Bacteroides expand the functional versatility of a conserved transcription factor and transcribed DNA to program capsule diversity
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In this work, we have developed a unique in situ multimodal corrosion system that is capable of acquiring electrochemical data, sample imaging/visualization and hydrogen collection, simultaneously. Each of these modalities yield valuable information pertaining to the ongoing corrosion process. Combining them can yield holistic information on the role of microstructure, processing history, presence of coatings, etc., on the sequence of steps occurring during the corrosion process, and how they correlate with the acquired electrochemical data. Four materials systems, namely AA6061-T6 aluminum alloy, AZ91 magnesium alloy, galvanized DP590 steel, and pure Zn, were investigated under open circuit potential and under potentiodynamic polarization. The multimodal corrosion system was utilized to observe processes such as surface passivation and dissolution, pit and filiform corrosion initiation and propagation, and was correlated with location and magnitude of hydrogen evolution. This approach is shown to yield a truly multimodal understanding of the ongoing corrosion processes.
Recent advances in two-dimensional (2D) materials have led to the renewed interest in intercalation as a powerful fabrication and processing tool. Intercalation is an effective method of modifying the interlayer interactions, doping 2D materials, modifying their electronic structure or even converting them into starkly different new structures or phases. Herein, we discuss different methods of intercalation and provide a comprehensive review of various roles and applications of intercalation in next-generation energy storage, optoelectronics, thermoelectrics, catalysis, etc. The recent progress in intercalation effects on crystal structure and structural phase transitions, including the emergence of quantum phases are also reviewed.
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We describe a new planar processing chemistry that allows the synthesis and patterning of dynamically self-actuating gels of diverse form. The chemical reaction covalently incorporates a methacrylate-modified ruthenium trisbipyridine monomer within a poly acrylamide (PAAm) gel, modified to provide a flexible chemistry for UV-curable, self-oscillating Belousov–Zhabotinsky (BZ) gels. The photoinitiated polymerization offers significant advantages over previously reported BZ gel chemistries – fast polymerization rates, broad flexibility in the structural and functional attributes that impact the BZ reaction driven mechanics, and a facility for net shape fabrication via projection mode photo lithographic exposure. The facility of the synthetic method enabled an opportunity to broadly explore the structure/property and structure/rate correlations characterizing the dynamics of these gels and develop means to both control and predict the detailed features of the self-oscillating chemical waves they embed. The PAAm systems initiate under the control of transport-dominated influences weighted heavily by the diffusion/depletion of reagents present in the ambient contacting fluid medium. These initiating modes of oscillation are generally unstable temporally, showing shape- and property-sensitive conversions to oscillating modes controlled by the attributes of the gel-phase environment. The present work establishes the nature of these sensitivities, developing insights related to such features in patterned gel objects or films as composition, size, thickness, shape, degree of crosslinking, and gradient forms of structure within the gel. We observed in this work that, across a broad design-rule and compositional space, the PAAm based BZ gel systems exhibit contractions in dimension for regions in which the Ru catalyst is present in the +3 oxidation state (PNIPAAm BZ gels expand in this state). The chemomechanics of the PAAm system are further differentiated from those of PNIPAAm in the generally (and relatively) fast oscillatory rates it can sustain. Furthermore, this work suggests the dynamics in the PAAm gels do not reflect a simple osmotic force driven by differences in the solvation of Ru(II/III) centers. Computational modeling supports a mechanism in which the charge state of Ru centers mediate a differential degree of intra/inter-chain segmental interactions – dynamics that mediate a temporally varying degree of reversibly formed association crosslinks within the gel.
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The solution synthesis of magnetic nanoparticles allows for precise control of a particle's shape, size, and crystal phase on the nanoscale, key parameters in tuning the intrinsic magnetic properties of nanoparticles. In this study, we investigate the role of polyhydric alcohols for the solution synthesis of cobalt carbide nanoparticles, a newly discovered hard ferromagnetic material. The oxidative stability of the polyhydric alcohol at reaction temperatures plays a significant role in the kinetics of carbide formation, as well as the phase produced (Co2C vs. Co3C). By tuning the oxidation rate of the polyhydric alcohol, composites of CoO, CoxC, and Co phases can be produced, allowing for magnetic composites comprised of anti ferromagnetic, hard ferromagnetic and soft ferromagnetic phases.
The thorium and uranium dihydride dimer complexes [(C 5 Me 5 ) 2 An(H)(μ-H)] 2 (An = Th, U) have been easily prepared using phenylsilane, which is an efficient and safer alternative to hydrogen gas. We demonstrated the synthetic utility of this new hydriding method by the preparation of a variety of organometallic complexes, including, for the first time, (C 5 Me 5 ) 2 U(SMe) 2 , (C 5 Me 5 ) 2 Th(C 4 Ph 4 ), (C 5 Me 5 ) 2 U(C 4 Ph 4 ), (C 5 Me 5 ) 2 ThS 5 , and (C 5 Me 5 ) 2 U(bipy) using [(C 5 Me 5 ) 2 An(H)(μ-H)] 2 (An = Th, U) as multi-electron reductants.
There is a facile method for introducing one or more deuterium atoms onto an aromatic nucleus via Br/D exchange with high functional group tolerance and high incorporation efficiency is disclosed. Deuterium-labeled aryl chlorides and aryl borates which could be used as substrates in cross-coupling reactions to construct more complicated deuterium-labeled compounds can also be synthesized by this method.
Thiol-based reactions were applied to enable the photochemical patterning of polymer brushes and green fluorescent protein on silicon oxide surfaces.
We herein propose a novel synthetic methodology for a series of nickel–tungsten bimetallics/carbon nanofiber catalysts (Ni, 0.37–2.08 wt%; W, 0.01–0.06 wt%) in situ fabricated by pyrolysis (950 °C) of Ni, W and Zn-containing metal organic framework (Ni0.6-x–Wx–ZnBTC, x = 0–0.6) fibers. The resulting catalysts (Ni0.6-x–Wx/CNF) have uniform particles (ca. 68 nm), evenly dispersed onto the hierarchically porous carbon nanofibers formed simultaneously. All of the Ni0.6-x–Wx/CNF catalysts prove to be highly active towards direct conversion of cellulose to ethylene glycol (EG). A large productivity ranging from 15.3 to 70.8 molEG h-1 gW-1 is shown, two orders of magnitude higher than those by using other W-based catalysts reported.
Nanomaterials engineering and synthetic chemistry continues to expand the range of applications for surface-enhanced Raman scattering spectroscopy.
Flash nanoprecipitation was validated for the facile fabrication and therapeutic loading of monodisperse polymeric bicontinuous nanospheres possessing primitive cubic mesophases.
Highly-stable ultrasmall superparamagnetic iron oxide nanoparticles (USPIONs) show great potential for the development of theranostic nanodevices.
A surface energy-driven strategy is proposed for ex situ hierarchical assembly of low-dimensional nanomaterials on graphene aerogels, which is applicable to a broad variety of low-dimensional nanomaterials regardless of their composition, shapes and dimensionalities.
A facile catalytic protocol achieves the homocoupling of pyrazole boronic esters, enabling access to the structurally-flexible metal–organic framework Co(bpz).