Hydrogen evolution enhancement of ultra-low loading, size-selected molybdenum sulfide nanoclusters by sulfur enrichment

Escalera‐López, Daniel; Niu, Yubiao; Park, Sung Jin; Isaacs, Mark A.; Wilson, Karen; Palmer, Richard E.; Rees, Neil V.

doi:10.1016/j.apcatb.2018.04.068

Cited by 61 publications

(36 citation statements)

References 89 publications

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“…For long‐term electrocatalytic applications, however, HER activity and stability of TMDs are paramount. In crystalline MoS 2 , basal plane activation, edge site exposure, and metal doping/incorporation/intercalation are the most employed strategies.…”

Section: Introductionmentioning

confidence: 99%

Benchmarking the Activity, Stability, and Inherent Electrochemistry of Amorphous Molybdenum Sulfide for Hydrogen Production

Escalera‐López

Lou

Rees

2019

Advanced Energy Materials

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can be efficiently produced on demand and in a decentralized manner with (photo) electrochemical methods via the hydrogen evolution reaction (HER). [1][2][3][4] Despite of being the best performing HER catalysts, [5,6] noble metals such as Pt, Ir, and Pd are scarce and consequently hamper the viability of water electrolysis technologies. Hence earth-abundant materials, and notably transition metal dichalcogenides (TMDs) such as molybdenum disulfide (MoS 2 ), have been extensively investigated as HER electrocatalysts. [7][8][9][10][11] The edge sites-driven hydrogen electroadsorption properties of TMDs [12,13] have prompted the fabrication of amorphous molybdenum sulfide materials (MoS x ) to minimize exposure of the electrocatalytically inert MoS 2 basal planes [14] for multiple applications. [15][16][17][18][19] A simple, yet scalable method to fabricate MoS x has been reported by substrate-insensitive electrodeposition from a [MoS 4 ] 2− precursor, [20,21] and critical properties in MoS x materials such as film thickness, [22] morphology, [23][24][25][26] Mo:S stoichiometry, [27] as well as incorporation of dopants [28][29][30] or nanocomposite formation, [31][32][33][34][35] have been easily tuned by experimental parameters.For long-term electrocatalytic applications, however, HER activity and stability of TMDs are paramount. In crystalline MoS 2 , basal plane activation, [36][37][38][39][40][41][42][43] edge site exposure, [44][45][46][47][48][49][50][51][52][53] and metal doping/incorporation/intercalation [54][55][56][57][58][59][60][61][62][63][64][65][66] are the most employed strategies.In contrast, the [Mo 3 S 13 ] 2− cluster-based polymeric structure of electrodeposited MoS x[67] requires alternative approaches to maximize activity. In addition, the detailed HER mechanism as well as the true catalytically active sites are still under debate. Whilst pioneering studies on ambient pressure X-ray photoelectron spectroscopy (XPS) indicated the MoS 2 edge-like sites formed after MoS 3 phase transformation under in operando conditions responsible for the HER performance, [68] in situ X-ray absorption spectroscopy experiments suggested terminal S 2 2− ligands (S 2 2− terminal ) to be the proton acceptor sites, [69] and more recently in situ Raman spectroscopy indicated these to be the electrochemically cleaved bridging S 2 2− ligands (S 2 2− bridging ). [70] Another study claimed that unsaturated Mo centers formed after cathodic dissolution of S 2 2− terminal to be the true HER Anodically electrodeposited amorphous molybdenum sulfide (AE-MoS x ) has attracted significant attention as a non-noble metal electrocatalyst for its high activity toward the hydrogen evolution reaction (HER). The [Mo 3 S 13 ] 2− polymerbased structure confers a high density of exposed sulfur moieties, widely regarded as the HER active sites. However, their intrinsic complexity conceals full understanding of their exact role in HER catalysis, hampering their full potential for water splitting applications. In this report, a unifying app...

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Section: Introductionmentioning

confidence: 99%

Benchmarking the Activity, Stability, and Inherent Electrochemistry of Amorphous Molybdenum Sulfide for Hydrogen Production

Escalera‐López

Lou

Rees

2019

Advanced Energy Materials

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“…20 Graphene-based two-dimensional (2D) transition metal dichalcogenide nanosheets, especially MoS 2 based heterostructures, have recently received much attention as a noble-metal-free catalyst and an anode material for energy storage devices. [21][22][23][24][25][26] Recently, Pi et al 27 demonstrated an extraordinary catalytic performance by TiO 2 nanostructures decorated with 1T-MoS 2 nanosheets under solar light. Thus, MoS 2 has now been recognized as an efficient co-catalyst incorporated with TiO 2 nanostructures due to its structural anisotropy, chemical inertness, good electroconductivity, and efficient catalytic properties.…”

Section: Journal Ofmentioning

confidence: 99%

“…S3, ESI †) which is reported to be benecial for the enhanced HER activity. 22 However, in the case of PTB, most of the Pt NPs are preferentially attached to the porous sites of TiO 2 nanostructures.…”

Section: Photoelectrocatalysis Measurements Under Visible Lightmentioning

confidence: 99%

“…This defect-rich structure leads to a higher exposure of unsaturated sulfur edge sites, which are widely regarded as the active sites responsible for the overall HER activity. 22,55 Additionally, the MoS 2 layers grown onto the TiO 2 NB surface present an n-type doping of MoS 2 , contributing to maximize HER activities aer MoS 2 basal plane activation.…”

Section: Mechanism Of Enhanced Her Activitymentioning

confidence: 99%

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Strongly enhanced visible light photoelectrocatalytic hydrogen evolution reaction in an n-doped MoS₂ /TiO₂(B) heterojunction by selective decoration of platinum nanoparticles at the MoS₂ edge sites

et al. 2018

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“…Cluster beam deposition (CBD) is one such method which offers a physical route to obtaining cluster catalysts with notable control over cluster size, composition and morphology. 18,19 Compared with traditional chemical methods, no solvents, salts or ligands are needed during the synthesis process, 20,21 making it an environmentally-friendly and in principle sustainable method. Since metal atoms are simply mixed together in the vacuum chamber to form clusters, it is relatively easy to develop recipes for new cluster systems.…”

Section: Introductionmentioning

confidence: 99%

Active site manipulation in MoS₂ cluster electrocatalysts by transition metal doping

et al. 2020

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Hydrogen evolution enhancement of ultra-low loading, size-selected molybdenum sulfide nanoclusters by sulfur enrichment

Cited by 61 publications

References 89 publications

Benchmarking the Activity, Stability, and Inherent Electrochemistry of Amorphous Molybdenum Sulfide for Hydrogen Production

Benchmarking the Activity, Stability, and Inherent Electrochemistry of Amorphous Molybdenum Sulfide for Hydrogen Production

Strongly enhanced visible light photoelectrocatalytic hydrogen evolution reaction in an n-doped MoS₂ /TiO₂(B) heterojunction by selective decoration of platinum nanoparticles at the MoS₂ edge sites

Active site manipulation in MoS₂ cluster electrocatalysts by transition metal doping

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Hydrogen evolution enhancement of ultra-low loading, size-selected molybdenum sulfide nanoclusters by sulfur enrichment

Cited by 61 publications

References 89 publications

Benchmarking the Activity, Stability, and Inherent Electrochemistry of Amorphous Molybdenum Sulfide for Hydrogen Production

Benchmarking the Activity, Stability, and Inherent Electrochemistry of Amorphous Molybdenum Sulfide for Hydrogen Production

Strongly enhanced visible light photoelectrocatalytic hydrogen evolution reaction in an n-doped MoS2 /TiO2(B) heterojunction by selective decoration of platinum nanoparticles at the MoS2 edge sites

Active site manipulation in MoS2 cluster electrocatalysts by transition metal doping

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Strongly enhanced visible light photoelectrocatalytic hydrogen evolution reaction in an n-doped MoS₂ /TiO₂(B) heterojunction by selective decoration of platinum nanoparticles at the MoS₂ edge sites

Active site manipulation in MoS₂ cluster electrocatalysts by transition metal doping