Organic Additive‐derived Films on Cu Electrodes Promote Electrochemical CO<sub>2</sub> Reduction to C<sub>2+</sub> Products Under Strongly Acidic Conditions

Nie, Weixuan; Heim, Gavin P.; Watkins, Nicholas B.; Agapie, Theodor; Peters, Jonas C.

doi:10.1002/ange.202216102

Cited by 18 publications

(22 citation statements)

References 52 publications

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“…The observed H + diffusion coefficient ( D H+ ), which is proportional to the proton diffusion rate, calculated based on the linear fitting of plateau current ( i plateau ) vs. rotation rate 1/2 ( ω 1/2 ), H + discussed here reflects using the Levich equation (Equation ()) 19

i_{plateau} goodbreak= 0.62 italicnFA D_{{normalH}^{+}}^{2 / 3} ω^{1 / 2} ʋ^{- 1 / 6} C_{{normalH}^{+}}^{*},

where ʋ is viscosity of electrolytes, which does not change much in systems without, and with CTAB.…”

Section: Methodsmentioning

confidence: 99%

Surfactant‐modified electrode–electrolyte interface for steering CO₂ electrolysis on Cu electrodes

Dong,

Ge,

Fan

et al. 2023

AIChE Journal

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Cu‐based catalysts exhibit the unique ability to generate high‐order products from electrochemical CO2 reduction reaction (CO2RR). The performance of electrochemical systems is jointly influenced by the catalysts and local microenvironment of the electrode–electrolyte interface. Here, Cu nanowires as a model catalyst, in combination with cetyl trimethyl ammonium bromide (CTAB) as electrolyte additives, are designed to steer CO2RR. By using the Cu rotating disc electrode and in situ vibrational spectroscopy, it is revealed that the hydrophobic interface microenvironment is built, and the interaction of interfacial water and surface‐adsorbed CO is disrupted by CTAB, which dramatically improve formate selectivity (from 5% to 63%) with a high partial current density of formate (13‐fold increase) at −1.0 V vs. reversible hydrogen electrode. The understanding of the surfactant‐modified electrode–electrolyte interface established here offers a distinct perspective to control the microenvironment on promoting electrosynthesis performance.

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i_{plateau} goodbreak= 0.62 italicnFA D_{{normalH}^{+}}^{2 / 3} ω^{1 / 2} ʋ^{- 1 / 6} C_{{normalH}^{+}}^{*},

where ʋ is viscosity of electrolytes, which does not change much in systems without, and with CTAB.…”

Section: Methodsmentioning

confidence: 99%

Surfactant‐modified electrode–electrolyte interface for steering CO₂ electrolysis on Cu electrodes

Dong,

Ge,

Fan

et al. 2023

AIChE Journal

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show abstract

“…Although the catalyst is the core of electrocatalysis, a GDL-based catalytic reaction system featuring a gas–solid–liquid triphasic interface can also play an influential role by improving the GDL and increasing the concentration of reactants around the catalyst. 32,289–291…”

Section: Optimization Of the Triphasic Interfacial Reaction Systemmentioning

confidence: 99%

“…The subsequent complex reaction pathway and HER competition directly lead to the low Faraday efficiency (FE) of C 2+ product formation. 32,33 Presently, the FE of C 2+ product formation can exceed 60%. 34–36 However, the poor selectivity limits the synthesis and subsequent applications of C 2+ products.…”

Section: Introductionmentioning

confidence: 99%

Electrochemical reduction of carbon dioxide to multicarbon (C₂₊) products: challenges and perspectives

Zhang¹,

Huang²,

Raziq³

et al. 2023

Energy Environ. Sci.

133

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“…9 Recently, techniques of CO 2 reduction with acidic electrolyte were developed to circumvent the asmentioned issues. [9][10][11][12][13][14][15][16][17][18][19][20][21] Alkali cations play an important role to suppress hydrogen evolution reaction (HER) and promote CO 2 reduction in acidic condition. However, alkali cations induce bicarbonate precipitation on the cathode during CO 2 reduction in acidic electrolyte, which is still an issue that hinders the sustainability of CO 2 reduction.…”

Section: Introductionmentioning

confidence: 99%

Surface-Immobilized Cross-linked Cationic Polyelectrolyte Enables CO2 Reduction with Metal Cation-free Acidic Electrolyte

Qin

Bai

et al. 2023

Preprint

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Conducting electrochemical CO2 reduction with acidic electrolyte is a promising strategy to achieve high utilization efficiency of CO2, which is an essential prerequisite for industrializable CO2 electroreduction technique. Recent progress of CO2 electroreduction in acidic electrolyte has validated that alkali cations in the electrolyte play a vital role to suppress hydrogen evolution and promote CO2 reduction. However, the addition of alkali cations causes precipitation of bicarbonate on gas diffusion electrode (GDE), flooding of electrolyte through GDE, and drifting of the pH of the electrolyte during electrolysis. In this work, we realized the electroreduction of CO2 in metal cation-free acidic electrolyte by covering the catalyst with cross-linked poly-diallyldimethylammonium chloride. This polyelectrolyte provides high density of cationic sites immobilized on the surface of catalyst, which suppresses the mass transport of H+ and modulates the interfacial field strength. By adopting this strategy, the Faradaic efficiency (FE) of CO reached 92% with Ag catalyst and the FE of formic acid reached 74% with In catalyst. More importantly, with metal cation-free acidic electrolyte, the amount of electrolyte flooding through the GDE decreased to 1% of that with alkali cation-containing acidic electrolyte, and the pH values of both catholyte and anolyte kept constant. Thanks to these features, the stability of CO2 reduction performance was greatly improved.

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Organic Additive‐derived Films on Cu Electrodes Promote Electrochemical CO₂ Reduction to C₂₊ Products Under Strongly Acidic Conditions

Cited by 18 publications

References 52 publications

Surfactant‐modified electrode–electrolyte interface for steering CO₂ electrolysis on Cu electrodes

Surfactant‐modified electrode–electrolyte interface for steering CO₂ electrolysis on Cu electrodes

Electrochemical reduction of carbon dioxide to multicarbon (C₂₊) products: challenges and perspectives

Surface-Immobilized Cross-linked Cationic Polyelectrolyte Enables CO2 Reduction with Metal Cation-free Acidic Electrolyte

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Organic Additive‐derived Films on Cu Electrodes Promote Electrochemical CO2 Reduction to C2+ Products Under Strongly Acidic Conditions

Cited by 18 publications

References 52 publications

Surfactant‐modified electrode–electrolyte interface for steering CO2 electrolysis on Cu electrodes

Surfactant‐modified electrode–electrolyte interface for steering CO2 electrolysis on Cu electrodes

Electrochemical reduction of carbon dioxide to multicarbon (C2+) products: challenges and perspectives

Surface-Immobilized Cross-linked Cationic Polyelectrolyte Enables CO2 Reduction with Metal Cation-free Acidic Electrolyte

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Product

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Organic Additive‐derived Films on Cu Electrodes Promote Electrochemical CO₂ Reduction to C₂₊ Products Under Strongly Acidic Conditions

Surfactant‐modified electrode–electrolyte interface for steering CO₂ electrolysis on Cu electrodes

Surfactant‐modified electrode–electrolyte interface for steering CO₂ electrolysis on Cu electrodes

Electrochemical reduction of carbon dioxide to multicarbon (C₂₊) products: challenges and perspectives