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Journal articleAugusto FF, Francisco M, Stephen E, et al., 2022,
Physicochemical Characterization of Two Protic Hydroxyethylammonium Carboxylate Ionic Liquids in Water and Their Mixture
, JOURNAL OF CHEMICAL AND ENGINEERING DATA, Vol: 67, Pages: 1309-1325, ISSN: 0021-9568- Cite
- Citations: 9
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Journal articleShmool TA, Constantinou A, Jirkas A, et al., 2022,
Next generation strategy for tuning the thermoresponsive properties of micellar and hydrogel drug delivery vehicles using ionic liquids
, Polymer Chemistry, Vol: 13, Pages: 2340-2350, ISSN: 1759-9954Amongst the greatest challenges in developing injectable controlled thermoresponsive micellar and hydrogel drug delivery vehicles include tuning the cloud point (CP) and reducing the gelation temperature (Tgel), below 37 °C, without compromising stability and solubility. Here, a unique strategy is employed using ionic liquid (IL) matrices to produce stable micellar and hydrogel delivery vehicles of distinct thermoresponsive properties. Each formulation includes the in-house synthesised polymer OEGMA30020-b-BuMA22-b-DEGMA11 with FITC-IgG. Both micellar-IL and hydrogel-IL formulations exhibit enhanced stability following 120 days of storage under 4 °C compared to in phosphate buffered saline (PBS). Visual tests demonstrate that the CP of the micellar-IL carriers can be finely tuned (31- 46 °C). Rheology measurements show that hydrogel strength is significantly increased and Tgel is reduced, from 40 °C in PBS to 30 °C with IL. Finally, a unique stabilisation mechanism is proposed, triggered by the synergetic action of the excipients and IL in each system
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Journal articleAl Ghatta A, Hallett JP, 2022,
High yield and isolation of 2,5-furandicarboxylic acid from HMF and sugars in ionic liquids, a new prospective for the establishment of a scalable and efficient catalytic route
, GREEN CHEMISTRY, Vol: 24, Pages: 3309-3313, ISSN: 1463-9262- Cite
- Citations: 25
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Journal articleAnuchi S, Campbell K, Hallett J, 2022,
Effective pretreatment of lignin-rich coconut wastes using a low-cost ionic liquid
, Scientific Reports, Vol: 12, ISSN: 2045-2322Coconut husks and shells are underutilised agricultural feedstocks in the bio-based industry. These biomass wastes have a higher lignin content than other woody biomass and have excellent potential as raw materials for the production of lignin-based materials. This work demonstrates the performance of a low-cost protic ionic liquid, N,N,N-dimethylbutylammonium hydrogen sulfate ([DMBA][HSO4]), for ionoSolv pretreatment of coconut husk and shell at 150 °C for 45 – 90 minutes and 170 °C for 15 - 60 minutes. Optimum pretreatment conditions were observed at 170 °C and 45 minutes for both feedstocks. At these conditions, [DMBA][HSO4] was able to remove almost 77 wt.% of the lignin from the husk; leaving a cellulosic rich pulp behind, which released 82 % of the theoretical maximum glucose after enzymatic saccharification. The pretreated shell, by comparison, achieved 82 wt.% lignin removal and 89 % glucose yield and these higher values could be attributed to the highly porous structure of coconut shell cell walls. The cleavage of the β-O-4 aryl ether linkages of lignin followed by extensive C-C condensation in the lignin at longer pretreatment times was shown by HSQC NMR analysis. This extensive condensation was evidenced by molecular weights > 10 000 g/mol exhibited by lignin precipitated after pretreatment at high temperature and long times. The high degree of lignin removal and high glucose release from both feedstocks demonstrate that [DMBA][HSO4] is an excellent ionic liquid for fractionation of very lignin-rich biomass.
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Journal articleBahzad H, Fennell P, Shah N, et al., 2022,
Techno-economic assessment for a pumped thermal energy storage integrated with open cycle gas turbine and chemical looping technology
, Energy Conversion and Management, Vol: 255, Pages: 1-23, ISSN: 0196-8904Pumped thermal energy storage offers a high energy density, potentially resulting in a relatively low cost per unit of energy stored. In this study, two novel energy storage systems were developed. The first system was developed by integrating pumped thermal energy storage and chemical looping technologies, whereas the second was formed by merging the first system with an open cycle gas turbine. Both systems used an oxygen depleted stream as a working fluid and iron-based oxygen carriers from a chemical looping water splitting process storage material for the pumped thermal energy storage system. In addition, hydrogen from the chemical looping process was employed for the gas turbine in the second system. Both systems were evaluated thermodynamically via the determination of the roundtrip efficiency. The results presented here indicate that the roundtrip efficiency of both systems developed was 77%. Furthermore, the capital requirements, operating costs, and daily profits from electricity generation were calculated for both systems over several days within the year. The capital and operating costs for the several days that were simulated for the integrated pumped thermal energy storage system were lower than that of a gas turbine based system. Consequently, the daily profit was estimated and found to be between 4.9% and 72.9% higher for the integrated pumped storage relative to the gas turbine based system. Moreover, an economic sensitivity analysis was performed to identify the factors that strongly affect the daily profits of the gas turbine system relative to the pumped storage system. Based on the analysis, the optimal hydrogen fuel percentage fed to the open cycle gas turbine was calculated for the days simulated. Finally, the impact of % error on the estimated capital and fuel production costs on daily profits were investigated. The outcome revealed a higher impact of computational errors on the fuel costs relative to the costs of the capital.
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Journal articleNakasu PYS, Barbara PV, Firth AEJ, et al., 2022,
Pretreatment of biomass with protic ionic liquids
, TRENDS IN CHEMISTRY, Vol: 4, Pages: 175-178- Cite
- Citations: 26
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Journal articleSantos Klienchen Dalari BL, Giroletti CL, Malaret FJ, et al., 2022,
Application of a phosphonium-based ionic liquid for reactive textile dye removal: Extraction study and toxicological evaluation
, JOURNAL OF ENVIRONMENTAL MANAGEMENT, Vol: 304, ISSN: 0301-4797- Cite
- Citations: 22
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PatentShmool T, Bhamra A, Chen R, et al., 2021,
Stable composition
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Journal articleBaaqel H, Hallett JP, Guillen-Gosalbez G, et al., 2021,
Sustainability assessment of alternative synthesis routs to aprotic ionic liquids: the case of 1-Butyl-3-methylimidazolium tetrafluoroborate for fuel desulfurization
, ACS Sustainable Chemistry and Engineering, Vol: 10, Pages: 323-331, ISSN: 2168-0485Advantages of ionic liquids (ILs) over volatile organic solvents in chemical processes include no or negligible evaporative losses and high tunability. However, the conventional production of aprotic ILs via metathesis can be unattractive (both economically and environmentally) because of its high complexity, while the performance of other synthesis routes remains unclear. Existing life-cycle assessments furthermore fail to combine the production and use phases of these solvents, leading to erroneous conclusion about their sustainability credentials. This paper compares a one-pot, halide-free production route to 1-butyl-3-methylimidazolium tetrafluoroborate [BMIM][BF4] against metathesis and two conventional fuel desulfurization solvents, namely, acetonitrile and dimethylformamide (DMF). Halide-free synthesis is predicted to reduce the cost and environmental impacts associated with the production of [BMIM][BF4] by 2–5-fold compared to metathesis. Upon including the use phase of the solvents in fuel desulfurization and accounting for the uncertainty in background data, halide-free [BMIM][BF4] consistently presents the lowest cost and environmental impacts, while DMF is the worst in class. As well as exemplifying the importance of synthesis routes of ILs on their sustainability, these results highlight the need to include the use phase of solvents for more comprehensive life-cycle assessments.
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Journal articleChambon CL, Verdía P, Fennell PS, et al., 2021,
Process intensification of the ionoSolv pretreatment: effects of biomass loading, particle size and scale-up from 10 mL to 1 L
, Scientific Reports, Vol: 11, Pages: 1-15, ISSN: 2045-2322The ionoSolv process is one of the most promising technologies for biomass pretreatment in a biorefinery context. In order to evaluate the transition of the ionoSolv pretreatment of biomass from bench-scale experiments to commercial scale, there is a need to get better insight in process intensification. In this work, the effects of biomass loading, particle size, pulp washing protocols and 100-fold scale up for the pretreatment of the grassy biomass Miscanthus giganteus with the IL triethylammonium hydrogen sulfate, [TEA][HSO4], are presented as a necessary step in that direction. At the bench scale, increasing biomass loading from 10 to 50 wt% reduced glucose yields from 68 to 23% due to re-precipitation of lignin onto the pulp surface. Omitting the pulp air-drying step maintained saccharification yields at 66% at 50 wt% loading due to reduced fiber hornification. 100-fold scale-up (from 10 mL to 1 L) improved the efficacy of ionoSolv pretreatment and increasing loadings from 10 to 20 wt% reduced lignin reprecipitation and led to higher glucose yields due to the improved heat and mass transfer caused by efficient slurry mixing in the reactor. Pretreatment of particle sizes of 1–3 mm was more effective than fine powders (0.18–0.85 mm) giving higher glucose yields due to reduced surface area available for lignin re-precipitation while reducing grinding energy needs. Stirred ionoSolv pretreatment showed great potential for industrialization and further process intensification after optimization of the pretreatment conditions (temperature, residence time, stirring speed), particle size and biomass loading. Pulp washing protocols need further improvement to reduce the incidence of lignin precipitation and the water requirements of lignin washing.
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