Defected MoS2: An efficient electrochemical nitrogen reduction catalyst under mild conditions

Ma, Chaoqun; Zhai, Naihua; Liu, Bingping; Yan, Shihai

doi:10.1016/j.electacta.2020.137695

Cited by 47 publications

(25 citation statements)

References 59 publications

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“…In contrast, in the 1T’ phase, they tend to disperse [24] . A number of studies have shown that sulphur vacancies in TMDs could activate N 2 and enhance the NRR performance of TMDs [17a,22m,n,23a] …”

Section: Introductionmentioning

confidence: 99%

NO Electroreduction by Transition Metal Dichalcogenides with Chalcogen Vacancies

Tursun

2021

ChemElectroChem

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Nitric oxide electroreduction reaction (NOER) is one of the most attractive routes for ammonia synthesis and NOx‐related pollutant treatment. However, current research on NOER catalysts mainly focus on noble metals and single atom catalysts, while low‐cost transition metal dichalcogenides (TMDs) are rarely considered, let alone their product selectivity. Herein, using first‐principles calculations, we systematically investigate the performance of a series of single‐layer TMDs (MoS2, MoSe2, MoTe2, TaTe2 and WTe2) in the 1T’ phase as electrocatalysts for NOER. Our results reveal that defective 1T’‐MoS2 and 1T’‐MoSe2 monolayers (with the most common sulphur and selenium vacancies, respectively) exhibit excellent activity for NOER as well as high selectivity for ammonia, which can be correspondingly yielded at 0 and −0.06 V potentials, comparable to the best Pt‐based and single atom catalysts. Furthermore, these two catalysts efficiently suppress the competing hydrogen evolution reaction (HER). Thus, single‐layer TMDs synthesized with chalcogen vacancies may serve as efficient catalysts for electrochemical ammonia synthesis from pollutants and electrocatalytic denitrification.

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Section: Introductionmentioning

confidence: 99%

NO Electroreduction by Transition Metal Dichalcogenides with Chalcogen Vacancies

Tursun

2021

ChemElectroChem

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“…In the potential range from −0.5 to −0.7 V versus RHE, the yield rate of NH 3 increases with the increasing of the negative applied potential, which is attributed to the increased current density and that NRR dominates the electrode process at the cathode. However, when the negative applied potential was below −0.7 V versus RHE, the NH 3 yield rate decreased, which can be attributed to the fact that hydrogen species adsorption on the electrode surface prevented N 2 adsorption and reduction. , …”

Section: Results and Discussionmentioning

confidence: 99%

“…However, when the negative applied potential was below −0.7 V versus RHE, the NH 3 yield rate decreased, which can be attributed to the fact that hydrogen species adsorption on the electrode surface prevented N 2 adsorption and reduction. 53,54 To identify that the produced NH 3 originated from the electrocatalytic conversion of N 2 by antimonene, the control experiments were carried out, including runs with an Arsaturated electrolyte at −0.7 V versus RHE and with a carbon paper electrode at −0.7 V versus RHE under N 2 , respectively. The feeble signals were found in the corresponding UV−vis absorption spectra compared with that of the fresh electrolyte (Figure 3c), which suggests that little NH 3 product was detected under these conditions due to the trace amount of NH 3 in air.…”

Section: Resultsmentioning

confidence: 99%

Defect Regulating of Few-Layer Antimonene from Acid-Assisted Exfoliation for Enhanced Electrocatalytic Nitrogen Fixation

Cao

Sun

Guo

et al. 2021

ACS Appl. Mater. Interfaces

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Nitrogen reduction reaction (NRR), as a green and sustainable technology, is far from a practical application due to the lack of efficient electrocatalysts. In this work, we found that antimonene, a group-VA elemental two-dimensional (2D) material, is attractive as an electrocatalyst for NRR. The antimonene here is acquired through chemical exfoliation of antimony (Sb) using H2SO4 for the first time, which simultaneously achieved efficient large-sized exfoliation and created a high density of active edge sites. Moreover, the concentration of defects shows a gradual increasing tendency as the treatment time extends. The obtained antimonene exhibited favorable average ammonia (NH3) yield and Faradaic efficiency as high as 2.08 μg h–1 cm–2 and 14.25% at −0.7 V versus RHE, respectively. Density functional theory calculations prove that the sufficient exposure of edge defects is favorable for reducing the reaction barrier and strengthening the interaction between antimonene and the intermediates of NRR, thus increasing the selectivity and yield rate of NH3. The chemical exfoliation of Sb reported here offers an alternative avenue to engineer the surface structures of group-VA elemental-based catalysts. Investigation of NRR using 2D antimonene can further provide deep insight into the mechanism and principle of NRR over group-VA elemental nanosheets.

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“…In addition, preparation of the working electrode, electrochemical NRR measurements, determination of NH 3 and N 2 H 4 as well as calculation of the NH 3 yield and FE are the same as our previous work. [58]…”

Section: Methodsmentioning

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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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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Defected MoS2: An efficient electrochemical nitrogen reduction catalyst under mild conditions

Cited by 47 publications

References 59 publications

NO Electroreduction by Transition Metal Dichalcogenides with Chalcogen Vacancies

NO Electroreduction by Transition Metal Dichalcogenides with Chalcogen Vacancies

Defect Regulating of Few-Layer Antimonene from Acid-Assisted Exfoliation for Enhanced Electrocatalytic Nitrogen Fixation

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

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Defected MoS2: An efficient electrochemical nitrogen reduction catalyst under mild conditions

Cited by 47 publications

References 59 publications

NO Electroreduction by Transition Metal Dichalcogenides with Chalcogen Vacancies

NO Electroreduction by Transition Metal Dichalcogenides with Chalcogen Vacancies

Defect Regulating of Few-Layer Antimonene from Acid-Assisted Exfoliation for Enhanced Electrocatalytic Nitrogen Fixation

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

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