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Journal articleYao JG, Tan S-Y, Metcalfe P, et al., 2021,
Demetallization of Sewage Sludge Using Low-Cost Ionic Liquids
, ENVIRONMENTAL SCIENCE & TECHNOLOGY, Vol: 55, Pages: 5291-5300, ISSN: 0013-936X- Author Web Link
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- Citations: 23
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Journal articleTan S-Y, Bedoya-Lora FE, Hallett JP, et al., 2021,
Evaluation of N,N,N-Dimethylbutylammonium methanesulfonate ionic liquid for electrochemical recovery of lead from lead-acid batteries
, Electrochimica Acta, Vol: 376, Pages: 1-9, ISSN: 0013-4686Physicochemical and electrochemical properties of N,N,N-dimethylbutylammonium methanesulfonate, [DMBA][MS], ionic liquid (IL) have been determined, and the potential application for electrochemical recovery of lead from lead-acid batteries is discussed. To optimise the transport properties of the IL, the dependences were measured of conductivity, density and viscosity with varying amounts of excess acid with water as a diluent in the electrolyte mixture. Molar conductivities obtained from the molar concentration and ionic conductivity measurements were used to quantify the ionicities of these IL mixtures. The solubility of PbII from PbCO3 was also shown to depend strongly on the IL composition. Preliminary results of the electrochemical kinetics of PbII reduction showed fast Pb deposition and potential-controlled electrodeposition morphologies of Pb, which may be advantageous for the design of up-scaled lead electrowinning processes.
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Journal articleBhatia R, Lad JB, Bosch M, et al., 2021,
Production of oligosaccharides and biofuels from <i>Miscanthus</i> using combinatorial steam explosion and ionic liquid pretreatment
, BIORESOURCE TECHNOLOGY, Vol: 323, ISSN: 0960-8524- Cite
- Citations: 51
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Journal articleClarke CJ, Matthews RP, Brogan APS, et al., 2021,
Controlling surface chemistry and mechanical properties of metal ionogels through Lewis acidity and basicity
, Journal of Materials Chemistry A, Vol: 9, Pages: 4679-4686, ISSN: 2050-7488Ionogels are emerging as soft materials with remarkable physical properties that can be tuned to suit application requirements. The liquid component—ionic liquids—are effectively involatile, which provides new opportunities to explore gel surfaces with UHV based analytical techniques. Here, we exploit the highly solvating nature of ionic liquids to fabricate poly(ethylene glycol) based ionogels with high concentrations of zinc, and then investigate their surfaces to show that tunability extends beyond the bulk to the interface. A unique relationship between Lewis acidity and basicity and the surface concentration of metal was revealed. Chemical state analysis and molecular dynamics showed that Lewis acidic metals templated polymers to give new architectures reduced brittleness and increased flexibility, while Lewis basic metals improved polymer uniformity and strengthened gels. Therefore, bulk structure, surface composition, and metal speciation were all found to be intimately related and dependent upon the coordination strengths of ionic liquid anions. Importantly, the highly controllable surface and structural properties of metal ionogels allow fine-tuning across a broad design space, which presents new opportunities for gel based applications.
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Journal articleLemus J, Santiago R, Hospital-Benito D, et al., 2021,
Process Analysis of Ionic Liquid-Based Blends as H<sub>2</sub>S Absorbents: Search for Thermodynamic/Kinetic Synergies
, ACS SUSTAINABLE CHEMISTRY & ENGINEERING, Vol: 9, Pages: 2080-2088, ISSN: 2168-0485- Cite
- Citations: 10
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Journal articleAl Ghatta A, Zhou X, Casarano G, et al., 2021,
Characterization and valorization of humins produced by HMF degradation in ionic liquids: a valuable carbonaceous material for antimony removal
, ACS Sustainable Chemistry and Engineering, Vol: 9, Pages: 2212-2223, ISSN: 2168-0485The processing of biomass in ionic liquids has demonstrated many benefits compared to organic solvents. This includes the maximization of 5-hydroxymethylfurfural (HMF) yield from sugars through the suppression of byproducts, such as formic acid and levulinic acid. Inefficiencies still exist due to the low stability of HMF at high temperature, leading to side reactions which ultimately result in the undesirable formation of humins. Valorization of this polymeric side product is thus needed to improve the economics of the biorefinery and could lead to humins being viewed as valuable materials for various applications. However, a much better understanding is needed of how humins form from HMF in the various ionic liquids proposed for the biorefinery. In this contribution, humin formation is probed by a range of analytical techniques, including FT-IR, SEM, solid-state 13C NMR, MS, GPC, and XPS analyses. This reveals that the structure and morphology of the humins formed does not resemble those reported in the literature and that the material displays a number of unique aspects. The hydrogen bonding proprieties of the ionic liquids employed exert a strong influence on the chemical functionality of the humins, and this is used to demonstrate their potential as functional materials. To demonstrate this, the humins produced in various ionic liquid environments are applied to metal extraction and compared with commercial activated carbon. This reveals that humins are superior for the extraction of antimony ions from wastewater, showing promise as an adsorbent additive for water purification.
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Journal articleCuellar-Franca RM, Garcia-Gutierrez P, Hallett JP, et al., 2021,
A life cycle approach to solvent design: challenges and opportunities for ionic liquids - application to CO<sub>2</sub> capture
, REACTION CHEMISTRY & ENGINEERING, Vol: 6, Pages: 258-278, ISSN: 2058-9883- Cite
- Citations: 15
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Journal articleBui-Le L, Brogan APS, Hallett JP, 2021,
Solvent-free liquid avidin as a step toward cold chain elimination
, BIOTECHNOLOGY AND BIOENGINEERING, Vol: 118, Pages: 592-600, ISSN: 0006-3592- Cite
- Citations: 9
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Journal articleBrandl P, Bui M, Hallett JP, et al., 2021,
Beyond 90% capture: Possible, but at what cost?
, International Journal of Greenhouse Gas Control, Vol: 105, Pages: 1-16, ISSN: 1750-5836Carbon capture and storage (CCS) will have an essential role in meeting our climate change mitigation targets. CCS technologies are technically mature and will likely be deployed to decarbonise power, industry, heat, and removal of CO2 from the atmosphere. The assumption of a 90% CO2 capture rate has become ubiquitous in the literature, which has led to doubt around whether CO2 capture rates above 90% are even feasible. However, in the context of a 1.5 °C target, going beyond 90% capture will be vital, with residual emissions needing to be indirectly captured via carbon dioxide removal (CDR) technologies. Whilst there will be trade-offs between the cost of increased rates of CO2 capture, and the cost of offsets, understanding where this lies is key to minimising the dependence on CDR. This study quantifies the maximum limit of feasible CO2 capture rate for a range of power and industrial sources of CO2, beyond which abatement becomes uneconomical. In no case, was a capture rate of 90% found to be optimal, with capture rates of up to 98% possible at a relatively low marginal cost. Flue gas composition was found to be a key determinant of the cost of capture, with more dilute streams exhibiting a more pronounced minimum. Indirect capture by deploying complementary CDR is also assessed. The results show that current policy initiatives are unlikely to be sufficient to enable the economically viable deployment of CCS in all but a very few niche sectors of the economy.
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Journal articleAl Ghatta A, Wilton-Ely J, Hallett J, 2021,
From sugars to FDCA: A techno-economic assessment using a design concept based on solvent selection and carbon dioxide emissions
, Green Chemistry, Vol: 23, Pages: 1716-1733, ISSN: 1463-9262The synthesis of the molecule 2,5-furandicarboxylic acid (FDCA) from sugars is key to unlocking the potential for the replacement of the oil derivative PET (polyethylene terephthalate) by polyethylene furanoate (PEF). Although much research and investment has been dedicated to the synthesis of FDCA, there remains limited commercial activity in this area due to the challenges related to the stability and isolation of the FDCA precursor, 5-hydroxymethylfurfural (HMF). High yields of HMF can be obtained from fructose at high loadings in water–organic solvent mixtures (methyl isobutyl ketone, MIBK; γ-valerolactone, GVL), dimethyl sulfoxide (DMSO) or ionic liquids. Each of these approaches suffers from various drawbacks in terms of catalyst development, product separation and environmental impact. It is therefore necessary to understand which of these processes has the potential for scale-up, while ensuring low environmental impact and a competitive selling price. In this study, a process simulation (rather than a life cycle assessment) was performed to evaluate the associated emissions and selling price of FDCA based on its production using different solvents. It was determined that the cost and CO2 emissions associated with the isolation of HMF undermine the economic and environmental viability of the transformation of sugars to FDCA. In contrast, a two-step, one-pot reaction represents an ideal solution to reduce both cost and environmental impact, making FDCA competitive with terephthalic acid (the corresponding precursor for PET). The choice of solvent and the process were then evaluated and ranked based on safety, CO2 emissions, selling price and state of development though a scoring methodology. A system based on a water/GVL mixture is closer to commercial applicability but the process is limited by extensive formation of humins, which reduces the overall yield of the process, increasing the minimum selling price of FDCA. Using DMSO or ionic liquids mi
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