Engineering active edge sites of fractal-shaped single-layer MoS2 catalysts for high-efficiency hydrogen evolution

Wan, Yi; Zhang, Zeyao; Xu, Xiaolong; Zhang, Zhihong; Li, Pan; Fang, Xin; Zhang, Kun; Yuan, Kai; Liu, Kaihui; Ran, Guangzhao; Li, Yan; Yang, Yu; Dai, Li‐Xin

doi:10.1016/j.nanoen.2018.02.027

Cited by 102 publications

(56 citation statements)

References 34 publications

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“…Two major strategies for improving the HER performance of LMDs‐based catalysts include: i) increasing the number of active sites and ii) enhancing their electrical conductivity . Several methods, such as doping with heteroatoms, shape controlling, and defect engineering with plasma treatment or chemical etching, have been developed to obtain more active sites . Introducing strain in the basal plane, synergizing with conductive materials or coupling with substrates have been extensively exploited to accelerate charge transfer .…”

Section: Introductionmentioning

confidence: 99%

Template‐Assisted Synthesis of Metallic 1T′‐Sn_0.3W_0.7S₂ Nanosheets for Hydrogen Evolution Reaction

Shao

Xue

et al. 2019

Adv Funct Materials

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Crystal phase control still remains a challenge for the precise synthesis of 2D layered metal dichalcogenide (LMD) materials. The T′ phase structure has profound influences on enhancing electrical conductivity, increasing active sites, and improving intrinsic catalytic activity, which are urgently needed for enhancing hydrogen evolution reaction (HER) activity. Theoretical calculations suggest that metastable T′ phase 2D Sn 1−x W x S 2 alloys can be formed by combining W with 1T tin disulfide (SnS 2 ) as a template to achieve a semiconductor-to-metallic transition. Herein, 2D Sn 1−x W x S 2 alloys with varying x are prepared by adjusting the molar ratio of reactants via hydrothermal synthesis, among which Sn 0.3 W 0.7 S 2 displays a maximum of concentration of 81% in the metallic phase and features a distorted octahedral-coordinated metastable 1T′ phase structure. The obtained 1T′-Sn 0.3 W 0.7 S 2 has high intrinsic electrical conductivity, lattice distortion, and defects, showing a prominently improved HER catalytic performance. Metallic Sn 0.3 W 0.7 S 2 coupled with carbon black exhibits at least a 215-fold improvement compared to pristine SnS 2 . It has excellent long-term durability and HER activity. This work reveals a general phase transition strategy by using T phase materials as templates and merging heteroatoms to achieve synthetic metastable phase 2D LMDs that have a significantly improved HER catalytic performance.

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Section: Introductionmentioning

confidence: 99%

Template‐Assisted Synthesis of Metallic 1T′‐Sn_0.3W_0.7S₂ Nanosheets for Hydrogen Evolution Reaction

Shao

Xue

et al. 2019

Adv Funct Materials

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“…Recent advances in strain engineering of 2D TMDs have shown that their electronic band structure is sensitive to strain, and could be used to tune the contact resistance at semiconductor–metal interfaces. Some work has demonstrated that strain engineering can also be used to improve the HER activity of TMDs by modifying Δ G H . Therefore, care must be taken to separate out the effects of strain on thermodynamics and charge injection.…”

Section: Resultsmentioning

confidence: 99%

“…For the hydrogen evolution reaction (HER), the Sabatier principle plots the catalytic activity of solid‐state catalysts as a function of the Gibbs free energy of hydrogen adsorption (Δ G H ) to a catalytic site and predicts optimal catalytic activity when Δ G H is close to zero . Many transition metal dichalcogenides (TMDs) have been investigated as potential electrocatalysts, including MoS 2 that exhibits small Δ G H , which has led to extensive effort to use MoS 2 as an HER catalyst via nanostructuring, strain‐engineering, and phase‐engineering . However, Δ G H alone does not determine the overall HER activity; charge injection into MoS 2 has a large effect on catalytic efficiency .…”

Section: Introductionmentioning

confidence: 99%

Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS₂/WTe₂ Hybrid Structures

Zhou

Pondick

Silva

et al. 2019

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Using the MoS2‐WTe2 heterostructure as a model system combined with electrochemical microreactors and density function theory calculations, it is shown that heterostructured contacts enhance the hydrogen evolution reaction (HER) activity of monolayer MoS2. Two possible mechanisms are suggested to explain this enhancement: efficient charge injection through large‐area heterojunctions between MoS2 and WTe2 and effective screening of mirror charges due to the semimetallic nature of WTe2. The dielectric screening effect is proven minor, probed by measuring the HER activity of monolayer MoS2 on various support substrates with dielectric constants ranging from 4 to 300. Thus, the enhanced HER is attributed to the increased charge injection into MoS2 through large‐area heterojunctions. Based on this understanding, a MoS2/WTe2 hybrid catalyst is fabricated with an HER overpotential of −140 mV at 10 mA cm−2, a Tafel slope of 40 mV dec−1, and long stability. These results demonstrate the importance of interfacial design in transition metal dichalcogenide HER catalysts. The microreactor platform presents an unambiguous approach to probe interfacial effects in various electrocatalytic reactions.

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“…Additionally, d‐band theory implies that the electron supply to the catalytic active sites increases due to the tensile strain in MoS 2 , which thus boosts the electrocatalytic HER activity . Likewise, Wan and co‐workers have prepared fractally shaped single‐layer MoS 2 with a large tensile strain on fused silica via a chemical vapor deposition (CVD) route and reported that the as‐synthesized MoS 2 has a large quantity of exposed edge sites, which is beneficial for superior HER activity compared with triangle‐shaped MoS 2 on a SiO 2 substrate. A low overpotential of 185 mV at a current density of 10 mA cm −2 , a Tafel slope of 45 mV dec −1 and an exchange current density of 50.9 µA cm −2 was obtained with fractal‐shaped single‐layer MoS 2 electrocatalysts, which correlates to an edge‐to‐substrate ratio of ≈0.33 µm −1 .…”

Section: Spe For Energy Conversion and Environmental Treatmentmentioning

confidence: 99%

Structural‐Phase Catalytic Redox Reactions in Energy and Environmental Applications

Uddin

Zhang

et al. 2020

Advanced Materials

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The structure–property engineering of phase‐based materials for redox‐reactive energy conversion and environmental decontamination nanosystems, which are crucial for achieving feasible and sustainable energy and environment treatment technology, is discussed. An exhaustive overview of redox reaction processes, including electrocatalysis, photocatalysis, and photoelectrocatalysis, is given. Through examples of applications of these redox reactions, how structural phase engineering (SPE) strategies can influence the catalytic activity, selectivity, and stability is constructively reviewed and discussed. As observed, to date, much progress has been made in SPE to improve catalytic redox reactions. However, a number of highly intriguing, unresolved issues remain to be discussed, including solar photon‐to‐exciton conversion efficiency, exciton dissociation into active reductive/oxidative electrons/holes, dual‐ and multiphase junctions, selective adsorption/desorption, performance stability, sustainability, etc. To conclude, key challenges and prospects with SPE‐assisted redox reaction systems are highlighted, where further development for the advanced engineering of phase‐based materials will accelerate the sustainable (active, reliable, and scalable) production of valuable chemicals and energy, as well as facilitate environmental treatment.

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Engineering active edge sites of fractal-shaped single-layer MoS2 catalysts for high-efficiency hydrogen evolution

Cited by 102 publications

References 34 publications

Template‐Assisted Synthesis of Metallic 1T′‐Sn_0.3W_0.7S₂ Nanosheets for Hydrogen Evolution Reaction

Template‐Assisted Synthesis of Metallic 1T′‐Sn_0.3W_0.7S₂ Nanosheets for Hydrogen Evolution Reaction

Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS₂/WTe₂ Hybrid Structures

Structural‐Phase Catalytic Redox Reactions in Energy and Environmental Applications

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Engineering active edge sites of fractal-shaped single-layer MoS2 catalysts for high-efficiency hydrogen evolution

Cited by 102 publications

References 34 publications

Template‐Assisted Synthesis of Metallic 1T′‐Sn0.3W0.7S2 Nanosheets for Hydrogen Evolution Reaction

Template‐Assisted Synthesis of Metallic 1T′‐Sn0.3W0.7S2 Nanosheets for Hydrogen Evolution Reaction

Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS2/WTe2 Hybrid Structures

Structural‐Phase Catalytic Redox Reactions in Energy and Environmental Applications

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Product

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About

Template‐Assisted Synthesis of Metallic 1T′‐Sn_0.3W_0.7S₂ Nanosheets for Hydrogen Evolution Reaction

Template‐Assisted Synthesis of Metallic 1T′‐Sn_0.3W_0.7S₂ Nanosheets for Hydrogen Evolution Reaction

Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS₂/WTe₂ Hybrid Structures