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Chemistry of Materials: a Publication of the American Chemical Society

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https://www.readbyqxmd.com/read/29910536/anisotropic-2d-cu-2-x-se-nanocrystals-from-dodecaneselenol-and-their-conversion-to-cdse-and-cuinse-2-nanoparticles
#1
Anne C Berends, Ward van der Stam, Quinten A Akkerman, Johannes D Meeldijk, Joost van der Lit, Celso de Mello Donega
We present the synthesis of colloidal anisotropic Cu2- x Se nanocrystals (NCs) with excellent size and shape control, using the unexplored phosphine-free selenium precursor 1-dodecaneselenol (DDSe). This precursor forms lamellar complexes with Cu(I) that enable tailoring the NC morphology from 0D polyhedral to highly anisotropic 2D shapes. The Cu2- x Se NCs are subsequently used as templates in postsynthetic cation exchange reactions, through which they are successfully converted to CdSe and CuInSe2 quantum dots, nanoplatelets, and ultrathin nanosheets...
June 12, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29910535/defect-engineering-of-earth-abundant-solar-absorbers-bisi-and-bisei
#2
Alex M Ganose, Saya Matsumoto, John Buckeridge, David O Scanlon
Bismuth-based solar absorbers have recently garnered attention due to their promise as cheap, nontoxic, and efficient photovoltaics. To date, however, most show poor efficiencies far below those seen in commercial technologies. In this work, we investigate two such promising materials, BiSI and BiSeI, using relativistic first-principles methods with the aim of identifying their suitability for photovoltaic applications. Both compounds show excellent optoelectronic properties with ideal band gaps and strong optical absorption, leading to high predicted device performance...
June 12, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29861547/supramolecular-loop-stitches-of-discrete-block-molecules-on-graphite-tunable-hydrophobicity-by-naphthalenediimide-end-capped-oligodimethylsiloxane
#3
José Augusto Berrocal, Joan Teyssandier, Olga J G M Goor, Steven De Feyter, E W Meijer
The noncovalent functionalization of surfaces has gained widespread interest in the scientific community, and it is progressively becoming an extremely productive research field offering brand new directions for both supramolecular and materials chemistry. As the end-groups often play a dominant role in the surface properties obtained, creating loops with end-groups only at the surface will lead to unexpected architectures and hence properties. Here we report the self-assembly of discrete block molecules-structures in-between block copolymers and liquid crystals-featuring oligodimethylsiloxanes (ODMS) end-capped with naphthalenediimides (NDIs) at the 1-phenyloctane/highly oriented pyrolytic graphite (1-PO/HOPG) interface...
May 22, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29861546/engineering-of-transition-metal-catalysts-confined-in-zeolites
#4
REVIEW
Nikolay Kosinov, Chong Liu, Emiel J M Hensen, Evgeny A Pidko
Transition metal-zeolite composites are versatile catalytic materials for a wide range of industrial and lab-scale processes. Significant advances in fabrication and characterization of well-defined metal centers confined in zeolite matrixes have greatly expanded the library of available materials and, accordingly, their catalytic utility. In this review, we summarize recent developments in the field from the perspective of materials chemistry, focusing on synthesis, postsynthesis modification, (operando) spectroscopy characterization, and computational modeling of transition metal-zeolite catalysts...
May 22, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29780208/the-role-of-the-side-chain-on-the-performance-of-n-type-conjugated-polymers-in-aqueous-electrolytes
#5
Alexander Giovannitti, Iuliana P Maria, David Hanifi, Mary J Donahue, Daniel Bryant, Katrina J Barth, Beatrice E Makdah, Achilleas Savva, Davide Moia, Matyáš Zetek, Piers R F Barnes, Obadiah G Reid, Sahika Inal, Garry Rumbles, George G Malliaras, Jenny Nelson, Jonathan Rivnay, Iain McCulloch
We report a design strategy that allows the preparation of solution processable n-type materials from low boiling point solvents for organic electrochemical transistors (OECTs). The polymer backbone is based on NDI-T2 copolymers where a branched alkyl side chain is gradually exchanged for a linear ethylene glycol-based side chain. A series of random copolymers was prepared with glycol side chain percentages of 0, 10, 25, 50, 75, 90, and 100 with respect to the alkyl side chains. These were characterized to study the influence of the polar side chains on interaction with aqueous electrolytes, their electrochemical redox reactions, and performance in OECTs when operated in aqueous electrolytes...
May 8, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29657360/interplay-between-surface-chemistry-precursor-reactivity-and-temperature-determines-outcome-of-zns-shelling-reactions-on-cuins-2-nanocrystals
#6
Anne C Berends, Ward van der Stam, Jan P Hofmann, Eva Bladt, Johannes D Meeldijk, Sara Bals, Celso de Mello Donega
ZnS shelling of I-III-VI2 nanocrystals (NCs) invariably leads to blue-shifts in both the absorption and photoluminescence spectra. These observations imply that the outcome of ZnS shelling reactions on I-III-VI2 colloidal NCs results from a complex interplay between several processes taking place in solution, at the surface of, and within the seed NC. However, a fundamental understanding of the factors determining the balance between these different processes is still lacking. In this work, we address this need by investigating the impact of precursor reactivity, reaction temperature, and surface chemistry (due to the washing procedure) on the outcome of ZnS shelling reactions on CuInS2 NCs using a seeded growth approach...
April 10, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29887671/polymer-based-black-phosphorus-bp-hybrid-materials-by-in-situ-radical-polymerization-an-effective-tool-to-exfoliate-bp-and-stabilize-bp-nanoflakes
#7
Elisa Passaglia, Francesca Cicogna, Federica Costantino, Serena Coiai, Stefano Legnaioli, Giulia Lorenzetti, Silvia Borsacchi, Marco Geppi, Francesca Telesio, Stefan Heun, Andrea Ienco, Manuel Serrano-Ruiz, Maurizio Peruzzini
Black phosphorus (bP) has been recently investigated for next generation nanoelectronic multifunctional devices. However, the intrinsic instability of exfoliated bP (the bP nanoflakes) toward both moisture and air has so far overshadowed its practical implementation. In order to contribute to fill this gap, we report here the preparation of new hybrid polymer-based materials where bP nanoflakes (bPn) exhibit a significantly improved stability. The new materials have been prepared by different synthetic paths including: (i) the mixing of conventionally liquid-phase exfoliated bP (in dimethyl sulfoxide, DMSO) with poly(methyl methacrylate) (PMMA) solution; (ii) the direct exfoliation of bP in a polymeric solution; (iii) the in situ radical polymerization after exfoliating bP in the liquid monomer (methyl methacrylate, MMA)...
March 27, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29606799/arrhenius-behavior-of-the-bulk-na-ion-conductivity-in-na-3-sc-2-po-4-3-single-crystals-observed-by-microcontact-impedance-spectroscopy
#8
Daniel Rettenwander, Günther J Redhammer, Marie Guin, Artur Benisek, Hannes Krüger, Olivier Guillon, Martin Wilkening, Frank Tietz, Jürgen Fleig
NASICON-based solid electrolytes with exceptionally high Na-ion conductivities are considered to enable future all solid-state Na-ion battery technologies. Despite 40 years of research the interrelation between crystal structure and Na-ion conduction is still controversially discussed and far from being fully understood. In this study, microcontact impedance spectroscopy combined with single crystal X-ray diffraction, and differential scanning calorimetry is applied to tackle the question how bulk Na-ion conductivity σbulk of sub-mm-sized flux grown Na3 Sc2 (PO4 )3 (NSP) single crystals is influenced by supposed phase changes (α, β, and γ phase) discussed in literature...
March 13, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29606798/popcorn-shaped-fe-x-o-w%C3%A3-stite-nanoparticles-from-a-single-source-precursor-colloidal-synthesis-and-magnetic-properties
#9
Christoph P Guntlin, Stefan T Ochsenbein, Michael Wörle, Rolf Erni, Kostiantyn V Kravchyk, Maksym V Kovalenko
Colloidal nanoparticles (NPs) with myriads of compositions and morphologies have been synthesized and characterized in recent years. For wüstite Fe x O, however, obtaining phase-pure NPs with homogeneous morphologies have remained challenging. Herein, we report the colloidal synthesis of phase-pure Fe x O ( x ≈ 0.94) popcorn-shaped NPs by decomposition of a single-source precursor, [Fe3 (μ3 -O)(CF3 COO)(μ-CF3 COO)6 (H2 O)2 ]·CF3 COOH. The popcorn shape and multigrain structure had been reconstructed using high-angle annular dark-field scanning transmission electron micrograph (HAADF-STEM) tomography...
February 27, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29515290/dopant-distribution-in-atomic-layer-deposited-zno-al-films-visualized-by-transmission-electron-microscopy-and-atom-probe-tomography
#10
Yizhi Wu, A Devin Giddings, Marcel A Verheijen, Bart Macco, Ty J Prosa, David J Larson, Fred Roozeboom, Wilhelmus M M Kessels
The maximum conductivity achievable in Al-doped ZnO thin films prepared by atomic layer deposition (ALD) is limited by the low doping efficiency of Al. To better understand the limiting factors for the doping efficiency, the three-dimensional distribution of Al atoms in the ZnO host material matrix has been examined on the atomic scale using a combination of high-resolution transmission electron microscopy (TEM) and atom probe tomography (APT). Although the Al distribution in ZnO films prepared by so-called "ALD supercycles" is often presented as atomically flat δ-doped layers, in reality a broadening of the Al-dopant layers is observed with a full-width-half-maximum of ∼2 nm...
February 27, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29503509/atomic-structure-of-intrinsic-and-electron-irradiation-induced-defects-in-mote-2
#11
Kenan Elibol, Toma Susi, Giacomo Argentero, Mohammad Reza Ahmadpour Monazam, Timothy J Pennycook, Jannik C Meyer, Jani Kotakoski
Studying the atomic structure of intrinsic defects in two-dimensional transition-metal dichalcogenides is difficult since they damage quickly under the intense electron irradiation in transmission electron microscopy (TEM). However, this can also lead to insights into the creation of defects and their atom-scale dynamics. We first show that MoTe2 monolayers without protection indeed quickly degrade during scanning TEM (STEM) imaging, and discuss the observed atomic-level dynamics, including a transformation from the 1H phase into 1T', 3-fold rotationally symmetric defects, and the migration of line defects between two 1H grains with a 60° misorientation...
February 27, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29503508/area-selective-atomic-layer-deposition-of-metal-oxides-on-noble-metals-through-catalytic-oxygen-activation
#12
Joseph A Singh, Nick F W Thissen, Woo-Hee Kim, Hannah Johnson, Wilhelmus M M Kessels, Ageeth A Bol, Stacey F Bent, Adriaan J M Mackus
Area-selective atomic layer deposition (ALD) is envisioned to play a key role in next-generation semiconductor processing and can also provide new opportunities in the field of catalysis. In this work, we developed an approach for the area-selective deposition of metal oxides on noble metals. Using O2 gas as co-reactant, area-selective ALD has been achieved by relying on the catalytic dissociation of the oxygen molecules on the noble metal surface, while no deposition takes place on inert surfaces that do not dissociate oxygen (i...
February 13, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29503507/electrochemistry-and-spectroelectrochemistry-of-lead-halide-perovskite-films-materials-science-aspects-and-boundary-conditions
#13
Gergely F Samu, Rebecca A Scheidt, Prashant V Kamat, Csaba Janáky
The unique optoelectronic properties of lead halide perovskites have triggered a new wave of excitement in materials chemistry during the past five years. Electrochemistry, spectroelectrochemistry, and photoelectrochemistry could be viable tools both for analyzing the optoelectronic features of these materials and for assembling them into hybrid architectures (e.g., solar cells). At the same time, the instability of these materials limits the pool of solvents and electrolytes that can be employed in such experiments...
February 13, 2018: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29307957/formation-of-au-nanoparticles-in-liquid-cell-transmission-electron-microscopy-from-a-systematic-study-to-engineered-nanostructures
#14
Yucheng Zhang, Debora Keller, Marta D Rossell, Rolf Erni
In this work, a systematic study of the effect of electron dose rate, solute concentration, imaging mode (broad beam vs scanning probe mode), and liquid cell setup (static vs flow mode) on the growth mechanism and the ultimate morphology of Au nanoparticles (NPs) was performed in chloroauric acid (HAuCl4 ) aqueous solutions using in situ liquid-cell TEM (LC-TEM). It was found that a diffusion limited growth dominates at high dose rates, especially for the solution with the lowest concentration (1 mM), resulting in formation of dendritic NPs...
December 26, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29725162/peptide-binding-nanoparticle-materials-with-tailored-recognition-sites-for-basic-peptides
#15
Shixin Fa, Yan Zhao
Peptides rich in basic residues such as lysine and arginine play important roles in biology such as bacterial defense and cell penetration. Although peptide-binding materials with high sequence-specificity have broad potential applications, the diverse functionalities of peptide side chains make their molecular recognition extremely difficult. By covalently capturing micelles of a doubly cross-linkable surfactant with solubilized peptide templates, we prepared water-soluble molecularly imprinted nanoparticles with high sequence-specificity for basic peptides...
November 14, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29606797/surface-engineered-cationic-nanocrystals-stable-in-biological-buffers-and-high-ionic-strength-solutions
#16
Ryan M Dragoman, Marcel Grogg, Maryna I Bodnarchuk, Peter Tiefenboeck, Donald Hilvert, Dmitry N Dirin, Maksym V Kovalenko
Progress in colloidal synthesis in the last two decades has enabled high-quality semiconductor, plasmonic, and magnetic nanocrystals (NCs). As synthesized, these NCs are usually capped with long-chain apolar ligands. Postsynthetic surface functionalization is required for rendering such NCs colloidally stable in polar media such as water. However, unlike small anionic molecules and polymeric coatings, producing positively charged stable NCs, especially at high ionic strengths, has remained challenging. Here, we present a general approach to achieve aqueously stable cationic NCs using a set of small (<2...
November 14, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29170602/theoretical-study-of-ripening-mechanisms-of-pd-clusters-on-ceria
#17
Ya-Qiong Su, Jin-Xun Liu, Ivo A W Filot, Emiel J M Hensen
We carried out density functional theory calculations to investigate the ripening of Pd clusters on CeO2 (111). Starting from stable Pd n clusters ( n = 1-21), we compared how these clusters can grow through Ostwald ripening and coalescence. As Pd atoms have mobility higher than that of Pd n clusters on the CeO2 (111) surface, Ostwald ripening is predicted to be the dominant sintering mechanism. Particle coalescence is possible only for clusters with less than 5 Pd atoms. These ripening mechanisms are facilitated by adsorbed CO through lowering barriers for the cluster diffusion, detachment of a Pd atom from clusters, and transformation of initial planar clusters...
November 14, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29545675/-in-situ-time-resolved-attenuated-total-reflectance-infrared-spectroscopy-for-probing-metal-organic-framework-thin-film-growth
#18
Junjie Zhao, Berc Kalanyan, Heather F Barton, Brent A Sperling, Gregory N Parsons
In situ chemical measurements of solution/surface reactions during metal-organic framework (MOF) thin film growth can provide valuable information about the mechanistic and kinetic aspects of key reaction steps, and allow control over crystal quality and material properties. Here, we report a new approach to study the growth of MOF thin films in a flow cell using attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR). Real-time spectra recorded during continuous flow synthesis were used to investigate the mechanism and kinetics that govern the formation of (Zn, Cu) hydroxy double salts (HDSs) from ZnO thin films and the subsequent conversion of HDS to HKUST-1...
October 24, 2017: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/29129959/cancer-targeting-ultrasmall-silica-nanoparticles-for-clinical-translation-physicochemical-structure-and-biological-property-correlations
#19
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
#20
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, t 1/2 = 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, t 1/2 = 78...
October 10, 2017: Chemistry of Materials: a Publication of the American Chemical Society
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