284 results match your criteria Chemistry Of Materials[Journal]


Annealing Supramolecular Gels by a Reaction Relay.

Chem Mater 2020 Jun 22;32(12):5264-5271. Epub 2020 May 22.

School of Chemistry, University of Glasgow, Glasgow G12 8QQ, U.K.

Supramolecular gels have potential in many areas. In many cases, a major drawback is that the gels are formed at a high rate. As a result, nonoptimal, kinetically trapped self-assembled structures are often formed, leading to gels that can be hard to reproduce and control. Read More

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http://dx.doi.org/10.1021/acs.chemmater.0c01483DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7315816PMC

Stability of Colloidal Iron Oxide Nanoparticles on Titania and Silica Support.

Chem Mater 2020 Jun 28;32(12):5226-5235. Epub 2020 May 28.

Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, Utrecht 3584 CG, The Netherlands.

Using model catalysts with well-defined particle sizes and morphologies to elucidate questions regarding catalytic activity and stability has gained more interest, particularly utilizing colloidally prepared metal(oxide) particles. Here, colloidally synthesized iron oxide nanoparticles (Fe O -NPs, size ∼7 nm) on either a titania (Fe O /TiO) or a silica (Fe O /SiO) support were studied. These model catalyst systems showed excellent activity in the Fischer-Tropsch to olefin (FTO) reaction at high pressure. Read More

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http://dx.doi.org/10.1021/acs.chemmater.0c01352DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7315821PMC

Bright Blue and Green Luminescence of Sb(III) in Double Perovskite CsMInCl (M = Na, K) Matrices.

Chem Mater 2020 Jun 8;32(12):5118-5124. Epub 2020 Jun 8.

Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Bioscience, ETH Zürich, Vladimir Prelog Weg 1, CH-8093 Zürich, Switzerland.

The vast structural and compositional space of metal halides has recently become a major research focus for designing inexpensive and versatile light sources; in particular, for applications in displays, solid-state lighting, lasing, etc. Compounds with isolated ns-metal halide centers often exhibit bright broadband emission that stems from self-trapped excitons (STEs). The Sb(III) halides are attractive STE emitters due to their low toxicity and oxidative stability; however, coupling these features with an appropriately robust, fully inorganic material containing Sb in an octahedral halide environment has proven to be a challenge. Read More

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http://dx.doi.org/10.1021/acs.chemmater.0c01004DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7315817PMC

Information Entropy as a Reliable Measure of Nanoparticle Dispersity.

Chem Mater 2020 May 13;32(9):3701-3706. Epub 2020 Apr 13.

University College London, Department of Chemical Engineering, Torrington Place, London, WC1E 6BT United Kingdom.

Nanoparticle size impacts properties vital to applications ranging from drug delivery to diagnostics and catalysis. As such, evaluating nanoparticle size dispersity is of fundamental importance. Conventional approaches, such as standard deviation, usually require the nanoparticle population to follow a known distribution and are ill-equipped to deal with highly poly- or heterodisperse populations. Read More

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http://dx.doi.org/10.1021/acs.chemmater.0c00539DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7304839PMC

Polyphenylene-Based Solid Acid as an Efficient Catalyst for Activation and Hydration of Alkynes.

Chem Mater 2020 May 1;32(10):4375-4382. Epub 2020 May 1.

Department of Chemical Engineering, University College London, Torrington Place, London WC1E 7JE, U.K.

Porous polymer catalysts possess the potential to combine the advantages of heterogeneous and homogeneous catalysis, namely, easy postreaction recycling and high dispersion of active sites. Here, we designed a -SOH functionalized polyphenylene (PPhen) framework with purely sp-hybridized carbons, which exhibited high activity in the hydration of alkynes including challenging aliphatic substrates such as 1-octyne. The superiority of the structure lies in its covalent crosslink in the -plane with a π-π stacking interaction between the planes, enabling simultaneously high swellability and porosity (653 m·g). Read More

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http://dx.doi.org/10.1021/acs.chemmater.0c01763DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7304856PMC

Understanding the Origin of Enhanced Li-Ion Transport in Nanocrystalline Argyrodite-Type LiPSI.

Chem Mater 2020 Jun 19;32(11):4754-4766. Epub 2020 May 19.

Institute for Chemistry and Technology of Materials, Christian Doppler Laboratory for Lithium Batteries, Graz University of Technology (NAWI Graz), Stremayrgasse 9, 8010 Graz, Austria.

Argyrodite-type LiPSX (X = Cl, Br) compounds are considered to act as powerful ionic conductors in next-generation all-solid-state lithium batteries. In contrast to LiPSBr and LiPSCl compounds showing ionic conductivities on the order of several mS cm, the iodine compound LiPSI turned out to be a poor ionic conductor. This difference has been explained by anion site disorder in LiPSBr and LiPSCl leading to facile through-going, that is, long-range ion transport. Read More

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http://dx.doi.org/10.1021/acs.chemmater.0c01367DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7304077PMC

Stability of Selected Hydrogen Bonded Semiconductors in Organic Electronic Devices.

Chem Mater 2019 Sep 11;31(17):6315-6346. Epub 2019 Jul 11.

Linz Institute for Organic Solar Cells (LIOS), Physical Chemistry, Johannes Kepler University Linz, Altenberger Str. Nr. 69, 4040 Linz, Austria.

The electronics era is flourishing and morphing itself into Internet of Everything, IoE. At the same time, questions arise on the issue of electronic materials employed: especially their natural availability and low-cost fabrication, their functional stability in devices, and finally their desired biodegradation at the end of their life cycle. Hydrogen bonded pigments and natural dyes like indigo, anthraquinone and acridone are not only biodegradable and of bio-origin but also have functionality robustness and offer versatility in designing electronics and sensors components. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b01405DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7297463PMC
September 2019

Impact of Defects and Crystal Size on Negative Gas Adsorption in DUT-49 Analyzed by Xe NMR Spectroscopy.

Chem Mater 2020 Jun 11;32(11):4641-4650. Epub 2020 May 11.

Chair of Bioanalytical Chemistry, Technische Universität Dresden, Bergstrasse 66, 01062 Dresden, Germany.

The origin of crystal-size-dependent adsorption behavior of flexible metal-organic frameworks is increasingly studied. In this contribution, we probe the solid-fluid interactions of DUT-49 crystals of different size by Xe NMR spectroscopy at 200 K. With decreasing size of the crystals, the average solid-fluid interactions are found to decrease reflected by a decrease in chemical shift of adsorbed xenon from 230 to 200 ppm, explaining the lack of adsorption-induced transitions for smaller crystals. Read More

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http://dx.doi.org/10.1021/acs.chemmater.0c01059DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7295370PMC

Conformal Ultrathin Film Metal-Organic Framework Analogues: Characterization of Growth, Porosity, and Electronic Transport.

Chem Mater 2019 Nov 15;31(21):8977-8986. Epub 2019 Oct 15.

Department of Chemistry, Hope College, Holland, Michigan 49423, United States.

Thin-film formation and transport properties of two copper-paddlewheel metal-organic framework (MOF) -based systems (MOF-14 and MOF-399) are investigated for their potential integration into electrochemical device architectures. Thin-film analogs of these two systems are fabricated by the sequential, alternating, solution-phase deposition of the inorganic and organic ligand precursors that result in conformal films via van der Merwe-like growth. Atomic force microscopy reveals smooth film morphologies with surface roughnesses determined by the underlying substrates and linear film growth of 1. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b03141DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7291877PMC
November 2019

Hierarchically Organized and Anisotropic Porous Carbon Monoliths.

Chem Mater 2020 May 20;32(9):3944-3951. Epub 2020 Apr 20.

Materials Chemistry, Paris Lodron University Salzburg, Jakob-Haringer Str. 2a, Salzburg 5020, Austria.

Anisotropy is a key factor regarding mechanical or transport properties and thus the functionality of porous materials. However, the ability to deliberately design the pore structure of hierarchically organized porous networks toward anisotropic features is limited. Here, we report two straightforward routes toward hierarchically structured porous carbon monoliths with an anisotropic alignment of the microstructure on the level of macro- and mesopores. Read More

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http://dx.doi.org/10.1021/acs.chemmater.0c00302DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7222333PMC

A Model System for Photocatalysis: Ti-Doped α-FeO(11̅02) Single-Crystalline Films.

Chem Mater 2020 May 9;32(9):3753-3764. Epub 2020 Apr 9.

Institute of Applied Physics, TU Wien, Wiedner Hauptstraβe 8-10/E134, 1040 Wien, Austria.

Hematite (α-FeO) is one of the most investigated anode materials for photoelectrochemical water splitting. Its efficiency improves by doping with Ti, but the underlying mechanisms are not understood. One hurdle is separating the influence of doping on conductivity, surface states, and morphology, which all affect performance. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b04908DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7222102PMC

Lithium Diffusion in Niobium Tungsten Oxide Shear Structures.

Chem Mater 2020 May 26;32(9):3980-3989. Epub 2020 Apr 26.

School of Metallurgy and Materials, University of Birmingham, Edgbaston, Birmingham B15 2TT, U.K.

Niobium tungsten oxides with crystallographic shear structures form a promising class of high-rate Li-ion anode materials. Lithium diffusion within these materials is studied in this work using density functional theory calculations, specifically nudged elastic band calculations and molecular dynamics simulations. Lithium diffusion is found to occur through jumps between 4-fold coordinated window sites with low activation barriers (80-300 meV) and is constrained to be effectively one-dimensional by the crystallographic shear planes of the structures. Read More

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http://dx.doi.org/10.1021/acs.chemmater.0c00483DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7222352PMC

Rapid Diels-Alder Cross-linking of Cell Encapsulating Hydrogels.

Chem Mater 2019 Oct 27;31(19):8035-8043. Epub 2019 Sep 27.

Department of Materials Science & Engineering, Stanford University, Stanford, California 94305, United States.

Recent efforts in the design of hydrogel biomaterials have focused on better mimicking the native cellular microenvironment to direct cell fate. To simultaneously control multiple material parameters, several orthogonal chemistries may be needed. However, present strategies to prepare cell-encapsulating hydrogels make use of relatively few chemical reactions. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b02485DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7224313PMC
October 2019

GeSe: Optical Spectroscopy and Theoretical Study of a van der Waals Solar Absorber.

Chem Mater 2020 Apr 13;32(7):3245-3253. Epub 2020 Mar 13.

Stephenson Institute for Renewable Energy and Department of Physics, University of Liverpool, Liverpool L69 7ZF, U.K.

The van der Waals material GeSe is a potential solar absorber, but its optoelectronic properties are not yet fully understood. Here, through a combined theoretical and experimental approach, the optoelectronic and structural properties of GeSe are determined. A fundamental absorption onset of 1. Read More

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http://dx.doi.org/10.1021/acs.chemmater.0c00453DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7161679PMC

Resonant Ta Doping for Enhanced Mobility in Transparent Conducting SnO.

Chem Mater 2020 Mar 18;32(5):1964-1973. Epub 2020 Feb 18.

Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, United Kingdom.

Transparent conducting oxides (TCOs) are ubiquitous in modern consumer electronics. SnO is an earth abundant, cheaper alternative to InO as a TCO. However, its performance in terms of mobilities and conductivities lags behind that of InO. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b04845DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7147269PMC

Modeling of Gas Transport through Polymer/MOF Interfaces: A Microsecond-Scale Concentration Gradient-Driven Molecular Dynamics Study.

Chem Mater 2020 Feb 7;32(3):1288-1296. Epub 2020 Jan 7.

Department of Chemical Engineering, University College London, London WC1E 7JE, U.K.

Membrane-based separation technologies offer a cost-effective alternative to many energy-intensive gas separation processes, such as distillation. Mixed matrix membranes (MMMs) composed of polymers and metal-organic frameworks (MOFs) have attracted a great deal of attention for being promising systems to manufacture durable and highly selective membranes with high gas fluxes and high selectivities. Therefore, understanding gas transport through these MMMs is of significant importance. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b04907DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7147253PMC
February 2020

Intrinsic Anomalous Hall Effect in Ni-Substituted Magnetic Weyl Semimetal CoSnS.

Chem Mater 2020 Feb 22;32(4):1612-1617. Epub 2020 Jan 22.

Max-Planck-Institute für Chemische Physik Fester Stoffe, 01187 Dresden, Germany.

Topological Weyl semimetals have recently attracted considerable attention among materials scientists as their properties are predicted to be protected against perturbations such as lattice distortion and chemical substitution. However, any experimental proof of such robustness is still lacking. In this study, we experimentally demonstrate that the topological properties of the ferromagnetic kagomé compound CoSnS are preserved upon Ni substitution. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b05009DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7045698PMC
February 2020

Anion Distribution, Structural Distortion, and Symmetry-Driven Optical Band Gap Bowing in Mixed Halide CsSnX Vacancy Ordered Double Perovskites.

Chem Mater 2019 Nov 5;31(22):9430-9444. Epub 2019 Nov 5.

Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, United Kingdom.

Mixed anion compounds in the vacancy ordered perovskite structure were synthesized and characterized experimentally and computationally with a focus on compounds where A = Cs. Pure anion CsSnX compounds were formed with X = Cl, Br, and I using a room temperature solution phase method. Mixed anion compounds were formed as solid solutions of CsSnCl and CsSnBr and a second series from CsSnBr and CsSnI. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b03267DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7046317PMC
November 2019

Computationally Guided Discovery of the Sulfide LiAlS in the Li-Al-S Phase Field: Structure and Lithium Conductivity.

Chem Mater 2019 Dec 23;31(23):9699-9714. Epub 2019 Oct 23.

Department of Chemistry, University of Liverpool, Crown Street, L69 7ZD Liverpool, U.K.

With the goal of finding new lithium solid electrolytes by a combined computational-experimental method, the exploration of the Li-Al-O-S phase field resulted in the discovery of a new sulfide LiAlS. The structure of the new phase was determined through an approach combining synchrotron X-ray and neutron diffraction with Li and Al magic-angle spinning nuclear magnetic resonance spectroscopy and revealed to be a highly ordered cationic polyhedral network within a sulfide anion -type sublattice. The originality of the structure relies on the presence of AlS repeating dimer units consisting of two edge-shared Al tetrahedra. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b03230DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7011735PMC
December 2019

Structurally Diverse Covalent Triazine-Based Framework Materials for Photocatalytic Hydrogen Evolution from Water.

Chem Mater 2019 Nov 27;31(21):8830-8838. Epub 2019 Sep 27.

Department of Chemistry and Materials Innovation Factory, University of Liverpool, 51 Oxford Street, Liverpool L7 3NY, U.K.

A structurally diverse family of 39 covalent triazine-based framework materials (CTFs) are synthesized by Suzuki-Miyaura polycondensation and tested as hydrogen evolution photocatalysts using a high-throughput workflow. The two best-performing CTFs are based on benzonitrile and dibenzo[,]thiophene sulfone linkers, respectively, with catalytic activities that are among the highest for this material class. The activities of the different CTFs are rationalized in terms of four variables: the predicted electron affinity, the predicted ionization potential, the optical gap, and the dispersibility of the CTFs particles in solution, as measured by optical transmittance. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b02825DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7011753PMC
November 2019

Brownmillerite-Type SrScGaO Oxide Ion Conductor: Local Structure, Phase Transition, and Dynamics.

Chem Mater 2019 Sep 6;31(18):7395-7404. Epub 2019 Aug 6.

Department of Chemistry, Durham University, Science Site, South Road, Durham DH1 3LE, United Kingdom.

Brownmillerite-type SrScGaO has been investigated by a range of experimental X-ray and neutron scattering techniques (diffraction, total scattering, and spectroscopy) and density functional theory calculations in order to characterize its structure and dynamics. The material undergoes a second-order phase transition on heating during which a rearrangement of the (GaO) tetrahedral chains occurs, such that they change from being essentially fully ordered in a polar structure at room temperature to being orientationally disordered above 400 °C. Pair distribution function analysis carried out using neutron total scattering data suggests that GaO tetrahedra remain as fairly rigid units above and below this transition, whereas coordination polyhedra in the (ScO) layers distort more. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b02051DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7011778PMC
September 2019

Ionic Hydrogel for Accelerated Dopamine Delivery via Retrodialysis.

Chem Mater 2019 Sep 29;31(17):7080-7084. Epub 2019 Jul 29.

Electrical Engineering Division, Department of Engineering, University of Cambridge, Cambridge CB3 0FA, United Kingdom.

Local drug delivery directly to the source of a given pathology using retrodialysis is a promising approach to treating otherwise untreatable diseases. As the primary material component in retrodialysis, the semipermeable membrane represents a critical point for innovation. This work presents a new ionic hydrogel based on polyethylene glycol and acrylate with dopamine counterions. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b02135DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7011752PMC
September 2019

Delayed Blue Fluorescence via Upper-Triplet State Crossing from C-C Bonded Donor-Acceptor Charge Transfer Molecules with Azatriangulene Cores.

Chem Mater 2019 Sep 22;31(17):6684-6695. Epub 2019 May 22.

Department of Chemistry, Durham University, Durham DH1 3LE, U.K.

We report the synthesis and structural and photophysical characterization of two series of molecules with functionalized azatriangulene electron donor cores and three pendant electron acceptor units. The presented donor and acceptor units are joined by C-C bonds, instead of the usual C-heteroatom bonds often found in thermally activated delayed fluorescence (TADF) emitters. The effects of the donor-acceptor strength and donor-acceptor dihedral angle on the emission properties are assessed. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b01184DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7011764PMC
September 2019

Interstitial Oxide Ion Conductivity in the Langasite Structure: Carrier Trapping by Formation of (Ga,Ge)O Units in LaGa Ge O (0 < ≤ 1.5).

Chem Mater 2019 Aug 8;31(15):5742-5758. Epub 2019 Jul 8.

Department of Chemistry, University of Liverpool, Crown Street, Liverpool L69 7ZD, United Kingdom.

Framework oxides with the capacity to host mobile interstitial oxide anions are of interest as electrolytes in intermediate temperature solid oxide fuel cells (SOFCs). High performance materials of this type are currently limited to the anisotropic oxyapatite and melilite structure types. The langasite structure is based on a corner-shared tetrahedral network similar to that in melilite but is three-dimensionally connected by additional octahedral sites that bridge the layers by corner sharing. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b01734DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7011757PMC

Room-Temperature Production of Nanocrystalline Molybdenum Disulfide (MoS) at the Liquid-Liquid Interface.

Chem Mater 2019 Aug 18;31(15):5384-5391. Epub 2019 Jul 18.

National Graphene Institute, School of Chemistry, School of Materials, and Photon Science Institute, University of Manchester, Oxford Road, Manchester M13 9PL, United Kingdom.

Scalable synthesis of 2D materials is a prerequisite for their commercial exploitation. Here, a novel method of producing nanocrystalline molybdenum disulfide (MoS) at the liquid-liquid interface is demonstrated by decomposing a molecular precursor (tetrakis(diethyldithiocarbamato) molybdenum(IV)) in an organic solvent. The decomposition occurs over a few hours at room temperature without stirring or the addition of any surfactants, producing MoS which can be isolated onto substrates of choice. Read More

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http://dx.doi.org/10.1021/acs.chemmater.8b05232DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7011726PMC

Putting the Squeeze on Lead Iodide Perovskites: Pressure-Induced Effects To Tune Their Structural and Optoelectronic Behavior.

Chem Mater 2019 Jun 14;31(11):4063-4071. Epub 2019 May 14.

Department of Physics and Department of Chemistry, University of Bath, Bath BA2 7AY, U.K.

Lattice compression through hydrostatic pressure has emerged as an effective means of tuning the structural and optoelectronic properties of hybrid halide perovskites. In addition to external pressure, the local strain present in solution-processed thin films also causes significant heterogeneity in their photophysical properties. However, an atomistic understanding of structural changes of hybrid perovskites under pressure and their effects on the electronic landscape is required. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b00648DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7011759PMC

Thermodynamics, Electronic Structure, and Vibrational Properties of Sn (S Se ) Solid Solutions for Energy Applications.

Chem Mater 2019 May 3;31(10):3672-3685. Epub 2019 May 3.

Department of Chemistry, University of Bath, Claverton Down, Bath BA2 1AG, U.K.

The tin sulfides and selenides have a range of applications spanning photovoltaics and thermoelectrics to photocatalysts and photodetectors. However, significant challenges remain to widespread use, including electrical and chemical incompatibilities between SnS and device contact materials and the environmental toxicity of selenium. Solid solutions of isostructural sulfide and selenide phases could provide scope for optimizing physical properties against sustainability requirements, but this has not been comprehensively explored. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b00362DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7011755PMC

Li NMR Chemical Shift Imaging To Detect Microstructural Growth of Lithium in All-Solid-State Batteries.

Chem Mater 2019 Apr 5;31(8):2762-2769. Epub 2019 Apr 5.

Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.

All-solid-state batteries potentially offer safe, high-energy-density electrochemical energy storage, yet are plagued with issues surrounding Li microstructural growth and subsequent cell death. We use Li NMR chemical shift imaging and electron microscopy to track Li microstructural growth in the garnet-type solid electrolyte, LiLaZrTaO. Here, we follow the early stages of Li microstructural growth during galvanostatic cycling, from the formation of Li on the electrode surface to dendritic Li connecting both electrodes in symmetrical cells, and correlate these changes with alterations observed in the voltage profiles during cycling and impedance measurements. Read More

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http://dx.doi.org/10.1021/acs.chemmater.8b04875DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7006347PMC

Synthesis and characterization of vacancy-doped neodymium telluride for thermoelectric applications.

Chem Mater 2019 Jun 11;31(12):4460-4468. Epub 2019 Jun 11.

Thermal Energy Conversion Technologies Research and Advancement Group, Jet Propulsion Laboratory, California Institute of Technology, 4800 Oak Grove Drive, Pasadena, California 91109-8099.

Thermoelectric materials exhibit a voltage under an applied thermal gradient and are the heart of radioisotope thermoelectric generators (RTGs), which are the main power system for space missions such as I, II, and the Mars rover. However, materials currently in use enable only modest thermal-to-electrical conversion efficiencies near 6.5% at the system level, warranting the development of material systems with improved thermoelectric performance. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b00964DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6961965PMC

Optimizing PEGylation of TiO Nanocrystals through a Combined Experimental and Computational Study.

Chem Mater 2019 Sep 9;31(18):7531-7546. Epub 2019 Aug 9.

Dipartimento di Scienza dei Materiali, Università di Milano-Bicocca, via R. Cozzi 55, 20125 Milano, Italy.

PEGylation of metal oxide nanoparticles is the common approach to improve their biocompatibility and in vivo circulation time. In this work, we present a combined experimental and theoretical study to determine the operating condition that guarantee very high grafting densities, which are desirable in any biomedical application. Moreover, we present an insightful conformational analysis spanning different coverage regimes and increasing polymer chain lengths. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b02329DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6924593PMC
September 2019

Low-Temperature Phase-Controlled Synthesis of Titanium Di- and Tri-sulfide by Atomic Layer Deposition.

Chem Mater 2019 Nov 28;31(22):9354-9362. Epub 2019 Oct 28.

Department of Applied Physics and Laboratory for Inorganic Materials and Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, The Netherlands.

Phase-controlled synthesis of two-dimensional (2D) transition-metal chalcogenides (TMCs) at low temperatures with a precise thickness control has to date been rarely reported. Here, we report on a process for the phase-controlled synthesis of TiS (metallic) and TiS (semiconducting) nanolayers by atomic layer deposition (ALD) with precise thickness control. The phase control has been obtained by carefully tuning the deposition temperature and coreactant composition during ALD. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b02895DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6883357PMC
November 2019

Methods and Protocols for Reliable Electrochemical Testing in Post-Li Batteries (Na, K, Mg, and Ca).

Chem Mater 2019 Nov 15;31(21):8613-8628. Epub 2019 Oct 15.

Institut de Ciència de Materials de Barcelona (ICMAB-CSIC), Campus UAB, 08193 Bellaterra, Catalonia, Spain.

While less mature than the Li-ion battery, technologies based on Na, K, Mg, and Ca are attracting more and more attention from the battery community. New material (cathode, anode, or electrolyte) testing for these post-Li systems commonly involves the use of an electrochemical setup called a half-cell in which metal counter and reference electrodes are used. Here we first describe the different issues that become critical when moving away from Li with respect to the cell hardware (cell design, current collector, separator, insulator) and the nature of the counter and reference electrodes. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b02776DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6854841PMC
November 2019

Electrochemical Modulation of the Photophysics of Surface-Localized Trap States in Core/Shell/(Shell) Quantum Dot Films.

Chem Mater 2019 Oct 24;31(20):8484-8493. Epub 2019 Sep 24.

Opto-Electronic Materials Section, Faculty of Applied Sciences, Delft University of Technology, van der Maasweg 9, 2629 HZ Delft, The Netherlands.

In this work, we systematically study the spectroelectrochemical response of CdSe quantum dots (QDs), CdSe/CdS core/shell QDs with varying CdS shell thicknesses, and CdSe/CdS/ZnS core/shell/shell QDs in order to elucidate the influence of localized surface trap states on the optoelectronic properties. By correlating the differential absorbance and the photoluminescence upon electrochemically raising the Fermi level, we reveal that trap states near the conduction band (CB) edge give rise to nonradiative recombination pathways regardless of the CdS shell thickness, evidenced by quenching of the photoluminescence before the CB edge is populated with electrons. This points in the direction of shallow trap states localized on the CdS shell surface that give rise to nonradiative recombination pathways. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b02908DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6814269PMC
October 2019

Black Phosphorus/Palladium Nanohybrid: Unraveling the Nature of P-Pd Interaction and Application in Selective Hydrogenation.

Chem Mater 2019 Jul 3;31(14):5075-5080. Epub 2019 Jul 3.

CNR-ICCOM, Via Madonna del Piano10, 50019 Sesto Fiorentino, Italy.

The burgeoning interest in two-dimensional (2D) black phosphorus (bP) contributes to the expansion of its applications in numerous fields. In the present study, 2D bP is used as a support for homogeneously dispersed palladium nanoparticles directly grown on it by a wet chemical process. Electron energy loss spectroscopy-scanning transmission electron microscopy analysis evidences a strong interaction between palladium and P atoms of the bP nanosheets. Read More

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https://pubs.acs.org/doi/10.1021/acs.chemmater.9b00851
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http://dx.doi.org/10.1021/acs.chemmater.9b00851DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6804426PMC
July 2019
1 Read

Supramolecular Self-Assembly To Control Structural and Biological Properties of Multicomponent Hydrogels.

Chem Mater 2019 Oct 12;31(19):7883-7897. Epub 2019 Sep 12.

Institute of Bioengineering, Queen Mary University of London, London E1 4NS, U.K.

Self-assembled nanofibers are ubiquitous in nature and serve as inspiration for the design of supramolecular hydrogels. A multicomponent approach offers the possibility of enhancing the tunability and functionality of this class of materials. We report on the synergistic multicomponent self-assembly involving a peptide amphiphile (PA) and a 1,3:2,4-dibenzylidene-d-sorbitol (DBS) gelator to generate hydrogels with tunable nanoscale morphology, improved stiffness, enhanced self-healing, and stability to enzymatic degradation. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b01882DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6792223PMC
October 2019
1 Read

Esterase-Cleavable 2D Assemblies of Magnetic Iron Oxide Nanocubes: Exploiting Enzymatic Polymer Disassembling To Improve Magnetic Hyperthermia Heat Losses.

Chem Mater 2019 Aug 26;31(15):5450-5463. Epub 2019 Jun 26.

Istituto Italiano di Tecnologia, via Morego 30, 16163 Genoa, Italy.

Here, we report a nanoplatform based on iron oxide nanocubes (IONCs) coated with a bioresorbable polymer that, upon exposure to lytic enzymes, can be disassembled increasing the heat performances in comparison with the initial clusters. We have developed two-dimensional (2D) clusters by exploiting benchmark IONCs as heat mediators for magnetic hyperthermia and a polyhydroxyalkanoate (PHA) copolymer, a biodegradable polymer produced by bacteria that can be digested by intracellular esterase enzymes. The comparison of magnetic heat performance of the 2D assemblies with 3D centrosymmetrical assemblies or single IONCs emphasizes the benefit of the 2D assembly. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b00728DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6795213PMC

Structural Insights into Poly(Heptazine Imides): A Light-Storing Carbon Nitride Material for Dark Photocatalysis.

Chem Mater 2019 Sep 12;31(18):7478-7486. Epub 2019 Aug 12.

Max-Planck-Institut für Festkörperforschung, Heisenbergstraße 1, 70569 Stuttgart, Germany.

Solving the structure of carbon nitrides has been a long-standing challenge due to the low crystallinity and complex structures observed within this class of earth-abundant photocatalysts. Herein, we report on two-dimensional layered potassium poly(heptazine imide) (K-PHI) and its proton-exchanged counterpart (H-PHI), obtained by ionothermal synthesis using a molecular precursor route. We present a comprehensive analysis of the in-plane and three-dimensional structure of PHI. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b02199DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6768190PMC
September 2019

Assembly of Bifunctional Aptamer-Fibrinogen Macromer for VEGF Delivery and Skin Wound Healing.

Chem Mater 2019 Feb 11;31(3):1006-1015. Epub 2019 Jan 11.

Department of Biomedical Engineering, The Pennsylvania State University, University Park, PA 16802, USA.

Macromolecular assembly has been studied for various applications. However, while macromolecules can recognize one another for assembly, their assembled structures usually lack the function of specific molecular recognition. We hypothesized that bifunctional aptamer-protein macromers would possess dual functions of molecular assembly and recognition. Read More

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http://dx.doi.org/10.1021/acs.chemmater.8b04486DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6761992PMC
February 2019
2 Reads

Tetragonal Superstructure of the Antiskyrmion Hosting Heusler Compound MnPtSn.

Chem Mater 2019 Aug 11;31(15):5876-5880. Epub 2019 Jul 11.

Max Planck Institute for Chemical Physics of Solids, 01187 Dresden, Germany.

Skyrmions in non-centrosymmetric magnets are vortex-like spin arrangements, viewed as potential candidates for information storage devices. The crystal structure and noncollinear magnetic structure together with magnetic and spin-orbit interactions define the symmetry of the skyrmion structure. We outline the importance of these parameters in the Heusler compound MnPtSn which hosts antiskyrmions, a vortex-like spin texture related to skyrmions. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b02013DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6694724PMC
August 2019
1 Read

Hybrid Oleate-Iodide Ligand Shell for Air-Stable PbSe Nanocrystals and Superstructures.

Chem Mater 2019 Aug 9;31(15):5808-5815. Epub 2019 Jul 9.

Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science, Utrecht University, P.O. Box 80000, 3508 TA Utrecht, The Netherlands.

A postsynthetic treatment is presented to improve the air stability of PbSe nanocrystals (NCs) and PbSe square superstructures. The addition of z-type Pb(oleate) ligands together with x-type iodide ligands creates a hybrid ligand shell containing both ligands. The air stability of the PbSe NCs is checked by enduring absorption spectroscopy under ambient conditions. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b01891DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6694723PMC

Edge-Site Nanoengineering of WS by Low-Temperature Plasma-Enhanced Atomic Layer Deposition for Electrocatalytic Hydrogen Evolution.

Chem Mater 2019 Jul 25;31(14):5104-5115. Epub 2019 Jun 25.

Department of Applied Physics and Laboratory for Inorganic Materials and Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, 5600 MB Eindhoven, The Netherlands.

Edge-enriched transition metal dichalcogenides, such as WS, are promising electrocatalysts for sustainable production of H through the electrochemical hydrogen evolution reaction (HER). The reliable and controlled growth of such edge-enriched electrocatalysts at low temperatures has, however, remained elusive. In this work, we demonstrate how plasma-enhanced atomic layer deposition (PEALD) can be used as a new approach to nanoengineer and enhance the HER performance of WS by maximizing the density of reactive edge sites at a low temperature of 300 °C. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b01008DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6662884PMC

Chemical Tuning of Specific Capacitance in Functionalized Fluorographene.

Chem Mater 2019 Jul 7;31(13):4698-4709. Epub 2019 Jun 7.

Regional Centre for Advanced Technologies and Materials, Department of Physical Chemistry, Faculty of Science, Palacký University Olomouc, 17. listopadu 1192/12, 771 46 Olomouc, Czech Republic.

Owing to its high surface area and excellent conductivity, graphene is considered an efficient electrode material for supercapacitors. However, its restacking in electrolytes hampers its broader utilization in this field. Covalent graphene functionalization is a promising strategy for providing more efficient electrode materials. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b00655DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6662882PMC
July 2019
1 Read

Thermally Activated in Situ Doping Enables Solid-State Processing of Conducting Polymers.

Chem Mater 2019 Apr 2;31(8):2770-2777. Epub 2019 Apr 2.

Department of Chemistry and Chemical Engineering, Chalmers University of Technology, 41296 Göteborg, Sweden.

Free-standing bulk structures encompassing highly doped conjugated polymers are currently heavily explored for wearable electronics as thermoelectric elements, conducting fibers, and a plethora of sensory devices. One-step manufacturing of such bulk structures is challenging because the interaction of dopants with conjugated polymers results in poor solution and solid-state processability, whereas doping of thick conjugated polymer structures after processing suffers from diffusion-limited transport of the dopant. Here, we introduce the concept of thermally activated latent dopants for in situ bulk doping of conjugated polymers. Read More

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http://dx.doi.org/10.1021/acs.chemmater.8b04895DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6614883PMC

Effect of Backbone Regiochemistry on Conductivity, Charge Density, and Polaron Structure of n-Doped Donor-Acceptor Polymers.

Chem Mater 2019 May 11;31(9):3395-3406. Epub 2019 Apr 11.

Laboratory of Organic Electronics, Department of Science and Technology, Linköping University, SE-60174 Norrköping, Sweden.

We investigated the influence of backbone regiochemistry on the conductivity, charge density, and polaron structure in the widely studied n-doped donor-acceptor polymer poly[,'-bis(2-octyldodecyl)-1,4,5,8-naphthalenediimide-2,6-diyl]--5,5'-(2,2'-bithiophene) [P(NDI2OD-T2)]. In contrast to classic semicrystalline polymers such as poly(3-hexylthiophene) (P3HT), the regioirregular (RI) structure of the naphthalenediimide (NDI)-bithiophene (T2) backbone does not alter the intramolecular steric demand of the chain versus the regioregular (RR) polymer, yielding RI-P(NDI2OD-T2) with similar energetics and optical features as its RR counterpart. By combining the electrical, UV-vis/infrared, X-ray diffraction, and electron paramagnetic resonance data and density functional theory calculations, we quantitatively characterized the conductivity, aggregation, crystallinity, and charge density, and simulated the polaron structures, molecular vibrations, and spin density distribution of RR-/RI-P(NDI2OD-T2). Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b00558DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6613787PMC
May 2019
8.354 Impact Factor

Role of Surface Reduction in the Formation of Traps in -Doped II-VI Semiconductor Nanocrystals: How to Charge without Reducing the Surface.

Chem Mater 2019 Jun 29;31(12):4575-4583. Epub 2019 May 29.

Optoelectronic Materials Section, Faculty of Applied Sciences, Delft University of Technology, Van der Maasweg 9, 2629 HZ Delft, The Netherlands.

The efficiency of nanocrystal (NC)-based devices is often limited by the presence of surface states that lead to localized energy levels in the bandgap. Yet, a complete understanding of the nature of these traps remains challenging. Although theoretical modeling has greatly improved our comprehension of the NC surface, several experimental studies suggest the existence of metal-based traps that have not yet been found with theoretical methods. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b01395DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6595709PMC

Data Mining for Parameters Affecting Polymorph Selection in Contorted Hexabenzocoronene Derivatives.

Chem Mater 2018 May 23;30(10):3330-3337. Epub 2018 Apr 23.

Department of Chemical and Biological Engineering, Princeton University, Princeton, New Jersey 08544, United States.

The macroscopic properties of molecular materials can be drastically influenced by their solid-state packing arrangements, of which there can be many (e.g., polymorphism). Read More

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http://dx.doi.org/10.1021/acs.chemmater.8b00679DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6550467PMC
May 2018
1 Read

Scaffold-Induced Diketopyrrolopyrrole Molecular Stacks in a Covalent Organic Framework.

Chem Mater 2019 Apr 6;31(8):2707-2712. Epub 2019 Feb 6.

Department of Chemistry and Center for NanoScience (CeNS), University of Munich (LMU), Butenandtstr. 5-13, 81377 Munich, Germany.

In recent years, covalent organic frameworks (COFs) have attracted considerable attention due to their crystalline and porous nature, which positions them as intriguing candidates for diverse applications such as catalysis, sensing, or optoelectronics. The incorporation of dyes or semiconducting moieties into a rigid two-dimensional COF can offer emergent features such as enhanced light harvesting or charge transport. However, this approach can be challenging when dealing with dye molecules that exhibit a large aromatic backbone, since the steric demand of solubilizing side chains also needs to be integrated into the framework. Read More

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http://pubs.acs.org/doi/10.1021/acs.chemmater.8b02882
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http://dx.doi.org/10.1021/acs.chemmater.8b02882DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6485259PMC
April 2019
19 Reads

Dispelling the Myth of Passivated Codoping in TiO.

Chem Mater 2019 Apr 17;31(7):2577-2589. Epub 2019 Mar 17.

Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, U.K.

Modification of TiO to increase its visible light activity and promote higher performance photocatalytic ability has become a key research goal for materials scientists in the past 2 decades. One of the most popular approaches proposed this as "passivated codoping", whereby an equal number of donor and acceptor dopants are introduced into the lattice, producing a charge neutral system with a reduced band gap. Using the archetypal codoping pairs of [Nb + N]- and [Ta + N]-doped anatase, we demonstrate using hybrid density functional theory that passivated codoping is not achievable in TiO. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b00257DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6483321PMC
April 2019
1 Read

Guanidinium and Mixed Cesium-Guanidinium Tin(II) Bromides: Effects of Quantum Confinement and Out-of-Plane Octahedral Tilting.

Chem Mater 2019 Mar 13;31(6):2121-2129. Epub 2019 Feb 13.

Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1, CH-8093 Zürich, Switzerland.

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(NH)] and mixed cesium-guanidinium cations: GSnBr, CsGSnBr, and CsGSnBr. GSnBr has a one-dimensional structure that consists of chains of corner-sharing [SnBr] square pyramids and G cations situated in between the chains. Read More

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http://dx.doi.org/10.1021/acs.chemmater.9b00038DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6438322PMC
March 2019
10 Reads

Molecular Insights into Carbon Dioxide Sorption in Hydrazone-Based Covalent Organic Frameworks with Tertiary Amine Moieties.

Chem Mater 2019 Mar 13;31(6):1946-1955. Epub 2019 Feb 13.

Max Planck Institute for Solid State Research, Heisenbergstraße 1, 70569 Stuttgart, Germany.

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 CO uptake, atomistic insights into CO 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. Read More

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http://dx.doi.org/10.1021/acs.chemmater.8b04643DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6438324PMC
March 2019
3 Reads