Boosting selectivity towards formate production using CuAl alloy nanowires by altering the CO<sub>2</sub>reduction reaction pathway

Badawy, I.; Khedr, Ghada E.; Hafez, Ahmad Mohammad; Ashour, Eman A.; Allam, Nageh K.

doi:10.1039/d3cc02235h

Cited by 12 publications

(10 citation statements)

References 38 publications

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“…As an important liquid-phase product of eCO 2 RR, formate has extensive applications in the pharmaceutical industry, animal feed, and hydrogen energy transportation. 151 Nowadays, indium (In), copper (Cu), and tin (Sn)-containing catalysts are widely studied in eCO 2 RR for CO 2 -to-formate production, 152–154 owing to the favorable *OCHO formation and suitable binding intensity with *HCOOH; but some limitations towards pragmatic application still exist, such as unsatisfied selectivity, moderate stability, and large overpotential. In fact, except for the shape and constituent control of the metal/oxides NPs, the electrocatalytic performance is also determined by the electronic and morphologic characteristics of carbon substrates to some extent.…”

Section: Electrocatalytic Co2 Conversion Of Hollow Carbon-based Mater...mentioning

confidence: 99%

Hollow carbon-based materials for electrocatalytic and thermocatalytic CO₂ conversion

Li,

Kuwahara,

Yamashita

2024

Chem. Sci.

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Section: Electrocatalytic Co2 Conversion Of Hollow Carbon-based Mater...mentioning

confidence: 99%

Hollow carbon-based materials for electrocatalytic and thermocatalytic CO₂ conversion

Li,

Kuwahara,

Yamashita

2024

Chem. Sci.

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“…To this end, the ability of the prepared photoanodes to split water was demonstrated and thoroughly explored. In addition, density functional theory (DFT) is an excellent tool for unveiling the reaction mechanism and electronic properties; , thus, it was implemented in this work to reveal the reason behind the observed oxygen evolution reaction (OER) photocatalytic activity. Furthermore, the impact of incorporating W into the TiO 2 photocatalyst followed by thermal treatment was thoroughly investigated using both experimental measurements as well as DFT modeling.…”

Section: Introductionmentioning

confidence: 99%

Transparent Sn-Decorated W-Doped TiO₂ Multiphase Nanotube Arrays as Efficient Photocatalysts for Solar-Driven Water Splitting

Elbanna,

Mohamed,

Ghanem

et al. 2024

ACS Appl. Eng. Mater.

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Photoelectrochemical water splitting is a crucial step in realizing a green hydrogen economy. Herein, we demonstrate, for the first time, the rational design and optimized fabrication of earth-abundant W-doped TiO 2 thin nanotubular structures decorated with Sn in mixed polymorphs (anatase/brookite/rutile) on F-doped tin oxide substrates via a direct-current sputtering technique and subsequent electrochemical anodization followed by thermal treatment. Sn decoration and W doping along with optimized annealing conditions were elucidated as determinant factors controlling the structural and optical features of the fabricated nanotubes. The resulting highly crystalline polymorphic nanotubes showed an enhanced photocurrent at 0.4 V SCE (1.75 mA/cm 2 ) with a noticeable narrowing in the optical band gap and 25 times compared to pristine TiO 2 nanotubes. The photoluminescence spectra revealed enriched oxygen (O) vacancies upon doping with W and decoration with Sn. The Mott−Schottky plot unveils the variations in the density of charge carriers upon annealing at different temperatures and their role in annihilating these O vacancies. Importantly, the electrochemical impedance spectroscopy elucidation helps to reveal the charge-transfer mechanism in the mixed polymorph junctions of the fabricated nanotubes under dark and illumination conditions, revealing reduced charge-transfer resistance under light-on conditions, which is consistent with the produced photocurrent, lifetime of the electrons, and density of the impurity levels. Moreover, the density functional theory investigation unraveled the development of a homojunction between the brookite and rutile phases that improved the photocatalytic activity toward the oxygen evolution reaction, in agreement with the experimental findings. The findings of this work represent a crucial milestone toward the development of visible-light, earth-abundant, light-absorbing photoanodes for solar-assisted water splitting.

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“…Herein, we demonstrate the design of novel and facile synthesis strategy to anchor iron atoms on N–C network in the form of nanosheet-like morphology, resulting in improved N 2 adsorption on the iron-modified catalyst while suppressing the competing HER. Density functional theory (DFT) calculations have also been employed to elucidate the reaction mechanisms, − electronic properties, and energy barriers. Both experimental and theoretical results are in agreement, confirming the successful design and fabrication of highly active NRR electrochemical catalysts.…”

Section: Introductionmentioning

confidence: 99%

Fe-Single-Atom Catalysts on Nitrogen-Doped Carbon Nanosheets for Electrochemical Conversion of Nitrogen to Ammonia

Agour,

Elkersh,

Khedr

et al. 2023

ACS Appl. Nano Mater.

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Electrochemical nitrogen reduction reaction (NRR) has been established as a promising and sustainable alternative to the Haber−Bosch process, which requires intensive energy to produce ammonia. Unfortunately, NRR is constrained by the high adsorption/activation of the N 2 energy barrier and the competing hydrogen evolution reaction, resulting in low faradic efficiency. Herein, a well-dispersed iron single-atom catalyst was successfully immobilized on nitrogen-doped carbon nanosheets (Fe SAC -N-C) synthesized from pre-hydrothermally derived Fe-doped carbon quantum dots with an average particle size of 2.36 nm and used for efficient electrochemical N 2 fixation at ambient conditions. The as-synthesized Fe SAC -N-C catalyst records an onset potential of 0.12 V RHE , exhibiting a considerable faradic efficiency of 23.7% and an NH 3 yield rate of 3.47 μg h −1 cm −2 in aqueous 0.1 M KOH electrolyte at a potential of −0.1 V RHE under continuous N 2 feeding conditions. The control experiments assert that the produced NH 3 molecules only emerge from the dissolved N 2 -gas, reflecting the remarkable stability of the nitrogen−carbon framework during electrolysis. The DFT calculations showed the Fe SAC -N-C catalyst to demonstrate a lower energy barrier during the rate-limiting step of the NRR process, consistent with the observed high activity of the catalyst. This study highlights the exceptional potential of single-atom catalysts for electrochemical NRR and offers a comprehensive understanding of the catalytic mechanisms involved. Ultimately, this work provides a facile synthesis strategy of Fe SAC -N-C nanosheets with high atomic-dispersion, creating a novel design avenue of Fe SAC -N-C that can vividly have a potential applicability in the large spectrum of electrocatalytic applications.

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Boosting selectivity towards formate production using CuAl alloy nanowires by altering the CO₂reduction reaction pathway

Abstract: Understanding the fundamentals behind an electrocatalyst’s selectivity enables the ability to steer product formation. Herein, we study Cu nanowires lowly doped with Al (12%) for CO2R that enhance formate production...

Cited by 12 publications

References 38 publications

Hollow carbon-based materials for electrocatalytic and thermocatalytic CO₂ conversion

Hollow carbon-based materials for electrocatalytic and thermocatalytic CO₂ conversion

Transparent Sn-Decorated W-Doped TiO₂ Multiphase Nanotube Arrays as Efficient Photocatalysts for Solar-Driven Water Splitting

Fe-Single-Atom Catalysts on Nitrogen-Doped Carbon Nanosheets for Electrochemical Conversion of Nitrogen to Ammonia

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Boosting selectivity towards formate production using CuAl alloy nanowires by altering the CO2reduction reaction pathway

Abstract: Understanding the fundamentals behind an electrocatalyst’s selectivity enables the ability to steer product formation. Herein, we study Cu nanowires lowly doped with Al (12%) for CO2R that enhance formate production...

Cited by 12 publications

References 38 publications

Hollow carbon-based materials for electrocatalytic and thermocatalytic CO2 conversion

Hollow carbon-based materials for electrocatalytic and thermocatalytic CO2 conversion

Transparent Sn-Decorated W-Doped TiO2 Multiphase Nanotube Arrays as Efficient Photocatalysts for Solar-Driven Water Splitting

Fe-Single-Atom Catalysts on Nitrogen-Doped Carbon Nanosheets for Electrochemical Conversion of Nitrogen to Ammonia

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Boosting selectivity towards formate production using CuAl alloy nanowires by altering the CO₂reduction reaction pathway

Hollow carbon-based materials for electrocatalytic and thermocatalytic CO₂ conversion

Hollow carbon-based materials for electrocatalytic and thermocatalytic CO₂ conversion

Transparent Sn-Decorated W-Doped TiO₂ Multiphase Nanotube Arrays as Efficient Photocatalysts for Solar-Driven Water Splitting