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Organic or inorganic (A) metal (M) halide (X) perovskites (AMX(3)) are semiconductor materials setting the basis for the development of highly efficient, low-cost and multijunction solar energy conversion devices. The best efficiencies nowadays are obtained with mixed compositions containing methylammonium, formamidinium, Cs and Rb as well as iodine, bromine and chlorine as anions. The understanding of fundamental properties such as crystal structure and its effect on the band gap, as well as their phase stability is essential. In this systematic study X-ray diffraction and photoluminescense spectroscopy were applied to evaluate structural and optoelectronic properties of hybrid perovskites with mixed compositions.
Calcium phosphate nanofibers with a diameter of only a few nanometers and a cotton-ball-like aggregate morphology have been reported several times in the literature. Although fiber formation seems reproducible in a variety of conditions, the crystal structure and chemical composition of the fibers have been elusive. Using scanning transmission electron microscopy, low dose electron (nano)diffraction, energy-dispersive X-ray spectroscopy, and energy- filtered transmission electron microscopy, we have assigned crystal structures and chemical compositions to the fibers. Moreover, we demonstrate that the mineralization process yields true polymer/calcium phosphate hybrid materials where the block copolymer template is closely associated with the calcium phosphate.
The lack of anionic carboxylate ligands on the surface of InP/ZnSe/ZnS quantum dots (QDs), where zinc carboxylate ligands can be converted to carboxylic acid or carboxylate ligands via proton transfer by 1-octanethiol, is demonstrated. The as-synthesized QDs initially have an under-coordinated vacancy surface, which is passivated by solvent ligands such as ethanol and acetone. Upon exposure of 1-octanethiol to the QD surface, 1-octanethiol effectively induces the surface binding of anionic carboxylate ligands (derived from zinc carboxylate ligands) by proton transfer, which consequently exchanges ethanol and acetone ligands that bind on the incomplete QD surface. These systematic chemical analyses, such as thermogravimetric analysis-mass spectrometry and proton nuclear magnetic resonance spectroscopy, directly show the interplay of surface ligands, and it associates with QD light-emitting diodes (QD-LEDs). It is believed that this better understanding can lead to industrially feasible QD-LEDs.
SpiderMAEn
(2019)
A growing energy demand requires new and preferably renewable energy sources. The infinite availability of solar radiation makes its conversion into storable and transportable energy forms attractive for research as well as for the industry. One promising example of a transportable fuel is hydrogen (H-2), making research into eco-friendly hydrogen production meaningful. Here, a hybrid system was developed using newly designed recombinant spider silk protein variants as a template for mineralization with inorganic titanium dioxide and gold. These bioinspired organic/inorganic hybrid materials allow for hydrogen production upon light irradiation. To begin with, recombinant spider silk proteins bearing titanium dioxide and gold-binding moieties were created and processed into structured films. These films were modified with gold and titanium dioxide in order to produce a photocatalyst. Subsequent testing revealed hydrogen production as a result of light-induced hydrolysis of water. Therefore, the novel setup presented here provides access to a new principle of generating advanced hybrid materials for sustainable hydrogen production and depicts a promising platform for further studies on photocatalytic production of hydrogen, the most promising future fuel.
The phase behavior of an amphiphilic block copolymer based on a poly(aspartic acid) hydrophilic block and a poly(n-butyl acrylate) hydrophobic block was investigated at the air–water and air–buffer interface. The polymer forms stable monomolecular films on both subphases. At low pH, the isotherms exhibit a plateau. Compression–expansion experiments and infrared reflection absorption spectroscopy suggest that the plateau is likely due to the formation of polymer bi- or multilayers. At high pH the films remain intact upon compression and no multilayer formation is observed. Furthermore, the mineralization of calcium phosphate beneath the monolayer was studied at different pH. The pH of the subphase and thus the polymer charge strongly affects the phase behavior of the film and the mineral formation. After 4 h of mineralization at low pH, atomic force microscopy shows smooth mineral films with a low roughness. With increasing pH the mineral films become inhomogeneous and the roughness increases. Transmission electron microscopy confirms this: at low pH a few small but uniform particles form whereas particles grown at higher pH are larger and highly agglomerated. Energy-dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy confirm the formation of calcium phosphate. The levels of mineralization are higher in samples grown at high pH.
Fully renewable pyridinium ionic liquids were synthesised via the hydrothermal decarboxylation of pyridinium zwitterions derived from furfural and amino acids in flow. The functionality of the resulting ionic liquid (IL) can be tuned by choice of different amino acids as well as different natural carboxylic acids as the counterions. A representative member of this new class of ionic liquids was successfully used for the synthesis of ionogels and as a solvent for the Heck coupling.
Mesoporous silica monoliths were prepared by the sol - gel technique and. lled with 1-ethyl-3-methyl imidazolium [Emim]-X (X = dicyanamide [N(CN)(2)], ethyl sulfate [EtSO4], thiocyanate [SCN], and triflate [TfO]) ionic liquids (ILs) using a methanol-IL exchange technique. The structure and behavior of the ILs inside the silica monoliths were studied using X-ray scattering, nitrogen sorption, IR spectroscopy, solid-state NMR, and thermal analysis. DSC finds shifts in both the glass transition temperature and melting points (where applicable) of the ILs. Glass transition and melting occur well below room temperature. There is thus no conflict with the NMR and IR data, which show that the ILs are as mobile at room temperature as the bulk (not confined) ILs. The very narrow line widths of the NMR spectra suggest that the ILs in our materials have the highest mobility reported for confined ILs so far. As a result, our data suggest that it is possible to generate IL/silica hybrid materials (ionogels) with bulk-like properties of the IL. This could be interesting for applications in, e.g., the solar cell or membrane fields.
Silica is an important mineral in biology and technology, and many protocols have been developed for the synthesis of complex silica architectures. The current report shows that silsesquioxane nanoparticles carrying polymer arms on their surface are efficient templates for the fabrication of silica particles with a star- or raspberry-like morphology. The shape of the resulting particles depends on the chemistry of the polymer arms. With poly(N,N- dimethylaminoethyl methacrylate) (PDMAEMA) arms, spherical particles with a less electron dense core form. With poly {[2- (methacryloyloxy)ethyl] trimethylammonium iodide} (PMETAI), star- or raspberry-like particles form. Electron microscopy, electron tomography, and small-angle X-ray scattering show that the resulting silica particles have a complex structure, where a silsequioxane nanoparticle carrying the polymer arms is in the center. Next is a region that is polymer-rich. The outermost region of the particle is a silica layer, where the outer parts of the polymer arms are embedded. Time- resolved zeta-potential and pH measurements, dynamic light scattering, and electron microscopy reveal that silica formation proceeds differently if PDMAEMA is exchanged for PMETAI.
Amphiphilic alkyl-poly(ethyleneimine)s (alkyl-PEI) with different degrees of polymerization have been produced by alkaline hydrolysis of alkyl-poly(2-methyl-2-oxazoline). Potentiometric titration of the alkyl-PEI shows the influence of the alkyl chain and the degree of polymerization on the titration curves and hence on the polymer conformation. Karl Fischer titration has been used to determine the water content in the polymers. Subsequent X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and differential scanning calorimetry (DSC) measurements prove the existence of different hydration states of the PEI even under dry storage conditions. Upon cooling from hot aqueous Solutions, hydrogels form. The gelation concentration decreases with increasing degree of polymerization of the PEI segment. Scanning electron microscopy (SEM and cryo-SEM) of the hydrogels reveal an alkyl-PEI fibrous network composed of fan-like units. DSC shows that the percentages of bound and free water in the hydrogels depend on the concentration of polar amino groups.
The report shows that simple LbL deposition of positively charged chitosan and negatively charged heparin can be used to efficiently modify the native surface of both NiTi and Ti without any previous treatments. Moreover, mineralization of the polymer multilayers with calcium phosphate leads to surfaces with low contact angles around 70 and 20 degrees for NiTi and Ti, respectively. This suggests that a polymer multilayer/calcium phosphate hybrid coating could be useful for making NiTi or Ti implants that are at the same time antibacterial (via the chitosan), suppress blood clot formation (via the heparin), and favor fast endothelialization (via the improved surface hydrophilicity compared to the respective neat material).