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  • Journal article
    Luan S, Nisar S, Phipps J, Ovejero-Perez A, Hallett JP, Barbara PVet al., 2025,

    Optimization of the ionoSolv process for the preservation of pulp fibre dimensions

    , INDUSTRIAL CROPS AND PRODUCTS, Vol: 236, ISSN: 0926-6690
  • Journal article
    Artime IF, Al Ghatta A, Ouitrakoon P, Damilano G, Brandt-Talbot A, Hallett JP, Barbara PVet al., 2025,

    Surfactant-assisted ionic liquid fractionation of spruce produces a low molar weight and less condensed lignin

    , INDUSTRIAL CROPS AND PRODUCTS, Vol: 235, ISSN: 0926-6690
  • Journal article
    Wesinger S, Rabiner A, Meyer N, Voß D, BrandtTalbot A, Hallett J, Albert Jet al., 2025,

    Sequential fractionation and polyoxometalate‐catalyzed oxidation of lignocellulosic biomass improves cellulose purity and formic acid yield

    , Biofuels, Bioproducts and Biorefining, Vol: 19, Pages: 1862-1874, ISSN: 1932-104X

    Lignocellulosic biomass is an important source of renewable chemicals and materials but its full valorization is necessary in order to achieve economic and sustainability goals. This study proposes a two-step approach for the valorization of lignocellulosic biomass combining solvent-assisted fractionation and catalytic oxidation with molecular oxygen to generate cellulose and formic acid. An industrially relevant lignocellulosic substrate, beech wood, was fractionated under a nitrogen atmosphere using either an organosolv (methanol or ethanol) or ionosolv (ionic liquid) aqueous solvent to produce dissolved hemicellulose and lignin as well as a cellulose-rich solid. The dissolved components were oxidized catalytically to formic acid and its derivatives in a second step using the fivefold vanadium substituted Keggin-type polyoxometalate H8[PV5Mo7O40]. Enzymatic hydrolysis of the cellulose-enriched solid generated purified glucose higher in yields than the single-step comparison method. The organosolv-fractionation increased enzymatic saccharification to 78% whereas the ionosolv-fractionation increased the saccharification yield to 68%, in comparison with 18% for the one-step conversion and only 8% for the untreated beech wood. In the oxidation step, a 28% formic acid yield was achieved under 125 °C, 1200 rpm, 30 bar oxygen, and 6.5 h reaction conditions. The improvements observed for the two-step approach are attributed to the influence of the solvent on the catalyst preventing the latter from interacting with the cellulose-enriched solid, which improved the quality of the pulp and increased the overall formic acid yield.

  • Journal article
    Wang W, Nakasu PYS, Costa JM, D'Acierno F, Ahmad N, Titirici MM, Pontiroli D, Ricco M, Hu C, Hallett JPet al., 2025,

    Pectin Extracted by a Recyclable Molecular Mixture: A Promising Material for Porous Membranes in Quasi-Solid-State Na-Ion Batteries

    , ACS SUSTAINABLE CHEMISTRY & ENGINEERING, Vol: 13, Pages: 18061-18074, ISSN: 2168-0485
  • Journal article
    Wesinger S, Rabiner A, Nisar S, Schill L, Kubus MG, Poller MJ, Riisager A, Brandt-Talbot A, Hallett JP, Albert Jet al., 2025,

    Boosting POM-ionosolv biorefining of lignocellulosic biomass by using redox-balanced polyoxometalate catalysts in methanolic ionic liquid reaction media

    , ChemSusChem, Vol: 18, ISSN: 1864-5631

    This article presents an advanced iteration of the polyoxometalate (POM)-Ionosolv concept to generate biobased methyl formate in high yield and a bleached cellulose pulp from lignocellulosic biomass in a single-step operation by using redox-balanced POM catalysts and molecular oxygen in alcoholic ionic liquid (IL) mixtures. The performance of the three Ionosolv-ILs triethylammonium hydrogen sulfate ([TEA][HSO4]), N,N-dimethylbutylammonium hydrogen sulfate ([DMBA][HSO4]), and tributylmethylphosphonium methyl sulfate ([TBMP][MeSO4]), mixed with methanol (MeOH) (30/70 wt%), is evaluated by methyl formate yield from extracted hemicellulose and lignin as well as purity of the bleached cellulose pulp in the presence of various Keggin-type POMs. The redox-balanced H8PVMnMo10O40 POM catalyst in [TBMP][MeSO4]/MeOH emerge as the most effective combination, achieving 20% methyl formate yield from commercial beech wood. The glucan content in the bleached cellulose-enriched solid consisted is over 90%, demonstrating that the use of MeOH drastically improved lignin extraction in parallel with full hemicellulose extraction. The cellulose is highly susceptible to enzymatic hydrolysis, generating a pure and concentrated cellulosic glucose stream. The formed solid catalyst complex is examined in detail to reveal its chemical nature as POM-IL-complex. The approach is applicable to disparate types of lignocellulosic biomass, including hardwood, softwood, and grass.

  • Journal article
    Nisar S, Barbará PV, Chachuat B, Hallett JP, Brandt-Talbot Aet al., 2025,

    Near-infrared spectroscopy for rapid compositional analysis of cellulose pulps after fractionation with ionic liquids

    , Biomass and Bioenergy, Vol: 201, ISSN: 0961-9534

    The composition of cellulose-enriched solids is typically monitored using a laborious and expensive wet-lab analytical method. Here, the development and application of an alternative tool that uses NIR spectroscopy and a software sensor is reported, drawing on a large data set (149 training samples) consisting of untreated grass, hardwood, and softwood biomass and cellulose pulps obtained after fractionation with the low-cost ionic liquids triethylammonium hydrogen sulfate ([TEA][HSO4]) or N,N-dimethylbutylammonium hydrogen sulfate ([DMBA][HSO4]) mixed with water. A partial least squares (PLS) model was trained on compositions determined with the traditional wet-lab procedure, followed by the application of an uncertainty quantification framework to estimate confidence in the predictions. Good agreement with the wet-lab experimental data (mean absolute errors on unseen samples below 5%) was found for ionic liquid fractionated cellulose and purified cellulose samples generated with non-ionoSolv approaches. Cellulose with low crystallinity and isolated lignins generated poor fits, suggesting that more specialised models are needed. The sugar-derived pseudo-lignin (humin) content in the cellulose pulp was estimated by comparing the model with a second PLS model that excluded charred (over-treated) pulps. The study shows that NIR soft-sensors can cost- and time-effectively estimate the composition of ionoSolv-based pulps, speeding up process and product development and facilitating process operation.

  • Journal article
    Suleman MY, Judah HL, Bexis P, Fennell P, Hallett JP, Brandt-Talbot Aet al., 2025,

    The acetate anion promotes hydrolysis of poly(ethylene terephthalate) in ionic liquid-water mixtures

    , GREEN CHEMISTRY, Vol: 27, Pages: 11475-11490, ISSN: 1463-9262
  • Journal article
    Polesca C, Sobreiro-Almeida R, Passos H, Coutinho JAP, Hallett JP, Mano JF, Freire MGet al., 2025,

    Engineered from Waste: Ionic Liquid Processing of Keratin for 3D Printing Biomedical Scaffolds

    , ACS MATERIALS LETTERS
  • Journal article
    Nakasu PYS, Martinez MA, Melanie S, Shmool TA, Hallett JPet al., 2025,

    Chitosan-Based Biocomposite Hydrogels with Squid Pen Protein for Anionic Dyes Adsorption (vol 7, pg 1012, 2025)

    , ACS MATERIALS LETTERS
  • Journal article
    Aljohani M, Lan L, Daly H, Barbara PV, Hu M, Nisar S, Ding S, Hallett J, Watkins N, Macalpine WJ, Rowe R, Brandt-Talbot A, Sanford G, Ralph J, Mansfield SD, D'Agostino C, Fan X, Hardacre Cet al., 2025,

    Enhancing Hydrogen Production from Bioenergy Crops via Photoreforming

    , JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, Vol: 147, Pages: 29679-29686, ISSN: 0002-7863

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