Rapid gram-scale microwave-assisted synthesis of organic anodes for sodium-ion batteries with environmental impact assessment.

Development of sustainable synthesis methods of organic electrode materials (OEMs) for sodium (Na)-ion batteries must take hold rapidly in large scale-synthesis if subsequent commercialisation is to occur. We report a facile and rapid gram-scale synthesis method based on microwave irradiation for disodium naphthalene-2,6-dicarboxylate (Na-NDC) and mono/disodium benzene-1,4-dicarboxylate (Na-BDC) as model compounds. Phase purity and formation of materials was confirmed by various characterisation techniques.

Does remission of type 2 diabetes matter? A qualitative study of healthcare professionals' perspectives and views about supporting remission in primary care.

Background: Trials conducted in highly selected populations have shown that type 2 diabetes (T2D) remission is possible, but the feasibility and acceptability of supporting remission in routine clinical practice remain uncertain.

Aim: We explored primary care professionals' perceptions and understandings of T2D remission and their views about supporting remission within routine clinical care.

Methods: Semi-structured interviews were conducted with 14 GPs and nine nurses working in Scottish general practices.

Kinetics of sulfur-transfer from titanocene (poly)sulfides to sulfenyl chlorides: rapid metal-assisted concerted substitution.

The kinetics of sulfur transfer from titanocene (poly)sulfides (CpTiS, CpTiSCMe, CpTi(SAr), CpTiCl(SAr)) to sulfenyl chlorides (SCl, RSCl) have been investigated by a combination of stopped-flow UV-Vis/NMR reaction monitoring, titration assays, numerical kinetic modelling and KS-DFT calculations. The reactions are rapid, proceeding to completion over timescales of milliseconds to minutes, a sequence of two S-S bond-forming steps ( , ). The archetypical polysulfides CpTiS (1a) and CpTiSC(Me) (2a) react with disulfur dichloride (SCl) through rate-limiting intermolecular S-S bond formation ( ) followed by a rapid intramolecular cyclization ( , with ≫ [RSCl]).

Rapid preparation of binary mixtures of sodium carboxylates as anodes in sodium-ion batteries.

Sodium-ion batteries are emerging as a sustainable solution to tackle the growing global energy demands. In this context, organic electrode materials complement such technologies as they are composed of earth-abundant elements. As organic anodes, sodium carboxylates exhibit promising applicability in a wide range of molecules.

Speciation and kinetics of fluoride transfer from tetra--butylammonium difluorotriphenylsilicate ('TBAT').

Tetra--butylammonium difluorotriphenylsilicate (TBAT) is a conveniently handled anhydrous fluoride source, commonly used as a surrogate for tetra--butylammonium fluoride (TBAF). While prior studies indicate that TBAT reacts rapidly with fluoride acceptors, little is known about the mechanism(s) of fluoride transfer. We report on the interrogation of the kinetics of three processes in which fluoride is transferred from TBAT, in THF and in MeCN, using a variety of NMR methods, including chemical exchange saturation transfer, magnetisation transfer, diffusion analysis, and 1D NOESY.

Site-directed cation ordering in chabazite-type AlGaPO-34 frameworks revealed by NMR crystallography.

We report the first synthesis of the mixed-metal chabazite-type AlGaPO-34(mim) solid solution, containing 1-methylimidazolium, mim, as structure directing agent (SDA), from the parent mixed-metal oxide solid solution, γ-(AlGa)O. This hitherto unreported family of materials exhibits complex disorder, arising from the possible distributions of cations over available sites, the orientation of the SDA and the presence of variable amounts of water, which provides a prototype for understanding structural subtleties in nanoporous materials. In the as-made forms of the phosphate frameworks, there are three crystallographically distinct metal sites: two tetrahedral MO and one octahedral MOF (M = Al, Ga).

Manganese catalysed dehydrogenative synthesis of polyureas from diformamide and diamines.

We report here the synthesis of polyureas from the dehydrogenative coupling of diamines and diformamides. The reaction is catalysed by a manganese pincer complex and releases H gas as the only by-product making the process atom-economic and sustainable. The reported method is greener in comparison to the current state-of-the-art production routes that involve diisocyanate and phosgene feedstock.

Rate and equilibrium constants for the addition of triazolium salt derived N-heterocyclic carbenes to heteroaromatic aldehydes.

Heteroaromatic aldehydes are often used preferentially or exclusively in a range of NHC-catalysed processes that proceed through the generation of a reactive diaminoenol or Breslow Intermediate (BI), with the reason for their unique reactivity currently underexplored. This manuscript reports measurement of rate and equilibrium constants for the reaction between -aryl triazolium NHCs and heteroaromatic aldehydes, providing insight into the effect of the NHC and heteroaromatic aldehyde structure up to formation of the BI. Variation in NHC catalyst and heteroaromatic aldehyde structure markedly affect the observed kinetic parameters of adduct formation, decay to starting materials and onward reaction to BI.

Exploring Helical Peptides and Foldamers for the Design of Metal Helix Frameworks: Current Trends and Future Perspectives.

Flexible and biocompatible metal peptide frameworks (MPFs) derived from short and ultra-short peptides have been explored for the storage of greenhouse gases, molecular recognition, and chiral transformations. In addition to short flexible peptides, peptides with specifically folded conformations have recently been utilized to fabricate a variety of metal helix frameworks (MHFs). The secondary structures of the peptides govern the structure-assembly relationship and thereby control the formation of three-dimensional (3D)-MHFs.

The lipidome of and its plasticity.

belongs to the trypanosomatidae order of protozoan parasites, bearing close relation to other kinetoplastid parasites such as and As an early diverging lineage of eukaryotes, the study of kinetoplastid parasites has provided unique insights into alternative mechanisms to traditional eukaryotic metabolic pathways. are a monogenetic parasite for mosquito species and have two distinct lifecycle stages both taking place in the mosquito gut. These consist of a motile choanomastigote form and an immotile amastigote form morphologically similar to amastigotes in .

flow pair distribution function analysis to probe the assembly-disassembly-organisation-reassembly (ADOR) mechanism of zeolite IPC-2 synthesis.

The assembly-disassembly-organisation-reassembly (ADOR) process is an important tool to access zeolite structures that are otherwise unfeasible hydrothermal methods. flow pair distribution function (PDF) analysis has been used to probe the mechanism of the disassembly and organisation steps, with the disassembly a rapid step that is often difficult to capture. Zeolite UTL was hydrolysed by 6 M hydrochloric acid, with PDF measurements used to monitor framework alterations as the reaction proceeded.

Benchmark Test and Guidelines for DEER/PELDOR Experiments on Nitroxide-Labeled Biomolecules.

Distance distribution information obtained by pulsed dipolar EPR spectroscopy provides an important contribution to many studies in structural biology. Increasingly, such information is used in integrative structural modeling, where it delivers unique restraints on the width of conformational ensembles. In order to ensure reliability of the structural models and of biological conclusions, we herein define quality standards for sample preparation and characterization, for measurements of distributed dipole-dipole couplings between paramagnetic labels, for conversion of the primary time-domain data into distance distributions, for interpreting these distributions, and for reporting results.

How Good is the Science That Informs Government Policy? A Lesson From the U.K.'s Response to 2020 CoV-2 Outbreak.

In an era when public faith in politicians is dwindling, yet trust in scientists remains relatively high, governments are increasingly emphasizing the role of science based policy-making in response to challenges such as climate change and global pandemics. In this paper we question the quality of some scientific advice given to governments and the robustness and transparency of the entire framework which envelopes such advice, all of which raise serious ethical concerns. In particular we focus on the so-called Imperial Model which heavily influenced the government of the United Kingdom in devising its response to the COVID-19 crisis.

Can we achieve better recruitment by providing better information? Meta-analysis of 'studies within a trial' (SWATs) of optimised participant information sheets.

Background: The information given to people considering taking part in a trial needs to be easy to understand if those people are to become, and then remain, trial participants. However, there is a tension between providing comprehensive information and providing information that is comprehensible. User-testing is one method of developing better participant information, and there is evidence that user-tested information is better at informing participants about key issues relating to trials.

Supramolecular packing of alkyl substituted Janus face all- 2,3,4,5,6-pentafluorocyclohexyl motifs.

This study uses X-ray crystallography, theory and Langmuir isotherm analysis to explore the conformations and molecular packing of alkyl all- 2,3,4,5,6-pentafluorocyclohexyl motifs, which are prepared by direct aryl hydrogenations from alkyl- or vinyl-pentafluoroaryl benzenes. Favoured conformations retain the more polar triaxial C-F bond arrangement of the all- 2,3,4,5,6-pentafluorocyclohexyl ring systems with the alkyl substituent adopting an equatorial orientation, and accommodating strong supramolecular interactions between rings. Langmuir isotherm analysis on a water subphase of a long chain fatty acid and alcohol carrying terminal all- 2,3,4,5,6-pentafluorocyclohexyl rings do not show any indication of monolayer assembly relative to their cyclohexane analogues, instead the molecules appear to aggregate and form higher molecular assemblies prior to compression.

Reverse ADOR: reconstruction of UTL zeolite from layered IPC-1P.

The assembly-disassembly-organisation-reassembly (ADOR) process has led to the discovery of numerous zeolite structures, albeit limited to materials with decreased pore size in relation to the parent germanosilicate zeolite. This limitation stems from the rapid decrease in -spacing upon hydrolysis (disassembly). Nevertheless, we have artificially increased the -spacing of layered IPC-1P by intercalating organic species.

Single-step synthesis and interface tuning of core-shell metal-organic framework nanoparticles.

Control over the spatial distribution of components in metal-organic frameworks has potential to unlock improved performance and new behaviour in separations, sensing and catalysis. We report an unprecedented single-step synthesis of multi-component metal-organic framework (MOF) nanoparticles based on the canonical ZIF-8 (Zn) system and its Cd analogue, which form with a core-shell structure whose internal interface can be systematically tuned. We use scanning transmission electron microscopy, X-ray energy dispersive spectroscopy and a new composition gradient model to fit high-resolution X-ray diffraction data to show how core-shell composition and interface characteristics are intricately controlled by synthesis temperature and reaction composition.

A general model to optimise Cu labelling efficiency of double-histidine motifs for pulse dipolar EPR applications.

Electron paramagnetic resonance (EPR) distance measurements are making increasingly important contributions to studies of biomolecules underpinning health and disease by providing highly accurate and precise geometric constraints. Combining double-histidine (dH) motifs with CuII spin labels shows promise for further increasing the precision of distance measurements, and for investigating subtle conformational changes. However, non-covalent coordination-based spin labelling is vulnerable to low binding affinity.

Isolation of 5'--sulfamyladenosine and related 3'--β-glucosylated adenosines from the nucleocidin producer .

The isolation of three adenosine based metabolites 6-8 from is reported. The metabolites are structurally related to the fluorine containing antibiotic nucleocidin 1 and two recently identified glycosylated fluoroadenosines 2 and 3, however in this case the three metabolites do not contain a fluorine, suggesting that the biosynthetic enzymes to the fluorometabolites also process their non-fluorinated counterparts.

Design of cross-linked polyisobutylene matrix for efficient encapsulation of quantum dots.

Photoluminescent quantum dots (QDs) are a prominent example of nanomaterials used in practical applications, especially in light-emitting and light-converting devices. Most of the current applications of QDs require formation of thin films or their incorporation in solid matrices. The choice of an appropriate host material capable of preventing QDs from degradation and developing a process of uniform incorporation of QDs in the matrix have become essential scientific and technological challenges.

Association of alcohol control policies with adolescent alcohol consumption and with social inequality in adolescent alcohol consumption: A multilevel study in 33 countries and regions.

Background Previous research found inconsistent associations between alcohol control policies and socioeconomic inequality with adolescent drinking outcomes. This study expands the focus beyond individual associations to examine whether a combination of policies is related to socioeconomic inequality in adolescent drinking outcomes and whether this relationship varies across survey years. Methods Multilevel modelling of 4 waves of repeat cross-sectional survey data (2001/02, 2005/06, 2009/10, and 2013/14) from the Health Behaviour in School-aged Children (HBSC) study was carried out.

Conversion of a microwave synthesized alkali-metal MOF to a carbonaceous anode for Li-ion batteries.

Hierarchical carbon-rich materials have shown immense potential for various electrochemical applications. Metal-organic frameworks (MOFs) are well suited precursors for obtaining such templated carbon matrices. Usually these conversions are carried out by energy intensive processes and lead to the presence of toxic transition metal residues.

Carbon Nanomembranes from Aromatic Carboxylate Precursors.

Self-assembled monolayers (SAMs) serve as convenient platform for fabricating carbon nanomembranes (CNMs) of extended lateral dimensions. Highly porous CNMs are emerging as interesting materials for membrane technologies as they exhibit selectivity for water permeation and, owing to their reduced dimensionality, promise increased energy efficiency compared to established systems. In the present study terphenylcarboxylate SAMs, prepared on silver underpotential deposited on Au and irradiated by 100 eV electrons, were successfully converted into free-standing CNMs.

Tandem sequential catalytic enantioselective synthesis of highly-functionalised tetrahydroindolizine derivatives.

An isothiourea-catalysed enantioselective synthesis of novel tetrahydroindolizine derivatives is reported through a one-pot tandem sequential process. The application of 2-(pyrrol-1-yl)acetic acid in combination with either a trifluoromethyl enone or an α-keto-β,γ-unsaturated ester in an enantioselective Michael addition-lactonisation process, followed by ring-opening and cyclisation, led to a range of 24 tetrahydroindolizine derivatives containing three stereocentres in up to >95 : 5 dr and >99 : 1 er.