New Enzymatically Produced Interpenetrating Starch-Cellulose Gels
Lead Research Organisation:
University of East Anglia
Department Name: Pharmacy
Abstract
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Publications
Calabrese V
(2018)
Surfactant controlled zwitterionic cellulose nanofibril dispersions
in Soft Matter
Calabrese V
(2019)
Understanding heat driven gelation of anionic cellulose nanofibrils: Combining saturation transfer difference (STD) NMR, small angle X-ray scattering (SAXS) and rheology.
in Journal of colloid and interface science
Courtenay JC
(2018)
Unravelling cationic cellulose nanofibril hydrogel structure: NMR spectroscopy and small angle neutron scattering analyses.
in Soft matter
De Andrade P
(2021)
Chemoenzymatic Synthesis of Fluorinated Cellodextrins Identifies a New Allomorph for Cellulose-Like Materials*.
in Chemistry (Weinheim an der Bergstrasse, Germany)
Fernández-García R
(2022)
Self-assembling, supramolecular chemistry and pharmacology of amphotericin B: Poly-aggregates, oligomers and monomers.
in Journal of controlled release : official journal of the Controlled Release Society
Gabrielli V
(2021)
Spin diffusion transfer difference (SDTD) NMR: An advanced method for the characterisation of water structuration within particle networks.
in Journal of colloid and interface science
Gabrielli V
(2021)
Molecular Recognition of Natural and Non-Natural Substrates by Cellodextrin Phosphorylase from Ruminiclostridium Thermocellum Investigated by NMR Spectroscopy
in Chemistry - A European Journal
Koev TT
(2020)
Structural heterogeneities in starch hydrogels.
in Carbohydrate polymers
Muñoz-García JC
(2019)
High Molecular Weight Mixed-Linkage Glucan as a Mechanical and Hydration Modulator of Bacterial Cellulose: Characterization by Advanced NMR Spectroscopy.
in Biomacromolecules
| Description | We have developed several novel hybrid NMR approaches for understanding the structure of gels. For instance, one of these NMR methodologies allow to better understand the role of the solvent on the gel structure and the resulting material properties, as well as the rationalisation of gelation mechanisms by observation of changes in solvent structuration in different gel samples. Also, we have found that the cell wall constituent Mixed Linkage Glucan can be used to control degree of water content and stiffness of cellulose hydrogels. Further, we have developed the production and characterisation of a novel type of cellulose structure using environmentally friendly methods, paving the grounds for the preparation of novel sustainable materials with tailored properties. Further advances in this are in progress. We have met the needed objectives for this stage of the grant. The details of key findings are below: - Development of a solution state NMR technique based on the Saturation Transfer Difference NMR (STD NMR) able to characterise and compare the degree of structuration of solvents in gels. - We have reported and characterised for the first time the role of high molecular weight mixed-linkage glucan (MLG) as a modulator of hydration of bacterial cellulose (BC) particles and weakening gel structure. By using advanced solid-state NMR techniques, we determined that MLG deposits at the surface of BC particles and acts as a water structuring agent that boosts BC hydration properties. - We have enzymatically synthesised for the first time chemically pure multiply 6-fluorinated cellodextrin (multi-6F-EpC), in aqueous media, in a sustainable manner. We have thoroughly characterised this novel material by solid-state NMR, x-ray diffraction, Raman spectroscopy and electron and atomic force microscopy. We have reported that multi-6F-EpC assembles into an unprecedented allomorph for a cellulose-like structure, and we have identified core and surface domains in the 13C solid-state NMR spectra. - We have developed a new NMR based methodology for understanding water structuration in carbohydrate particulate hydrogels (SDTD NMR) (this is now published) |
| Exploitation Route | The NMR methods we have developed are easy to setup and of general use for the community of gel-like materials. Our novel STD NMR approach to characterise the degree of solvent structuration in gels might be extended further to the study or other types of soft matter such as living tissue. For example, this method opens promising avenues for the characterisation of tissue integrity in a clinical context. |
| Sectors | Agriculture, Food and Drink,Environment,Healthcare,Manufacturing, including Industrial Biotechology,Pharmaceuticals and Medical Biotechnology |
| URL | https://www.gelenz.com/ |
| Description | The impact of this work is recorded against grant ref EP/N03340X/2' |
| First Year Of Impact | 2022 |
| Sector | Manufacturing, including Industrial Biotechology |
| Impact Types | Policy & public services |
| Title | Novel NMR method for characterisation of hydration in soft matter |
| Description | We developed novel STD NMR methodology using residual HDO in D2O solvated hydrogel samples of particulate gelators to monitor changes in the populations of surface-confined water molecules with temperature. The ease of the STD NMR methodology may allow a future boost in the use of HDO-based STD NMR experiments to correlate changes in confined water populations with rheology, within the hydrogel research community. |
| Type Of Material | Technology assay or reagent |
| Year Produced | 2019 |
| Provided To Others? | Yes |
| Impact | This methodology forms a part of our programme of developing of advanced NMR tools for soft materials . |
| Title | Novel NMR method for studying water structuration in carbohydrate based hydrogels (SDTD NMR) |
| Description | The classical STD NMR protocol to monitor water interactions in gels is strongly dependent on gelator and solvent concentrations and does not report on the degree of structuration of the solvent at the particle/solvent interface. We hypothesised that, for suspensions of large gelator particles, solvent structuration could be characterised by STD NMR when taking into account the particle-to-solvent 1H-1H spin diffusion transfer using the 1D diffusion equation. We have carried out a systematic study on effect of gelator and solvent concentrations, and gelator surface charge, affecting the behaviour of the classical STD NMR build-up curves. To do so, we have characterised solvent interactions in dispersions of starch and cellulose-like particles prepared in deuterated water and alcohol/D2O mixtures. The Spin Diffusion Transfer Difference (SDTD) NMR protocol is independent of the gelator and solvent concentrations, hence allowing the estimation of the degree of solvent structuration within different particle networks. In addition, the simulation of SDTD build-up curves using the general onedimensional diffusion equation allows the determination of minimum distances (r) and spin diffusion rates (D) at the particle/solvent interface. This novel NMR protocol can be readily extended to characterise the solvent(s) organisation in any type of colloidal systems constituted by large particles. |
| Type Of Material | Technology assay or reagent |
| Year Produced | 2020 |
| Provided To Others? | Yes |
| Impact | This novel NMR protocol can be readily extended to characterise the solvent(s) organisation in any type of colloidal systems constituted by large particles. |
| Title | Dataset for "Surfactant controlled zwitterionic cellulose nanofibril dispersions" |
| Description | Dataset for each figure appearing in the manuscript, "Surfactant controlled zwitterionic cellulose nanofibril dispersions". Fig. 2 shows the z-potential (mV) of ZCNF and OCNF dispersions as a function of pH. The average and standard deviation of values obtained for duplicate samples are reported. Fig. 3 shows the z-potential (mV) of ZCNF dispersions at 0.01 wt% upon addition of 25 mM SDS, 25 mM DTAB and 25 mM TW80 is presented as an average of measurements on duplicate samples. Fig. 4 shows the surface tension at the air-water interface (gamma-aw) of 0.001 wt% ZCNF dispersions upon addition of (a) 125 mMSDS,(b) 125 mM DTAB and (c) 2.5 mM TW80. The average of duplicate measurements is reported. Fig. 6 shows the relative viscosity (eta-r) as a function of shear rate (s-1) for 0.5 wt% ZCNF dispersions containing (a) SDS, (b) DTAB and (c) TW80. Fig. 7 shows the relative viscosity (eta-r) as a function of the shear rate (s-1) for 0.5 wt% ZCNF containing 50 mM SDS, 50 mM DTAB and 50 mM TW80. Fig. 8 shows the SANS data for 0.5 wt% ZCNF dispersions in the presence of 1 mM d-SDS and 5mMd-DTAB in D2O. The data were fitted with a model of cylinder with an elliptical cross section. The intensity (I) is given in arbitrary units (A.U.). |
| Type Of Material | Database/Collection of data |
| Year Produced | 2018 |
| Provided To Others? | Yes |
| Title | Dataset for Charge-driven interfacial gelation of cellulose nanofibrils across the water/oil interface |
| Description | The Dataset for Charge-driven interfacial gelation of cellulose nanofibrils across the water/oil interface contains data, in the form of Excel files, for the figures shown in the associated manuscript and the supplementary information. Each Excel file is specific for a set of data acquired utilising the same protocol. In the Excel file named "Data_rheology_Fig2_3_S4_S5", the rheological data presented in Figures 2 and 3 of the manuscript and Figures S4 and S5 from the supplementary information are shown. The data are subdivided in different spreadsheets in according to the concentration of oxidised cellulose nanofibrils (OCNF) and ionic strength employed (NaCl concentration in mM), as specified at the top of each spreadsheet. In the Excel file named "Data_rheology_Fig4", the rheological data presented in Figure 4 are shown. For all the rheological data, parameters as Gi* (N/m), tani(d) (-), Gi' (N/m) and Gi'' (N/m) are given as function of time (h) or strain amplitude (%) as shown in the relative figures. In the Excel file named "Data_surface tension_Fig_S1", the surface tension measured at the oil-air interface (gamma, mN/m) as a function of Oleylamine (OA) concentration (mM) is given as illustrated in Figure S1 from the supplementary material. Specification of the materials and methods employed throughout the data collection are available in the associated manuscript. |
| Type Of Material | Database/Collection of data |
| Year Produced | 2019 |
| Provided To Others? | Yes |
| URL | https://researchdata.bath.ac.uk/id/eprint/662 |