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ReportCastillo Castillo A, Brophy K, Hallett J, et al., 2023,
Addressing plastic additives
, London, Publisher: Institute for Molecular Science and Engineering, Briefing topic No. 10Hundreds of chemicals with known toxicity to humans and the environment are still widely used as additives in plastics. The average consumer’s knowledge of what goes into plastic products is not sufficient to make informed choices about exposure. The data collection needed to make these choices often does not exist, especially for recycled products made of mixtures of existing plastics. Though data on the toxicology of single additives in isolation may be available, there is very little data on the interaction of multiple additives in real world situations, either within a single product or between many products in a single place. Most substances are not restricted until proven toxic. As a result, damage comes first and action second. Substance-by-substance testing often results in the substitution of one hazardous molecule by another with similar toxicology. Governments and consumers should demand the use of non-toxic chemicals for use in plastics, especially given the risk of admixture of toxic substances in recycled plastic products. Consumers and producers should demand full supply chain transparency on additive presence in plastic products. Understanding the toxicology of mixtures of additives requires the generation of substantial new datasets. This data should include biomonitoring to characterise the complexity of real-world exposures. Assessments of toxicity should not assume that a low dose always means a low risk. Hazardous substances should be regulated by group rather than one-by-one to avoid substituting one harmful chemical for another. A molecular science and engineering approach is crucial to finding chemical and functional alternatives to toxic additives, and also for developing new processes to better manage the toxicity of additives which cannot be replaced or omitted.
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Journal articleAnuchi SO, Campbell KLS, Hallett JP, 2023,
Effects of the Ionic Liquid Structure on Porosity of Lignin-Derived Carbon Materials
, ACS SUSTAINABLE CHEMISTRY & ENGINEERING, Vol: 11, Pages: 15228-15241, ISSN: 2168-0485 -
Journal articleShmool TA, Martin LK, Jirkas A, et al., 2023,
Unveiling the rational development of stimuli-responsive silk fibroin-based ionogel formulations
, Chemistry of Materials, Vol: 35, Pages: 5798-5808, ISSN: 0897-4756We present an approach for the rational development of stimuli-responsive ionogels which can be formulated for precise control of multiple unique ionogel features and fill niche pharmaceutical applications. Ionogels are captivating materials, exhibiting self-healing characteristics, tunable mechanical and structural properties, high thermal stability, and electroconductivity. However, the majority of ionogels developed require complex chemistry, exhibit high viscosity, poor biocompatibility, and low biodegradability. In our work, we overcome these limitations. We employ a facile production process and strategically integrate silk fibroin, the biocompatible ionic liquids (ILs) choline acetate ([Cho][OAc]), choline dihydrogen phosphate ([Cho][DHP]), and choline chloride ([Cho][Cl]), traditional pharmaceutical excipients, and the model antiepileptic drug phenobarbital. In the absence of ILs, we failed to observe gel formation; yet in the presence of ILs, thermoresponsive ionogels formed. Systems were assessed via visual tests, transmission electron microscopy, confocal reflection microscopy, dynamic light scattering, zeta potential and rheology measurements. We formed diverse ionogels of strengths ranging between 18 and 642 Pa. Under 25 °C storage, formulations containing polyvinylpyrrolidone (PVP) showed an ionogel formation period ranging over 14 days, increasing in the order of [Cho][DHP], [Cho][OAc], and [Cho][Cl]. Formulations lacking PVP showed an ionogel formation period ranging over 32 days, increasing in the order of [Cho][OAc], [Cho][DHP] and [Cho][Cl]. By heating from 25 to 60 °C, immediately following preparation, thermoresponsive ionogels formed below 41 °C in the absence of PVP. Based on our experimental results and density functional theory calculations, we attribute ionogel formation to macromolecular crowding and confinement effects, further enhanced upon PVP inclusion. Holistically, applying our rational development strategy enables the pr
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Journal articleAl Ghatta A, Hallett JP, 2023,
Bioderived furanic compounds as replacements for BTX in chemical intermediate applications
, RSC SUSTAINABILITY, Vol: 1, Pages: 698-745 -
Conference paperShmool TA, Hallett JP, 2023,
A novel biophysical-based approach to understand the stabilisation and suppressed aggregation of protein therapeutics in ionic liquid formulations
, Publisher: SPRINGER, Pages: S105-S105, ISSN: 0175-7571 -
Journal articleBarbara PV, Rafat AA, Hallett JP, et al., 2023,
Purifying cellulose from major waste streams using ionic liquids and deep eutectic solvents
, Current Opinion in Green and Sustainable Chemistry, Vol: 41, ISSN: 2452-2236Cellulose is the main component in woody plant parts and a commodity industrial product, whose importance is set to increase as fossil hydrocarbons are phased out. Cellulose provided after a prior application can help secure stable, sustainable and cost-effective supplies of cellulosic glucose or cellulose fibers; however, the previous life poses additional challenges. Here, we discuss recent research efforts in recycling cellulose from waste biomass using ionic liquids and deep eutectic solvents, promising designer solvents for biopolymer separations. The review identifies large cellulosic waste streams that are not paper and cardboard waste, promising processing approaches employing ionic liquids and deep eutectic solvents to purify the waste cellulose, and discusses the opportunities and challenges in finding applications for the recovered cellulose. While the field of cellulosic waste recycling is relatively new, and hence decontamination and purification processes are at an early stage of development, further development has substantial potential to promote a more circular economy for cellulose.
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Journal articleAl Ghatta A, Nakasu PYS, Hallett JP, 2023,
Implementation of furan-based building blocks in commodity chemical production: An opinion on scientific progress and economic viability
, CURRENT OPINION IN GREEN AND SUSTAINABLE CHEMISTRY, Vol: 41, ISSN: 2452-2236- Cite
- Citations: 6
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Journal articlePolesca C, Al Ghatta A, Passos H, et al., 2023,
Sustainable keratin recovery process using a bio-based ionic liquid aqueous solution and its techno-economic assessment
, GREEN CHEMISTRY, Vol: 25, Pages: 3995-4003, ISSN: 1463-9262- Cite
- Citations: 16
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Journal articleBaaqel HA, Bernardi A, Hallett JP, et al., 2023,
Global sensitivity analysis in life-cycle assessment of early-stage technology using detailed process simulation: application to dialkylimidazolium ionic liquid production.
, ACS Sustainable Chemistry and Engineering, Vol: 11, Pages: 7157-7169, ISSN: 2168-0485The ability to assess the environmental performance of early-stage technologies at production scale is critical for sustainable process development. This paper presents a systematic methodology for uncertainty quantification in life-cycle assessment (LCA) of such technologies using global sensitivity analysis (GSA) coupled with a detailed process simulator and LCA database. This methodology accounts for uncertainty in both the background and foreground life-cycle inventories, and is enabled by lumping multiple background flows, either downstream or upstream of the foreground processes, in order to reduce the number of factors in the sensitivity analysis. A case study comparing the life-cycle impacts of two dialkylimidazolium ionic liquids is conducted to illustrate the methodology. Failure to account for the foreground process uncertainty alongside the background uncertainty is shown to underestimate the predicted variance of the end-point environmental impacts by a factor of two. Variance-based GSA furthermore reveals that only few foreground and background uncertain parameters contribute significantly to the total variance in the end-point environmental impacts. As well as emphasizing the need to account for foreground uncertainties in LCA of early-stage technologies, these results illustrate how GSA can empower more reliable decision-making in LCA.
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Journal articleQu S, Hadjittofis E, Malaret F, et al., 2023,
Controlling simonkolleite crystallisation <i>via</i> metallic Zn oxidation in a betaine hydrochloride solution
, NANOSCALE ADVANCES, Vol: 5, Pages: 2437-2452, ISSN: 2516-0230
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