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Synthesis and Stability of an Eight‐Coordinated Fe 3 O 4 High‐Pressure Phase: Implications for the Mantle Structure of Super‐Earths
Abstract Super‐Earths ranging up to 10 Earth masses (M E ) with Earth‐like density are common among the observed exoplanets thus far, but their measured masses and radii do not uniquely elucidate their internal structure. Exploring the phase transitions in the Mg‐silicates that define the mantle‐structure of super‐Earths is critical to characterizing their interiors, yet the relevant terapascal conditions are experimentally challenging for direct structural analysis. Here we investigated the crystal chemistry of Fe 3 O 4 as a low‐pressure analog to Mg 2 SiO 4 between 45–115 GPa and up to 3000 K using powder and single crystal X‐ray diffraction in the laser‐heated diamond anvil cell. Between 60–115 GPa and above 2000 K, Fe 3 O 4 adopts an 8‐fold coordinated Th 3 P 4 ‐type structure ( I ‐43d, Z = 4) with disordered Fe 2+ and Fe 3+ into one metal site. This Fe‐oxide phase is isostructural with that predicted for Mg 2 SiO 4 above 500 GPa in super‐Earth mantles and suggests that Mg 2 SiO 4 can incorporate both ferric and ferrous iron at these conditions. The pressure‐volume behavior observed in this 8‐fold coordinated Fe 3 O 4 indicates a maximum 4% density increase across the 6‐ to 8‐fold coordination transition in the analog Mg‐silicate. Reassessment of the FeO—Fe 3 O 4 fugacity buffer considering the Fe 3 O 4 phase relationships identified in this study reveals that increasing pressure and temperature to 120 GPa and 3000 K in Earth and planetary mantles drives iron toward oxidation.
The initiation of mammalian protein synthesis and mRNA scanning mechanism
Abstract not provided
Synthesis of sodium polyhydrides at high pressures
Archetypal ionic NaH is the only known compound of sodium and hydrogen. Application of high pressure is known to promote states with higher atomic coordination, but extensive searches for polyhydrides with unusual stoichiometry have had only limited success in spite of several theoretical predictions. Here we report the first observation of the formation of polyhydrides of Na (NaH 3 and NaH 7 ) above 40 GPa and 2,000 K. Moreover, we combine synchrotron X-ray diffraction and Raman spectroscopy in a laser-heated diamond anvil cell and theoretical random structure searching, which both agree on the stable structures and compositions. Our results support the formation of multicenter bonding in a material with unusual stoichiometry. These results are applicable to the design of new energetic solids and high-temperature superconductors based on hydrogen-rich materials.
Detonation synthesis of carbon nano-onions via liquid carbon condensation
Abstract not provided
A multi-species synthesis of physiological mechanisms in drought-induced tree mortality
Widespread tree mortality associated with drought has been observed on all forested continents and global change is expected to exacerbate vegetation vulnerability. Forest mortality has implications for future biosphere–atmosphere interactions of carbon, water and energy balance, and is poorly represented in dynamic vegetation models. Reducing uncertainty requires improved mortality projections founded on robust physiological processes. However, the proposed mechanisms of drought-induced mortality, including hydraulic failure and carbon starvation, are unresolved. A growing number of empirical studies have investigated these mechanisms, but data have not been consistently analysed across species and biomes using a standardized physiological framework. Here in this work, we show that xylem hydraulic failure was ubiquitous across multiple tree taxa at drought-induced mortality. All species assessed had 60% or higher loss of xylem hydraulic conductivity, consistent with proposed theoretical and modelled survival thresholds. We found diverse responses in non-structural carbohydrate reserves at mortality, indicating that evidence supporting carbon starvation was not universal. Reduced non-structural carbohydrates were more common for gymnosperms than angiosperms, associated with xylem hydraulic vulnerability, and may have a role in reducing hydraulic function. In conclusion, our finding that hydraulic failure at drought-induced mortality was persistent across species indicates that substantial improvement in vegetation modelling can be achieved using thresholds in hydraulic function.
Mechanism of error-free DNA synthesis across N1-methyl-deoxyadenosine by human DNA polymerase-$\iota$
N1-methyl-deoxyadenosine (1-MeA) is formed by methylation of deoxyadenosine at the N1 atom. 1-MeA presents a block to replicative DNA polymerases due to its inability to participate in Watson-Crick (W-C) base pairing. Here we determine how human DNA polymerase-ι (Pol$\iota$) promotes error-free replication across 1-MeA. Steady state kinetic analyses indicate that Pol$\iota$ is ~100 fold more efficient in incorporating the correct nucleotide T versus the incorrect nucleotide C opposite 1-MeA. To understand the basis of this selectivity, we determined ternary structures of Polι bound to template 1-MeA and incoming dTTP or dCTP. In both structures, template 1-MeA rotates to the syn conformation but pairs differently with dTTP versus dCTP. Thus, whereas dTTP partakes in stable Hoogsteen base pairing with 1-MeA, dCTP fails to gain a “foothold” and is largely disordered. Together, our kinetic and structural studies show how Polι maintains discrimination between correct and incorrect incoming nucleotide opposite 1-MeA in preserving genome integrity.
Synthesis, Ligation and Solvent Extraction Properties of NCMPO-decorated Pyridine and Pyridine N-oxide Platforms
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Poly(methyl methacrylate-block-vinyl-m-triphenylamine): synthesis by RAFT polymerization and melt-state self-assembly
Abstract not provided
Core–shell PdPb@Pd aerogels with multiply-twinned intermetallic nanostructures: facile synthesis with accelerated gelation kinetics and their enhanced electrocatalytic properties
Delicately engineering well-defined noble metal aerogels with favorable structural and compositional features is of vital importance for wide applications. Here, we reported a one-pot and facile method for synthesizing core–shell PdPb@Pd hydrogels/aerogels with multiply-twinned grains and an ordered intermetallic phase using sodium hypophosphite as a multifunctional reducing agent. Due to the accelerated gelation kinetics induced by increased reaction temperature and the specific function of sodium hypophosphite, the formation of hydrogels can be completed within 4 h. As a result, owing to their unique porous structure and favorable geometric and electronic effects, the optimized PdPb@Pd aerogels exhibit enhanced electrochemical performance towards ethylene glycol oxidation with a mass activity of 5.8 times higher than Pd black.
Synthesis of uranium-in-cryptand complexes
Uranium-in-cryptand complexes can be readily synthesized by reacting UI 3 with 2.2.2-cryptand.
Synthesis of first row transition metal selenomaltol complexes
Complexation of selenomaltol to transition metal ions promotes a zwitterionic resonance form.
Direct synthesis of functionalized PCN-333 via linker design for Fe 3+ detection in aqueous media
Functionalized PCN-333 was synthesized for Fe 3+ ion detection via one-pot solvothermal reaction.
Synthesis of highly-active Fe–N–C catalysts for PEMFC with carbide-derived carbons
We study the physico-chemical properties and electrocatalytic activity towards oxygen reduction of two Fe–N–C catalysts based on carbide derived carbon.
Design and synthesis of capped-paddlewheel-based porous coordination cages
A novel cluster capping strategy is employed to leverage the structural diversity of metal–organic cages toward the isolation of porous cages.
Efficient electrochemical synthesis of robust, densely functionalized water soluble quinones
Robust, highly water-soluble quinone derivatives are efficiently prepared by a scalable electrosynthetic protocol employing low-cost commercially available precursors.
Solvothermal synthesis of porous organic cage CC3 in the presence of dimethylformamide as solvent
Morphology, and crystal product of porous organic cage CC3, was modified by the use of a novel and non-traditional high dielectric constant solvent dimethyl formamide.