| 1. |
- Cao, Wei, et al.
(author)
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Self-Assembly of Large Magnetic Nanoparticles in Ultrahigh Molecular Weight Linear Diblock Copolymer Films
- 2020
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In: ACS Applied Materials and Interfaces. - : AMER CHEMICAL SOC. - 1944-8244 .- 1944-8252. ; 12:6, s. 7557-7564
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Journal article (peer-reviewed)abstract
- The development of diblock copolymer (DBC) nanocomposite films containing magnetic nanoparticles (NPs) with diameters (D) over 20 nm is a challenging task. To host large iron oxide NPs (Fe3O4, D = 27 +/- 0.6 nm), an ultrahigh molecular weight (UHMW) linear DBC polystyrene-block-poly(methyl methacrylate) (PS-b-PMMA) is used as a template in the present work. Due to hydrogen bonding between the carboxylic acid ligands of the NPs and the ester groups in PMMA, the NPs show an affinity to the PMMA block. The localization of the NPs inside the DBC is investigated as a function of the NP concentration. At low NP concentrations, NPs are located preferentially at the interface between PS and PMMA domains to minimize the interfacial tension caused by the strong segregation strength of the UHMW DBC. At high NP concentrations (>= 10 wt %), chain-like NP aggregates (a head-to-tail orientation) are observed in the PMMA domains, resulting in a change of the morphology from sphere to ellipsoid for part of the PMMA domains. Magnetic properties of the hybrid films are probed via superconducting quantum interference device magnetometry. All hybrid films show ferrimagnetism and are promising for potential applications in magnetic data storage.
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| 2. |
- Hohn, Nuri, et al.
(author)
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Impact of Catalytic Additive on Spray Deposited and Nanoporous Titania in Films Observed via in Situ X-ray Scattering : Implications for hanced Photovoltaics
- 2018
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In: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 1:8, s. 4227-4235
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Journal article (peer-reviewed)abstract
- With the aim of obtaining nanostructured titania thin films for the tential use in hybrid or dye sensitized solar cells, the amphiphilic block copolymer polystyrene-b-poly(ethylene oxide) is employed as a ructure directing template in combination with solgel chemistry. For sy upscaling, spraying is used as a deposition technique. In situ azing incidence small-angle X-ray scattering (GISAXS) measurements are rformed during spraying and show that most titania structures are ready formed within the solution prior to deposition. However, ructural rearrangement is enabled during the deposition period when all amounts of hydrochloric acid (HCl) are used as a catalytic ditive to the spray solution. This behavior is ascribed to an altering the reaction dynamics and phase separation in the presence of HCl, ich significantly improves the templating effect of the employed block copolymer. With HCl as an additive the final nanoscale rphologies exhibit smaller pore sizes and strongly enhanced order as mpared to thin films sprayed from solutions that do not contain HCl as antified with atomic force microscopy, scanning electron microscopy, d GISAXS.
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| 3. |
- Li, Nian, et al.
(author)
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Morphology Phase Diagram of Slot-Die Printed TiO2 Films Based on Sol-Gel Synthesis
- 2019
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In: Advanced Materials Interfaces. - : WILEY. - 2196-7350. ; 6:12
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Journal article (peer-reviewed)abstract
- Mesoporous titania films with tailored nanostructures are fabricated via slot-die printing, which is a simple and cost-effective thin-film deposition technique with the possibility of a large-scale manufacturing. Based on this technique, which is favorable in industry, TiO2 films possess the similar advantage with polymer semiconducting devices like ease of large-scale production. The titania morphologies, including foam-like nanostructures, nanowire aggregates, collapsed vesicles and nanogranules, are achieved via a so-called block-copolymer-assisted sol-gel synthesis. By adjusting the weight fraction of reactants, the ternary morphology phase diagram of the printed titania films is probed after template removal. The surface and inner morphology evolutions are explored with scanning electron microscopy and grazing incidence small-angle X-ray scattering, respectively. Special focus is set on foam-like titania nanostructures as they are of especial interest for, e.g., solar cell applications. At a low weight fraction of the titania precursor titanium(IV)isopropoxide (TTIP), foam-like titania films are achieved, which exhibit a high uniformity and possess large pore sizes. The anatase phase of the highly crystalline titania films is verified with X-ray diffraction and transmission electron microscopy.
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| 4. |
- Schwartzkopf, Matthias, et al.
(author)
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In Situ Monitoring of Scale Effects on Phase Selection and Plasmonic Shifts during the Growth of AgCu Alloy Nanostructures for Anticounterfeiting Applications
- 2022
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In: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 5:3, s. 3832-3842
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Journal article (peer-reviewed)abstract
- Tailoring of plasmon resonances is essential for applications in anticounterfeiting. This is readily achieved by tuning the composition of alloyed metal clusters; in the simplest case, binary alloys are used. Yet, one challenge is the correlation of cluster morphology and composition with the changing optoelectronic properties. Hitherto, the early stages of metal alloy nanocluster formation in immiscible binary systems such as silver and copper have been accessible by molecular dynamics (MD) simulations and transmission electron microscopy (TEM). Here, we investigate in real time the formation of supported silver, copper, and silver-copper-alloy nanoclusters during sputter deposition on poly(methyl methacrylate) by combining in situ surface-sensitive X-ray scattering with optical spectroscopy. While following the transient growth morphologies, we quantify the early stages of phase separation at the nanoscale, follow the shifts of surface plasmon resonances, and quantify the growth kinetics of the nanogranular layers at different thresholds. We are able to extract the influence of scaling effects on the nucleation and phase selection. The internal structure of the alloy cluster shows a copper-rich core/silver-rich shell structure because the copper core yields a lower mobility and higher crystallization tendency than the silver fraction. We compare our results to MD simulation and TEM data. This demonstrates a route to tailor accurately the plasmon resonances of nanosized, polymer-supported clusters which is a crucial prerequisite for anticounterfeiting.
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| 5. |
- Wang, Kun, et al.
(author)
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Comparison of UV Irradiation and Sintering on Mesoporous Spongelike ZnO lms Prepared from PS-b-P4VP Templated Sol-Gel Synthesis
- 2018
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In: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 1:12, s. 7139-7148
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Journal article (peer-reviewed)abstract
- Mesoporous ZnO films with large surface-area-to-volume ratio show great omise in multiple applications, among which solid-state dye-sensitized lar cells (ssDSSCs) have attracted great attention in the field of otovoltaics. An appropriate mesopore size in the nanostructured ZnO lms significantly plays an indispensable role in improving the device ficiency that resulted from an efficient penetration of dye molecules d solid hole transport material. In the present work, mesoporous ongelike ZnO films are prepared using sol-gel synthesis templated by a block copolymer polystyrene-block-poly(4-vinylpyridine). Two different mplate removal techniques, ultraviolet (UV) irradiation and gh-temperature sintering, are used to compare their respective impact the pore sizes of the final ZnO thin films. Both the surface rphology and the inner morphology show that mesopores obtained via UV radiation are smaller as compared to their sintered counterparts. reover, increasing the template-to-ZnO precursor ratio is found to rther enlarge present mesopores. Accordingly, a strong correlation tween the pore sizes of sol-gel synthesized ZnO films and photovoltaic rformance of fabricated ssDSSCs is demonstrated. In contrast with the vices fabricated from the UV-irradiated ZnO films, those obtained from ntered samples show >2 times higher efficiency.
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| 6. |
- Xia, Senlin, et al.
(author)
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Magnetic nanoparticle-containing soft-hard diblock copolymer films with high order
- 2018
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In: Nanoscale. - : ROYAL SOC CHEMISTRY. - 2040-3364 .- 2040-3372. ; 10:25, s. 11930-11941
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Journal article (peer-reviewed)abstract
- For sensor applications, superparamagnetic anisotropy is an indispensable property, which is typically achieved by employing an external field to guide the arrangement of magnetic nanoparticles (NPs). In the present investigation, the diblock copolymer polystyrene-block-poly(N-isopropylacrylamide) (PS-b-PNIPAM) is printed as a template to localize magnetic iron oxide NPs without any external field. Via microphase separation, cylindrical nanostructures of PS in a PNIPAM matrix are obtained, aligned perpendicular to the substrate. Since the magnetite NPs (Fe3O4) are functionalized with hydrophobic organic chains showing affinity to the PS blocks, they can selectively aggregate inside the PS cylinders. Moreover, solvent vapor annealing allows the achievement of nanostructures inside the hybrid system with a very high order, even at a high NP loading. Therefore, NPs can accumulate within PS domains to form perpendicularly aligned aggregates with high periodicity. The magnetic properties of the hybrid films are determined at various temperatures in two orthogonal directions (with PS cylinders vertical and parallel to the applied magnetic field). All hybrid films show superparamagnetism and a remarkable magnetic anisotropy is achieved at certain NP concentrations. This investigation shows a facile route to prepare superparamagnetic films with magnetic anisotropy and offers a novel possibility to future magnetic sensor fabrication.
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| 7. |
- Xia, Senlin, et al.
(author)
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Printed Thin Diblock Copolymer Films with Dense Magnetic Nanostructure
- 2019
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In: ACS Applied Materials and Interfaces. - : AMER CHEMICAL SOC. - 1944-8244 .- 1944-8252. ; 11:24, s. 21935-21945
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Journal article (peer-reviewed)abstract
- Thin hybrid films with dense magnetic structures for sensor applications are printed using diblock copolymer (DBC) templating magnetic nanoparticles (MNPs). To achieve a high-density magnetic structure, the printing ink is prepared by mixing polystyrene-block-poly(methyl methacrylate) (PS-b-PMMA) with a large PS volume fraction and PS selective MNPs. Solvent vapor annealing is applied to generate a parallel cylindrical film morphology (with respect to the substrate), in which the MNP-residing PS domains are well separated by the PMMA matrix, and thus, the formation of large MNP agglomerates is avoided. Moreover, the morphologies of the printed thin films are determined as a function of the MNP concentration with real and reciprocal space characterization techniques. The PS domains are found to be saturated with MNPs at 1 wt %, at which the structural order of the hybrid films reaches a maximum within the studied range of MNP concentration. As a beneficial aspect, the MNP loading improves the morphological order of the thin DBC films. The dense magnetic structure endows the thin films with a faster superparamagnetic responsive behavior, as compared to thick films where identical MNPs are used, but dispersed inside the minority domains of the DBC.
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| 8. |
- Xia, Senlin, et al.
(author)
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Spray-Coating Magnetic Thin Hybrid Films of PS-b-PNIPAM and Magnetite Nanoparticles
- 2019
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In: Advanced Functional Materials. - : WILEY-V C H VERLAG GMBH. - 1616-301X .- 1616-3028. ; 29:15
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Journal article (peer-reviewed)abstract
- Spray coating is employed to fabricate magnetic thin films composed of the diblock copolymer polystyrene-block-poly(N-isopropylacrylamide) and Fe3O4 magnetic nanoparticles (MNPs) functionalized with hydrophobic coatings. The kinetics of structure formation of the hybrid films is followed in situ with grazing incidence small angle X-ray scattering during the spray deposition. To gain a better understanding of the influence of MNPs on the overall structure formation, the pure polymer film is also deposited as a reference via an identical spray protocol. At the initial spraying stage, the hybrid film (containing 2 wt% of MNPs) exhibits a faster formation process of a complete film as compared to the reference. The existence of MNPs depresses the dewetting behavior of polymer films on the substrate at macroscale and simultaneously alters the polymer microphase separation structure orientation from parallel to vertical. As spraying proceeds, MNPs aggregate into agglomerates with increasing sizes. After the spray deposition is finished, both samples gradually reach an equilibrium state and magnetic films with stable structures are achieved in the end. Superconducting quantum interference device investigation reveals the superparamagnetic property of the sprayed hybrid film. Consequently, potential application of sprayed films in fields such as magnetic sensors or data storage appears highly promising.
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