A Guideline to Determine Faradaic Efficiency in Electrochemical CO<sub>2</sub> Reduction

Dutta, Nilutpal; Bagchi, Debabrata; Chawla, Geetansh; Peter, Sebastian C.

doi:10.1021/acsenergylett.3c02362

Cited by 9 publications

(4 citation statements)

References 39 publications

(71 reference statements)

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“…The catalytic performance along with current density has been further increased by the use of a flow cell and gas diffusion electrode (Figures S20a,b and S21a,b) by proper optimization of the gas–catalyst–electrolyte (Figure S22a) interface. − The basic design of a flow cell and its various components have been demonstrated pictorially in Figure S21a,b. In the flow cell, the current density (Figure S21a) and FE of all the CO 2 -reduced products (Figure S21b) have increased than that of obtained in the H-cell suppressing the hydrogen evolution reaction .…”

Section: Resultsmentioning

confidence: 99%

Unraveling the Cooperative Mechanisms in Ultralow Copper-Loaded WC@NGC for Enhanced CO₂ Electroreduction to Acetic Acid

Bagchi,

Riyaz,

Raj

et al. 2024

Chem. Mater.

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Electrochemical CO2 reduction reaction (eCO2RR) has been explored on tungsten carbide (WC) nanoparticles embedded on N-doped graphitic carbon (NGC), demonstrating excellent activity toward the formation of acetic acid at an extremely lower potential. The activity has been further enhanced by loading ultralow copper sites into the catalyst system, exhibiting 80.02% Faradaic efficiency (FE) toward acetic acid at an applied potential of −0.3 V (vs RHE). Potential-dependent in situ infrared (IR), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, ex situ extended X-ray absorption fine structure (EXAFS) studies, and computational analysis confirm that synergy between uniformly dispersed Cu atoms and WC lattice plays a crucial role in the formation of acetic acid with high FE at a lower potential. It has been observed that the W atom of WC strongly chemisorbs CO2 with a significant change in the C–O bond length and the O–C–O bond angle, in contrast to weaker adsorption on Cu-based catalyst surfaces. The presence of a Cu site enhances the adsorption of CO2, thereby increasing the possibility of C–C coupling kinetically. Most importantly, hydrogen evolution predominates on the catalyst’s surface at higher applied potentials (−0.5 to −1.1 V vs RHE), elucidating the mechanism underlying enhanced charge transfer between copper and WC, a phenomenon ascertained through in situ IR spectroscopy and ex situ XPS analysis

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Section: Resultsmentioning

confidence: 99%

Unraveling the Cooperative Mechanisms in Ultralow Copper-Loaded WC@NGC for Enhanced CO₂ Electroreduction to Acetic Acid

Bagchi,

Riyaz,

Raj

et al. 2024

Chem. Mater.

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“…Prior to the CO 2 reduction studies, the GC was calibrated with known concentrations of both CO and H 2 . After quantification of the gaseous products, the faradaic efficiency was calculated using the following eq: FE g = n × x × F × ϑ flowrate × P R × T × I where n = number of electrons required to convert 1 mol of a particular product. x = concentration of obtained gaseous products, F = Faraday constant (96485 C/mol), ϑ flow rate = volumetric flow rate, P = 101325 Pa, R = gas constant (8.314 J/mol K), T = 298 K, and I = average current density after steady state (A).…”

Section: Methodsmentioning

confidence: 99%

Bilayer Porous Electrocatalysts for Stable and Selective Electrochemical Reduction of CO₂ to Formate in the Presence of Flue Gas Containing NO and SO₂

Prasad,

Chandiran,

Chetty

2024

ACS Appl. Mater. Interfaces

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The development of stable and selective electrocatalysts for converting CO 2 to value-added chemicals or fuels has gained much interest in terms of their potential to mitigate anthropogenic carbon emissions. Most of the electrocatalysts are tested under pure CO 2 ; however, industrial outlet flue gas contains numerous impurities, such as NO and SO 2 , which poison the electrocatalysts and alter the product selectivity. Developing electrocatalysts that are resistant to such impurities is essential for commercial implementation. Herein, we prepared bilayer porous electrocatalysts, namely, Sn, Bi, and In, on porous Cu foam mesh (Sn/Cu-f, Bi/Cu-f, and In/Cu-f) by a two-step electrodeposition process and employed these electrodes for the electrochemical reduction of CO 2 to formate. It was observed that the bilayer porous electrocatalysts exhibited high CO 2 reduction activity compared to catalysts coated on a Cu mesh. Among bilayer porous electrocatalysts, Sn/Cu-f and Bi/Cu-f electrocatalysts showed more than 80% faradaic efficiency (FE) toward formate production, with a formate partial current density of around −16 and −10.4 mA cm −2 , respectively, at −1.02 V vs RHE. In/Cu-f electrocatalyst showed nearly 40% formate FE with formate partial current density of −15 mA cm −2 at −1.22 V vs RHE. We investigated the effect of NO and SO 2 impurities (500 ppm of NO, 800 ppm of SO 2 , and 500 ppm of NO + 800 ppm of SO 2 ) on these electrocatalysts' selectivity and stability toward formate. It was observed that the Bi/Cu-f electrocatalyst showed 50 h stability with 80 ± 5% formate FE, and Sn/Cu-f showed 18 h stability with above 80 ± 5% efficiency in the presence of NO and SO 2 mixed with CO 2 . Furthermore, we studied the effect of CO 2 concentration with Sn/Cu-f and Bi/Cu-f catalysts in the range of 15−100% CO 2 , for which formate FEs of 45−80% were observed.

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“…Addressing this urgent issue necessitates the development of innovative methodologies, such as the electrochemical conversion of CO 2 using renewable energy sources, to mitigate its harmful impacts. Notwithstanding significant advancements in this domain, a fundamental understanding of the mechanisms governing the synthesis of higher carbon (>C 2 ) products from CO 2 remains elusive, impeding the rational design of effective catalysts. − …”

Section: Introductionmentioning

confidence: 99%

Lattice Charge Tuning-Driven Multi-Carbon Products from Carbon Dioxide

Chawla,

Sarma,

Raj

et al. 2024

ACS Sustainable Chem. Eng.

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A Guideline to Determine Faradaic Efficiency in Electrochemical CO₂ Reduction

Cited by 9 publications

References 39 publications

Unraveling the Cooperative Mechanisms in Ultralow Copper-Loaded WC@NGC for Enhanced CO₂ Electroreduction to Acetic Acid

Unraveling the Cooperative Mechanisms in Ultralow Copper-Loaded WC@NGC for Enhanced CO₂ Electroreduction to Acetic Acid

Bilayer Porous Electrocatalysts for Stable and Selective Electrochemical Reduction of CO₂ to Formate in the Presence of Flue Gas Containing NO and SO₂

Lattice Charge Tuning-Driven Multi-Carbon Products from Carbon Dioxide

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A Guideline to Determine Faradaic Efficiency in Electrochemical CO2 Reduction

Cited by 9 publications

References 39 publications

Unraveling the Cooperative Mechanisms in Ultralow Copper-Loaded WC@NGC for Enhanced CO2 Electroreduction to Acetic Acid

Unraveling the Cooperative Mechanisms in Ultralow Copper-Loaded WC@NGC for Enhanced CO2 Electroreduction to Acetic Acid

Bilayer Porous Electrocatalysts for Stable and Selective Electrochemical Reduction of CO2 to Formate in the Presence of Flue Gas Containing NO and SO2

Lattice Charge Tuning-Driven Multi-Carbon Products from Carbon Dioxide

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A Guideline to Determine Faradaic Efficiency in Electrochemical CO₂ Reduction

Unraveling the Cooperative Mechanisms in Ultralow Copper-Loaded WC@NGC for Enhanced CO₂ Electroreduction to Acetic Acid

Unraveling the Cooperative Mechanisms in Ultralow Copper-Loaded WC@NGC for Enhanced CO₂ Electroreduction to Acetic Acid

Bilayer Porous Electrocatalysts for Stable and Selective Electrochemical Reduction of CO₂ to Formate in the Presence of Flue Gas Containing NO and SO₂