A DFT screening of single transition atoms supported on MoS<sub>2</sub> as highly efficient electrocatalysts for the nitrogen reduction reaction

Zhai, Xingwu; Li, Lei; Liu, Xiaoyue; Li, Yafei; Yang, Jueming; Yang, Dezheng; Zhang, Jinli; Yan, Hongxia; Ge, Guixian

doi:10.1039/d0nr00030b

Cited by 112 publications

(89 citation statements)

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“…As shown in Figure 2a, for the MoS 2 system, the Mo atoms contribute to the valence band maximum (VBM) near the Fermi level (−0.03 eV), which also contribute to the conduction band minimum (CBM) about 1.65 eV. Therefore, the predicted bandgap of the MoS 2 monolayer is 1.68 eV, which is comparable to the literature [45,60] . Regarding the D‐MoS 2 system, the peak of Mo and S atoms are noticeably down‐shifted to 1.20 eV, and a new sharp peak appears above the Fermi level about 0.75 eV, which is primarily attributed to the formation of the vacancy defect.…”

Section: Resultssupporting

confidence: 72%

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Sulfur‐Vacancy Defective MoS₂ as a Promising Electrocatalyst for Nitrogen Reduction Reaction under Mild Conditions

Liu

et al. 2021

ChemElectroChem

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Developing low‐cost and efficient nanomaterials to transform nitrogen to ammonia under mild conditions is an attractive topic in chemistry and is significant for sustaining agriculture and life. In this work, the catalytic performance of three types of MoS2 electrocatalysts is systematically investigated. The density of states shows noticeable improvement in the electrical conductivity for sulfur‐vacancy defective MoS2 (VS‐MoS2) than that of pure MoS2, as it facilitates the following electrocatalytic nitrogen reduction reaction (NRR). VS‐MoS2 possesses excellent NRR catalytic performance with a limiting potential of −0.48 V, an outstanding NH3 average yield of 29.55 μg h−1 mgcat.−1 at −0.5 V versus reversible hydrogen electrode (RHE), and a high faraday efficiency of 4.58 % at −0.3 V vs RHE. The hydrogenation of *N‐NH to *NH‐NH is the rate determining step of the enzymatic mechanism. These results demonstrate the feasibility of VS‐MoS2 for electrocatalytic ammonia synthesis.

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Section: Resultssupporting

confidence: 72%

“…have predicted that the single Mo‐atom embedded MoS 2 nanosheets is an efficient NRR catalyst with an energy barrier of 0.53 eV [44] . Ge et al reported the excellent NRR performance of the single Re atom supported on MoS 2 [45] . Moreover, Zeng et al.…”

Section: Introductionmentioning

confidence: 99%

Sulfur‐Vacancy Defective MoS₂ as a Promising Electrocatalyst for Nitrogen Reduction Reaction under Mild Conditions

Liu

et al. 2021

ChemElectroChem

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“…At present, the DFT method is widely used for systems of TM atoms supported on 2D materials as SACs. Therefore, for calculational cost reasons and to facilitate comparisons with similar previous reports, [28][29][30][31] we adopted the DFT method in this study. Figure 9.…”

Section: Thermodynamic Stabilitymentioning

confidence: 99%

Computational Screening of 3 d Transition Metal Atoms Anchored on Defective Graphene for Efficient Electrocatalytic N₂ Fixation

et al. 2021

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The synthesis of ammonia (NH 3 ) through the electrochemical reduction of molecular nitrogen (N 2 ) is a promising strategy for significantly reducing energy consumption compared to traditional industrial processes. Herein, we report the design of a series of monovacancy and divacancy defective graphenes decorated with single 3d transition metal atoms (TM@MVG and TM@DVG; TM=ScÀ Zn) as electrocatalysts for the nitrogenreduction reaction (NRR) aided by density functional theory (DFT) calculations. By comparing energies for N 2 adsorption as well as the free energies associated with *N 2 activation and *N 2 H formation, we successfully identified V@MVG, with the lowest potential of À 0.63 V, to be an effective catalytic substrate for the NRR in an enzymatic mechanism. Electronic properties, including Bader charges, charge density differences, partial densities of states, and crystal orbital Hamilton populations, are further analyzed in detail. We believe that these results help to explain recent observations in this field and provide guidance for the exploration of efficient electrocatalysts for the NRR.

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“…(e) Atomic models of single transition metal atom catalysts anchored on the B monovacancy of the h-BN monolayer [44] . [48] , Copyright © 2020, Royal Society of Chemistry Figure 5 (Color online) Catalytic performance of 2D MoS 2 for electroreduction of N 2 . (a) The optimized configurations (top and side views) of diatomic boron and single-atom boron doped MoS 2 nanosheets, as well as the main Mo-B bond lengths and binding energy [46] , Copyright © 2019, Royal Society of Chemistry.…”

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confidence: 99%

“…(b) Screening results of TM@MoS 2 systems for NRR processes using the free energy changes of two thermodynamically unfavorable protonation steps (ΔG(*N 2 -*NNH) and ΔG(*NH 2 -*NH 3 )) [47] , Copyright © 2017, John Wiley & Sons. (c), (d) Relationships between φ and ΔG(*NNH) and ΔG* [48] , Copyright © 2020, Royal Society of Chemistry [53] , Copyright © 2016, American Chemical Society. (b) NRR和HER的起始电位之差 [53] , Copyright © 2020, Royal Society of Chemistry.…”

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confidence: 99%

Advances in two dimensional electrochemical catalysts for ammonia synthesis

Zhu¹,

Li²

2020

Chin. Sci. Bull.

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A DFT screening of single transition atoms supported on MoS₂ as highly efficient electrocatalysts for the nitrogen reduction reaction

Abstract: Re@MoS2 possesses the best NRR catalytic activity with a limiting potential of −0.43 V among TM@MoS2 systems.

Cited by 112 publications

References 70 publications

Sulfur‐Vacancy Defective MoS₂ as a Promising Electrocatalyst for Nitrogen Reduction Reaction under Mild Conditions

Sulfur‐Vacancy Defective MoS₂ as a Promising Electrocatalyst for Nitrogen Reduction Reaction under Mild Conditions

Computational Screening of 3 d Transition Metal Atoms Anchored on Defective Graphene for Efficient Electrocatalytic N₂ Fixation

Advances in two dimensional electrochemical catalysts for ammonia synthesis

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A DFT screening of single transition atoms supported on MoS2 as highly efficient electrocatalysts for the nitrogen reduction reaction

Abstract: Re@MoS2 possesses the best NRR catalytic activity with a limiting potential of −0.43 V among TM@MoS2 systems.

Cited by 112 publications

References 70 publications

Sulfur‐Vacancy Defective MoS2 as a Promising Electrocatalyst for Nitrogen Reduction Reaction under Mild Conditions

Sulfur‐Vacancy Defective MoS2 as a Promising Electrocatalyst for Nitrogen Reduction Reaction under Mild Conditions

Computational Screening of 3 d Transition Metal Atoms Anchored on Defective Graphene for Efficient Electrocatalytic N2 Fixation

Advances in two dimensional electrochemical catalysts for ammonia synthesis

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A DFT screening of single transition atoms supported on MoS₂ as highly efficient electrocatalysts for the nitrogen reduction reaction

Sulfur‐Vacancy Defective MoS₂ as a Promising Electrocatalyst for Nitrogen Reduction Reaction under Mild Conditions

Sulfur‐Vacancy Defective MoS₂ as a Promising Electrocatalyst for Nitrogen Reduction Reaction under Mild Conditions

Computational Screening of 3 d Transition Metal Atoms Anchored on Defective Graphene for Efficient Electrocatalytic N₂ Fixation