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Chemistry of Materials: a Publication of the American Chemical Society

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https://read.qxmd.com/read/30930536/guanidinium-and-mixed-cesium-guanidinium-tin-ii-bromides-effects-of-quantum-confinement-and-out-of-plane-octahedral-tilting
#1
Olga Nazarenko, Martin R Kotyrba, Sergii Yakunin, Michael Wörle, Bogdan M Benin, Gabriele Rainò, Frank Krumeich, Mikaël Kepenekian, Jacky Even, Claudine Katan, Maksym V Kovalenko
Hybrid organic-inorganic main-group metal halide compounds are the subject of intense research owing to their unique optoelectronic characteristics. In this work, we report the synthesis, structure, and electronic and optical properties of a family of hybrid tin (II) bromide compounds comprising guanidinium [G, C(NH2 )3 + ] and mixed cesium-guanidinium cations: G2 SnBr4 , CsGSnBr4 , and Cs2 GSn2 Br7 . G2 SnBr4 has a one-dimensional structure that consists of chains of corner-sharing [SnBr5 ]2- square pyramids and G cations situated in between the chains...
March 26, 2019: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30930535/molecular-insights-into-carbon-dioxide-sorption-in-hydrazone-based-covalent-organic-frameworks-with-tertiary-amine-moieties
#2
Kerstin Gottschling, Linus Stegbauer, Gökcen Savasci, Nathan A Prisco, Zachariah J Berkson, Christian Ochsenfeld, Bradley F Chmelka, Bettina V Lotsch
Tailorable sorption properties at the molecular level are key for efficient carbon capture and storage and a hallmark of covalent organic frameworks (COFs). Although amine functional groups are known to facilitate CO2 uptake, atomistic insights into CO2 sorption by COFs modified with amine-bearing functional groups are scarce. Herein, we present a detailed study of the interactions of carbon dioxide and water with two isostructural hydrazone-linked COFs with different polarities based on the 2,5-diethoxyterephthalohydrazide linker...
March 26, 2019: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30918420/directed-functionalization-tailors-the-polarized-emission-and-waveguiding-properties-of-anthracene-based-molecular-crystals
#3
Andrea Camposeo, Devin B Granger, Sean R Parkin, Davide Altamura, Cinzia Giannini, John E Anthony, Dario Pisignano
Organic semiconducting crystals are characterized by anisotropic optical and electronic properties, which can be tailored by controlling the packing of the constituent molecules in the crystal unit cell. Here, the synthesis, structural characterization, and emission of anthracene derivatives are focused to correlate directed functionalization and optical properties. These compounds are easily and scalably prepared by standard synthesis techniques, and alterations in functional groups yield materials with either exclusive edge-to-face or face-to-face solid-state interactions...
March 12, 2019: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30894784/sizing-curve-absorption-coefficient-surface-chemistry-and-aliphatic-chain-structure-of-pbte-nanocrystals
#4
Joep L Peters, Jur de Wit, Daniël Vanmaekelbergh
For colloidal semiconductor nanocrystals (NCs), the knowledge of the chemical structure and the size-dependent optical properties is of crucial importance, both from a practical and fundamental perspective. Here, we report the basic properties of PbTe NCs in order to complement the already existing knowledge on PbS and PbSe NCs. The band gap versus NC diameter (sizing) curve was determined by combining transmission electron microscopy with absorption spectroscopy; the energy of the primary optical absorption follows 1/ d dependence with the diameter...
March 12, 2019: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30886456/quantitative-measure-of-the-size-dispersity-in-ultrasmall-fluorescent-organic-inorganic-hybrid-core-shell-silica-nanoparticles-by-small-angle-x-ray-scattering
#5
Katherine P Barteau, Kai Ma, Ferdinand F E Kohle, Thomas C Gardinier, Peter A Beaucage, Richard Edward Gillilan, Ulrich Wiesner
Small-angle X-ray scattering (SAXS) was performed on dispersions of ultrasmall (d < 10 nm) fluorescent organic-inorganic hybrid core-shell silica nanoparticles synthesized in aqueous solutions (C' dots) by using an oscillating flow cell to overcome beam induced particle degradation. Form factor analysis and fitting was used to determine the size and size dispersity of the internal silica core containing covalently encapsulated fluorophores. The structure of the organic poly(ethylene glycol) (PEG) shell was modelled as a monodisperse corona containing concentrated and semi-dilute regimes of decaying density and as a simple polydisperse shell to determine the bounds of dispersity in the overall hybrid particle...
February 12, 2019: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30828131/band-gap-tuning-of-solution-processed-ferroelectric-perovskite-bife-1-x-co-x-o-3-thin-films
#6
Pamela Machado, Mateusz Scigaj, Jaume Gazquez, Estel Rueda, Antonio Sánchez-Díaz, Ignasi Fina, Martí Gibert-Roca, Teresa Puig, Xavier Obradors, Mariano Campoy-Quiles, Mariona Coll
Ferroelectric perovskite oxides are emerging as a promising photoactive layer for photovoltaic applications because of their very high stability and their alternative ferroelectricity-related mechanism for solar energy conversion that could lead to extraordinarily high efficiencies. One of the biggest challenges so far is to reduce their band gap toward the visible region while simultaneously retaining ferroelectricity. To address these two issues, herein an elemental composition engineering of BiFeO3 is performed by substituting Fe by Co cations, as a means to tune the characteristics of the transition metal-oxygen bond...
February 12, 2019: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30686859/water-dispersible-copper-sulfide-nanocrystals-via-ligand-exchange-of-1-dodecanethiol
#7
Christina H M van Oversteeg, Freddy E Oropeza, Jan P Hofmann, Emiel J M Hensen, Petra E de Jongh, Celso de Mello Donega
In colloidal Cu2- x S nanocrystal synthesis, thiols are often used as organic ligands and the sulfur source, as they yield high-quality nanocrystals. However, thiol ligands on Cu2- x S nanocrystals are difficult to exchange, limiting the applications of these nanocrystals in photovoltaics, biomedical sensing, and photocatalysis. Here, we present an effective and facile procedure to exchange native 1-dodecanethiol on Cu2- x S nanocrystals by 3-mercaptopropionate, 11-mercaptoundecanoate, and S2- in formamide under inert atmosphere...
January 22, 2019: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30686858/shaping-silica-rods-by-tuning-hydrolysis-and-condensation-of-silica-precursors
#8
Fabian Hagemans, Ravi Kumar Pujala, Danisha S Hotie, Dominique M E Thies-Weesie, D A Matthijs de Winter, Johannes D Meeldijk, Alfons van Blaaderen, Arnout Imhof
We present the synthesis of colloidal silica particles with new shapes by manipulating the growth conditions of rods that are growing from polyvinylpyrrolidone-loaded water-rich droplets containing ammonia and ethanol. The silica rods grow by ammonia-catalyzed hydrolysis and condensation of tetraethoxysilane (TEOS). The lengthwise growth of these silica rods gives us the opportunity to change the conditions at any time during the reaction. In this work, we vary the availability of hydrolyzed monomers as a function of time and study how the change in balance between the hydrolysis and condensation reactions affects a typical synthesis (as described in more detail by our group earlier1)...
January 22, 2019: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30774194/from-the-bottom-up-toward-area-selective-atomic-layer-deposition-with-high-selectivity
#9
REVIEW
Adriaan J M Mackus, Marc J M Merkx, Wilhelmus M M Kessels
Bottom-up nanofabrication by area-selective atomic layer deposition (ALD) is currently gaining momentum in semiconductor processing, because of the increasing need for eliminating the edge placement errors of top-down processing. Moreover, area-selective ALD offers new opportunities in many other areas such as the synthesis of catalysts with atomic-level control. This Perspective provides an overview of the current developments in the field of area-selective ALD, discusses the challenge of achieving a high selectivity, and provides a vision for how area-selective ALD processes can be improved...
January 8, 2019: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30487664/spectroelectrochemical-signatures-of-surface-trap-passivation-on-cdte-nanocrystals
#10
Ward van der Stam, Indy du Fossé, Gianluca Grimaldi, Julius O V Monchen, Nicholas Kirkwood, Arjan J Houtepen
The photoluminescence (PL) quantum yield of semiconductor nanocrystals (NCs) is hampered by in-gap trap states due to dangling orbitals on the surface of the nanocrystals. While crucial for the rational design of nanocrystals, the understanding of the exact origin of trap states remains limited. Here, we treat CdTe nanocrystal films with different metal chloride salts and we study the effect on their optical properties with in situ spectroelectrochemistry, recording both changes in absorption and photoluminescence...
November 13, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30487663/reactivity-of-amorphous-carbon-surfaces-rationalizing-the-role-of-structural-motifs-in-functionalization-using-machine-learning
#11
Miguel A Caro, Anja Aarva, Volker L Deringer, Gábor Csányi, Tomi Laurila
Systematic atomistic studies of surface reactivity for amorphous materials have not been possible in the past because of the complexity of these materials and the lack of the computer power necessary to draw representative statistics. With the emergence and popularization of machine learning (ML) approaches in materials science, systematic (and accurate) studies of the surface chemistry of disordered materials are now coming within reach. In this paper, we show how the reactivity of amorphous carbon (a-C) surfaces can be systematically quantified and understood by a combination of ML interatomic potentials, ML clustering techniques, and density functional theory calculations...
November 13, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30344371/ab-initio-study-of-sodium-insertion-in-the-%C3%AE-mn-2-o-4-and-dis-ordered-%C3%AE-mn-1-5-ni-0-5-o-4-spinels
#12
Alexandros Vasileiadis, Brian Carlsen, Niek J J de Klerk, Marnix Wagemaker
The main challenge of sodium-ion batteries is cycling stability, which is usually compromised due to strain induced by sodium insertion. Reliable high-voltage cathode materials are needed to compensate the generally lower operating voltages of Na-ion batteries compared to Li-ion ones. Herein, density functional theory (DFT) computations were used to evaluate the thermodynamic, structural, and kinetic properties of the high voltage λ-Mn2 O4 and λ-Mn1.5 Ni0.5 O4 spinel structures as cathode materials for sodium-ion batteries...
October 9, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30270987/one-pot-gram-scale-synthesis-of-hydrogen-terminated-silicon-nanoparticles
#13
Sidharam P Pujari, Hafedh Driss, Fatma Bannani, Barend van Lagen, Han Zuilhof
Silicon nanoparticles (Si NPs) are highly attractive materials for typical quantum dots functions, such as in light-emitting and bioimaging applications, owing to silicon's intrinsic merits of minimal toxicity, low cost, high abundance, and easy and highly stable functionalization. Especially nonoxidized Si NPs with a covalently bound coating serve well in these respects, given the minimization of surface defects upon hydrosilylation of H-terminated Si NPs. However, to date, methods to obtain such H-terminated Si NPs are still not easy...
September 25, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30319176/reversible-photoswitching-function-in-atomic-molecular-layer-deposited-zno-azobenzene-superlattice-thin-films
#14
Aida Khayyami, Maarit Karppinen
We report new types of reversibly photoresponsive ZnO:azobenzene superlattice thin films fabricated through atomic/molecular-layer deposition (ALD/MLD) from diethylzinc, water, and 4,4'-azobenzene dicarboxylic acid precursors. In these ultrathin films, crystalline ZnO layers are interspersed with monomolecular photoactive azobenzene dicarboxylate layers. The thickness of the individual ZnO layers is precisely controlled by the number ( m ) of ALD cycles applied between two subsequent MLD cycles for the azobenzene layers; in our {[(Zn-O) m +(Zn-O2 -C-C6 H4 -N=N-C6 H4 -C-O2 )] n +(Zn-O) m } samples, m ranges from 0 to 240...
September 11, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30270986/colloidal-phase-change-materials-synthesis-of-monodisperse-gete-nanoparticles-and-quantification-of-their-size-dependent-crystallization
#15
Olesya Yarema, Aleksandr Perevedentsev, Vladimir Ovuka, Paul Baade, Sebastian Volk, Vanessa Wood, Maksym Yarema
Phase-change memory materials refer to a class of materials that can exist in amorphous and crystalline phases with distinctly different electrical or optical properties, as well as exhibit outstanding crystallization kinetics and optimal phase transition temperatures. This paper focuses on the potential of colloids as phase-change memory materials. We report a novel synthesis for amorphous GeTe nanoparticles based on an amide-promoted approach that enables accurate size control of GeTe nanoparticles between 4 and 9 nm, narrow size distributions down to 9-10%, and synthesis upscaling to reach multigram chemical yields per batch...
September 11, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30197470/unveiling-the-outstanding-oxygen-mass-transport-properties-of-mn-rich-perovskites-in-grain-boundary-dominated-la-0-8-sr-0-2-mn-1-x-co-x-0-85-o-3%C3%A2-%C3%AE-nanostructures
#16
Aruppukottai M Saranya, Alex Morata, Dolors Pla, Mónica Burriel, Francesco Chiabrera, Iñigo Garbayo, Aitor Hornés, John A Kilner, Albert Tarancón
Ion transport in solid-state devices is of great interest for current and future energy and information technologies. A superior enhancement of several orders of magnitude of the oxygen diffusivity has been recently reported for grain boundaries in lanthanum-strontium manganites. However, the significance and extent of this unique phenomenon are not yet established. Here, we fabricate a thin film continuous composition map of the La0.8 Sr0.2 (Mn1- x Co x )0.85 O3±δ family revealing a substantial enhancement of the grain boundary oxygen mass transport properties for the entire range of compositions...
August 28, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30197469/soft-nondamaging-contacts-formed-from-eutectic-ga-in-for-the-accurate-determination-of-dielectric-constants-of-organic-materials
#17
Evgenia Douvogianni, Xinkai Qiu, Li Qiu, Fatemeh Jahani, Floris B Kooistra, Jan C Hummelen, Ryan C Chiechi
A method for accurately measuring the relative dielectric constant (εr ) of thin films of soft, organic materials is described. The effects of the bombardment of these materials with hot Al atoms, the most commonly used top electrode, are mitigated by using electrodes fabricated from eutectic gallium-indium (EGaIn). The geometry of the electrode is defined by injection into microchannels to form stable structures that are nondamaging and that conform to the topology of the organic thin film. The εr of a series of references and new organic materials, polymers, and fullerene derivatives was derived from impedance spectroscopy measurements for both Al and EGaIn electrodes showing the specific limitations of Al with soft, organic materials and overcoming them with EGaIn to determine their dielectric properties and provide realistic values of εr ...
August 28, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30270985/tuning-exciton-mn-2-energy-transfer-in-mixed-halide-perovskite-nanocrystals
#18
Kunyuan Xu, Andries Meijerink
Doping nanocrystals (NCs) with luminescent activators provides additional color tunability for these highly efficient luminescent materials. In CsPbCl3 perovskite NCs the exciton-to-activator energy transfer (ET) has been observed to be less efficient than in II-VI semiconductor NCs. Here we investigate the evolution of the exciton-to-Mn2+ ET efficiency as a function of composition (Br/Cl ratio) and temperature in CsPbCl3- x Br x :Mn2+ NCs. The results show a strong dependence of the transfer efficiency on Br- content...
August 14, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30245549/mono-and-multilayer-silicene-type-honeycomb-lattices-by-oriented-attachment-of-pbse-nanocrystals-synthesis-structural-characterization-and-analysis-of-the-disorder
#19
Joep L Peters, Thomas Altantzis, Ivan Lobato, Maryam Alimoradi Jazi, Carlo van Overbeek, Sara Bals, Daniel Vanmaekelbergh, Sophia Buhbut Sinai
Nanocrystal (NC) solids are commonly prepared from nonpolar organic NC suspensions. In many cases, the capping on the NC surface is preserved and forms a barrier between the NCs. More recently, superstructures with crystalline connections between the NCs, implying the removal of the capping, have been reported, too. Here, we present large-scale uniform superstructures of attached PbSe NCs with a silicene-type honeycomb geometry, resulting from solvent evaporation under nearly reversible conditions. We also prepared multilayered silicene honeycomb structures by using larger amounts of PbSe NCs...
July 24, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://read.qxmd.com/read/30930534/raft-polymerization-of-an-intrinsically-stretchable-water-soluble-block-copolymer-scaffold-for-pedot
#20
Laure V Kayser, Madeleine D Russell, Daniel Rodriquez, Sami N Abuhamdieh, Charles Dhong, Salik Khan, Alexander N Stein, Julian Ramírez, Darren J Lipomi
Despite the common association of π-conjugated polymers with flexible and stretchable electronics, these materials can be rigid and brittle unless they are designed otherwise. For example, low modulus, high extensibility, and high toughness are treated as prerequisites for integration with soft and biological structures. One of the most successful and commercially available organic electronic materials is the conductive and brittle polyelectrolyte complex poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS)...
July 10, 2018: Chemistry of Materials: a Publication of the American Chemical Society
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