Most recently, much attention has been devoted to 1T phase MoS2 because of its distinctive phase-engineering nature and promising applications in catalysts, electronics, and energy storage devices. While alkali metal intercalation and exfoliation methods have been well developed to realize unstable 1T-MoS2 , but the aqueous synthesis for producing stable metallic phase remains big challenging. Herein, a new synthetic protocol is developed to mass-produce colloidal metallic 1T-MoS2 layers highly stabilized by intercalated ammonium ions (abbreviated as N-MoS2). In combination with density functional calculations, the X-ray diffraction pattern and Raman spectra elucidate the excellent stability of metallic phase. As clearly depicted by high-angle annular dark-field imaging in an aberration-corrected scanning transmission electron microscope and extended X-ray absorption fine structure, the N-MoS2 exhibits a distorted octahedral structure with a 2a0 × a0 basal plane superlattice and 2.72 Å Mo-Mo bond length. In a proof-of-concept demonstration for the obtained material's applications, highly efficient photocatalytic activity is achieved by simply hybridizing metallic N-MoS2 with semiconducting CdS nanorods due to the synergistic effect. As a direct outcome, this CdS:N-MoS2 hybrid shows giant enhancement of hydrogen evolution rate, which is almost 21-fold higher than pure CdS and threefold higher than corresponding annealed CdS:2H-MoS2.
Designing advanced electrocatalysts for hydrogen evolution reaction is of far-reaching significance. Active sites and conductivity play vital roles in such a process. Herein, we demonstrate a heteronanostructure for hydrogen evolution reaction, which consists of metallic 1T-MoS2 nanopatches grown on the surface of flexible single-walled carbon nanotube (1T-MoS2/SWNT) films. The simulated deformation charge density of the interface shows that 0.924 electron can be transferred from SWNT to 1T-MoS2, which weakens the absorption energy of H atom on electron-doped 1T-MoS2, resulting in superior electrocatalytic performance. The electron doping effect via interface engineering renders this heteronanostructure material outstanding hydrogen evolution reaction (HER) activity with initial overpotential as small as approximately 40 mV, a low Tafel slope of 36 mV/dec, 108 mV for 10 mA/cm2, and excellent stability. We propose that such interface engineering could be widely used to develop new catalysts for energy conversion application.
Stable metallic 1T-WS2 nanoribbons with zigzag chain superlattices, highly stabilized by ammonia-ion intercalation, are produced using a facile bottom-up process. The atomic structure of the nanoribbons, including W-W reconstruction and W-S distorted octahedral coordination, results in distinctive electrical transport and optical Raman scattering properties that are very different from semiconducting 2H-WS2 . The correlations between structure and properties are further confirmed by theory calculations.
Vertical 1T-MoS nanosheets with an expanded interlayer spacing of 9.8 Å were successfully grown on a graphene surface via a one-step solvothermal method. Such unique hybridized structures provided strong electrical and chemical coupling between the vertical nanosheets and graphene layers by means of C-O-Mo bonding. The merits are very beneficial for a high-efficiency electron/ion transport pathway and structural stability. As a proof of concept, the lithium ion battery with the as-obtained hybrid's electrode exhibited excellent rate performance with a 666 mA h g capacity at a high current density of 3500 mA g. We can extend this method to produce various metallic 1T-MX (M = transition metal; X = chalcogen) vertically edged on a graphene frame as one of the promising hetero-structures for several specific applications in the fields of electronics, optics and catalysis.
Two-dimensional stable metallic 1T-MoSe with expanded interlayer spacing of 10.0 Å in situ grown on SWCNTs film is fabricated via a one-step solvothermal method. Combined with X-ray absorption near-edge structures, our characterization reveals that such 1T-MoSe and single-walled carbon nanotubes (abbreviated as 1T-MoSe/SWCNTs) hybridized structure can provide strong electrical and chemical coupling between 1T-MoSe nanosheets and SWCNT film in a form of C-O-Mo bonding, which significantly benefits a high-efficiency electron/ion transport pathway and structural stability, thus directly enabling high-performance lithium storage properties. In particular, as a flexible and binder-free Li-ion anode, the 1T-MoSe/SWCNTs electrode exhibits excellent rate capacity, which delivers a capacity of 630 mAh/g at 3000 mA/g. Meanwhile, the strong C-O-Mo bonding of 1T-MoSe/SWCNTs accommodates volume alteration during the repeated charge/discharge process, which gives rise to 89% capacity retention and a capacity of 971 mAh/g at 300 mA/g after 100 cycles. This synthetic route of a multifunctional MoSe/SWCNTs hybrid might be extended to fabricate other 2D layer-based flexible and light electrodes for various applications such as electronics, optics, and catalysts.
Layered tungsten disulfide (WS2) has attracted great attention because of its high potential for electrochemical energy applications.
The replacement of expensive noble‐metals cocatalysts with inexpensive, earth‐abundant, metallic nonmetal materials in most semiconductor‐based photocatalytic systems is highly desirable. Herein, we report the fabrication of stable 1T‐MoS2 slabs in situ grown on CdS nanorods (namely, 1T‐MoS2@CdS) by using a solvothermal method. As demonstrated by ultrafast transient absorption spectroscopy, in combination with steady‐state and time‐resolved photoluminescence, the synergistic effects resulting from formation of the intimate nanojunction between the interfaces and effective electron transport in the metallic phase of 1T‐MoS2 largely contribute to boosting the photocatalytic activity of CdS. Notably, the heterostructure with an optimum loading of 0.2 wt % 1T‐MoS2 exhibits an almost 39‐fold enhancement in the photocatalytic activity relative to that exhibited by bare CdS. This work represents a step towards the in situ realization of a 1T‐phase MoS2‐based heterostructure as a promising cocatalyst with high performance and low cost.
a variety of applications, such as drug delivery or biocatalysis accessible. [2] In addition, mesoporous silica offers a wide variety of transport characteristics achieved by introducing organic functions into the silica framework. Those silica hybrid materials are a common motive in separation processes, drug delivery, or sensor technology. [3] Key properties, such as high specific surface area, stability, adjustable pore geometries, as well as high diversity regarding surface chemistry allow their application in such diverse areas. [4] Especially the responsive, so-called smart, organo-silica materials have been established as a new fascinating field of research over the last decades. [5] Using responsive polymers, gates are created in silica nanopores which react to triggers, such as light, [6] pH, [7] or temperature [8] and thus control pore accessibility, transport, or the release of drugs. [9] Applications for mesoporous silica strongly depend on charge generation and the corresponding gating behavior of the mesopores, which result from interactions with pH adjusted solutions.Controlled polymerization and thus precise control on pore filling and charge density in nanopores has been demonstrated by atom transfer radical polymerization, reversible additionfragmentation chain transfer, or surface initiated photoiniferter polymerization. [10] Only very recently it has been shown that not only the amount of polymer but also the architecture of the polymer chains can be controlled and block-cooligomers in pores can be generated. [10a,11] Thereby, pH responsive polymers Functionalized ordered mesoporous materials are relevant in technologies, such as drug release, sensing, and separation. To design functionality, the silica framework can be functionalized with responsive molecules or polymers. Often, the pH value in those hybrid materials determines performance. Even though pH/pKa differences between polymers in bulk solutions and nanoscale confinement have been observed, the influence of confinement on pH-and pore filling dependent polyelectrolyte oligomer chain charge has yet not been investigated systematically. Here, mesoporous silica films are functionalized with (2-dimethylamino) ethyl methacrylate) (DMAEMA) and 2-(methacryloyloxy)ethyl phosphate (MEP) oligomers using photoiniferter initiated polymerization. This approach allows a controlled and environmentally friendly mesopore functionalization in water. The obtained oligomer functionalized pores are tunable with respect to pore filling. For both, poly(2-(dimethylamino) ethyl methacrylate) (PDMAEMA) and poly(2-(methacryloxy)ethyl phosphate) (PMEP), the charge generation inside mesopore confinement is significantly delayed toward harsher pH conditions resulting in pKa shifts of 1-2 pH units. Polymer amount and ionic strength show to further influence the pKa of PDMAEMA in mesopores. The technological importance of the pH value in confinement and its effect on enzyme stabilization is demonstrated. Lipase from Aspergillus oryzae loses its activity upo...
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