Tetrameric self-assembling of water-lean solvents enables carbamate anhydride-based CO capture chemistry.

Carbon capture, utilization and storage is a key yet cost-intensive technology for the fight against climate change. Single-component water-lean solvents have emerged as promising materials for post-combustion CO capture, but little is known regarding their mechanism of action. Here we present a combined experimental and modelling study of single-component water-lean solvents, and we find that CO capture is accompanied by the self-assembly of reverse-micelle-like tetrameric clusters in solution.

Oxide- and Silicate-Water Interfaces and Their Roles in Technology and the Environment.

Interfacial reactions drive all elemental cycling on Earth and play pivotal roles in human activities such as agriculture, water purification, energy production and storage, environmental contaminant remediation, and nuclear waste repository management. The onset of the 21st century marked the beginning of a more detailed understanding of mineral aqueous interfaces enabled by advances in techniques that use tunable high-flux focused ultrafast laser and X-ray sources to provide near-atomic measurement resolution, as well as by nanofabrication approaches that enable transmission electron microscopy in a liquid cell. This leap into atomic- and nanometer-scale measurements has uncovered scale-dependent phenomena whose reaction thermodynamics, kinetics, and pathways deviate from previous observations made on larger systems.

Soft nanoconfinement of ionic liquids in lyotropic liquid crystals.

Nanoconfinement of ionic liquids (ILs) influences their physicochemical properties. In this study, we investigate the effect of soft nanoconfinement imposed by lyotropic liquid crystals (LLCs) on ILs. The LLC ion gels are obtained through self-assembly of a short chain block copolymer (BCP) of polyethylene--poly(ethylene oxide), PE--PEO, in ILs.

Subtle changes in hydrogen bond orientation result in glassification of carbon capture solvents.

Water-lean CO capture solvents show promise for more efficient and cost-effective CO capture, although their long-term behavior in operation has yet to be well studied. New observations of extended structure solvent behavior show that some solvent formulations transform into a glass-like phase upon aging at operating temperatures after contact with CO. The glassification of a solvent would be detrimental to a carbon-capture process due to plugging of infrastructure, introducing a critical need to decipher the underlying principles of this phenomenon to prevent it from happening.

Formation of ion gels by polymerization of block copolymer/ionic liquid/oil mesophases.

In this study, we introduce a new method of developing ion gels through polymerization of lyotropic liquid crystal (LLC) templates of monomer (styrene), cross-linker (divinylbenzene), ionic liquid (1-ethyl-3-methylimidazolium tetrafluoroborate), and amphiphilic block copolymers (Pluronic F127). The polymerization of the oil phase boosts the mechanical properties of the ion-conducting electrolytes. We discuss the effect of tortuosity induced by crystalline domains and LLC structure on the conductivity of ion gels.

Fate of Liposomes in the Presence of Phospholipase C and D: From Atomic to Supramolecular Lipid Arrangement.

Understanding the origins of lipid membrane bilayer rearrangement in response to external stimuli is an essential component of cell biology and the bottom-up design of liposomes for biomedical applications. The enzymes phospholipase C and D (PLC and PLD) both cleave the phosphorus-oxygen bonds of phosphate esters in phosphatidylcholine (PC) lipids. The atomic position of this hydrolysis reaction has huge implications for the stability of PC-containing self-assembled structures, such as the cell wall and lipid-based vesicle drug delivery vectors.

Toward understanding the structural heterogeneity and ion pair stability in dicationic ionic liquids.

The structural and dynamical properties of dicationic ionic liquids (DILs) [Cn(mim)2](Tf2N)2, that is, 3-methylimidazolium dications separated by an alkyl chain and with bis(trifluoromethylsulfonyl)amide as the anion, were investigated by molecular dynamics (MD) simulation in combination with small/wide-angle X-ray scattering (SWAXS) measurements. Enhanced spatial heterogeneity is observed as the DIL chain length is increased, characterized by the changes in the scattering and the increased heterogeneity order parameter (HOP). Temperature variation imposes only slight influences on the local structures of DILs compared to monocationic ionic liquids (MILs).

Pore-size-dependent calcium carbonate precipitation controlled by surface chemistry.

Induced mineral precipitation is potentially important for the remediation of contaminants, such as during mineral trapping during carbon or toxic metal sequestration. The prediction of precipitation reactions is complicated by the porous nature of rocks and soils and their interaction with the precipitate, introducing transport and confinement effects. Here X-ray scattering measurements, modeling, and electron microscopies were used to measure the kinetics of calcium carbonate precipitation in a porous amorphous silica (CPG) that contained two discrete distributions of pore sizes: nanopores and macropores.

High-pressure cell for neutron reflectometry of supercritical and subcritical fluids at solid interfaces.

A new high-pressure cell design for use in neutron reflectometry (NR) for pressures up to 50 MPa and a temperature range of 300-473 K is described. The cell design guides the neutron beam through the working crystal without passing through additional windows or the bulk fluid, which provides for a high neutron transmission, low scattering background, and low beam distortion. The o-ring seal is suitable for a wide range of subcritical and supercritical fluids and ensures high chemical and pressure stability.