished for a substantial part of the ; 56 [R] Zhong et al 57 Any "missing letters" in the legend are due to the study not reporting the property in the figure, cf. Table S1.…”

“…Table S1. ; 56 [R] Zhong et al 57 Any "missing letters" in the legend are due to the study not reporting the property in the figure, cf. Table S1.…”

Tuning Electronic Structures of Covalent Co Porphyrin Polymers for Electrocatalytic CO 2 Reduction in Aqueous Solutions

“…8,9 More seriously, the hydrogen evolution reaction (HER) is often kinetically more favored, resulting in unsatisfied CO 2 RR selectivity in aqueous solutions. [10][11][12][13][14][15] Several strategies have been reported to improve the selectivity of CO 2 RR over HER in aqueous solutions, including using strong basic solutions, 16,17 introducing cationic surfactants on electrode surfaces, 18,19 employing gas diffusion electrodes, 20,21 and utilizing supercritical CO 2 . 22,23 However, designing and developing electrocatalysts, whose active sites have intrinsically high selectivity for CO 2 RR, and understanding the underlaying mechanisms, are of fundamental significance.…”

Improved electrochemical conversion of CO2 to multicarbon products by using molecular doping

“…Organic species such as N-aryl pyridinium salts 31 , 32 , imidazole 33 – 35 , thiol 36 , 37 , and cysteamine 38 have been reported as an effective lever to tune the reaction selectivity toward the formation of specific products by stabilizing key reaction intermediates. Functionalization of alkyl chains can also lead to better CO 2 RR performance by suppressing the competitive hydrogen evolution reaction (HER) via the creation of hydrophobic regions on the surface of the catalyst 37 , 39 , 40 .…”