Notes

Methane service in single-atom Ir-doped material nanoparticles via very first principles.
Bio-active molecules having N-heteroarene core are widely used for numerous medicinal applications and as lifesaving drugs. In this direction, dehydrogenation of partially saturated aromatic N-heterocycles shows utmost importance for the synthesis of heterocycles. This feature article highlights the recent advances, from 2009 to April 2021, on the dehydrogenation of N-heteroaromatics. Notable features considering the development of newer catalysis for dehydrogenations are (i) approaches based on precious metal catalysis, (ii) newer strategies and catalyst development technology using non-precious metal-catalysts for N-heterocycles having one or more heteroatoms, (iii) Synthesis of five or six-membered N-heterocycles using photocatalysis, electrocatalytic, and organo-catalytic approaches using different homogeneous and heterogeneous conditions' (iv) metal free (base and acid-promoted) dehydrogenation along with I2, N-hydroxyphthalimide (NHPI) and bio catalyzed miscellaneous examples have also been discussed, (v) mechanistic studies for various dehydrogenation reactions and (vi) synthetic applications of various bio-active molecules including post-drug derivatization are discussed.TiO2-based nanosheet materials with a core-shell structure are expected to be one of the promising photocatalysts for the degradation of organic pollution. It is a challenge to synthesize TiO2 by the desired nucleation and growth process, so most reported TiO2 core-shell photocatalysts are prepared using TiO2 as a core material. Layered double hydroxides (LDHs) are considered ideal platforms to grow TiO2in situ and further serve as additional components to improve the separation of photogenerated charge carriers. In this work, we report the design and fabrication of anatase TiO2-coated ZnAl-layered double oxide (LDO@TiO2) nanosheets, which involve the in situ growth of TiO2 on ZnAl-LDH followed by subsequent calcination treatment. The resulting LDO@TiO2 photocatalyst yields typical core-shell nanosheet morphology with a mesoporous structure, exhibiting excellent photodegradation and mineralization efficiency for organic pollution.Both polyesters and polycarbonates have been proposed as alternatives to polyethers as host materials for future polymer electrolytes for solid-state lithium-ion batteries. While being comparatively similar functional groups, the electron density on the coordinating carbonyl oxygen is different, thereby rendering different coordinating strength towards lithium ions. In this study, the transport properties of poly(ε-caprolactone) and poly(trimethylene carbonate) as well as random copolymers of systematically varied composition of the two have been investigated, in order to better elucidate the role of the coordination strength. The cationic transference number, a property well-connected with the complexing ability of the polymer, was shown to depend almost linearly on the ester content of the copolymer, increasing from 0.49 for the pure poly(ε-caprolactone) to 0.83 for pure poly(trimethylene carbonate). Contradictory to the transference number measurements that suggest a stronger lithium-to-ester coordination, DFT calculations showed that the carbonyl oxygen in the carbonate coordinates more strongly to the lithium ion than that of the ester. FT-IR measurements showed the coordination number to be higher in the polyester system, resulting in a higher total coordination strength and thereby resolving the paradox. selleck chemicals llc This likely originates in properties that are specific of polymeric solvent systems, e.g. steric properties and chain dynamics, which influence the coordination chemistry. These results highlight the complexity in polymeric systems and their ion transport properties in comparison to low-molecular-weight analogues, and how polymer structure and steric effects together affect the coordination strength and transport properties.Fasciola gigantica is one of the aetiological trematodes associated with fascioliasis, which heavily impacts food-production systems and human and animal welfare on a global scale. In the absence of a vaccine, fascioliasis control and treatment is restricted to pasture management, such as clean grazing, and a limited array of chemotherapies, to which signs of resistance are beginning to appear. Research into novel control strategies is therefore urgently required and the advent of 'omics technologies presents considerable opportunity for novel drug and vaccine target discovery. Here, interrogation of the first available F. gigantica newly excysted juvenile (NEJ) transcriptome revealed several protein families of current interest to parasitic flatworm vaccine research, including orthologues of mammalian complement regulator CD59 of the Ly6 family. Ly6 proteins have previously been identified on the tegument of Schistosoma mansoni and induced protective immunity in vaccination trials. Incorporating the recently available F. gigantica genome, the current work revealed 20 novel Ly6 family members in F. gigantica and, in parallel, significantly extended the F. hepatica complement from 3 to 18 members. Phylogenetic analysis revealed several distinct clades within the family, some of which are unique to Fasciola spp. trematodes. Analysis of available proteomic databases also revealed three of the newly discovered FhLy6s were present in extracellular vesicles, which have previously been prioritised in studying the host-parasite interface. The presentation of this new transcriptomic resource, in addition to the Ly6 family proteins here identified, represents a wealth of opportunity for future vaccine research.We study the isomeric effects using time resolved photoelectron circular dichroism (TR-PECD). Using a (1 + 1') pump-probe ionisation scheme with photoelectrons collected by the velocity map imaging technique, we compare the relaxation dynamics from the 3s-Rydberg state in 1R,4R-(+)-camphor with the one in its chiral isomer, 1R,4S-(-)-fenchone [Comby et al., 2016, JPCL, 7, 4514]. Our measurements revealed a similar lifetime for both isomers. However, the circular dichroism in the photoelectron angular distribution decays exponentially in ∼730 fs from a +9% forward amplitude during the first hundreds of femtoseconds to reach an asymptotic -2% backward amplitude. This time-scale is drastically shorter than in fenchone. Our analysis allows us to evaluate the impact of the anisotropy of excitation; the relaxation dynamics, following photoexcitation by the linearly polarized pump, is then compared to that induced by a circularly polarized pump pulse (CPL). With such a CPL pump, we then retrieve time constants of our chiral observables similar to the ones recorded in fenchone. Quantum and classical simulations are developed and used to decipher the dependence of the PECD on the anisotropy of excitation and the spatial distribution of the 3s-Rydberg electron wavefunction. Our experimental investigations, supported by our simulations, suggest that varying the pump ellipticity enables us to reveal the breakdown of the Franck-Condon approximation.We report the design of 'slippery' nanoemulsion-infused porous surfaces (SNIPS). These materials are strongly anti-fouling to a broad range of substances, including microorganisms. Infusion with water-in-oil nanoemulsions also endows these slippery coatings with the ability to host and control or sustain the release of water-soluble agents, including polymers, peptides, and nucleic acids, opening the door to new applications of liquid-infused materials.Adhesion between similar and dissimilar materials is essential to many biological systems and synthetic materials, devices, and machines. Since the inception of adhesion science more than five decades ago, adhesion to a surface has long been recognized as beyond two-dimensional. Similarly, molecular conformation - the three-dimensional arrangement of atoms in a molecule - is ubiquitous in biology and fundamental to the binding of biomolecules. However, the connection between these concepts, which could link molecular conformation in biology to micro- and macroscopic adhesion in materials science, remains elusive. Herein, we examine this connection by manipulating the molecular conformation of a mussel-inspired universal coating, which imparts a memory for recognizing different hydrogels. This approach leads to significantly (several fold) increased interfacial adhesion between the coating and hydrogels across a broad range of length scales, from molecular to macroscopic. Furthermore, we demonstrate that imparting memory is a general and facile noncovalent approach for enhancing interfacial adhesion that, with suitable energy dissipation, can be used for the bonding of materials.Digitally aligned long continuous ZnO NWs with distinct widths and microstructures are prepared and used for tuning the plasticity of synaptic transistors (STs) for the first time. Intrinsically controlled synaptic plasticity, i.e. short-term plasticity (STP) and long-term plasticity (LTP), was achieved using the same source material and post-fabrication condition for the first time, which is essential for simple and low-cost fabrication. Moreover, these versatile properties of ZnO STs enable the integration of STP and LTP as realized by multiplexed neurotransmission of different neurotransmitters dopamine and acetylcholine, which promote learning and memory in organisms, so the device may utilize these processes in neuroelectronic devices. Devices with well-controlled synaptic plasticity can simulate the "learning-forgetting-erase" and "instant display" processes. ZnO NWs may enable the development of neuromorphic computers that can use the same material to achieve both short-term computation and long-term memory.Adverse dendritic growth destabilizes Li metal anodes (LMAs), dramatically limiting the commercial applications of Li metal batteries (LMBs). Herein, ZIF-67 with unsaturated coordinative metal sites is used to construct a protective coating to immobilize anions, which is capable of increasing the Li+ transference number (tLi+) to mitigate the electrolyte concentration gradient in the vicinity of LMAs. In addition, the ZIF-67-based layer provides highly ordered ionic diffusion pathways, thus enabling dendrite-free Li deposition. With a considerable Li+ transference number of 0.57, ZIF-67-Cu@Li symmetric cells deliver a superior long-term performance (over 1000 h), and Li-O2 full batteries with ZIF-67-Cu@Li electrodes display a high energy density of 1911.61 W h kg-1.Emerging studies have shown that lipid metabolism plays an important role in aging. High resolution in situ imaging of lipid metabolic dynamics inside cells and tissues affords a novel and potent approach for understanding many biological processes such as aging. Here we established a new optical imaging platform that combines D2O-probed stimulated Raman scattering (DO-SRS) imaging microscopy and a Drosophila model to directly visualize metabolic activities in situ during aging. The sub-cellular spatial distribution of de novo lipogenesis in the fat body was quantitatively imaged and examined. We discovered a dramatic decrease in lipid turnover in 35-day-old flies. Decreases in protein turnover occurred earlier than lipids (25-day vs. 35-day), and there are many proteins localized on the cell and lipid droplet membrane. This suggests that protein metabolism may act as a prerequisite for lipid metabolism during aging. This alteration of maintenance of protein turnover indicates disrupted lipid metabolism. We further found a significantly higher lipid turnover rate in large LDs, indicating more active metabolism in large LDs, suggesting that large and small LDs play different roles in metabolism to maintain cellular homeostasis.
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