Machine-learned modeling of PM exposures in rural Lao PDR.

This study presents a machine-learning-enhanced method of modeling PM personal exposures in a data-scarce, rural, solid fuel use context. Data collected during a cookstove (Africa Clean Energy (ACE)-1 solar-battery-powered stove) intervention program in rural Lao PDR are presented and leveraged to explore advanced techniques for predicting personal exposures to particulate matter with aerodynamic diameter smaller than 2.5 μm (PM).

Advanced Spectroelectrochemical Techniques to Study Electrode Interfaces Within Lithium-Ion and Lithium-Oxygen Batteries.

Lithium battery technologies have revolutionized mobile energy storage, but improvements in the technology are still needed. Critical to delivering new light weight, high capacity, safe devices is an improved understanding of the dynamic processes occurring at the electrode-electrolyte interfaces. Therefore, alongside advances in materials there has been a parallel progression in advanced characterization methods.

The Role of Cation-Vacancies for the Electronic and Optical Properties of Aluminosilicate Imogolite Nanotubes: A Non-local, Linear-Response TDDFT Study.

We report a combined non-local (PBE-TC-LRC) Density Functional Theory (DFT) and linear-response time-dependent DFT (LR-TDDFT) study of the structural, electronic, and optical properties of the cation-vacancy based defects in aluminosilicate (AlSi) imogolite nanotubes (Imo-NTs) that have been recently proposed on the basis of Nuclear Magnetic Resonance (NMR) experiments. Following numerical determination of the smallest AlSi Imo-NT model capable of accommodating the defect-induced relaxation with negligible finite-size errors, we analyse the defect-induced structural deformations in the NTs and ensuing changes in the NTs' electronic structure. The NMR-derived defects are found to introduce both shallow and deep occupied states in the pristine NTs' band gap (BG).

Identification of different carbenium ion intermediates in zeolites with identical chabazite topology C-C through-bond NMR correlations.

C-C through-bond NMR correlation experiments reveal the stabilization of different carbenium ion intermediates in two zeolites possessing identical CHA topology (H-SAPO-34 and H-SSZ-13) during the methanol to olefins reaction.

Oxygen reactions on Pt{} in a non-aqueous Na electrolyte: site selective stabilisation of a sodium peroxy species.

Sodium-oxygen battery cathodes utilise the reversible redox species of oxygen in the presence of sodium ions. However, the oxygen reduction and evolution reaction mechanism is yet to be conclusively determined. In order to examine the part played by surface structure in sodium-oxygen electrochemistry for the development of catalytic materials and structures, a method of preparing clean, well-defined Pt electrode surfaces for adsorption studies in aprotic solvents is described.

Stabilization of O-O Bonds by d Cations in LiNiWO (0 ≤ x ≤ 0.25) Rock Salt Oxides as the Origin of Large Voltage Hysteresis.

Multinary lithium oxides with the rock salt structure are of technological importance as cathode materials in rechargeable lithium ion batteries. Current state-of-the-art cathodes such as LiNiMnCoO rely on redox cycling of earth-abundant transition-metal cations to provide charge capacity. Recently, the possibility of using the oxide anion as a redox center in Li-rich rock salt oxides has been established as a new paradigm in the design of cathode materials with enhanced capacities (>200 mAh/g).

Synthesis and Characterization of Renewable Polyester Coil Coatings from Biomass-Derived Isosorbide, FDCA, 1,5-Pentanediol, Succinic Acid, and 1,3-Propanediol.

Biomass-derived polyester coatings for coil applications have been successfully developed and characterized. The coatings were constituted by carbohydrate-derived monomers, namely 2,5-furan dicarboxylic acid, isosorbide, succinic acid, 1,3-propanediol, and 1,5-pentanediol, the latter having previously been used as a plasticizer rather than a structural building unit. The effect of isosorbide on the coatings is widely studied.

Synthesis, Characterization and Adsorptive Performances of a Composite Material Based on Carbon and Iron Oxide Particles.

The aim of this paper was to produce a new composite material based on carbon and iron oxides, starting from soluble starch and ferric chloride. The composite material was synthesized by simple thermal decomposition of a reaction mass obtained from starch and iron chloride, in an inert atmosphere. Starch used as a carbon source also efficiently stabilizes the iron oxides particles obtained during the thermal decomposition.

In situ study of the low overpotential "dimer pathway" for electrocatalytic carbon dioxide reduction by manganese carbonyl complexes.

The electrocatalytic reduction of CO2 using [fac-Mn(bpy)(CO)3Br] (bpy = 2,2'-bipyridine) and its derivatives has been the subject of numerous recent studies. However the mechanisms of catalysis are still debated. Here we carry out in situ vibrational sum-frequency generation (VSFG) spectroelectrochemistry to examine how this catalyst behaves at an electrode surface.

Nanocontainer-based self-healing coatings: current progress and future perspectives.

Here, we summarize the recent achievements in the field of the nanocontainer-based self-healing coatings made during the last 8 years. The development of nanocontainer-based self-healing coatings was started 15 years ago from the study of nanocontainers with stimuli-responsive release properties able to release anticorrosion agent (inhibitor) on demand only into a corroded area thus preventing its spontaneous leakage. Since then, many different types of nanocontainers have been demonstrated: from polymer capsules to porous inorganic nanoparticles with sophisticated mechanisms of release triggering.

Nanocontainer-Based Active Systems: From Self-Healing Coatings to Thermal Energy Storage.

We highlight the development of nanocontainer-based active materials started in 2006 at the Max Planck Institute of Colloids and Interfaces under the supervision of Prof. Helmuth Möhwald. The active materials encapsulated in the nanocontainers with controlled shell permeability have been first applied for self-healing coatings with controlled release of the corrosion inhibitor.

Mussel-Inspired Self-Healing Coatings Based on Polydopamine-Coated Nanocontainers for Corrosion Protection.

The mussel-inspired properties of dopamine have attracted immense scientific interest for surface modification of nanoparticles due to the high potential of dopamine functional groups to increase the adhesion of nanoparticles to flat surfaces. Here, we report for the first time a novel type of inhibitor-loaded nanocontainer using polydopamine (PDA) as a pH-sensitive gatekeeper for mesoporous silica nanoparticles (MSNs). The encapsulated inhibitor (benzotriazole) was loaded into MSNs at neutral pH, demonstrating fast release in an acidic environment.

Energy communities in the transition to a low-carbon future: A taxonomical approach and some policy dilemmas.

In calls for transition to a society in which energy production is based on renewable sources, a fundamental role is increasingly assigned to so-called 'energy communities'. The term 'energy communities' is, however, used to denote a range of different circumstances thus risking overly simplifying the phenomenon. The intention of this article is to discuss what these communities really are or could be.

Evaluating chemical bonding in dioxides for the development of metal-oxygen batteries: vibrational spectroscopic trends of dioxygenyls, dioxygen, superoxides and peroxides.

Dioxides (dioxygenyl (O2+), dioxygen (O2), superoxide (O2˙-) and peroxide (O22-)) are of immense biological, chemical and environmental importance. The ability to accurately detect and measure the changing strength of their chemical bonding and coordination in situ or operando is extremely beneficial in order to evaluate their chemical properties, this has been particularly important recently in the field of metal-oxygen batteries, where understanding the reactivity of the O2˙- intermediate is crucial in the development of more stable electrolytes. Meta-analysis of the collated vibrational Raman and IR spectral bands of numerous (>200) dioxygen species was used to interpret the effect that the immediate chemical environment has on the O-O bond.

Fast detection and structural identification of carbocations on zeolites by dynamic nuclear polarization enhanced solid-state NMR.

Acidic zeolites are porous aluminosilicates used in a wide range of industrial processes such as adsorption and catalysis. The formation of carbocation intermediates plays a key role in reactivity, selectivity and deactivation in heterogeneous catalytic processes. However, the observation and determination of carbocations remain a significant challenge in heterogeneous catalysis due to the lack of selective techniques of sufficient sensitivity to detect their low concentrations.

Wet-Chemical Synthesis of Surface-Passivated Halide Perovskite Microwires for Improved Optoelectronic Performance and Stability.

One-dimensional (1D) halide perovskite materials with intrinsic high carrier mobility and long diffusion length hold great promises for high-performance optoelectronic devices, in which the passivation of the surface defects is of significance for further boosting its optoelectronic performance as well as its moisture stability. Herein, we demonstrate a simple room-temperature wet-chemical synthetic protocol for perovskite microwires with controlled morphologies and passivated surface states. This strategy allows for facile assembly of hydrophobic 1 H,1 H-perfluorooctylamine (PFA) molecules on the surface of the perovskite microwires owing to the coordination binding between the amino groups of PFA and Pb.

Understanding structure-activity relationships in linear polymer photocatalysts for hydrogen evolution.

Conjugated polymers have sparked much interest as photocatalysts for hydrogen production. However, beyond basic considerations such as spectral absorption, the factors that dictate their photocatalytic activity are poorly understood. Here we investigate a series of linear conjugated polymers with external quantum efficiencies for hydrogen production between 0.

Publisher Correction: Liquid phase blending of metal-organic frameworks.

The original version of this Article contained an error in Figure 1b, where the blue '(ZIF-4-Zn) (ZIF-62) blend' data curve was omitted from the enthalpy response plot. This has now been corrected in both the PDF and HTML versions of the Article.

Acyclic and Cyclic Alkyl and Ether-Functionalised Sulfonium Ionic Liquids Based on the [TFSI] and [FSI] Anions as Potential Electrolytes for Electrochemical Applications.

This work provides a study based on acyclic and cyclic sulfonium ionic liquids (ILs) with alkyl and ether-functionality on the cation paired with the bis{(trifluoromethyl)sulfonyl}imide, [TFSI] , or the bis(fluorosulfonyl)imide, [FSI] , as the counter anion. Herein, thermophysical characterisation of nine sulfonium-based ILs concerning the density, viscosity and conductivity and thermal properties including phase transition behaviour and decomposition temperature is reported. The electrochemical stability of the ILs was also measured by cyclic voltammetry at a glassy carbon macro-disk electrode.

Size-controlled electron transfer rates determine hydrogen generation efficiency in colloidal Pt-decorated CdS quantum dots.

Semiconducting quantum dots (QDs) have been considered as promising building blocks of solar energy harvesting systems because of size-dependent electronic structures, e.g. QD-metal heterostructures for solar-driven H2 production.

Highly efficient removal of ammonia nitrogen from wastewater by dielectrophoresis-enhanced adsorption.

A new approach, based on dielectrophoresis (DEP), was developed in this work to enhance traditional adsorption for the removal of ammonia nitrogen (NH-N) from wastewater. The factors that affected the removal efficiency were systematically investigated, which allowed us to determine optimal operation parameters. With this new method we found that the removal efficiency was significantly improved from 66.

Liquid phase blending of metal-organic frameworks.

The liquid and glass states of metal-organic frameworks (MOFs) have recently become of interest due to the potential for liquid-phase separations and ion transport, alongside the fundamental nature of the latter as a new, fourth category of melt-quenched glass. Here we show that the MOF liquid state can be blended with another MOF component, resulting in a domain structured MOF glass with a single, tailorable glass transition. Intra-domain connectivity and short range order is confirmed by nuclear magnetic resonance spectroscopy and pair distribution function measurements.

Structural resolution of inorganic nanotubes with complex stoichiometry.

Determination of the atomic structure of inorganic single-walled nanotubes with complex stoichiometry remains elusive due to the too many atomic coordinates to be fitted with respect to X-ray diffractograms inherently exhibiting rather broad features. Here we introduce a methodology to reduce the number of fitted variables and enable resolution of the atomic structure for inorganic nanotubes with complex stoichiometry. We apply it to recently synthesized methylated aluminosilicate and aluminogermanate imogolite nanotubes of nominal composition (OH)AlOSi(Ge)CH.

Near-Ideal Xylene Selectivity in Adaptive Molecular Pillar[ n]arene Crystals.

The energy-efficient separation of alkylaromatic compounds is a major industrial sustainability challenge. The use of selectively porous extended frameworks, such as zeolites or metal-organic frameworks, is one solution to this problem. Here, we studied a flexible molecular material, perethylated pillar[ n]arene crystals ( n = 5, 6), which can be used to separate C8 alkylaromatic compounds.