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End date: 2021 × Start date: 2021 × Has files: Yes × Publisher: Weinheim : Wiley-VCH × WGL Institute: IPF ×

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Now showing 1 - 10 of 23
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    A Two-Dimensional Polyimide-Graphene Heterostructure with Ultra-fast Interlayer Charge Transfer
    (Weinheim : Wiley-VCH, 2021) Liu, Kejun; Li, Jiang; Qi, Haoyuan; Hambsch, Mike; Rawle, Jonathan; Vázquez, Adrián Romaní; Nia, Ali Shaygan; Pashkin, Alexej; Schneider, Harald; Polozij, Mirosllav; Heine, Thomas; Helm, Manfred; Mannsfeld, Stefan C.B.; Kaiser, Ute; Dong, Renhao; Feng, Xinliang
    Two-dimensional polymers (2DPs) are a class of atomically/molecularly thin crystalline organic 2D materials. They are intriguing candidates for the development of unprecedented organic–inorganic 2D van der Waals heterostructures (vdWHs) with exotic physicochemical properties. In this work, we demonstrate the on-water surface synthesis of large-area (cm2), monolayer 2D polyimide (2DPI) with 3.1-nm lattice. Such 2DPI comprises metal-free porphyrin and perylene units linked by imide bonds. We further achieve a scalable synthesis of 2DPI-graphene (2DPI-G) vdWHs via a face-to-face co-assembly of graphene and 2DPI on the water surface. Remarkably, femtosecond transient absorption spectroscopy reveals an ultra-fast interlayer charge transfer (ca. 60 fs) in the resultant 2DPI-G vdWH upon protonation by acid, which is equivalent to that of the fastest reports among inorganic 2D vdWHs. Such large interlayer electronic coupling is ascribed to the interlayer cation–π interaction between 2DP and graphene. © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH
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    Prospects of Coupled Organic-Inorganic Nanostructures for Charge and Energy Transfer Applications
    (Weinheim : Wiley-VCH, 2021) Steiner, Anja Maria; Lissel, Franziska; Fery, Andreas; Lauth, Jannika; Scheele, Marcus
    We review the field of organic–inorganic nanocomposites with a focus on materials that exhibit a significant degree of electronic coupling across the hybrid interface. These nanocomposites undergo a variety of charge and energy transfer processes, enabling optoelectronic applications in devices which exploit singlet fission, triplet energy harvesting, photon upconversion or hot charge carrier transfer. We discuss the physical chemistry of the most common organic and inorganic components. Based on those we derive synthesis and assembly strategies and design criteria on material and device level with a focus on photovoltaics, spin memories or optical upconverters. We conclude that future research in the field should be directed towards an improved understanding of the binding motif and molecular orientation at the hybrid interface. © 2020 The Authors. Published by Wiley-VCH GmbH
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    Plasmonic Properties of Colloidal Assemblies
    (Weinheim : Wiley-VCH, 2021) Rossner, Christian; König, Tobias A.F.; Fery, Andreas
    The assembly of metal nanoparticles into supracolloidal structures unlocks optical features, which can go beyond synergistic combinations of the properties of their primary building units. This is due to inter-particle plasmonic coupling effects, which give rise to emergent properties. The motivation for this progress report is twofold: First, it is described how simulation approaches can be used to predict and understand the optical properties of supracolloidal metal clusters. These simulations may form the basis for the rational design of plasmonic assembly architectures, based on the desired functional cluster properties, and they may also spark novel material designs. Second, selected scalable state-of-the-art preparative strategies based on synthetic polymers to guide the supracolloidal assembly are discussed. These routes also allow for equipping the assembly structures with adaptive properties, which in turn enables (inter-)active control over the cluster optical properties. © 2021 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
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    Chemokine‐Capturing Wound Contact Layer Rescues Dermal Healing
    (Weinheim : Wiley-VCH, 2021) Schirmer, Lucas; Atallah, Passant; Freudenberg, Uwe; Werner, Carsten
    Excessive inflammation often impedes the healing of chronic wounds. Scavenging of chemokines by multiarmed poly(ethylene glycol)-glycosaminoglycan (starPEG-GAG) hydrogels has recently been shown to support regeneration in a diabetic mouse chronic skin wound model. Herein, a textile-starPEG-GAG composite wound contact layer (WCL) capable of selectively sequestering pro-inflammatory chemokines is reported. Systematic variation of the local and integral charge densities of the starPEG-GAG hydrogel component allows for tailoring its affinity profile for biomolecular signals of the wound milieu. The composite WCL is subsequently tested in a large animal (porcine) model of human wound healing disorders. Dampening excessive inflammatory signals without affecting the levels of pro-regenerative growth factors, the starPEG-GAG hydrogel-based WCL treatment induced healing with increased granulation tissue formation, angiogenesis, and deposition of connective tissue (collagen fibers). Thus, this biomaterials technology expands the scope of a new anti-inflammatory therapy toward clinical use.
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    Poly(2-alkyl-2-oxazoline)-Heparin Hydrogels—Expanding the Physicochemical Parameter Space of Biohybrid Materials
    (Weinheim : Wiley-VCH, 2021) Hahn, Dominik; Sonntag, Jannick M.; Lück, Steffen; Maitz, Manfred F.; Freudenberg, Uwe; Jordan, Rainer; Werner, Carsten
    Poly(ethylene glycol) (PEG)-glycosaminoglycan (GAG) hydrogel networks are established as very versatile biomaterials. Herein, the synthetic gel component of the biohybrid materials is systematically varied by combining different poly(2-alkyl-2-oxazolines) (POx) with heparin applying a Michael-type addition crosslinking scheme: POx of gradated hydrophilicity and temperature-responsiveness provides polymer networks of distinctly different stiffness and swelling. Adjusting the mechanical properties and the GAG concentration of the gels to similar values allows for modulating the release of GAG-binding growth factors (VEGF165 and PDGF-BB) by the choice of the POx and its temperature-dependent conformation. Adsorption of fibronectin, growth of fibroblasts, and bacterial adhesion scale with the hydrophobicity of the gel-incorporated POx. In vitro hemocompatibility tests with freshly drawn human whole blood show advantages of POx-based gels compared to the PEG-based reference materials. Biohybrid POx hydrogels can therefore enable biomedical technologies requiring GAG-based materials with customized and switchable physicochemical characteristics. © 2021 The Authors. Advanced Healthcare Materials published by Wiley-VCH GmbH.
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    Complex Metal Nanostructures with Programmable Shapes from Simple DNA Building Blocks
    (Weinheim : Wiley-VCH, 2021) Ye, Jingjing; Aftenieva, Olha; Bayrak, Türkan; Jain, Archa; König, Tobias A.F.; Erbe, Artur; Seidel, Ralf
    Advances in DNA nanotechnology allow the design and fabrication of highly complex DNA structures, uisng specific programmable interactions between smaller nucleic acid building blocks. To convey this concept to the fabrication of metallic nanoparticles, an assembly platform is developed based on a few basic DNA structures that can serve as molds. Programming specific interactions between these elements allows the assembly of mold superstructures with a range of different geometries. Subsequent seeded growth of gold within the mold cavities enables the synthesis of complex metal structures including tightly DNA-caged particles, rolling-pin- and dumbbell-shaped particles, as well as T-shaped and loop particles with high continuity. The method further supports the formation of higher-order assemblies of the obtained metal geometries. Based on electrical and optical characterizations, it is expected that the developed platform is a valuable tool for a self-assembly-based fabrication of nanoelectronic and nanooptic devices. © 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH
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    Amphiphilic Copolymers for Versatile, Facile, and In Situ Tunable Surface Biofunctionalization
    (Weinheim : Wiley-VCH, 2021) Ruland, André; Schenker, Saskia; Schirmer, Lucas; Friedrichs, Jens; Meinhardt, Andrea; Schwartz, Véronique B.; Kaiser, Nadine; Konradi, Rupert; MacDonald, William; Helmecke, Tina; Sikosana, Melissa K.L.N.; Valtin, Juliane; Hahn, Dominik; Renner, Lars D.; Werner, Carsten; Freudenberg, Uwe
    Precision surface engineering is key to advanced biomaterials. A new platform of PEGylated styrene-maleic acid copolymers for adsorptive surface biofunctionalization is reported. Balanced amphiphilicity renders the copolymers water-soluble but strongly affine for surfaces. Fine-tuning of their molecular architecture provides control over adsorptive anchorage onto specific materials-which is why they are referred to as "anchor polymers" (APs)-and over structural characteristics of the adsorbed layers. Conjugatable with an array of bioactives-including cytokine-complexing glycosaminoglycans, cell-adhesion-mediating peptides and antimicrobials-APs can be applied to customize materials for demanding biotechnologies in uniquely versatile, simple, and robust ways. Moreover, homo- and heterodisplacement of adsorbed APs provide unprecedented means of in situ alteration and renewal of the functionalized surfaces. The related options are exemplified with proof-of-concept experiments of controlled bacterial adhesion, human umbilical vein endothelial cell, and induced pluripotent cell growth on AP-functionalized surfaces.
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    Controlling Surface Wettability for Automated In Situ Array Synthesis and Direct Bioscreening
    (Weinheim : Wiley-VCH, 2021) Lin, Weilin; Gandhi, Shanil; Oviedo Lara, Alan Rodrigo; Thomas, Alvin K.; Helbig, Ralf; Zhang, Yixin
    The in situ synthesis of biomolecules on glass surfaces for direct bioscreening can be a powerful tool in the fields of pharmaceutical sciences, biomaterials, and chemical biology. However, it is still challenging to 1) achieve this conventional multistep combinatorial synthesis on glass surfaces with small feature sizes and high yields and 2) develop a surface which is compatible with solid-phase syntheses, as well as the subsequent bioscreening. This work reports an amphiphilic coating of a glass surface on which small droplets of polar aprotic organic solvents can be deposited with an enhanced contact angle and inhibited motion to permit fully automated multiple rounds of the combinatorial synthesis of small-molecule compounds and peptides. This amphiphilic coating can be switched into a hydrophilic network for protein- and cell-based screening. Employing this in situ synthesis method, chemical space can be probed via array technology with unprecedented speed for various applications, such as lead discovery/optimization in medicinal chemistry and biomaterial development.
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    Thiophene-Bridged Donor–Acceptor sp2-Carbon-Linked 2D Conjugated Polymers as Photocathodes for Water Reduction
    (Weinheim : Wiley-VCH, 2021) Xu, Shunqi; Sun, Hanjun; Addicoat, Matthew; Biswal, Bishnu P.; He, Fan; Park, SangWook; Paasch, Silvia; Zhang, Tao; Sheng, Wenbo; Brunner, Eike; Hou, Yang; Richter, Marcus; Feng, Xinliang
    Photoelectrochemical (PEC) water reduction, converting solar energy into environmentally friendly hydrogen fuel, requires delicate design and synthesis of semiconductors with appropriate bandgaps, suitable energy levels of the frontier orbitals, and high intrinsic charge mobility. In this work, the synthesis of a novel bithiophene-bridged donor–acceptor-based 2D sp2-carbon-linked conjugated polymer (2D CCP) is demonstrated. The Knoevenagel polymerization between the electron-accepting building block 2,3,8,9,14,15-hexa(4-formylphenyl) diquinoxalino[2,3-a:2′,3′-c]phenazine (HATN-6CHO) and the first electron-donating linker 2,2′-([2,2′-bithiophene]-5,5′-diyl)diacetonitrile (ThDAN) provides the 2D CCP-HATNThDAN (2D CCP-Th). Compared with the corresponding biphenyl-bridged 2D CCP-HATN-BDAN (2D CCP-BD), the bithiophene-based 2D CCP-Th exhibits a wide light-harvesting range (up to 674 nm), a optical energy gap (2.04 eV), and highest energy occupied molecular orbital–lowest unoccupied molecular orbital distributions for facilitated charge transfer, which make 2D CCP-Th a promising candidate for PEC water reduction. As a result, 2D CCP-Th presents a superb H2-evolution photocurrent density up to ≈7.9 µA cm−2 at 0 V versus reversible hydrogen electrode, which is superior to the reported 2D covalent organic frameworks and most carbon nitride materials (0.09–6.0 µA cm−2). Density functional theory calculations identify the thiophene units and cyano substituents at the vinylene linkage as active sites for the evolution of H2. © 2020 The Authors. Advanced Materials published by Wiley-VCH GmbH
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    Nanoimprint Lithography Facilitated Plasmonic-Photonic Coupling for Enhanced Photoconductivity and Photocatalysis
    (Weinheim : Wiley-VCH, 2021) Gupta, Vaibhav; Sarkar, Swagato; Aftenieva, Olha; Tsuda, Takuya; Kumar, Labeesh; Schletz, Daniel; Schultz, Johannes; Kiriy, Anton; Fery, Andreas; Vogel, Nicolas; König, Tobias A.F.
    Imprint lithography has emerged as a reliable, reproducible, and rapid method for patterning colloidal nanostructures. As a promising alternative to top-down lithographic approaches, the fabrication of nanodevices has thus become effective and straightforward. In this study, a fusion of interference lithography (IL) and nanosphere imprint lithography on various target substrates ranging from carbon film on transmission electron microscope grid to inorganic and dopable polymer semiconductor is reported. 1D plasmonic photonic crystals are printed with 75% yield on the centimeter scale using colloidal ink and an IL-produced polydimethylsiloxane stamp. Atomically smooth facet, single-crystalline, and monodisperse colloidal building blocks of gold (Au) nanoparticles are used to print 1D plasmonic grating on top of a titanium dioxide (TiO2) slab waveguide, producing waveguide-plasmon polariton modes with superior 10 nm spectral line-width. Plasmon-induced hot electrons are confirmed via two-terminal current measurements with increased photoresponsivity under guiding conditions. The fabricated hybrid structure with Au/TiO2 heterojunction enhances photocatalytic processes like degradation of methyl orange (MO) dye molecules using the generated hot electrons. This simple colloidal printing technique demonstrated on silicon, glass, Au film, and naphthalenediimide polymer thus marks an important milestone for large-scale implementation in optoelectronic devices. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH