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Chemistry of Materials: a Publication of the American Chemical Society

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https://www.readbyqxmd.com/read/27818575/structural-evolution-of-electrochemically-lithiated-mos2-nanosheets-and-the-role-of-carbon-additive-in-li-ion-batteries
#1
Chandramohan George, Andrew J Morris, Mohammad H Modarres, Michael De Volder
Understanding the structure and phase changes associated with conversion-type materials is key to optimizing their electrochemical performance in Li-ion batteries. For example, molybdenum disulfide (MoS2) offers a capacity up to 3-fold higher (∼1 Ah/g) than the currently used graphite anodes, but they suffer from limited Coulombic efficiency and capacity fading. The lack of insights into the structural dynamics induced by electrochemical conversion of MoS2 still hampers its implementation in high energy-density batteries...
October 25, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27713598/shape-control-of-colloidal-cu2-x-s-polyhedral-nanocrystals-by-tuning-the-nucleation-rates
#2
Ward van der Stam, Sabine Gradmann, Thomas Altantzis, Xiaoxing Ke, Marc Baldus, Sara Bals, Celso de Mello Donega
Synthesis protocols for colloidal nanocrystals (NCs) with narrow size and shape distributions are of particular interest for the successful implementation of these nanocrystals into devices. Moreover, the preparation of NCs with well-defined crystal phases is of key importance. In this work, we show that Sn(IV)-thiolate complexes formed in situ strongly influence the nucleation and growth rates of colloidal Cu2-x S polyhedral NCs, thereby dictating their final size, shape, and crystal structure. This allowed us to successfully synthesize hexagonal bifrustums and hexagonal bipyramid NCs with low-chalcocite crystal structure, and hexagonal nanoplatelets with various thicknesses and aspect ratios with the djurleite crystal structure, by solely varying the concentration of Sn(IV)-additives (namely, SnBr4) in the reaction medium...
September 27, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27656042/electroconductive-hydrogel-based-on-functional-poly-ethylenedioxy-thiophene
#3
Damia Mawad, Arbel Artzy-Schnirman, Joanne Tonkin, Jose Ramos, Sahika Inal, Muzamir M Mahat, Nadim Darwish, Limor Zwi-Dantsis, George G Malliaras, J Justin Gooding, Antonio Lauto, Molly M Stevens
Poly(ethylene dioxythiophene) with functional pendant groups bearing double bonds is synthesized and employed for the fabrication of electroactive hydrogels with advantageous characteristics: covalently cross-linked porous 3D scaffolds with notable swelling ratio, appropriate mechanical properties, electroactivity in physiological conditions, and suitability for proliferation and differentiation of C2C12 cells. This is a new approach for the fabrication of conductive engineered constructs.
September 13, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27594765/thermodynamic-insight-in-the-high-pressure-behavior-of-uio-66-effect-of-linker-defects-and-linker-expansion
#4
Sven M J Rogge, Jelle Wieme, Louis Vanduyfhuys, Steven Vandenbrande, Guillaume Maurin, Toon Verstraelen, Michel Waroquier, Veronique Van Speybroeck
In this Article, we present a molecular-level understanding of the experimentally observed loss of crystallinity in UiO-66-type metal-organic frameworks, including the pristine UiO-66 to -68 as well as defect-containing UiO-66 materials, under the influence of external pressure. This goal is achieved by constructing pressure-versus-volume profiles at finite temperatures using a thermodynamic approach relying on ab initio derived force fields. On the atomic level, the phenomenon is reflected in a sudden drop in the number of symmetry operators for the crystallographic unit cell because of the disordered displacement of the organic linkers with respect to the inorganic bricks...
August 23, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27570369/fast-li-ion-conducting-garnet-related-li7-3x-fe-x-la3zr2o12-with-uncommon-i4%C3%AC-3d-structure
#5
Reinhard Wagner, Günther J Redhammer, Daniel Rettenwander, Gerold Tippelt, Andreas Welzl, Stefanie Taibl, Jürgen Fleig, Alexandra Franz, Werner Lottermoser, Georg Amthauer
Fast Li-ion-conducting Li oxide garnets receive a great deal of attention as they are suitable candidates for solid-state Li electrolytes. It was recently shown that Ga-stabilized Li7La3Zr2O12 crystallizes in the acentric cubic space group I4̅3d. This structure can be derived by a symmetry reduction of the garnet-type Ia3̅d structure, which is the most commonly found space group of Li oxide garnets and garnets in general. In this study, single-crystal X-ray diffraction confirms the presence of space group I4̅3d also for Li7-3x Fe x La3Zr2O12...
August 23, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27551163/ph-responsive-and-oxidation-resistant-wet-adhesive-based-on-reversible-catechol-boronate-complexation
#6
Ameya R Narkar, Brett Barker, Matthew Clisch, Jingfeng Jiang, Bruce P Lee
A smart adhesive capable of binding to a wetted surface was prepared by copolymerizing dopamine methacrylamide (DMA) and 3-acrylamido phenylboronic acid (AAPBA). pH was used to control the oxidation state and the adhesive property of the catechol side chain of DMA and to trigger the catechol-boronate complexation. FTIR spectroscopy confirmed the formation of the complex at pH 9, which was not present at pH 3. The formation of the catechol-boronate complex increased the cross-linking density of the adhesive network...
August 9, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27346923/operando-x-ray-investigation-of-electrode-electrolyte-interfaces-in-model-solid-oxide-fuel-cells
#7
Sergey Volkov, Vedran Vonk, Navid Khorshidi, Dirk Franz, Markus Kubicek, Volkan Kilic, Roberto Felici, Tobias M Huber, Edvinas Navickas, Ghislain M Rupp, Jürgen Fleig, Andreas Stierle
We employed operando anomalous surface X-ray diffraction to investigate the buried interface between the cathode and the electrolyte of a model solid oxide fuel cell with atomic resolution. The cell was studied under different oxygen pressures at elevated temperatures and polarizations by external potential control. Making use of anomalous X-ray diffraction effects at the Y and Zr K-edges allowed us to resolve the interfacial structure and chemical composition of a (100)-oriented, 9.5 mol % yttria-stabilized zirconia (YSZ) single crystal electrolyte below a La0...
June 14, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27563171/polymer-free-films-of-inorganic-halide-perovskite-nanocrystals-as-uv-to-white-color-conversion-layers-in-leds
#8
Francisco Palazon, Francesco Di Stasio, Quinten A Akkerman, Roman Krahne, Mirko Prato, Liberato Manna
No abstract text is available yet for this article.
May 10, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27212793/highly-fluorescent-ribonuclease-a-encapsulated-lead-sulfide-quantum-dots-for-ultrasensitive-fluorescence-in-vivo-imaging-in-the-second-near-infrared-window
#9
Yifei Kong, Jun Chen, Hongwei Fang, George Heath, Yan Wo, Weili Wang, Yunxia Li, Yuan Guo, Stephen D Evans, Shiyi Chen, Dejian Zhou
Ribonuclease-A (RNase-A) encapsulated PbS quantum dots (RNase-A@PbS Qdots) which emit in the second near-infrared biological window (NIR-II, ca. 1000-1400 nm) are rapidly synthesized under microwave heating. Photoluminescence (PL) spectra of the Qdots can be tuned across the entire NIR-II range by simply controlling synthesis temperature. The size and morphology of the Qdots are examined by transmission electron microscopy (TEM), atomic force microscopy (AFM), and dynamic light scattering (DLS). Quantum yield (Φf) measurement confirms that the prepared Qdots are one of the brightest water-soluble NIR-II emitters for in vivo imaging...
May 10, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27212792/self-assembled-heteroepitaxial-oxide-nanocomposite-for-photoelectrochemical-solar-water-oxidation
#10
Seungho Cho, Ji-Wook Jang, Leigang Li, Jie Jian, Haiyan Wang, Judith L MacManus-Driscoll
We report on spontaneously phase ordered heteroepitaxial SrTiO3 (STO):ZnFe2O4 (ZFO) nanocomposite films that give rise to strongly enhanced photoelectrochemical solar water oxidation, consistent with enhanced photoinduced charge separation. The STO:ZFO nanocomposite yielded an enhanced photocurrent density of 0.188 mA/cm(2) at 1.23 V vs a reversible hydrogen electrode, which was 7.9- and 2.6-fold higher than that of the plain STO film and ZFO film cases under 1-sun illumination, respectively. The photoelectrode also produced stable photocurrent and Faradaic efficiencies of H2 and O2 formation that were more than 90%...
May 10, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27212791/multiprobe-study-of-the-solid-electrolyte-interphase-on-silicon-based-electrodes-in-full-cell-configuration
#11
N Dupré, P Moreau, E De Vito, L Quazuguel, M Boniface, A Bordes, C Rudisch, P Bayle-Guillemaud, D Guyomard
The failure mechanism of silicon-based electrodes has been studied only in a half-cell configuration so far. Here, a combination of (7)Li, (19)F MAS NMR, XPS, TOF-SIMS, and STEM-EELS, provides an in-depth characterization of the solid electrolyte interphase (SEI) formation on the surface of silicon and its evolution upon aging and cycling with LiNi1/3Mn1/3Co1/3O2 as the positive electrode in a full Li-ion cell configuration. This multiprobe approach indicates that the electrolyte degradation process observed in the case of full Li-ion cells exhibits many similarities to what has been observed in the case of half-cells in previous works, in particular during the early stages of the cycling...
April 26, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27274616/interplay-of-orbital-and-relativistic-effects-in-bismuth-oxyhalides-biof-biocl-biobr-and-bioi
#12
Alex M Ganose, Madeleine Cuff, Keith T Butler, Aron Walsh, David O Scanlon
No abstract text is available yet for this article.
April 12, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27110064/structural-and-electrochemical-consequences-of-al-and-ga-cosubstitution-in-li7la3zr2o12-solid-electrolytes
#13
Daniel Rettenwander, Günther Redhammer, Florian Preishuber-Pflügl, Lei Cheng, Lincoln Miara, Reinhard Wagner, Andreas Welzl, Emmanuelle Suard, Marca M Doeff, Martin Wilkening, Jürgen Fleig, Georg Amthauer
Several "Beyond Li-Ion Battery" concepts such as all solid-state batteries and hybrid liquid/solid systems envision the use of a solid electrolyte to protect Li-metal anodes. These configurations are very attractive due to the possibility of exceptionally high energy densities and high (dis)charge rates, but they are far from being realized practically due to a number of issues including high interfacial resistance and difficulties associated with fabrication. One of the most promising solid electrolyte systems for these applications is Al or Ga stabilized Li7La3Zr2O12 (LLZO) based on high ionic conductivities and apparent stability against reduction by Li metal...
April 12, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27041820/drug-initiated-synthesis-of-polymer-prodrugs-combining-simplicity-and-efficacy-in-drug-delivery
#14
Julien Nicolas
In the field of nanomedicine, the global trend over the past few years has been toward the design of highly sophisticated drug delivery systems with active targeting and/or imaging capabilities, as well as responsiveness to various stimuli to increase their therapeutic efficacy. However, providing sophistication generally increases complexity that could be detrimental in regards to potential pharmaceutical development. An emerging concept to design efficient yet simple drug delivery systems, termed the "drug-initiated" method, consists of growing short polymer chains from drugs in a controlled fashion to yield well-defined drug-polymer prodrugs...
March 22, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27019548/crystal-structure-of-garnet-related-li-ion-conductor-li7-3x-ga-x-la3zr2o12-fast-li-ion-conduction-caused-by-a-different-cubic-modification
#15
Reinhard Wagner, Günther J Redhammer, Daniel Rettenwander, Anatoliy Senyshyn, Walter Schmidt, Martin Wilkening, Georg Amthauer
Li-oxide garnets such as Li7La3Zr2O12 (LLZO) are among the most promising candidates for solid-state electrolytes to be used in next-generation Li-ion batteries. The garnet-structured cubic modification of LLZO, showing space group Ia-3d, has to be stabilized with supervalent cations. LLZO stabilized with Ga(3+) shows superior properties compared to LLZO stabilized with similar cations; however, the reason for this behavior is still unknown. In this study, a comprehensive structural characterization of Ga-stabilized LLZO is performed by means of single-crystal X-ray diffraction...
March 22, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27458325/thermoreversible-and-injectable-abc-polypeptoid-hydrogels-controlling-the-hydrogel-properties-through-molecular-design
#16
Sunting Xuan, Chang-Uk Lee, Cong Chen, Andrew B Doyle, Yueheng Zhang, Li Guo, Vijay T John, Daniel Hayes, Donghui Zhang
A series of ABC triblock copolypeptoids [i.e., poly(N-allyl glycine)-b-poly(N-methyl glycine)-b-poly(N-decyl glycine) (AMD)] with well-defined structure and varying composition have been synthesized by sequential primary amine-initiated ring-opening polymerization of the corresponding N-substituted N-carboxyanhydride monomers (Al-NCA, Me-NCA, and De-NCA). The ABC block copolypeptoids undergo sol-to-gel transitions with increasing temperature in water and biological media at low concentrations (2.5-10 wt %)...
February 9, 2016: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/26834315/stimuli-responsive-supramolecular-hydrogels-with-high-extensibility-and-fast-self-healing-via-precoordinated-mussel-inspired-chemistry
#17
Sen Hou, Peter X Ma
Supramolecular hydrogels have the advantages of stimuli responsiveness and self-healing compared to covalently crosslinked hydrogels. However, the existing supramolecular hydrogels are usually poor in mechanical properties especially in extensibility. In addition, these supramolecular hydrogels need a long self-healing time and have low self-healing efficiency. In this manuscript, we report a novel strategy to develop highly extensible and fast self-healing supramolecular hydrogels by using pre-coordinated mussel-inspired catechol-Fe(3+) complexes as dynamic crosslinkers...
November 24, 2015: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/26617434/nanoscale-transformations-in-covellite-cus-nanocrystals-in-the-presence-of-divalent-metal-cations-in-a-mild-reducing-environment
#18
Yi Xie, Giovanni Bertoni, Andreas Riedinger, Ayyappan Sathya, Mirko Prato, Sergio Marras, Renyong Tu, Teresa Pellegrino, Liberato Manna
We studied the structural and compositional transformations of colloidal covellite (CuS) nanocrystals (and of djurleite (Cu1.94S) nanocrystals as a control) when exposed to divalent cations, as Cd(2+) and Hg(2+), at room temperature in organic solvents. All the experiments were run in the absence of phosphines, which are a necessary ingredient for cation exchange reactions involving copper chalcogenides, as they strongly bind to the expelled Cu(+) ions. Under these experimental conditions, no remarkable reactivity was indeed seen for both CuS and Cu1...
November 10, 2015: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27182110/3d-magnetic-induction-maps-of-nanoscale-materials-revealed-by-electron-holographic-tomography
#19
Daniel Wolf, Luis A Rodriguez, Armand Béché, Elsa Javon, Luis Serrano, Cesar Magen, Christophe Gatel, Axel Lubk, Hannes Lichte, Sara Bals, Gustaaf Van Tendeloo, Amalio Fernández-Pacheco, José M De Teresa, Etienne Snoeck
The investigation of three-dimensional (3D) ferromagnetic nanoscale materials constitutes one of the key research areas of the current magnetism roadmap and carries great potential to impact areas such as data storage, sensing, and biomagnetism. The properties of such nanostructures are closely connected with their 3D magnetic nanostructure, making their determination highly valuable. Up to now, quantitative 3D maps providing both the internal magnetic and electric configuration of the same specimen with high spatial resolution are missing...
October 13, 2015: Chemistry of Materials: a Publication of the American Chemical Society
https://www.readbyqxmd.com/read/27293311/self-assembly-of-pluronic-f127-silica-spherical-core-shell-nanoparticles-in-cubic-close-packed-structures
#20
Stef Kerkhofs, Tom Willhammar, Heleen Van Den Noortgate, Christine E A Kirschhock, Eric Breynaert, Gustaaf Van Tendeloo, Sara Bals, Johan A Martens
A new ordered mesoporous silica material (COK-19) with cubic symmetry is synthesized by silicate polycondensation in a citric acid/citrate buffered micellar solution of Pluronic F127 triblock copolymer near neutral pH. SAXS, nitrogen adsorption, TEM, and electron tomography reveal the final material has a cubic close packed symmetry (Fm3̅m) with isolated spherical mesopores interconnected through micropores. Heating of the synthesis medium from room temperature to 70 °C results in a mesopore size increase from 7...
August 11, 2015: Chemistry of Materials: a Publication of the American Chemical Society
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