Carbon capture and storage (CCS) is broadly recognised as having the potential to play a key role in meeting climate change targets, delivering low carbon heat and power, decarbonising industry and, more recently, its ability to facilitate the net removal of CO2 from the atmosphere. However, despite this broad consensus and its technical maturity, CCS has not yet been deployed on a scale commensurate with the ambitions articulated a decade ago. Thus, in this paper we review the current state-of-the-art of CO2 capture, transport, utilisation and storage from a multi-scale perspective, moving from the global to molecular scales. In light of the COP21 commitments to limit warming to less than 2 °C, we extend the remit of this study to include the key negative emissions technologies (NETs) of bioenergy with CCS (BECCS), and direct air capture (DAC). Cognisant of the non-technical barriers to deploying CCS, we reflect on recent experience from the UK's CCS commercialisation programme and consider the commercial and political barriers to the large-scale deployment of CCS. In all areas, we focus on identifying and clearly articulating the key research challenges that could usefully be addressed in the coming decade.

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Carbon capture and storage (CCS): the way forward

Structure and nanostructure in ionic liquids.

: The unpolarized absorption and circular dichroism spectra of the fundamental vibrational transitions of the chiral molecule, 4-methyl-2-oxetanone, are calculated ab initio. Harmonic force fields are obtained using Density Functional Theory (DFT), MP2, and SCF methodologies and a 5S4P2D/3S2P (TZ2P) basis set. DFT calculations use the Local Spin Density Approximation (LSDA), BLYP, and Becke3LYP (B3LYP) density functionals. Mid-IR spectra predicted using LSDA, BLYP, and B3LYP force fields are of significantly different quality, the B3LYP force field yielding spectra in clearly superior, and overall excellent, agreement with experiment. The MP2 force field yields spectra in slightly worse agreement with experiment than the B3LYP force field. The SCF force field yields spectra in poor agreement with experiment.The basis set dependence of B3LYP force fields is also explored: the 6-31G* and TZ2P basis sets give very similar results while the 3-21G basis set yields spectra in substantially worse agreements with experiment. jg

Ab initio calculation of vibrational absorption and circular dichroism spectra using density functional force fields

https://pubs.rsc.org/en/Content/ArticlePDF/2013/GC/C2GC36364J

Deconstruction of lignocellulosic biomass with ionic liquids

Until recently, “room-temperature” (<100–150 °C) liquid-state electrochemistry was mostly electrochemistry of diluted electrolytes(1)–(4) where dissolved salt ions were surrounded by a considerable amount of solvent molecules. Highly concentrated liquid electrolytes were mostly considered in the narrow (albeit important) niche of high-temperature electrochemistry of molten inorganic salts(5-9) and in the even narrower niche of “first-generation” room temperature ionic liquids, RTILs (such as chloro-aluminates and alkylammonium nitrates).(10-14) The situation has changed dramatically in the 2000s after the discovery of new moisture- and temperature-stable RTILs.(15, 16) These days, the “later generation” RTILs attracted wide attention within the electrochemical community.(17-31) Indeed, RTILs, as a class of compounds, possess a unique combination of properties (high charge density, electrochemical stability, low/negligible volatility, tunable polarity, etc.) that make them very attractive substances from fundamental and application points of view.(32-38) Most importantly, they can mix with each other in “cocktails” of one’s choice to acquire the desired properties (e.g., wider temperature range of the liquid phase(39, 40)) and can serve as almost “universal” solvents.(37, 41, 42) It is worth noting here one of the advantages of RTILs as compared to their high-temperature molten salt (HTMS)(43) “sister-systems”.(44) In RTILs the dissolved molecules are not imbedded in a harsh high temperature environment which could be destructive for many classes of fragile (organic) molecules.

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Ionic Liquids at Electrified Interfaces

Simple ionic liquids have long been held to be designer solvents, based upon the ability to independently vary their cations and anions. The formation of mixtures of ionic liquids increases this synthetic flexibility. We review the available literature of these ionic liquid mixtures to identify how their properties change and the possibility for their application.

/pdf/mixtures-of-ionic-liquids-1nyvyn3p46.pdf

Mixtures of ionic liquids.

The polarities of a wide range of ionic liquids have been determined using the Kamlet–Taft empirical polarity scales α, β and π*, with the dye set Reichardt's Dye, N,N-diethyl-4-nitroaniline and 4-nitroaniline. These have been compared to measurements of these parameters with different dye sets and to different polarity scales. The results emphasise the importance of recognising the role that the nature of the solute plays in determining these scales. It is particularly noted that polarity scales based upon charged solutes can give very different values for the polarity of ionic liquids compared to those based upon neutral probes. Finally, the effects of commonplace impurities in ionic liquids are reported.

/pdf/understanding-the-polarity-of-ionic-liquids-a5oep12tzz.pdf

Understanding the polarity of ionic liquids

https://spiral.imperial.ac.uk/bitstream/10044/1/9955/4/Welton%2c%20T%20-%20Self%20assembly%20in%20the%20electrical.pdf

Self-assembly in the electrical double layer of ionic liquids

Solvents and solutions are ubiquitous in chemistry. For instance, in synthesis the solvent allows reagents to mix intimately so that reactions between these may occur. Consequently, understanding how solutes behave in solutions has been one of the major themes of chemistry throughout its history. Ionic liquids (liquid salts) are an exciting recent addition to the range of available solvents. Here we show that these solvents interact with dissolved salts to give solutions that are completely different from those of salts in either traditional organic solvents or water. Observations of these ideal salt solutions will require new models of solvation and polarity and have the potential to lead to new chemical processes.

Salts dissolved in salts: ionic liquid mixtures

Ionic liquids have earned the reputation of being ‘designer solvents’ due to the wide range of accessible properties and the degree of fine-tuning afforded by varying the constituent ions. Mixtures of ionic liquids offer the opportunity for further fine-tuning of properties. A broad selection of common ionic liquid cations and anions are employed to create a sample of binary and reciprocal binary ionic liquid mixtures, which are analysed and described in this paper. Physical properties such as the conductivity, viscosity, density and phase behaviour (glass transition temperatures) are examined. In addition, thermal stabilities of the mixtures are evaluated. The physical properties examined for these formulations are found to generally adhere remarkably closely to ideal mixing laws, with a few consistent exceptions, allowing for the facile prediction and control of properties of ionic liquid mixtures.

/pdf/a-physicochemical-investigation-of-ionic-liquid-mixtures-clxgzx9doo.pdf

Heiko Niedermeyer

Papers

Mixtures of ionic liquids.

Understanding the polarity of ionic liquids

Self-assembly in the electrical double layer of ionic liquids

Salts dissolved in salts: ionic liquid mixtures

A physicochemical investigation of ionic liquid mixtures