Incorporated oxygen in MoS<sub>2</sub> ultrathin nanosheets for efficient ORR catalysis

Huang, Hao; Feng, Xiang; Du, Cuicui; Wu, Siyuan; Song, Wenbo

doi:10.1039/c5ta01600b

Cited by 98 publications

(62 citation statements)

References 36 publications

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“…The advent of doped TMDs as activated electrocatalysts in clean‐energy production, due to the enhanced intrinsic activity, conductivity, and higher density of actives sites for the TMDs upon doping, has cast the spotlight on the electrocatalytic performance of Group 5 transition‐metal‐doped WSe 2 . Replete with brilliant expectations, we investigated the electrocatalytic properties of WSe 2 before and after doping with V, Nb, and Ta metals for the hydrogen‐evolution reaction (HER) and the oxygen‐reduction reaction (ORR) by using linear sweep voltammetry (LSV).…”

Section: Resultsmentioning

confidence: 66%

Morphological Effects and Stabilization of the Metallic 1T Phase in Layered V‐, Nb‐, and Ta‐Doped WSe₂ for Electrocatalysis

Chia

Sutrisnoh

Sofer

et al. 2018

Chemistry A European J

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Layered transition-metal dichalcogenides (TMDs) are valued for their electrocatalytic properties toward the hydrogen-evolution reaction (HER) and oxygen-reduction reaction (ORR). One effective strategy to activate the electrocatalytic properties of TMDs is through doping. The optimistic outlook of doped-MoS as an electrocatalyst witnessed in previous reports spurred us to examine the effect of doping WSe with Group 5 transition-metal species, namely V, Nb, and Ta, in aspects of inherent electroactivities and catalysis. Apart from the mild reduction signal unique to the Group 5 transition-metal dopants, the Group 5 transition-metal-doped WSe materials are found to possess largely identical inherent electrochemistry to the undoped WSe with a characteristic anodic peak. Living up to expectations, the Group 5 transition-metal-doped WSe materials exhibit improved electrocatalytic HER efficiency, as evident by the lower HER overpotentials and Tafel slopes relative to undoped WSe . After doping with V, Nb, or Ta species, an increased number of active sites is observed given the distinct changes in morphology from thick bulky pieces in undoped WSe to thinner fragments in doped WSe . Although undoped WSe exists in the semiconducting 2H phase, the Group 5 transition-metal-doped WSe materials are dominated by the metallic 1T phase. Doping WSe with V, Nb, or Ta stabilizes the catalytic 1T phase and appears to induce the transition from the 2H to 1T phase. In contrast to the enhanced HER performance of WSe upon doping, Group 5 transition-metal dopants proved futile in activating the ORR electrocatalytic behavior of WSe , for which the ORR efficiency is unchanged. Therefore, these findings facilitate the understanding of the role of Group 5 transition-metal dopants in the electrochemical and catalytic properties of WSe relative to their morphological features and provide an evaluation of the efficacy of doping TMDs in electrocatalytic applications.

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Section: Resultsmentioning

confidence: 66%

Morphological Effects and Stabilization of the Metallic 1T Phase in Layered V‐, Nb‐, and Ta‐Doped WSe₂ for Electrocatalysis

Chia

Sutrisnoh

Sofer

et al. 2018

Chemistry A European J

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“…In addition, heteroatom doping in MoS 2 has also shown some encouraging results for ORR both experimentally and theoretically where the dopant act as a catalytic site. [62][63][64][65][66][67][68][69][70]71] Thus, motivated by these ongoing advancements, in this paper we perform a detailed analysis of various N-and P-doped TMDs (MoS 2 , MoSe 2 , WS 2, and WSe 2 ) for their possible application as a high-performance electrocatalyst for ORR. Our density functional theory (DFT) computations reveal that N-/Pdoping at a single S/Se vacancy is energetically more favourable in metal-rich conditions.…”

Section: Introductionmentioning

confidence: 99%

Activating Transition Metal Dichalcogenides by Substitutional Nitrogen‐Doping for Potential ORR Electrocatalysts

2018

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One of the challenging goals in the large‐scale realization of hydrogen‐based fuel cells is to replace or minimize the use of expensive Pt‐based electrocatalysts to reduce molecular oxygen at the cathode. Recently, non‐metal doped nanosheets of transition metal dichalcogenides (TMDs) have emerged as a promising Pt‐free electrocatalyst for hydrogen evolution reaction. Herein, we investigate the potential of nitrogen‐ and phosphorus‐ (N‐ and P‐) doped TMDs (MoS2, MoSe2, WS2, and WSe2) as high‐performing electrocatalysts for ORR using first principle calculations, motivated by recent experimental advances to incorporate single S/Se vacancies on the surface of TMD monolayers using electrochemical methods. We observed a strong hybridization of p‐orbitals of N/P atom with the p‐ and d‐orbitals of neighbouring S/Se and Mo/W atoms, respectively, activating pristine TMDs by increasing density of states near Fermi‐level. Based on the free energy profiles of the four‐electron reduction process, we expect that N‐TMDs to be efficient in catalyzing ORR, whereas, too strong binding of reaction intermediates prevents ORR on P‐TMDs. Among the candidates considered, N‐WS2 is found to be a promising TMD as ORR catalyst with the overpotential as low as 0.31 V, stimulating further experimental studies.

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“…In contrast to the tremendous research of MoS 2 for HER, there are only few reports considering their applications for ORR or OER . The abundant Mo edge sites in MoS 2 nanoparticles and the spin densities altered by heteroatom doping (such as N and P) are revealed to be responsible for the ORR/OER activity of MoS 2 ‐based electrocatalysts. Most recently, the topological defects in porous graphene are also believed to be a kind of effective active centers toward ORR, OER, and HER .…”

mentioning

confidence: 97%

“…The efficient catalysis for HER coupled with OER is of paramount importance to the clean hydrogen production by electrochemical water splitting; meanwhile, the ORR and OER electrocatalysis is crucial for some renewable energy technologies, such as fuel cells and metal–air batteries . In contrast to the tremendous research of MoS 2 for HER, there are only few reports considering their applications for ORR or OER . The abundant Mo edge sites in MoS 2 nanoparticles and the spin densities altered by heteroatom doping (such as N and P) are revealed to be responsible for the ORR/OER activity of MoS 2 ‐based electrocatalysts.…”

mentioning

confidence: 99%

3D Mesoporous van der Waals Heterostructures for Trifunctional Energy Electrocatalysis

et al. 2017

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The emergence of van der Waals (vdW) heterostructures of 2D materials has opened new avenues for fundamental scientific research and technological applications. However, the current concepts and strategies of material engineering lack feasibilities to comprehensively regulate the as-obtained extrinsic physicochemical characters together with intrinsic properties and activities for optimal performances. A 3D mesoporous vdW heterostructure of graphene and nitrogen-doped MoS via a two-step sequential chemical vapor deposition method is constructed. Such strategy is demonstrated to offer an all-round engineering of 2D materials including the morphology, edge, defect, interface, and electronic structure, thereby leading to robustly modified properties and greatly enhanced electrochemical activities. The hydrogen evolution is substantially accelerated on MoS , while the oxygen reduction and evolution are significantly improved on graphene. This work provides a powerful overall engineering strategy of 2D materials for electrocatalysis, which is also enlightening for other nanomaterials and energy-related applications.

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Incorporated oxygen in MoS₂ ultrathin nanosheets for efficient ORR catalysis

Abstract: Controllable engineering of high-electronegativity oxygen (O)-heteroatoms into MoS2 ultrathin nanosheets is realized via a facile post-modification process.

Cited by 98 publications

References 36 publications

Morphological Effects and Stabilization of the Metallic 1T Phase in Layered V‐, Nb‐, and Ta‐Doped WSe₂ for Electrocatalysis

Morphological Effects and Stabilization of the Metallic 1T Phase in Layered V‐, Nb‐, and Ta‐Doped WSe₂ for Electrocatalysis

Activating Transition Metal Dichalcogenides by Substitutional Nitrogen‐Doping for Potential ORR Electrocatalysts

3D Mesoporous van der Waals Heterostructures for Trifunctional Energy Electrocatalysis

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Incorporated oxygen in MoS2 ultrathin nanosheets for efficient ORR catalysis

Abstract: Controllable engineering of high-electronegativity oxygen (O)-heteroatoms into MoS2 ultrathin nanosheets is realized via a facile post-modification process.

Cited by 98 publications

References 36 publications

Morphological Effects and Stabilization of the Metallic 1T Phase in Layered V‐, Nb‐, and Ta‐Doped WSe2 for Electrocatalysis

Morphological Effects and Stabilization of the Metallic 1T Phase in Layered V‐, Nb‐, and Ta‐Doped WSe2 for Electrocatalysis

Activating Transition Metal Dichalcogenides by Substitutional Nitrogen‐Doping for Potential ORR Electrocatalysts

3D Mesoporous van der Waals Heterostructures for Trifunctional Energy Electrocatalysis

Contact Info

Product

Resources

About

Incorporated oxygen in MoS₂ ultrathin nanosheets for efficient ORR catalysis

Morphological Effects and Stabilization of the Metallic 1T Phase in Layered V‐, Nb‐, and Ta‐Doped WSe₂ for Electrocatalysis

Morphological Effects and Stabilization of the Metallic 1T Phase in Layered V‐, Nb‐, and Ta‐Doped WSe₂ for Electrocatalysis