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  • Journal article
    Zhang C, Ovejero-Pérez A, Fennell PS, Hallett JP, Ghatta AAet al., 2026,

    Design and Optimization of a New Efficient Furfural Production Technology via a Protic Ionic Liquid at “Quasi-Economic” Viability

    , ACS Sustainable Chemistry & Engineering

    <jats:title>Abstract</jats:title> <jats:p>Furfural is a versatile bio-based aromatic building block with great potential for many applications. State-of-the-art processes rely on acid hydrolysis, with the main drawback being excessive wastewater generation with high biochemical oxygen demand. This implies environmental and regulatory challenges and requires extensive capital expenditure for large-scale adoption. Solvent-based approaches can improve process economics and reduce waste generation if criteria for recyclability and energy efficiency are met, thereby delivering a more cost-effective, sustainable process. Here, a protic ionic liquid-based approach is assessed using N,N-dimethylbutylammonium hydrogen sulfate ([DMBA][HSO4]), which previous studies have proven to be effective in biomass fractionation. This study shows that, under strict reaction control in terms of furfural separation, temperature regulation, and biomass feeding, competitive furfural yields can be achieved at a high biomass loading of 30 wt %, reducing energy demand and making this methodology competitive with traditional processes. This advance holds promise for reducing hazardous waste generation while improving the economic and environmental footprint of furfural manufacturing. This is the first study to combine high yield (∼75%), high biomass loading, solvent recyclability, and process economics for furfural production using a solvent-based approach.</jats:p>

  • Journal article
    Kumar P, Nakasu PYS, Shmool TA, Hallett JP, Brandt-Talbot Aet al., 2026,

    Optimized Isolation of Protein Fractions from Brewer’s Spent Grain by Extraction with Ethanol and Mild Alkali

    , ACS Sustainable Chemistry &amp; Engineering

    <jats:title>Abstract</jats:title> <jats:p>Spent grain is the largest by-product of ethanol production from cereal grains. While spent grains can be used as livestock feed, fractionation could enable a wider range of applications. This study investigated multistep fractionation of an air-dried mixed Brewer’s Spent Grain (BSG) with 23% protein content from a small brewery to obtain protein concentrates, an organic solvent-soluble fraction, and a protein-depleted BSG residue. After screening of pre-extraction solvents (hot water, cyclohexane, ethanol, and water + ethanol), hot ethanol was selected followed by a three-step protein extraction with 0.1 M aqueous alkali at ambient temperature and by isoelectric precipitation at pH 3.5. The conditions yielded two protein products: an alkali-soluble protein precipitate (32% protein yield, 75% protein content) and an alkali-insoluble protein concentrate (18% protein yield, 44% protein content), which was separated from the protein-depleted residue based on density. The combined protein yield (up to 50%) exceeds previously reported yields for precipitated BSG protein products. Glucan analysis revealed that the protein products contained significant amounts of starch resistant to enzymatic hydrolysis. Comprehensive compositional analysis of the starting material, protein products, and residue enabled detailed mass balances. Although selective protein separation remains challenging due to coextraction of other biopolymers, the composition of the isolated protein concentrates supports potential valorization beyond livestock feed, including human nutrition and packaging materials. Identifying applications for the protein-depleted fraction remains important.</jats:p>

  • Journal article
    Zhang C, Nisar S, Liu Y, Verdía Barbará P, Nakasu PYS, Fennell PS, Hallett JPet al., 2026,

    Process intensification via probe sonication in protic ionic liquid pretreatment of biomass

    , Chemical Engineering Journal, Vol: 541, ISSN: 1385-8947

    Protic ionic liquids have proven to be feasible and cost-effective for the fractionation of lignocellulosic biomass into renewable fuels and materials (the ionoSolv process). This study tested probe sonication as a process accelerator for the ionoSolv pretreatment of Miscanthus × giganteus (grass) and spruce (softwood) using the low-cost PIL, N,N-dimethylbutylammonium hydrogen sulfate ([DMBA][HSO<inf>4</inf>], 20 wt% water content). Treatments were run at moderate temperatures (110 and 130 °C for Miscanthus; 130 and 150 °C for spruce). Results showed that sonication greatly improved softwood pretreatment, whereas its effect on grass biomass was less pronounced. At 130 °C, spruce displayed high recalcitrance to the conventional ionoSolv process, yielding only 18.1% glucose after 4 h of treatment. In contrast, with sonication, an equivalent saccharification yield was achieved after only 0.5 h of treatment, and the yield further exceeded 40% after 2 h. Monitoring the temperature profile showed that the main driver of this improvement was the temperature rise induced by sonication, rather than enhanced mass transfer. Additionally, sonication was observed to produce two pulp layers, with the upper layer having finer particles. For spruce, this upper layer was markedly more digestible than the lower layer. A preliminary techno-economic analysis indicated that applying sonication during spruce fractionation could reduce the minimum selling price of spruce-derived ethanol relative to the conventional ionoSolv route, although the magnitude of the benefit depends on the extent to which the sonication-induced, laboratory-scale temperature increase can be maintained at an industrial scale.

  • Journal article
    Krueger J-DH, Saedi P, Poller MJ, Collauto A, Hallett JP, Robinson D, Roessler MM, Albert Jet al., 2026,

    Enhancing Biogenic Formic Acid Production in the Modified OxFA Process by Acetonitrile Addition.

    , Adv Sci (Weinh), Vol: 13

    Developing homogeneously catalyzed, selective biomass transformation techniques toward an industrially viable biomass valorization process is one of the major tasks of a more sustainable chemical industry. Specifically, the production of short-chain carboxylic acids like formic acid (FA) in the OxFA process is a promising strategy. In this study, we show the beneficial effect of using acetonitrile as a co-solvent in the modified OxFA process outperforming methanol, demonstrating improved reaction kinetics combined with high selectivity for the HPA-2 (H5PV2Mo10O40) catalyzed oxidation of xylose to FA. Ex situ spectroscopic 51V-NMR as well as optical UV-vis and electrochemical SWV investigations in combination with advanced pulse EPR measurements and DFT calculations clearly reveal the direct interactions of the co-solvents methanol and acetonitrile with the HPA-2 catalyst. This leads to improved selectivity for methanol addition whereby acetonitrile addition leads to both enhanced kinetics and improved selectivity on the kinetics of xylose oxidation to FA compared to the classical OxFA process in pure aqueous solution. This study shows interesting new correlations allowing us to further push the limits of the OxFA technology toward higher productivity.

  • Journal article
    Firth AEJ, Nakasu PYS, Amako RS, Fennell PS, Hallett JPet al., 2026,

    Effects of Cation Structure and Acidity on Hydrogen Sulfate-Based Protic Ionic Liquid Fractionation Efficacy of Lignocellulosic Biomass

    , ACS Sustainable Chemistry and Engineering, Vol: 14, Pages: 13355-13364

    Alkylammonium hydrogen sulfate ([HSO<inf>4</inf>]<sup>–</sup>) ionic liquids (ILs) have proven effective fractionation solvents for lignocellulosic biomass. While a number of process parameters have been studied, there has been relatively little investigation into the effect of cation structure for these tunable solvents. Four alkylammonium cations were screened in this study, with three different degrees of substitution. Decreasing degree of substitution was found to enhance solution acidity as measured by the Hammett acidity function, strongly affecting fractionation behavior. Excess acid was added to a tertiary alkylammonium [HSO<inf>4</inf>]<sup>–</sup> IL to replicate the behavior of primary and secondary alkylammonium [HSO<inf>4</inf>]<sup>–</sup> ILs. The Hammett acidity scale alone was not sufficient to predict and compare the different PIL acidities and their effect on fractionation severity. Methylbutylammmonium hydrogen sulfate ([MBA][HSO<inf>4</inf>]) was identified as a promising fractionation solvent, generating pulps with high cellulose content (>90%) and saccharification yield (>90%) at a range of different conditions, and at shorter durations than current benchmark ILs. Primary alkylammonium [HSO<inf>4</inf>]<sup>–</sup> ILs were found to be ineffective fractionation solvents, due to insufficient lignin removal despite reasonable cellulose pulp contents. Sustainability metrics showed that despite low E-factors, process mass intensity can be significantly high due to high solvent use during washing steps.

  • Journal article
    Polesca C, Nisar S, Law RV, Ovejero-Pérez A, Hallett JPet al., 2026,

    An Integrated ionoSolv Process with Ethanol-Free Pulp Washing for Lignocellulosic Biomass Valorisation and High-Purity Cellulose Pulp Production

    , ACS Sustainable Chemistry and Engineering, Vol: 14, Pages: 12601-12616

    Sustainable and cost-effective lignocellulosic biomass valorisation is essential for the transition from fossil to renewable feedstocks. The ionoSolv process, which employs protic ionic liquids (PILs) to selectively extract hemicellulose and lignin while preserving cellulose, has demonstrated effectiveness across various feedstocks. Nevertheless, current laboratory protocols rely on ethanol for cellulose pulp washing, raising safety and sustainability concerns and failing to accurately represent commercial-scale process dynamics. Herein, we report for the first time an ethanol-free pulp washing strategy based on an additional IL washing step using a low-cost PIL, enabling enhanced cellulose pulp purity. Miscanthus × giganteus was used as a model feedstock, and a statistical design of experiments was applied to optimise washing conditions, including IL concentration, pulp:IL ratio, and temperature. Enhanced lignin removal was achieved, yielding a cellulose pulp with up to 92.7% glucan content and up to 90.5% enzymatic digestibility (7 days, Ctec-3, 50 °C). Eliminating ethanol and increasing solid loading did not affect cellulose structure. Techno-economic analysis indicates a minimum cellulose selling price of ≤0.80 $·kg<sup>–1</sup> at ≥10% solid loading. Overall, the proposed ethanol-free pulp washing strategy enhances safety and process simplification while delivering high-purity cellulose for biorefining and advanced material applications.

  • Journal article
    Polesca C, Passos H, Hallett JP, Coutinho JAP, Freire MGet al., 2026,

    Sustainable Recovery of Keratin from Chicken Feather Waste and Its Processing for Biomedical Applications

    , Accounts of Materials Research, Vol: 7, Pages: 499-509

    Conspectus: The global poultry industry has grown significantly in recent decades and is currently producing vast amounts of chicken feather waste, corresponding to around 7 wt % of the total weight of an adult chicken. This waste, which is typically incinerated or landfilled, poses both environmental and economic challenges, while being inconsistent with the principles of the circular economy. Chicken feathers are composed primarily of keratin (approximately 90 wt % on a dry weight basis), a natural protein with valuable properties, namely, anti-inflammatory and antioxidant activities, superior cytocompatibility, and ability to promote cellular migration. These characteristics make keratin an ideal candidate for various biomedical applications. However, traditional methods of recovering keratin from natural biomass are inefficient and costly and involve the use of toxic chemicals, limiting the broader use of this waste. In this Account, we discuss a sustainable and efficient process for keratin recovery and processing using ionic liquids. By employing acetate-based ionic liquids (80 wt % in water), we have developed a method that not only dissolves chicken feathers but also allows for high-yield keratin recovery. The developed process significantly reduces the need for harmful chemicals and energy-intensive steps traditionally associated with keratin recovery. Furthermore, the ionic liquids can be recovered and reused, which are important elements highlighted by our technoeconomic assessment. According to the process simulation, the minimum selling price for keratin is 22 $ per kg, based on a productivity of 350 tons of keratin per year, which is suitable for biomedical applications. The recovered keratin has been used to develop biocompatible films and hydrogels for wound healing, incorporated into biocomposites with melanin, cellulose, and chitin to enable tunable material properties, and integrated into advanced 3D printing technologies for tissue engineering ap

  • Journal article
    Chakrabarti BK, Hayyan M, Syed Putra SS, İnan TY, Mu T, Zulkifli LS, Manan NSA, Basirun WJ, Qiao Y, Bayazıt MK, Hayat Soytaş S, Rubio-Garcia J, Shah N, AlNashef IM, Hallett JP, Hajimolana YS, Low CTJet al., 2026,

    Deep eutectic solvents in battery recycling: A sustainable path forward

    , Journal of Power Sources, Vol: 670, ISSN: 0378-7753

    The recycling of various energy storage materials, including but not limited to lithium-based batteries, has become increasingly important due to the rapid growth of the battery sector and its potential to strain global material supply chains. Recycling not only helps recover valuable metals and minerals but also reduces reliance on environmentally harmful mining practices and creates local economic opportunities. However, current recycling methods often involve chemical processes that are not entirely environmentally friendly. As a greener alternative, deep eutectic solvents (DESs) are drawing attention for their potential in battery recycling technologies. This review explores the progress on DESs in this field. It also examines the recycling of polymer components, often overlooked but crucial for a complete recycling strategy. Furthermore, a brief life-cycle-assessment (LCA) is included to evaluate the environmental benefits and limitations of DES-based recycling. Early integration of LCA can guide sustainable process development, identify environmental trade-offs, and support sound decision-making, aligning emerging recycling technologies with sustainability targets and regulatory frameworks. While energy storage represents the bottleneck to a successful energy transition, the recycling of materials used in storage devices constitutes the foundation of a true circular economy, in which DES systems possess the potential to play a pivotal role.

  • Book chapter
    Hallett J, 2026,

    DYERECYCLE – Materials and Longevity

    , Fashion Works, Publisher: Springer Nature Switzerland, Pages: 67-71, ISBN: 9783032020697
  • Journal article
    Ewulonu CM, Akromah S, Lee K-Y, Seddon AM, Polesca C, Hallett JP, Eichhorn SJet al., 2025,

    Looking beyond pure cellulose to lignocellulose for regenerated continuous spun filaments

    , ACS Omega, Vol: 10, Pages: 63583-63596, ISSN: 2470-1343

    The need to use naturally abundant, renewable, and sustainable precursors, such as lignin and cellulose, to produce technical textile fibers for a range of applications is rapidly growing. Being able to spin fibers directly from the biomass feedstock, without separation and purification, could significantly reduce processing costs, energy consumption, and pollution, and also retain carbon for subsequent use in carbon fiber production and other applications. Going beyond the approach of either spinning pure lignin, cellulose, or combinations of the two, continuous regenerated spun fibers have been successfully produced from dissolved and unbleached miscanthus grass pulp. The rheological and microscopic properties of the spinning dope were fully characterized as well as the structure and mechanical properties of the spun lignocellulose pulp (LCP) fibers. The highly viscous spinning dope had a zero-shear viscosity in the range 26–256 kPa·s, which resulted in spun fibers with a rough surface texture, with some undissolved lignocellulose components in the dope. The LCP fiber’s orientation was determined using X-ray diffraction, displaying low- to mid-range values of <sin2 θ> (0.2–0.5), which was expected at the low draw ratios used to ensure fiber consistency. Despite this, the filaments were found to have strengths in the range of 114–173 MPa, similar to wool or wet viscose rayon, and moduli of 9–12 GPa comparable to lower-range lyocell fibers. Interestingly, the micrometer-scale undissolved lignocellulose components did not inhibit the spinning process, allowing the production of what resembles continuous natural fibers. This approach shows promise for generating sustainable continuous spun fibers, without excessive pretreatment of the precursor, for technical textiles from lignocellulose pulps.

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