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Two-dimensional (2D) materials1,2 and the associated van der Waals (vdW) heterostructures3-7 have provided great flexibility for integrating distinct atomic layers beyond the traditional limits of lattice-matching requirements, through layer-by-layer mechanical restacking or sequential synthesis. However, the 2D vdW heterostructures explored so far have been usually limited to relatively simple heterostructures with a small number of blocks8-18. The preparation of high-order vdW superlattices with larger number of alternating units is exponentially more difficult, owing to the limited yield and material damage associated with each sequential restacking or synthesis step8-29. Here we report a straightforward approach to realizing high-order vdW superlattices by rolling up vdW heterostructures. We show that a capillary-force-driven rolling-up process can be used to delaminate synthetic SnS2/WSe2 vdW heterostructures from the growth substrate and produce SnS2/WSe2 roll-ups with alternating monolayers of WSe2 and SnS2, thus forming high-order SnS2/WSe2 vdW superlattices. The formation of these superlattices modulates the electronic band structure and the dimensionality, resulting in a transition of the transport characteristics from semiconducting to metallic, from 2D to one-dimensional (1D), with an angle-dependent linear magnetoresistance. This strategy can be extended to create diverse 2D/2D vdW superlattices, more complex 2D/2D/2D vdW superlattices, and beyond-2D materials, including three-dimensional (3D) thin-film materials and 1D nanowires, to generate mixed-dimensional vdW superlattices, such as 3D/2D, 3D/2D/2D, 1D/2D and 1D/3D/2D vdW superlattices. This study demonstrates a general approach to producing high-order vdW superlattices with widely variable material compositions, dimensions, chirality and topology, and defines a rich material platform for both fundamental studies and technological applications.
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The junctions formed at the contact between metallic electrodes and semiconductor materials are crucial components of electronic and optoelectronic devices 1 . Metal-semiconductor junctions are characterized by an energy barrier known as the Schottky barrier, whose height can, in the ideal case, be predicted by the Schottky-Mott rule2-4 on the basis of the relative alignment of energy levels. Such ideal physics has rarely been experimentally realized, however, because of the inevitable chemical disorder and Fermi-level pinning at typical metal-semiconductor interfaces2,5-12. Here we report the creation of van der Waals metal-semiconductor junctions in which atomically flat metal thin films are laminated onto two-dimensional semiconductors without direct chemical bonding, creating an interface that is essentially free from chemical disorder and Fermi-level pinning. The Schottky barrier height, which approaches the Schottky-Mott limit, is dictated by the work function of the metal and is thus highly tunable. By transferring metal films (silver or platinum) with a work function that matches the conduction band or valence band edges of molybdenum sulfide, we achieve transistors with a two-terminal electron mobility at room temperature of 260 centimetres squared per volt per second and a hole mobility of 175 centimetres squared per volt per second. Furthermore, by using asymmetric contact pairs with different work functions, we demonstrate a silver/molybdenum sulfide/platinum photodiode with an open-circuit voltage of 1.02 volts. Our study not only experimentally validates the fundamental limit of ideal metal-semiconductor junctions but also defines a highly efficient and damage-free strategy for metal integration that could be used in high-performance electronics and optoelectronics.
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Artificial superlattices, based on van der Waals heterostructures of two-dimensional atomic crystals such as graphene or molybdenum disulfide, offer technological opportunities beyond the reach of existing materials. Typical strategies for creating such artificial superlattices rely on arduous layer-by-layer exfoliation and restacking, with limited yield and reproducibility. The bottom-up approach of using chemical-vapour deposition produces high-quality heterostructures but becomes increasingly difficult for high-order superlattices. The intercalation of selected two-dimensional atomic crystals with alkali metal ions offers an alternative way to superlattice structures, but these usually have poor stability and seriously altered electronic properties. Here we report an electrochemical molecular intercalation approach to a new class of stable superlattices in which monolayer atomic crystals alternate with molecular layers. Using black phosphorus as a model system, we show that intercalation with cetyl-trimethylammonium bromide produces monolayer phosphorene molecular superlattices in which the interlayer distance is more than double that in black phosphorus, effectively isolating the phosphorene monolayers. Electrical transport studies of transistors fabricated from the monolayer phosphorene molecular superlattice show an on/off current ratio exceeding 107, along with excellent mobility and superior stability. We further show that several different two-dimensional atomic crystals, such as molybdenum disulfide and tungsten diselenide, can be intercalated with quaternary ammonium molecules of varying sizes and symmetries to produce a broad class of superlattices with tailored molecular structures, interlayer distances, phase compositions, electronic and optical properties. These studies define a versatile material platform for fundamental studies and potential technological applications.
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NiCo2 O4 nanowire array on carbon cloth (NiCo2 O4 /CC) is proposed as a highly active electrocatalyst for ambient nitrate (NO3 - ) reduction to ammonia (NH3 ). In 0.1 m NaOH solution with 0.1 m NaNO3 , such NiCo2 O4 /CC achieves a high Faradic efficiency of 99.0% and a large NH3 yield up to 973.2 µmol h-1 cm-2 . The superior catalytic activity of NiCo2 O4 comes from its half-metal feature and optimized adsorption energy due to the existence of Ni in the crystal structure. A Zn-NO3 - battery with NiCo2 O4 /CC cathode also shows a record-high battery performance.
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Electrocatalytic NO reduction is regarded as an attractive strategy to degrade the NO contaminant into useful NH3 , but the lack of efficient and stable electrocatalysts to facilitate such multiple proton-coupled electron-transfer processes impedes its applications. Here, we report on developing amorphous B2.6 C supported on a TiO2 nanoarray on a Ti plate (a-B2.6 C@TiO2 /Ti) as an NH3 -producing nanocatalyst with appreciable activity and durability toward the NO electroreduction. It shows a yield of 3678.6â µg h-1 cm-2 and a FE of 87.6 %, superior to TiO2 /Ti (563.5â µg h-1 cm-2 , 42.6 %) and a-B2.6 C/Ti (2499.2â µg h-1 cm-2 , 85.6 %). An a-B2.6 C@TiO2 /Ti-based Zn-NO battery achieves a power density of 1.7â mW cm-2 with an NH3 yield of 1125â µg h-1 cm-2 . An in-depth understanding of catalytic mechanisms is gained by theoretical calculations.
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Electrocatalysis plays an essential role in diverse electrochemical energy conversion processes that are vital for improving energy utilization efficiency and mitigating the aggravating global warming challenge. The noble metals such as platinum are generally the most frequently used electrocatalysts to drive these reactions and facilitate the relevant energy conversion processes. The high cost and scarcity of these materials pose a serious challenge for the wide-spread adoption and the sustainability of these technologies in the long run, which have motivated considerable efforts in searching for alternative electrocatalysts with reduced loading of precious metals or based entirely on earth-abundant metals. Of particular interest are graphene-supported single atom catalysts (G-SACs) that integrate the merits of heterogeneous catalysts and homogeneous catalysts, such as high activity, selectivity, stability, maximized atom utilization efficiency and easy separation from reactants/products. The graphene support features a large surface area, high conductivity and excellent (electro)-chemical stability, making it a highly attractive substrate for supporting single atom electrocatalysts for various electrochemical energy conversion processes. In this review, we highlight the recent advancements in G-SACs for electrochemical energy conversion, from the synthetic strategies and identification of the atomistic structure to electrocatalytic applications in a variety of reactions, and finally conclude with a brief prospect on future challenges and opportunities.
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A facile and versatile microwave-assisted and shell-confined Kirkendall diffusion strategy is used to fabricate ultrasmall hollow nanoparticles by modulating the growth and thermal conversion of metal-organic framework (MOF) nanocrystals on graphene. This method involves that the adsorption of microwave by graphene creates a high-energy environment in a short time to decompose the inâ situ grown MOF nanocrystals into well-dispersed uniform core-shell nanoparticles with ultrasmall size. Upon a shell-confined Kirkendall diffusion process, hollow nanoparticles of multi-metal oxides, phosphides, and sulfides with the diameter below 20â nm and shell thickness below 3â nm can be obtained for the first time. Ultrasmall hollow nanostructures such as Fe2O3 can promote much faster charge transport and expose more active sites as well as migrate the volume change stress more efficiently than the solid and large hollow counterparts, thus demonstrating remarkable lithium-ion storage performance.
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The designable structure with 3D structure, ultrathin 2D nanosheets, and heteroatom doping are considered as highly promising routes to improve the electrochemical performance of carbon materials as anodes for lithium-ion batteries. However, it remains a significant challenge to efficiently integrate 3D interconnected porous frameworks with 2D tunable heteroatom-doped ultrathin carbon layers to further boost the performance. Herein, a novel nanostructure consisting of a uniform ultrathin N-doped carbon layer in situ coated on a 3D graphene framework (NC@GF) through solvothermal self-assembly/polymerization and pyrolysis is reported. The NC@GF with the nanosheets thickness of 4.0 nm and N content of 4.13 at% exhibits an ultrahigh reversible capacity of 2018 mA h g-1 at 0.5 A g-1 and an ultrafast charge-discharge feature with a remarkable capacity of 340 mA h g-1 at an ultrahigh current density of 40 A g-1 and a superlong cycle life with a capacity retention of 93% after 10 000 cycles at 40 A g-1 . More importantly, when coupled with LiFePO4 cathode, the fabricated lithium-ion full cells also exhibit high capacity and excellent rate and cycling performances, highlighting the practicability of this NC@GF.
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Negative transconductance (NTC) devices have been heavily investigated for their potential in low power logical circuit, memory, oscillating, and high-speed switching applications. Previous NTC devices are largely attributed to two working mechanisms: quantum mechanical tunneling, and mobility degradation at high electrical field. Herein we report a systematic investigation of charge transport in multilayer two-dimensional semiconductors (2DSCs) with optimized van der Waals contact and for the first time demonstrate NTC and antibipolar characteristics in multilayer 2DSCs (such as MoS2, WSe2). By varying the measurement temperature, bias voltage, and body thickness, we found the NTC behavior can be attributed to a vertical potential barrier in the multilayer 2DSCs and the competing mechanisms between intralayer lateral transport and interlayer vertical transport, thus representing a new working mechanism for NTC operation. Importantly, this vertical potential barrier arises from inhomogeneous carrier distribution in 2DSC from the near-substrate region to the bulk region, which is in contrast to conventional semiconductors with homogeneous doping defined by bulk dopants. We further show that the unique NTC behavior can be explored for creating frequency doublers and phase shift keying circuits with only one transistor, greatly simplifying the circuit design compared to conventional technology.
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Facile and controllable integration of metal cyanides (MCs) into three-dimensional graphene (3DG) with advantageous structures is of fundamental importance for the development of superior MC-based electrode materials for electrochemical energy storage and catalysis. Here a facile and versatile spatially-confined Ostwald ripening strategy was developed to synthesize a series of 3DG wrapped MC aerogels with different compositions, size, and structure based on the chemical instability of MC in the reaction system. Remarkably, the integration of Prussian blue (PB) into 3DG, with such unique architecture, largely improves the rate performance and long-term cycling stability of PB as a cathode material for sodium ion batteries.
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Two-dimensional semiconductors (2DSCs) such as molybdenum disulfide (MoS2) have attracted intense interest as an alternative electronic material in the postsilicon era. However, the ON-current density achieved in 2DSC transistors to date is considerably lower than that of silicon devices, and it remains an open question whether 2DSC transistors can offer competitive performance. A high current device requires simultaneous minimization of the contact resistance and channel length, which is a nontrivial challenge for atomically thin 2DSCs, since the typical low contact resistance approaches for 2DSCs either degrade the electronic properties of the channel or are incompatible with the fabrication process for short channel devices. Here, we report a new approach toward high-performance MoS2 transistors by using a physically assembled nanowire as a lift-off mask to create ultrashort channel devices with pristine MoS2 channel and self-aligned low resistance metal/graphene hybrid contact. With the optimized contact in short channel devices, we demonstrate sub-100 nm MoS2 transistor delivering a record high ON-current of 0.83 mA/µm at 300 K and 1.48 mA/µm at 20 K, which compares well with that of silicon devices. Our study, for the first time, demonstrates that the 2DSC transistors can offer comparable performance to the 2017 target for silicon transistors in International Technology Roadmap for Semiconductors (ITRS), marking an important milestone in 2DSC electronics.
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Leaching of the internal apolar phase from the biopolymeric microparticles during storage is a great concern as it undoes the beneficial effects of encapsulation. In this paper, a novel formulation was prepared by encapsulating the sunflower oil-based organogels in alginate microparticles. Salicylic acid and metronidazole were used as the model drugs. The microparticles were prepared by double emulsion methodology. Physico-chemical characterization of the microparticles was done by microscopy, FTIR, XRD, and DSC studies. Oil leaching studies, biocompatibility, mucoadhesivity, in vitro drug release, and the antimicrobial efficiency of the microparticles were also performed. The microparticles were found to be spherical in shape. Gelation of the sunflower oil prevented leaching of the internal phase from the microparticles. Release of drugs from the microparticles followed Fickian kinetics and non-Fickian kinetics in gastric and intestinal environments, respectively. Microparticles showed good antimicrobial activity against both Gram-positive (Bacillus subtilis) and Gram-negative (Escherichia coli) bacteria. The results suggested that the developed formulations hold promise to carry oils without leakage of the internal phase. Encapsulation of organogels within the microparticles has improved the drug entrapment efficiency and improved characteristics for controlled delivery applications.
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Alginatos/química , Cápsulas/química , Composición de Medicamentos/métodos , Geles/química , Polisorbatos/química , Antibacterianos/administración & dosificación , Antibacterianos/farmacología , Ésteres , Ensayo de Materiales , Metronidazol/administración & dosificación , Metronidazol/química , Tamaño de la Partícula , Ácido Salicílico/administración & dosificación , Ácido Salicílico/químicaRESUMEN
Exploring new strategies to design non-precious and efficient electrocatalysts can provide a solution for sluggish electrocatalytic kinetics and sustainable hydrogen energy. Transition metal selenides are potential contenders for bifunctional electrocatalysis owing to their unique layered structure, low band gap, and high intrinsic activities. However, insufficient access to active sites, lethargic water dissociation, and structural degradation of active materials during electrochemical reactions limit their activities, especially in alkaline media. In this article, we report a useful strategy to assemble vanadium diselenide (VSe2) into a 3D MXene/rGO-based sponge-like architecture (VSe2@G/MXe) using hydrothermal and freeze-drying approaches. The 3D hierarchical meso/macro-pore rich sponge-like morphology not only prevents aggregation of VSe2 nanosheets but also offers a kinetics-favorable framework and high robustness to the electrocatalyst. Synergistic coupling of VSe2 and a MXene/rGO matrix yields a heterostructure with a large specific surface area, high conductivity, and multi-dimensional anisotropic pore channels for uninterrupted mass transport and gas diffusion. Consequently, VSe2@G/MXe presented superior electrochemical activity for both the HER and OER compared to its counterparts (VSe2 and VSe2@G), in alkaline media. The overpotentials required to reach a cathodic and anodic current density of 10 mA cm-2 were 153 mV (Tafel slope = 84 mV dec-1) and 241 mV (Tafel slope = 87 mV dec-1), respectively. The Rct values at the open circuit voltage were as low as 9.1 Ω and 1.41 Ω for the HER and OER activity, respectively. Importantly, VSe2@G/MXe withstands a steady current output for a long 24 h operating time. Hence, this work presents a rational design for 3D microstructures with optimum characteristics for efficient bifunctional alkaline water-splitting.
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This study explores the iodine and nickel-doped cobalt hydroxide (I & Ni-co-doped-Co(OH)2) as a potential material for energy storage and conversion applications owing to its excellent electrochemical characteristics. According to our analysis, it was revealed that this material exhibits pseudocapacitive-like behavior, as evident from distinct redox peaks observed in cyclic voltammetry, which confirms its ability to store charges. The diffusion coefficient analysis reveals that this material possesses conductivity and rapid diffusion kinetics, making it particularly advantageous compared to materials synthesized in previous studies. Charge-discharge measurements were performed to analyze the charge storage capacity and stability of this material after 3000 consecutive cycles, showing its excellent stability with minimum loss of capacitance. Furthermore, its anodic and cathodic linear sweep voltammetry curves were measured to evaluate its oxygen evolution and hydrogen evolution reaction performance. The results showed that the material exhibited an excellent water splitting performance, which suggests its potential practical application for hydrogen production. This increased activity was attributed to the doping of α-Co(OH)2, which improved its structural stability, electrical conductivity, and charge transfer efficiency. Thus, I & Ni-co-doped-Co(OH)2 possesses enhanced properties that make it an excellent material for both energy storage and hydrogen generation applications.
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In the current study, CuO, ZnCo2O4, CuO/ZnCo2O4, and CuO/ZnCo2O4/CNTs photocatalysts were prepared to remove crystal violet (CV) and colorless pollutants (diclofenac sodium and phenol) from wastewater. Herein, sol-gel and co-precipitation methods were used to synthesize CuO and ZnCo2O4, respectively. The sonication method was used to synthesize CuO/ZnCo2O4 and a CNTs-based composite (CuO/ZnCo2O4/CNTs). From the UV-Vis spectra of CuO, ZnCo2O4, CuO/ZnCo2O4, and CuO/ZnCo2O4/CNTs, the optical band gap value was calculated to be 2.11, 2.18, 1.71 and 1.63 eV respectively. The photocatalytic results revealed that CuO/ZnCo2O4/CNTs exhibited higher degradation of 87.7% against CV dye, 82% against diclofenac sodium, and 72% against phenol as compared to other prepared photocatalysts. The OHË radical is identified as the active species in the photocatalytic process over CuO/ZnCo2O4/CNTs. The impact of several parameters, such as pH, concentration, and catalyst dosage, has also been investigated. The better activity of the CNTs-based composite was due to the synergic effect of both CuO/ZnCo2O4 nanocomposite and carbon nanotubes. Therefore, the synthesized CuO/ZnCo2O4/CNTs photocatalyst has the potential to degrade organic wastewater effluents effectively.
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The rapid recombination of charges of photogenerated electrons and holes severely limits single semiconductor photocatalytic applications. In this study, a simple and facile sol-gel approach was used to synthesize Ba2-xHoxSr2-yNiyFe12O22 (x = 0, 0.1 and y = 0, 0.5). The composite of holmium-nickel doped barium-strontium ferrite with MXene (Ba1.9Ho0.1Sr1.5Ni0.5Fe12O22@MXene) was synthesized by ultrasonication method. These synthesized samples were subsequently used to photodegrade rhodamine B (RhB) and pendimethalin under visible light illumination. The results of the experiments demonstrated that MXene, as a cocatalyst, considerably reduces the rate of recombination of charges and broadens absorption of visible light by providing increased surface functional groups to improve the photocatalytic activity of synthesized samples. MXene is thermally stable, have high electrical conductivity, have adjustable bandgap, and hydrophilic in nature. The optimized Ba1.9Ho0.1Sr1.5Ni0.5Fe12O22@MXene composite demonstrated an excellent photocatalytic rate by degrading 78.88% RhB and 75.59% pendimethalin in 140 minutes. Moreover, the scavenging experiment revealed that photogenerated electrons and holes were the primary active species involved in RhB and pendimethalin photodegradation, respectively. Ba1.9Ho0.1Sr1.5Ni0.5Fe12O22@MXene showed increased photocatalytic behavior because it has increased surface area which decreases rate of recombination of electron and hole pair, hence photocatalytic activity increases. It is observed that Ba1.9Ho0.1Sr1.5Ni0.5Fe12O22@MXene has potential application in photocatalytic degradation of harmful pollutants.
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Since the discovery of single-layer graphene in 2004, the family of 2D inorganic nanosheets is considered as ideal membrane materials due to their ultrathin atomic thickness and fascinating physicochemical properties. However, the intrinsically nonporous feature of 2D inorganic nanosheets hinders their potential to achieve a higher flux to some extent. Recently, 2D polymer nanosheets, originated from the regular and periodic covalent connection of the building units in 2D plane, have emerged as promising candidates for preparing ultrafast and highly selective membranes owing to their inherently tunable and ordered pore structure, light weight, and high specific surface. In this review, the synthetic methodologies (including top-down and bottom-up methods) of 2D polymer nanosheets are first introduced, followed by the summary of 2D polymer nanosheets-based membrane fabrication as well as membrane applications in the fields of gas separation, water purification, organic solvent separation, and ion exchange/transport in fuel cells and lithium-sulfur batteries. Finally, based on their current achievements, the authors' personal insights are put forward into the existing challenges and future research directions of 2D polymer nanosheets for membrane separation. The authors believe this comprehensive review on 2D polymer nanosheets-based membrane separation will definitely inspire more studies in this field.
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Tungsten oxide (WO3), MXene, and an WO3/MXene nanocomposite were synthesized to study their photocatalytic and biological applications. Tungsten oxide was synthesized by an easy and cost-effective hydrothermal method, and its composite with MXene was prepared through the sonication method. The synthesized tungsten oxide, MXene, and its composite were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), Fourier transform infrared (FTIR), energy-dispersive X-ray analysis (EDX), and Brunauer-Emmett-Teller (BET) for their structural, morphological, spectral, elemental and surface area analysis, respectively. The crystallite size of WO3 calculated from XRD was ~10 nm, the particle size of WO3 was 130 nm, and the average thickness of MXene layers was 175 nm, which was calculated from FESEM. The photocatalytic activity of as-synthesized samples was carried out for the degradation of methylene blue under solar radiation, MXene, the WO3/MXene composite, and WO3 exhibited 54%, 89%, and 99% photocatalytic degradation, respectively. WO3 showed maximal degradation ability; by adding WO3 to MXene, the degradation ability of MXene was enhanced. Studies on antibacterial activity demonstrated that these samples are good antibacterial agents against positive strains, and their antibacterial activity against negative strains depends upon their concentration. Against positive strains, the WO3/MXene composite's inhibition zone was at 7 mm, while it became 9 mm upon increasing the concentration. This study proves that WO3, MXene, and the WO3/MXene nanocomposite could be used in biological and environmental applications.
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2D layered materials typically feature strong in-plane covalent chemical bonding within each atomic layer and weak out-of-plane van der Waals (vdW) interactions between adjacent layers. The non-bonding nature between neighboring layers naturally results in a vdW gap, in which various foreign species may be inserted without breaking the in-plane covalent bonds. By tailoring the composition, size, structure, and electronic properties of the intercalated guest species and the hosting layered materials, an expansive family of layered intercalation materials may be produced with highly variable compositional and structural features as well as widely tunable physical/chemical properties, invoking unprecedented opportunities in fundamental studies of property modulation and potential applications in diverse technologies, including electronics, optics, superconductors, thermoelectrics, catalysis, and energy storage. Here, the principles and protocols for various intercalation methods, including wet chemical intercalation, gas-phase intercalation, electrochemical intercalation, and ion-exchange intercalation, are comprehensively reviewed and how the intercalated species alter the crystal structure and the interlayer coupling of the host 2D layered materials, introducing unusual physical and chemical properties and enabling devices with superior performance or unique functions, is discussed. To conclude, a brief summary on future research opportunities and emerging challenges in the layered intercalation materials is given.
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An efficient, environment-friendly and economical catalyst to control contaminants of environment is an enduring interest in recent years. In this study, a new composite, DyxMnFe2-xO4nanoparticles decorated over mesoporous silica was synthesized and utilized for removal of organic pollutant. Highly crystalline nature of DyxMnFe2-xO4 nanoparticles and amorphous nature of material was confirmed by XRD (X-ray diffraction) technique. Infrared spectra of fabricated material before and after adsorption of dye molecules evidenced the successful adsorption of dye molecules by fabricated adsorbent. From field emission scanning electron microscopic (FESEM) images of Dy3+ substituted MnFe2O4 composite with mesoporous silica, it was clearly observed that ferrite particles of size 20-30 nm were decorated on the surface of mesoporous silica particles and distributed well over spherical silica balls homogeneously. Its magnificent mesoporous nature was revealed from BET (nitrogen adsorption-desorption measurements) analysis. Surface area, pore volume and average pore size was found 387.95 m2/g, 0.390 cm3/g and 4.02 nm respectively. Tri-modal pore size distribution showed its effective utilization in adsorption. The abundant (SiOH) hydroxyl groups of mesoporous silica, the broad diffraction hump of silica depicted its superior loading capacity of target molecular specie inside its porous network. From band gap analysis, a red shift of 2.43 eV exhibited semiconductor photocatalysis of DyxMnFe2-xO4 nanoparticles. Degradation efficiency of bare MnFe2O4, DyxMnFe2-xO4 and mesoporous silica-based composite was tested using crystal violet dye. Its explored adsorption-photocatalysis synergy, degradation mechanism, kinetic investigation, easily recovery and remarkable recycling ability suggested that the new fabricated composite is best for environmental remediation.