Biomimetic electro-oxidation of alkyl sulfides from exfoliated molybdenum disulfide nanosheets

Maachou, Lahcene; Qi, Kun; Petit, Eddy; Qin, Zhaodan; Zhang, Yang; Cot, Didier; Flaud, Valérie; Reibel, Corine; El-Maghrbi, Heba; Li, Lei; Miele, Philippe; Kaplan, Daniel; Chhowalla, Manish; Voiry, Damien

doi:10.1039/d0ta09045j

Cited by 9 publications

(5 citation statements)

References 52 publications

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“…We have recently identified chemically exfoliated MoS2 nanosheets as two-dimensional electrocatalysts for efficient oxidation of organic sulfides to sulfoxides with near-unity selectivity. 32 The nitrate reductase enzyme possesses a Mo (IV) active site coordinated with sulfur coordinating ligands similar to the dimethyl sulfoxide (DMSO) reductase, whereas the nitrogenase is a multinuclear enzyme with MoFe7 clusters as the active sites. Fe-based catalysts have been reported to be promising for NO3RR but the Faradaic efficiency is low because of the competing hydrogen evolution reaction and the formation of nitrogen via the five-electron transfer pathway.…”

Section: Main Textmentioning

confidence: 99%

3.4% Solar‐to‐Ammonia Efficiency from Nitrate Using Fe Single Atomic Catalyst Supported on MoS₂ Nanosheets

Zhang

Liu

et al. 2021

Adv Funct Materials

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Electrochemical synthesis of NH3 is a carbon-free alternative to the traditional Haber-Bosch process. The challenge with nitrogen reduction reaction (NRR) to NH3 is cleavage of the inert N≡N triple bond of nitrogen gas. Obtaining NH3 from environmental pollutants, such as nitrates or nitrites, is a more practical route than NRR. However, reduction of nitrates or nitrites to ammonia is currently hampered by modest Faradaic efficiencies, typically below 10 %. Here, we report a novel heterogeneous catalyst based on iron (Fe) single-atoms supported on two-dimensional MoS2 (Fe-MoS2) for the nitrate reduction reaction (NO3RR). We have found that Fe-MoS2 exhibits remarkable performance with a maximum Faradaic efficiency of 98 % for NO3RR to NH3 at an overpotential of -0.48 V vs. the reversible hydrogen electrode (RHE) as confirmed by our isotopic nuclear magnetic resonance (NMR) analyses. Density function theory (DFT) calculations reveal that the enhanced selectivity for the production of NH3 from single Fe atoms supported on MoS2 is attributed to a reduced energy barrier of 0.38 eV associated with de-oxidation of *NO to *N -the usual potential limiting step in NO3RR. We assembled our catalyst in a two-electrode electrolyzer coupled to an InGaP/GaAs/Ge triple-junction solar cell to demonstrate a solar-to-ammonia (STA) conversion efficiency of 3.4 % and a yield rate of 0.03 mmol h -1 cm -2 equivalent to 510 µg h -1 cm -2 . Our results open new avenues for design of single-atom catalysts (SAC) for the realization of solar-driven ammonia production.

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Section: Main Textmentioning

confidence: 99%

3.4% Solar‐to‐Ammonia Efficiency from Nitrate Using Fe Single Atomic Catalyst Supported on MoS₂ Nanosheets

Zhang

Liu

et al. 2021

Adv Funct Materials

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“…For alkaline HER, the adsorption of H 2 O, OH – , and H + play a crucial role in promoting the kinetics of the catalytic process. The weak gravitational force between the catalyst and the H 2 O molecule or the strong adsorption of OH – retarded the Volmer step, slowed down the proton supply, and resulted in slow kinetics. , The theoretical voltage of OER is 1.23 V, and the reaction process is more complex than HER. Among them, the breaking of the O–H bond and the formation of the O–O bond require high energy to overcome the kinetic energy barrier and drive the reaction, which is considered to be the rate-limiting step in electrocatalytic water decomposition. , Therefore, in practical applications, reducing the overpotential in the HER/OER is a difficult problem to overcome.…”

Section: Introductionmentioning

confidence: 99%

Oxygen Vacancy and Heterostructure Modulation of Co₂P/Fe₂P Electrocatalysts for Improving Total Water Splitting

Liu,

Hu,

Zhao

et al. 2024

ACS Appl. Mater. Interfaces

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Designing a stable and highly active catalyst for hydrogen evolution and oxygen evolution reactions (HER/OER) is essential for the industrialization of hydrogen energy but remains a major challenge. This work reports a simple approach to fabricating coupled Co 2 P/Fe 2 P nanorod array catalyst for overall water decomposition, demonstrating the source of excellent activity in the catalytic process. Under alkaline conditions, Co 2 P/Fe 2 P heterostructures exhibit an overpotential of 96 and 220 mV for HER and OER, respectively, at 10 mA cm −2 . For total water splitting, a low voltage of 1.56 V is required to provide a current density of 10 mA cm −2 . And the catalyst exhibits long-term durability for 30 h at a high current density of 250 mA cm −2 . The analysis of the results revealed that the presence of interfacial oxygen vacancies and the strong interaction between Co 2 P/Fe 2 P provided the catalyst with more electrochemically active sites and a faster charge transfer capability, which improved the hydrolysis dissociation process. Electrochemically active metal (oxygen) hydroxide phases were produced after OER stability testing. The results of this study prove its great potential in practical industrial electrolysis and provide a reasonable and feasible strategy for the design of nonprecious metal phosphide electrocatalysts.

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“…Hydrogen, as a clean and sustainable energy source, has become a vital substitute for fossil fuels. [1][2][3][4][5][6] At present, hydrogen is mainly produced through the electrolysis of water, which involves the hydrogen evolution reaction (HER) at the cathode and the oxygen evolution reaction (OER) at the anode. The noble metal-based catalysts, such as Pt, Ru and their alloys, [7][8][9][10] have been proven to be highly efficient for HER, but the scarce resources and high prices severely limit their large-scale applications.…”

Section: Introductionmentioning

confidence: 99%

Molybdenum phosphide nanoparticles encapsulated with biomolecule-derived N, P-codoped carbon nanosheets for the synergistic hydrogen evolution reaction

Peng,

Liu,

Huang

2024

New J. Chem.

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Biomimetic electro-oxidation of alkyl sulfides from exfoliated molybdenum disulfide nanosheets

Abstract: High electrocatalytic performance of biomimetic exfoliated molybdenum disulfide nanosheets towards the electro-oxidation of alkyl sulfides.

Cited by 9 publications

References 52 publications

3.4% Solar‐to‐Ammonia Efficiency from Nitrate Using Fe Single Atomic Catalyst Supported on MoS₂ Nanosheets

3.4% Solar‐to‐Ammonia Efficiency from Nitrate Using Fe Single Atomic Catalyst Supported on MoS₂ Nanosheets

Oxygen Vacancy and Heterostructure Modulation of Co₂P/Fe₂P Electrocatalysts for Improving Total Water Splitting

Molybdenum phosphide nanoparticles encapsulated with biomolecule-derived N, P-codoped carbon nanosheets for the synergistic hydrogen evolution reaction

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Biomimetic electro-oxidation of alkyl sulfides from exfoliated molybdenum disulfide nanosheets

Abstract: High electrocatalytic performance of biomimetic exfoliated molybdenum disulfide nanosheets towards the electro-oxidation of alkyl sulfides.

Cited by 9 publications

References 52 publications

3.4% Solar‐to‐Ammonia Efficiency from Nitrate Using Fe Single Atomic Catalyst Supported on MoS2 Nanosheets

3.4% Solar‐to‐Ammonia Efficiency from Nitrate Using Fe Single Atomic Catalyst Supported on MoS2 Nanosheets

Oxygen Vacancy and Heterostructure Modulation of Co2P/Fe2P Electrocatalysts for Improving Total Water Splitting

Molybdenum phosphide nanoparticles encapsulated with biomolecule-derived N, P-codoped carbon nanosheets for the synergistic hydrogen evolution reaction

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Product

Resources

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3.4% Solar‐to‐Ammonia Efficiency from Nitrate Using Fe Single Atomic Catalyst Supported on MoS₂ Nanosheets

3.4% Solar‐to‐Ammonia Efficiency from Nitrate Using Fe Single Atomic Catalyst Supported on MoS₂ Nanosheets

Oxygen Vacancy and Heterostructure Modulation of Co₂P/Fe₂P Electrocatalysts for Improving Total Water Splitting