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Chemistry of Materials: a Publication of the American Chemical Society

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https://www.readbyqxmd.com/read/29129959/cancer-targeting-ultrasmall-silica-nanoparticles-for-clinical-translation-physicochemical-structure-and-biological-property-correlations
#1
Feng Chen, Kai Ma, Miriam Benezra, Li Zhang, Sarah M Cheal, Evan Phillips, Barney Yoo, Mohan Pauliah, Michael Overholtzer, Pat Zanzonico, Sonia Sequeira, Mithat Gonen, Thomas Quinn, Ulrich Wiesner, Michelle S Bradbury
Although a large body of literature exists on the potential use of nanoparticles for medical applications, the number of probes translated into human clinical trials is remarkably small. A major challenge of particle probe development and their translation is the elucidation of safety profiles associated with their structural complexity, not only in terms of size distribution and heterogeneities in particle composition but also their effects on biological activities and the relationship between particle structure and pharmacokinetics...
October 24, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29123332/target-or-clear-zirconium-89-labeled-silica-nanoparticles-for-enhanced-cancer-directed-uptake-in-melanoma-a-comparison-of-radiolabeling-strategies
#2
Feng Chen, Kai Ma, Li Zhang, Brian Madajewski, Pat Zanzonico, Sonia Sequeira, Mithat Gonen, Ulrich Wiesner, Michelle S Bradbury
Designing a nanomaterials platform with high target-to-background ratios has long been one of the major challenges in the field of nanomedicine. Here, we introduce a "target-or-clear" multifunctional nanoparticle platform that demonstrates high tumor-targeting efficiency and retention while minimizing off-target effects. Encouraged by the favorable preclinical and clinical pharmacokinetic profiles derived after fine-tuning surface chemical properties of radioiodinated ((124)I, t1/2 = 100.2 h) ultrasmall cRGDY-conjugated fluorescent silica nanoparticles (C dots), we sought to investigate how the biological properties of these radioconjugates could be influenced by the conjugation of radiometals such as zirconium-89 ((89)Zr, t1/2 = 78...
October 10, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28989232/setting-directions-anisotropy-in-hierarchically-organized-porous-silica
#3
Florian Putz, Roland Morak, Michael S Elsaesser, Christian Balzer, Stephan Braxmeier, Johannes Bernardi, Oskar Paris, Gudrun Reichenauer, Nicola Hüsing
Structural hierarchy, porosity, and isotropy/anisotropy are highly relevant factors for mechanical properties and thereby the functionality of porous materials. However, even though anisotropic and hierarchically organized, porous materials are well known in nature, such as bone or wood, producing the synthetic counterparts in the laboratory is difficult. We report for the first time a straightforward combination of sol-gel processing and shear-induced alignment to create hierarchical silica monoliths exhibiting anisotropy on the levels of both, meso- and macropores...
September 26, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28852267/fabrication-and-postmodification-of-nanoporous-liquid-crystalline-networks-via-dynamic-covalent-chemistry
#4
Dirk J Mulder, Luc M W Scheres, Jingjin Dong, Giuseppe Portale, Dirk J Broer, Albertus P H J Schenning
No abstract text is available yet for this article.
August 22, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29123331/aptamer-functionalized-hydrogel-for-self-programmed-protein-release-via-sequential-photoreaction-and-hybridization
#5
Jinping Lai, Pinliang Jiang, Erin R Gaddes, Nan Zhao, Lidya Abune, Yong Wang
A dynamic hydrogel that sequentially responds to two independent but interrelated physical and biomolecular signals was reported in this work. Once hit by an external light signal, an immobilized internal molecular signal is activated and freed via photoreaction; and subsequently the freed molecular signal works as a self-programming factor of the hydrogel to induce the dissociation of a biomolecular complex to release protein via hybridization reaction. Notably, pulsatile external light input can be converted to periodical protein output from the hydrogel to regulate cell migration...
July 25, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28890605/highly-planarized-naphthalene-diimide-bifuran-copolymers-with-unexpected-charge-transport-performance
#6
Rukiya Matsidik, Alessandro Luzio, Özge Askin, Daniele Fazzi, Alessandro Sepe, Ullrich Steiner, Hartmut Komber, Mario Caironi, Michael Sommer
The synthesis, characterization, and charge transport performance of novel copolymers PNDIFu2 made from alternating naphthalene diimide (NDI) and bifuran (Fu2) units are reported. Usage of potentially biomass-derived Fu2 as alternating repeat unit enables flattened polymer backbones due to reduced steric interactions between the imide oxygens and Fu2 units, as seen by density functional theory (DFT) calculations and UV-vis spectroscopy. Aggregation of PNDIFu2 in solution is enhanced if compared to the analogous NDI-bithiophene (T2) copolymers PNDIT2, occurring in all solvents and temperatures probed...
July 11, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28713199/isothermal-crystallization-kinetics-and-time-temperature-transformation-of-the-conjugated-polymer-poly-3-2-ethyl-hexylthiophene
#7
Liyang Yu, Emily Davidson, Anirudh Sharma, Mats R Andersson, Rachel Segalman, Christian Müller
Thermal annealing strongly impacts the nano- and microstructure of conjugated polymers. Despite the fundamental importance for the resulting optoelectronic behavior of this class of materials, the underlying crystallization processes have not received the same attention that is encountered in other disciplines of materials science. The question arises whether classical treatment of nucleation and growth phenomena is truly applicable to conjugated polymers? Here, the isothermal crystallization behavior of the conjugated polymer poly(3-(2'-ethyl)hexylthiophene) (P3EHT) is monitored with differential scanning calorimetry (DSC)...
July 11, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28706347/ga-for-zn-cation-exchange-allows-for-highly-luminescent-and-photostable-inznp-based-quantum-dots
#8
Francesca Pietra, Nicholas Kirkwood, Luca De Trizio, Anne W Hoekstra, Lennart Kleibergen, Nicolas Renaud, Rolf Koole, Patrick Baesjou, Liberato Manna, Arjan J Houtepen
In this work, we demonstrate that a preferential Ga-for-Zn cation exchange is responsible for the increase in photoluminescence that is observed when gallium oleate is added to InZnP alloy QDs. By exposing InZnP QDs with varying Zn/In ratios to gallium oleate and monitoring their optical properties, composition, and size, we conclude that Ga(3+) preferentially replaces Zn(2+), leading to the formation of InZnP/InGaP core/graded-shell QDs. This cation exchange reaction results in a large increase of the QD photoluminescence, but only for InZnP QDs with Zn/In ≥ 0...
June 27, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28638177/highly-luminescent-water-dispersible-nir-emitting-wurtzite-cuins2-zns-core-shell-colloidal-quantum-dots
#9
Chenghui Xia, Johannes D Meeldijk, Hans C Gerritsen, Celso de Mello Donega
Copper indium sulfide (CIS) quantum dots (QDs) are attractive as labels for biomedical imaging, since they have large absorption coefficients across a broad spectral range, size- and composition-tunable photoluminescence from the visible to the near-infrared, and low toxicity. However, the application of NIR-emitting CIS QDs is still hindered by large size and shape dispersions and low photoluminescence quantum yields (PLQYs). In this work, we develop an efficient pathway to synthesize highly luminescent NIR-emitting wurtzite CIS/ZnS QDs, starting from template Cu2-x S nanocrystals (NCs), which are converted by topotactic partial Cu(+) for In(3+) exchange into CIS NCs...
June 13, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28572705/monodisperse-iron-oxide-nanoparticles-by-thermal-decomposition-elucidating-particle-formation-by-second-resolved-in-situ-small-angle-x-ray-scattering
#10
A Lassenberger, T A Grünewald, P D J van Oostrum, H Rennhofer, H Amenitsch, R Zirbs, H C Lichtenegger, E Reimhult
The synthesis of iron oxide nanoparticles (NPs) by thermal decomposition of iron precursors using oleic acid as surfactant has evolved to a state-of-the-art method to produce monodisperse, spherical NPs. The principles behind such monodisperse syntheses are well-known: the key is a separation between burst nucleation and growth phase, whereas the size of the population is set by the precursor-to-surfactant ratio. Here we follow the thermal decomposition of iron pentacarbonyl in the presence of oleic acid via in situ X-ray scattering...
May 23, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28572704/multiporous-supramolecular-microspheres-for-artificial-photosynthesis
#11
Kai Tao, Bin Xue, Samuel Frere, Inna Slutsky, Yi Cao, Wei Wang, Ehud Gazit
Artificial photosynthesis shows a promising potential for sustainable supply of nutritional ingredients. While most studies focus on the assembly of the light-sensitive chromophores to 1-D architectures in an artificial photosynthesis system, other supramolecular morphologies, especially bioinspired ones, which may have more efficient light-harvesting properties, have been far less studied. Here, MCpP-FF, a bioinspired building block fabricated by conjugating porphyrin and diphenylalanine, was designed to self-assemble into nanofibers-based multiporous microspheres...
May 23, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28572703/efficient-and-stable-luminescence-from-mn-2-in-core-and-core-isocrystalline-shell-cspbcl3-perovskite-nanocrystals
#12
Kunyuan Xu, Chun Che Lin, Xiaobin Xie, Andries Meijerink
There has been a growing interest in applying CsPbX3 (X = Cl, Br, I) nanocrystals (NCs) for optoelectronic application. However, research on doping of this new class of promising NCs with optically active and/or magnetic transition metal ions is still limited. Here we report a facile room temperature method for Mn(2+) doping into CsPbCl3 NCs. By addition of a small amount of concentrated HCl acid to a clear solution containing Mn(2+), Cs(+), and Pb(2+) precursors, Mn(2+)-doped CsPbCl3 NCs with strong orange luminescence of Mn(2+) at ∼600 nm are obtained...
May 23, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28572702/changing-the-dimensionality-of-cesium-lead-bromide-nanocrystals-by-reversible-postsynthesis-transformations-with-amines
#13
Francisco Palazon, Guilherme Almeida, Quinten A Akkerman, Luca De Trizio, Zhiya Dang, Mirko Prato, Liberato Manna
No abstract text is available yet for this article.
May 23, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28539702/one-step-synthesis-of-hierarchical-zsm-5-using-cetyltrimethylammonium-as-mesoporogen-and-structure-directing-agent
#14
Lingqian Meng, Brahim Mezari, Maarten G Goesten, Emiel J M Hensen
Hierarchical ZSM-5 zeolite is hydrothermally synthesized in a single step with cetyltrimethylammonium (CTA) hydroxide acting as mesoporogen and structure-directing agent. Essential to this synthesis is the replacement of NaOH with KOH. An in-depth solid-state NMR study reveals that, after early electrostatic interaction between condensed silica and the head group of CTA, ZSM-5 crystallizes around the structure-directing agent. The crucial aspect of using KOH instead of NaOH lies in the faster dissolution of silica, thereby providing sufficient nutrients for zeolite nucleation...
May 9, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28503030/ligand-induced-shape-transformation-of-pbse-nanocrystals
#15
Joep L Peters, Karel H W van den Bos, Sandra Van Aert, Bart Goris, Sara Bals, Daniël Vanmaekelbergh
We present a study of the relation between the surface chemistry and nanocrystal shape of PbSe nanocrystals with a variable Pb-to-Se stoichiometry and density of oleate ligands. The oleate ligand density and binding configuration are monitored by nuclear magnetic resonance and Fourier transform infrared absorbance spectroscopy, allowing us to quantify the number of surface-attached ligands per NC and the nature of the surface-Pb-oleate configuration. The three-dimensional shape of the PbSe nanocrystals is obtained from high-angle annular dark field scanning transmission electron microscopy combined with an atom counting method...
May 9, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28989233/extremely-slow-spontaneous-electron-trapping-in-photodoped-n-type-cdse-nanocrystals
#16
Emily Y Tsui, Gerard M Carroll, Brigit Miller, Arianna Marchioro, Daniel R Gamelin
The trapping dynamics of conduction-band electrons in colloidal degenerately doped n-CdSe nanocrystals prepared by photochemical reduction (photodoping) were measured by direct optical methods. The nanocrystals show spontaneous electron trapping with distributed kinetics that extend to remarkably long timescales. Shifts in nanocrystal band-edge potentials caused by quantum confinement and surface ion stoichiometry were also measured by spectroelectrochemical techniques, and their relationship to the slow electron trapping is discussed...
April 25, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28572706/electroactive-nanoporous-metal-oxides-and-chalcogenides-by-chemical-design
#17
Christopher H Hendon, Keith T Butler, Alex M Ganose, Yuriy Román-Leshkov, David O Scanlon, Geoffrey A Ozin, Aron Walsh
The archetypal silica- and aluminosilicate-based zeolite-type materials are renowned for wide-ranging applications in heterogeneous catalysis, gas-separation and ion-exchange. Their compositional space can be expanded to include nanoporous metal chalcogenides, exemplified by germanium and tin sulfides and selenides. By comparison with the properties of bulk metal dichalcogenides and their 2D derivatives, these open-framework analogues may be viewed as three-dimensional semiconductors filled with nanometer voids...
April 25, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28435185/influence-of-rb-cs-cation-exchange-on-inorganic-sn-halide-perovskites-from-chemical-structure-to-physical-properties
#18
Young-Kwang Jung, Ji-Hwan Lee, Aron Walsh, Aloysius Soon
CsSnI3 is a potential lead-free inorganic perovskite for solar energy applications due to its nontoxicity and attractive optoelectronic properties. Despite these advantages, photovoltaic cells using CsSnI3 have not been successful to date, in part due to low stability. We demonstrate how gradual substitution of Rb for Cs influences the structural, thermodynamic, and electronic properties on the basis of first-principles density functional theory calculations. By examining the effect of the Rb:Cs ratio, we reveal a correlation between octahedral distortion and band gap, including spin-orbit coupling...
April 11, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28413261/sculpting-silica-colloids-by-etching-particles-with-nonuniform-compositions
#19
Fabian Hagemans, Wessel Vlug, Chiara Raffaelli, Alfons van Blaaderen, Arnout Imhof
We present the synthesis of new shapes of colloidal silica particles by manipulating their chemical composition and subsequent etching. Segments of silica rods, prepared by the ammonia catalyzed hydrolysis and condensation of tetraethylorthosilicate (TEOS) from polyvinylpyrrolidone loaded water droplets, were grown under different conditions. Upon decreasing temperature, delaying ethanol addition, or increasing monomer concentration, the rate of dissolution of the silica segment subsequently formed decreased...
April 11, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28413260/missing-linkers-an-alternative-pathway-to-uio-66-electronic-structure-engineering
#20
Arthur De Vos, Kevin Hendrickx, Pascal Van Der Voort, Veronique Van Speybroeck, Kurt Lejaeghere
UiO-66 is a promising metal-organic framework for photocatalytic applications. However, the ligand-to-metal charge transfer of an excited electron is inefficient in the pristine material. Herein, we assess the influence of missing linker defects on the electronic structure of UiO-66 and discuss their ability to improve ligand-to-metal charge transfer. Using a new defect classification system, which is transparent and easily extendable, we identify the most promising photocatalysts by considering both relative stability and electronic structure...
April 11, 2017: Chemistry of Materials: a Publication of the American Chemical Society
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