Advanced characterization of regioselectively substituted methylcellulose model compounds by DNP enhanced solid-state NMR spectroscopy

Berruyer, Pierrick; Gericke, Martin; Moutzouri, Pinelopi; Jakobi, Dörthe; Bardet, Michel; Karlson, Leif; Schantz, Staffan; Heinze, Thomas; Emsley, Lyndon

doi:10.1016/j.carbpol.2021.117944

Cited by 25 publications

(21 citation statements)

References 54 publications

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“…It can be speculated that these phenyl groups are more flexible compared to ones that are attached to secondary positions C-2 and C-3 and that this flexibility enables secondary interaction (e.g., π-π stacking) of the aromatic groups resulting in stronger attraction of the polymer chains and aggregation into larger agglomerates. It might be possible to verify this hypothesis in future studies by using regioselectively modified 2,3- O -CPC, which can be synthesized using protecting group strategies [ 29 ].…”

Section: Resultsmentioning

confidence: 99%

Reactive Nanoparticles Derived from Polysaccharide Phenyl Carbonates

et al. 2021

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Polysaccharide (PS) based nanoparticles (NP) are of great interest for biomedical applications. A key challenge in this regard is the functionalization of these nanomaterials. The aim of the present work was the development of reactive PS-NP that can be coupled with an amino group containing compounds under mild aqueous conditions. A series of cellulose phenyl carbonates (CPC) and xylan phenyl carbonates (XPC) with variable degrees of substitution (DS) was obtained by homogeneous synthesis. The preparation of PS-NP by self-assembling of these hydrophobic derivatives was studied comprehensively. While CPC mostly formed macroscopic aggregates, XPC formed well-defined spherical NP with diameters around 100 to 200 nm that showed a pronounced long-term stability in water against both particle aggregation as well as cleavage of phenyl carbonate moieties. Using an amino group functionalized dye it was demonstrated that the novel XPC-NP are reactive towards amines. A simple coupling procedure was established that enables direct functionalization of the reactive NP in an aqueous dispersion. Finally, it was demonstrated that dye functionalized XPC-NP are non-cytotoxic and can be employed in advanced biomedical applications.

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Section: Resultsmentioning

confidence: 99%

Reactive Nanoparticles Derived from Polysaccharide Phenyl Carbonates

et al. 2021

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“…Recently, SCREAM-DNP has been investigated by Sergeyev et al in HIV-1 CA assemblies where the authors analyzed the CP-based indirect DNP, direct DNP, as well as SCREAM-DNP pathways providing an overview of their dependence on the PA . Furthermore, SCREAM-DNP was used for characterization of regioselectivity in two cellulose methyl ethers with a well-defined molecular structure in terms of overall degree of substitution with methyl groups . Besides methyl groups, Park et al have proven that similar dynamics in primary amine and ammonium groups support the indirect polarization transfer from hyperpolarized 1 H to their nitrogen under direct 15 N DNP .…”

Section: Perspectives Developments and Outlookmentioning

confidence: 99%

Dynamic Nuclear Polarization for Sensitivity Enhancement in Biomolecular Solid-State NMR

et al. 2022

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Solid-state NMR with magic-angle spinning (MAS) is an important method in structural biology. While NMR can provide invaluable information about local geometry on an atomic scale even for large biomolecular assemblies lacking long-range order, it is often limited by low sensitivity due to small nuclear spin polarization in thermal equilibrium. Dynamic nuclear polarization (DNP) has evolved during the last decades to become a powerful method capable of increasing this sensitivity by two to three orders of magnitude, thereby reducing the valuable experimental time from weeks or months to just hours or days; in many cases, this allows experiments that would be otherwise completely unfeasible. In this review, we give an overview of the developments that have opened the field for DNP-enhanced biomolecular solid-state NMR including state-of-the-art applications at fast MAS and high magnetic field. We present DNP mechanisms, polarizing agents, and sample constitution methods suitable for biomolecules. A wide field of biomolecular NMR applications is covered including membrane proteins, amyloid fibrils, large biomolecular assemblies, and biomaterials. Finally, we present perspectives and recent developments that may shape the field of biomolecular DNP in the future.

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“…Natural-abundance DNP has also been used to determine the extent of delignification in wood material subjected to pretreatment (lignin extraction) and to analyze the monolignol units and linkages in wild-type poplar and a mutant with a high content of S-units (Figure B) . DNP has also been employed to characterize cellulose derivatives and understand the regioselectivity of cellulose methylation . The DNP-enabled 2D 13 C– 13 C INADEQUATE spectra of unlabeled cellulose derivatives provided sufficient resolution for identifying the methylation site.…”

Section: Solid-state Nmr Studies Of Plant Materialsmentioning

confidence: 99%

Solid-State NMR Investigations of Extracellular Matrixes and Cell Walls of Algae, Bacteria, Fungi, and Plants

et al. 2021

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Extracellular matrixes (ECMs), such as the cell walls and biofilms, are important for supporting cell integrity and function and regulating intercellular communication. These biomaterials are also of significant interest to the production of biofuels and the development of antimicrobial treatment. Solid-state nuclear magnetic resonance (ssNMR) and magic-angle spinning-dynamic nuclear polarization (MAS-DNP) are uniquely powerful for understanding the conformational structure, dynamical characteristics, and supramolecular assemblies of carbohydrates and other biomolecules in ECMs. This review highlights the recent high-resolution investigations of intact ECMs and native cells in many organisms spanning across plants, bacteria, fungi, and algae. We spotlight the structural principles identified in ECMs, discuss the current technical limitation and underexplored biochemical topics, and point out the promising opportunities enabled by the recent advances of the rapidly evolving ssNMR technology.

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Advanced characterization of regioselectively substituted methylcellulose model compounds by DNP enhanced solid-state NMR spectroscopy

Cited by 25 publications

References 54 publications

Reactive Nanoparticles Derived from Polysaccharide Phenyl Carbonates

Reactive Nanoparticles Derived from Polysaccharide Phenyl Carbonates

Dynamic Nuclear Polarization for Sensitivity Enhancement in Biomolecular Solid-State NMR

Solid-State NMR Investigations of Extracellular Matrixes and Cell Walls of Algae, Bacteria, Fungi, and Plants

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