There is, I think, something ethereal about i —the square root of minus one. I remember first hearing about it at school. It seemed an odd beast at that time—an intruder hovering on the edge of reality.

Usually familiarity dulls this sense of the bizarre, but in the case of i it was the reverse: over the years the sense of its surreal nature intensified. It seemed that it was impossible to write mathematics that described the real world in …

I and i

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

In recent years, Carbon Capture and Storage (Sequestration) (CCS) has been proposed as a potential method to allow the continued use of fossil-fuelled power stations whilst preventing emissions of CO2 from reaching the atmosphere. Gas, coal (and biomass)-fired power stations can respond to changes in demand more readily than many other sources of electricity production, hence the importance of retaining them as an option in the energy mix. Here, we review the leading CO2 capture technologies, available in the short and long term, and their technological maturity, before discussing CO2 transport and storage. Current pilot plants and demonstrations are highlighted, as is the importance of optimising the CCS system as a whole. Other topics briefly discussed include the viability of both the capture of CO2 from the air and CO2 reutilisation as climate change mitigation strategies. Finally, we discuss the economic and legal aspects of CCS.

Carbon capture and storage update

Structure and nanostructure in ionic liquids.

Ionic liquids offer a unique suite of properties that make them important candidates for a number of energy related applications. Cation–anion combinations that exhibit low volatility coupled with high electrochemical and thermal stability, as well as ionic conductivity, create the possibility of designing ideal electrolytes for batteries, super-capacitors, actuators, dye sensitised solar cells and thermo-electrochemical cells. In the field of water splitting to produce hydrogen they have been used to synthesize some of the best performing water oxidation catalysts and some members of the protic ionic liquid family co-catalyse an unusual, very high energy efficiency water oxidation process. As fuel cell electrolytes, the high proton conductivity of some of the protic ionic liquid family offers the potential of fuel cells operating in the optimum temperature region above 100 °C. Beyond electrochemical applications, the low vapour pressure of these liquids, along with their ability to offer tuneable functionality, also makes them ideal as CO2 absorbents for post-combustion CO2 capture. Similarly, the tuneable phase properties of the many members of this large family of salts are also allowing the creation of phase-change thermal energy storage materials having melting points tuned to the application. This perspective article provides an overview of these developing energy related applications of ionic liquids and offers some thoughts on the emerging challenges and opportunities.

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Energy applications of ionic liquids

As an emerging carbon dioxide (CO2) capture technology, separating CO2 from industrial gases with ionic liquids is increasingly attracting remarkable interests. In this paper, the research progress on CO2 capture with ionic liquids is reviewed with particular attention on the viewpoint of potential industrial applications. We investigate and compare the CO2 capture capacities of pure ionic liquids, including conventional and task-specific ionic liquids, and ionic liquid-based mixtures. The mechanisms of chemisorption and physisorption are explained with experimental characteristics and molecular simulation, which show more and more important roles for screening suitable ionic liquids from tremendous candidates. Considering the scaling up of novel units for ionic liquid-based fluids, the studies on the transport properties and hydrodynamics of ionic liquid fluids are presented. The process design and assessment of ionic liquid processes are discussed, including the research progress on thermodynamic properties and prediction models. Besides giving an overview of research for each issue above, we also provide discussions for future work to try to identify the gap between the current work and the demand by real industrial applications. Finally, we present some perspectives of ionic liquid-based novel technologies, and the challenges which will be faced while developing industrially available technologies.

Carbon capture with ionic liquids: overview and progress

Ionic liquids (ILs) offer a wide range of promising applications because of their much enhanced properties. However, further development of such materials depends on the fundamental understanding of their hierarchical structures and behaviors, which requires multiscale strategies to provide coupling among various length scales. In this review, we first introduce the structures and properties of these typical ILs. Then, we introduce the multiscale modeling methods that have been applied to the ILs, covering from molecular scale (QM/MM), to mesoscale (CG, DPD), to macroscale (CFD for unit scale and thermodynamics COSMO-RS model and environmental assessment GD method for process scale). In the following section, we discuss in some detail their applications to the four scales of ILs, including molecular scale structures, mesoscale aggregates and dynamics, and unit scale reactor design and process design and optimization of typical IL applications. Finally, we address the concluding remarks of multiscale strat...

Multiscale Studies on Ionic Liquids

Developing effective catalysts based on earth abundant elements is critical for CO2 electroreduction. However, simultaneously achieving a high Faradaic efficiency (FE) and high current density of CO (jCO) remains a challenge. Herein, we prepare a Mn single-atom catalyst (SAC) with a Mn-N3 site embedded in graphitic carbon nitride. The prepared catalyst exhibits a 98.8% CO FE with a jCO of 14.0 mA cm−2 at a low overpotential of 0.44 V in aqueous electrolyte, outperforming all reported Mn SACs. Moreover, a higher jCO of 29.7 mA cm−2 is obtained in an ionic liquid electrolyte at 0.62 V overpotential. In situ X-ray absorption spectra and density functional theory calculations demonstrate that the remarkable performance of the catalyst is attributed to the Mn-N3 site, which facilitates the formation of the key intermediate COOH* through a lowered free energy barrier. Developing effective catalysts based on earth abundant elements is critical for electrochemical CO2 reduction. Here, the authors prepare a manganese single atom catalyst with high CO2 reduction performance, which can be attributed to the Mn-N3 site embedded in graphitic carbon nitride.

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A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction.

To study the effect of water on the properties of choline chloride (ChCl)/urea mixtures (1:2 on a molar basis), the density and viscosity of ChCl/urea (1:2) with water were measured at temperatures from 298.15 K to 333.15 K at atmospheric pressure, the CO2 solubility in ChCl/urea (1:2) with water was determined at 308.2 K, 318.2 K, and 328.2 K and at pressures up to 4.5 MPa. The results show that the addition of water significantly decreases the viscosity of ChCl/urea (1:2), whereas the effects on their density and CO2 solubility are much weaker. The CO2 solubility in ChCl/urea (1:2) with water was represented with the Nonrandom-Two-Liquid Redlich–Kwong (NRTL-RK) model. The excess molar volume and excess molar activation energy were further determined. The CO2 absorption enthalpy was calculated and dominated by the CO2 dissolution enthalpy, and the magnitude of the CO2 dissolution enthalpy decreases with the increase of water content.

Haifeng Dong

Papers

Carbon capture with ionic liquids: overview and progress

Multiscale Studies on Ionic Liquids

A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction.

Effect of Water on the Density, Viscosity, and CO2 Solubility in Choline Chloride/Urea

Efficient and reversible capture of SO2 by pyridinium-based ionic liquids