Robust carbon dioxide reduction on molybdenum disulphide edges

Asadi, Mohammad; Kumar, Bijandra; Behranginia, Amirhossein; Rosen, Brian A.; Baskin, Artem; Repnin, Nikita; Pisasale, Davide; Phillips, Patrick J.; Zhu, Wei; Haasch, Richard T.; Klie, Robert F.; Král, Petr; Abiade, Jeremiah T.; Salehi‐Khojin, Amin

doi:10.1038/ncomms5470

Cited by 670 publications

(601 citation statements)

References 44 publications

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“…In 2014, Salehi‐Khojin and co‐workers first experimentally demonstrated bulk MoS 2 as a highly efficient electrocatalyst for selectively reducing CO 2 to CO with a small overpotential of 54 mV in a mixture of 96 mol% water and 4 mol% EMIM‐BF 4 101. An impressive cathodic current density of ≈65 mA cm −2 and a CO Faradaic efficient of 98% were delivered at η = 0.65 V, much improved than Au and Ag NPs.…”

Section: Electrocatalytic Materials For Co2 Reductionmentioning

confidence: 99%

CO₂ Reduction: From the Electrochemical to Photochemical Approach

et al. 2017

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Increasing CO2 concentration in the atmosphere is believed to have a profound impact on the global climate. To reverse the impact would necessitate not only curbing the reliance on fossil fuels but also developing effective strategies capture and utilize CO2 from the atmosphere. Among several available strategies, CO2 reduction via the electrochemical or photochemical approach is particularly attractive since the required energy input can be potentially supplied from renewable sources such as solar energy. In this Review, an overview on these two different but inherently connected approaches is provided and recent progress on the development, engineering, and understanding of CO2 reduction electrocatalysts and photocatalysts is summarized. First, the basic principles that govern electrocatalytic or photocatalytic CO2 reduction and their important performance metrics are discussed. Then, a detailed discussion on different CO2 reduction electrocatalysts and photocatalysts as well as their generally designing strategies is provided. At the end of this Review, perspectives on the opportunities and possible directions for future development of this field are presented.

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Section: Electrocatalytic Materials For Co2 Reductionmentioning

confidence: 99%

CO₂ Reduction: From the Electrochemical to Photochemical Approach

et al. 2017

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“…In HER, electrons from the external circuit combine with protons from an electrolyte at a catalytic site resulting in the formation of H2 molecules. For the semiconducting 2H polytype of many TMDs, it is known that the catalytic active sites reside on the nanosheet edge [36][37][38][39][40][41] and are probably terminal disulphide groups. 38 reported using MoS2 nanosheets of different sizes to catalyse the HER.…”

Section: Introductionmentioning

confidence: 99%

Electrochemical Applications of Two-Dimensional Nanosheets: The Effect of Nanosheet Length and Thickness

et al. 2016

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Although many electrochemical properties of 2D materials depend sensitively on the nanosheet dimensions, there are no systematic, quantitative studies which analyse the effect of nanosheet size and thickness on electrochemical parameters. Here we use size-selected WS2 nanosheets as a model system to determine the effect of nanosheet dimensions in two representative areas -hydrogen evolution electrocatalytic electrodes and electrochemical double layer capacitor electrodes. We chose these applications as they depend on the interaction of ions with the nanosheet edge and basal plane, respectively, and so would be expected to be nanosheet-size-dependent. The data shows the catalytic current density to scale inversely with mean nanosheet length while the volumetric double layer capacitance scales inversely with mean nanosheet thickness. Both of these results are consistent with simple models allowing use to extract intrinsic quantities, namely the turnover frequency and the double layer thickness respectively.3

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“…MoS 2 for instance has been widely used as an efficient catalyst for water splitting 22,23 and hydrodesulphurization, 24,25 whereas a recent report has shown its superior CO 2 reduction performance in an ionic liquid, compared to the noble metals, with a a) Electronic addresses: N.Y.Dzade@uu.nl and N.H.Deleeuw@uu.nl high current density and low overpotential (54 mV). 26 Ironnickel sulfide membranes formed in hydrothermal systems in the deep ocean floor are increasingly considered to be the early catalysts for a series of biochemical reactions leading to the emergence of life. [27][28][29][30] The anaerobic production of acetate, formaldehyde, and amino acids, and the nucleic acid bases (the organic precursors for larger biomolecules) are thought to have been catalyzed by small cubane (Fe, Ni)S clusters (for example, Fe 5 NiS 8 ), which are structurally similar to the surfaces of present day sulfide minerals such as greigite (Fe 3 S 4 ), 31 violarite (FeNi 2 S 4 ), 32 and mackinawite (FeS).…”

Section: Introductionmentioning

confidence: 99%

Activation and dissociation of CO2 on the (001), (011), and (111) surfaces of mackinawite (FeS): A dispersion-corrected DFT study

Dzade

Roldan

Leeuw

2015

The Journal of Chemical Physics

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Iron sulfide minerals, including mackinawite (FeS), are relevant in origin of life theories, due to their potential catalytic activity towards the reduction and conversion of carbon dioxide (CO 2 ) to organic molecules, which may be applicable to the production of liquid fuels and commodity chemicals. However, the fundamental understanding of CO 2 adsorption, activation, and dissociation on FeS surfaces remains incomplete. Here, we have used density functional theory calculations, corrected for long-range dispersion interactions (DFT-D2), to explore various adsorption sites and configurations for CO 2 on the low-index mackinawite (001), (110), and (111) surfaces. We found that the CO 2 molecule physisorbs weakly on the energetically most stable (001) surface but adsorbs relatively strongly on the (011) and (111) FeS surfaces, preferentially at Fe sites. The adsorption of the CO 2 on the (011) and (111) surfaces is shown to be characterized by significant charge transfer from surface Fe species to the CO 2 molecule, which causes a large structural transformation in the molecule (i.e., forming a negatively charged bent CO 2 −δ species, with weaker C-O confirmed via vibrational frequency analyses). We have also analyzed the pathways for CO 2 reduction to CO and O on the mackinawite (011) and (111) surfaces. CO 2 dissociation is calculated to be slightly endothermic relative to the associatively adsorbed states, with relatively large activation energy barriers of 1.25 eV and 0.72 eV on the (011) and (111)

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Robust carbon dioxide reduction on molybdenum disulphide edges

Cited by 670 publications

References 44 publications

CO₂ Reduction: From the Electrochemical to Photochemical Approach

CO₂ Reduction: From the Electrochemical to Photochemical Approach

Electrochemical Applications of Two-Dimensional Nanosheets: The Effect of Nanosheet Length and Thickness

Activation and dissociation of CO2 on the (001), (011), and (111) surfaces of mackinawite (FeS): A dispersion-corrected DFT study

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Robust carbon dioxide reduction on molybdenum disulphide edges

Cited by 670 publications

References 44 publications

CO2 Reduction: From the Electrochemical to Photochemical Approach

CO2 Reduction: From the Electrochemical to Photochemical Approach

Electrochemical Applications of Two-Dimensional Nanosheets: The Effect of Nanosheet Length and Thickness

Activation and dissociation of CO2 on the (001), (011), and (111) surfaces of mackinawite (FeS): A dispersion-corrected DFT study

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CO₂ Reduction: From the Electrochemical to Photochemical Approach

CO₂ Reduction: From the Electrochemical to Photochemical Approach