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Chemistry of Materials: a Publication of the American Chemical Society

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https://www.readbyqxmd.com/read/28713199/isothermal-crystallization-kinetics-and-time-temperature-transformation-of-the-conjugated-polymer-poly-3-2-ethyl-hexylthiophene
#1
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
#2
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
#3
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
#4
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
#5
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
#6
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
#7
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
#8
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
#9
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/28572706/electroactive-nanoporous-metal-oxides-and-chalcogenides-by-chemical-design
#10
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
#11
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
#12
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
#13
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
https://www.readbyqxmd.com/read/28413259/materials-genome-in-action-identifying-the-performance-limits-of-physical-hydrogen-storage
#14
Aaron W Thornton, Cory M Simon, Jihan Kim, Ohmin Kwon, Kathryn S Deeg, Kristina Konstas, Steven J Pas, Matthew R Hill, David A Winkler, Maciej Haranczyk, Berend Smit
The Materials Genome is in action: the molecular codes for millions of materials have been sequenced, predictive models have been developed, and now the challenge of hydrogen storage is targeted. Renewably generated hydrogen is an attractive transportation fuel with zero carbon emissions, but its storage remains a significant challenge. Nanoporous adsorbents have shown promising physical adsorption of hydrogen approaching targeted capacities, but the scope of studies has remained limited. Here the Nanoporous Materials Genome, containing over 850 000 materials, is analyzed with a variety of computational tools to explore the limits of hydrogen storage...
April 11, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28413258/fluorinated-polyurethane-scaffolds-for-19-f-magnetic-resonance-imaging
#15
Twan Lammers, Marianne E Mertens, Philipp Schuster, Khosrow Rahimi, Yang Shi, Volkmar Schulz, Alexander J C Kuehne, Stefan Jockenhoevel, Fabian Kiessling
Polymers are increasingly employed in implant materials. To reduce the incidence of complications, which in the case of vascular grafts include incorrect placement and restenosis, materials are needed which allow for image-guided implantation, as well as for accurate and efficient postoperative implant imaging. We here describe amorphous fluorinated polymers based on thermoplastic polyurethane ((19)F-TPU), and show that are useful starting materials for developing tissue-engineered vascular grafts which can be detected using (19)F MRI...
April 11, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28405059/uniform-atomic-layer-deposition-of-al2o3-on-graphene-by-reversible-hydrogen-plasma-functionalization
#16
René H J Vervuurt, Bora Karasulu, Marcel A Verheijen, Wilhelmus Erwin M M Kessels, Ageeth A Bol
A novel method to form ultrathin, uniform Al2O3 layers on graphene using reversible hydrogen plasma functionalization followed by atomic layer deposition (ALD) is presented. ALD on pristine graphene is known to be a challenge due to the absence of dangling bonds, leading to nonuniform film coverage. We show that hydrogen plasma functionalization of graphene leads to uniform ALD of closed Al2O3 films down to 8 nm in thickness. Hall measurements and Raman spectroscopy reveal that the hydrogen plasma functionalization is reversible upon Al2O3 ALD and subsequent annealing at 400 °C and in this way does not deteriorate the graphene's charge carrier mobility...
March 14, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28356613/atomic-layer-deposition-of-titanium-oxide-on-single-layer-graphene-an-atomic-scale-study-toward-understanding-nucleation-and-growth
#17
Yucheng Zhang, Carlos Guerra-Nuñez, Ivo Utke, Johann Michler, Piyush Agrawal, Marta D Rossell, Rolf Erni
Controlled synthesis of a hybrid nanomaterial based on titanium oxide and single-layer graphene (SLG) using atomic layer deposition (ALD) is reported here. The morphology and crystallinity of the oxide layer on SLG can be tuned mainly with the deposition temperature, achieving either a uniform amorphous layer at 60 °C or ∼2 nm individual nanocrystals on the SLG at 200 °C after only 20 ALD cycles. A continuous and uniform amorphous layer formed on the SLG after 180 cycles at 60 °C can be converted to a polycrystalline layer containing domains of anatase TiO2 after a postdeposition annealing at 400 °C under vacuum...
March 14, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28413257/tuning-and-locking-the-localized-surface-plasmon-resonances-of-cus-covellite-nanocrystals-by-an-amorphous-cupd-x-s-shell
#18
Yi Xie, Wenhui Chen, Giovanni Bertoni, Ilka Kriegel, Mo Xiong, Neng Li, Mirko Prato, Andreas Riedinger, Ayyappan Sathya, Liberato Manna
We demonstrate the stabilization of the localized surface plasmon resonance (LSPR) in a semiconductor-based core-shell heterostructure made of a plasmonic CuS core embedded in an amorphous-like alloyed CuPd x S shell. This heterostructure is prepared by reacting the as-synthesized CuS nanocrystals (NCs) with Pd(2+) cations at room temperature in the presence of an electron donor (ascorbic acid). The reaction starts from the surface of the CuS NCs and proceeds toward the center, causing reorganization of the initial lattice and amorphization of the covellite structure...
February 28, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28316369/understanding-the-electrochemical-formation-and-decomposition-of-li2o2-and-lioh-with-operando-x-ray-diffraction
#19
Zhaolong Li, Swapna Ganapathy, Yaolin Xu, Jouke R Heringa, Quanyao Zhu, Wen Chen, Marnix Wagemaker
The lithium air, or Li-O2, battery system is a promising electrochemical energy storage system because of its very high theoretical specific energy, as required by automotive applications. Fundamental research has resulted in much progress in mitigating detrimental (electro)chemical processes; however, the detailed structural evolution of the crystalline Li2O2 and LiOH discharge products, held at least partially responsible for the limited reversibility and poor rate performance, is hard to measure operando under realistic electrochemical conditions...
February 28, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/28260837/facet-dependent-interactions-of-islet-amyloid-polypeptide-with-gold-nanoparticles-implications-for-fibril-formation-and-peptide-induced-lipid-membrane-disruption
#20
Shih-Ting Wang, Yiyang Lin, Nevena Todorova, Yingqi Xu, Manuel Mazo, Subinoy Rana, Vincent Leonardo, Nadav Amdursky, Christopher D Spicer, Bruce D Alexander, Alison A Edwards, Steve J Matthews, Irene Yarovsky, Molly M Stevens
A comprehensive understanding of the mechanisms of interaction between proteins or peptides and nanomaterials is crucial for the development of nanomaterial-based diagnostics and therapeutics. In this work, we systematically explored the interactions between citrate-capped gold nanoparticles (AuNPs) and islet amyloid polypeptide (IAPP), a 37-amino acid peptide hormone co-secreted with insulin from the pancreatic islet. We utilized diffusion-ordered spectroscopy, isothermal titration calorimetry, localized surface plasmon resonance spectroscopy, gel electrophoresis, atomic force microscopy, transmission electron microscopy (TEM), and molecular dynamics (MD) simulations to systematically elucidate the underlying mechanism of the IAPP-AuNP interactions...
February 28, 2017: Chemistry of Materials: a Publication of the American Chemical Society
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