Selective oxidation of silanes into silanols with water using [MnBr(CO)<sub>5</sub>] as a precatalyst

Antico, Emanuele; Leutzsch, Markus; Wessel, Niklas; Weyhermüller, Thomas; Werlé, Christophe; Leitner, Walter

doi:10.1039/d2sc05959b

Cited by 13 publications

(6 citation statements)

References 64 publications

(41 reference statements)

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“…The water infiltrated into the nanonetwork seemed to trigger the reaction of unreacted functions during the nanofiber fabrication process as shown by the increase of the gel fractions (figure 3(C)) just after immersion in the degradation medium (PLA -Si-XL, (PLA/ G 40 −0.2%) -Si-XL, and (PLA/G 40 −2%) -Si-XL ). The aqueous catalysis of silane functions is well described in the literature as well as the water-ageing of this kind of materials [33,34]. According to our results, this new link formation occurred in the first three days, and did not interfere with the gradual decrease of the gel fraction over the following 30 d.…”

Section: Hybrid Nanofibers Degradationsupporting

confidence: 82%

Development of hybrid bioactive nanofibers composed of star Poly(lactic acid) and gelatin by sol–gel crosslinking during the electrospinning process

Belabbes,

Simon,

Leon-Valdivieso

et al. 2023

Nanotechnology

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The design of a biomimetic scaffold is a major challenge in tissue engineering to promote tissue reconstruction. The use of synthetic polymer nanofibers is widely described as they provide biocompatible matrices whose topography mimics natural extracellular matrix (ECM). To closely match the biochemical composition of the ECM, bioactive molecules such as gelatin are added to the nanofibers to enhance cell adhesion and proliferation. To overcome the rapid solubilization of gelatin in biological fluids and to allow a lasting biological effect, the covalent crosslinking of this macromolecule in the network is crucial. The sol–gel route offers the possibility of gentle crosslinking during shaping but is rarely combined with electrospinning. In this study, we present the creation of Poly(lactic acid)/Gelatin hybrid nanofibers by sol–gel route during electrospinning. To enable sol–gel crosslinking, we synthesized star-shaped PLA and functionalized it with silane groups; then we functionalized gelatin with the same groups for their subsequent reaction with the polymer and thus the creation of the hybrid nanonetwork. We evaluated the impact of the presence of gelatin in Poly(lactic acid)/Gelatin hybrid nanofibers at different percentages on the mechanical properties, nanonetwork crosslinking, degradation and biological properties of the hybrid nanofibers. The addition of gelatin modulated nanonetwork crosslinking that impacted the stiffness of the nanofibers, resulting in softer materials for the cells. Moreover, these hybrid nanofibers also showed a significant improvement in fibroblast proliferation and present a degradation rate suitable for tissue reconstruction. Finally, the bioactive hybrid nanofibers possess versatile properties, interesting for various potential applications in tissue reconstruction.

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Section: Hybrid Nanofibers Degradationsupporting

confidence: 82%

Development of hybrid bioactive nanofibers composed of star Poly(lactic acid) and gelatin by sol–gel crosslinking during the electrospinning process

Belabbes,

Simon,

Leon-Valdivieso

et al. 2023

Nanotechnology

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“…Following from this, auto-VTNA was applied to kinetic data from 22 publications, including stoichiometric and catalytic reactions (Table 4, entries 1-14) containing up to 6 reaction species (reactants, reagents, catalyst and additives). 5,8,9,34,[37][38][39][40][41][42][43][44][45][46] The current approach to VTNA experimentation involves performing a "standard" reaction, under synthetically relevant conditions, followed by "different excess" experiments, where only the initial concentration of each reaction species is altered.…”

Section: Automatic Determination Of Rate Equations Using Auto-vtnamentioning

confidence: 99%

Auto-VTNA: An Automatic VTNA platform for Determination of Global Rate Equations

Dalland,

Schrecker,

Hii

2024

Preprint

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The ability and desire to generate kinetic data has greatly increased in recent years, requiring more automated and quantitative methods for analysis. In this work, an automated program (Auto-VTNA) is developed, to simplify the kinetic analysis workflow. The Auto-VTNA solver allows all the reaction orders to be determined concurrently, expediting the process of kinetic analysis. Auto-VTNA performs well on noisy or sparse data sets and can handle complex reactions involving changing reaction orders. Quantitative error analysis and facile visualisation allows users to numerically justify and robustly present their findings. Auto-VTNA can be used through a free graphical user interface (GUI), requiring no coding or kinetic knowledge from the user, or can be customised and built on if required.

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“…Mechanism study based on spectroscopic techniques and the reaction kinetics shows that cationic tricarbonyl Mn(I) is the active species in the catalytic cycle (Scheme 5). [21] In addition, Chan and Meng described the dehydrogenative coupling of silanes with hydroxyl compounds (alcohols, phenols, indoles, and water) catalyzed by Mn(CO) 10 and phosphineoxide under heating conditions (> 91 examples, up to 99 % yield) (Scheme 6). In this study, they found phosphineoxide ligand is essential for this catalytic system, because the conversion of silane to silanol was slow in the absence of phosphineoxide.…”

Section: Mn-catalyzed Oxidation Of Hydrosilanesmentioning

confidence: 99%

“…Mechanism study based on spectroscopic techniques and the reaction kinetics shows that cationic tricarbonyl Mn(I) is the active species in the catalytic cycle (Scheme 5). [21] …”

Section: Transition‐metal‐catalyzed Hydroxylation Of Hydrosilanesmentioning

confidence: 99%

Catalytic Synthesis of Silanols by Hydroxylation of Hydrosilanes: From Chemoselectivity to Enantioselectivity

Huang,

Xu,

Yang

et al. 2023

Chemistry A European J

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As a crucial class of functional molecules in organosilicon chemistry, silanols are found valuable applications in the fields of modern science and will be a potentially powerful framework for biologically active compounds or functional materials. It has witnessed an increasing demand for non‐natural organosilanols, as well as the progress in the synthesis of these structural features. From the classic preparative methods to the catalytic selective oxidation of hydrosilanes, electrochemical hydrolysis of hydrosilanes, and then the construction of the most challenging silicon‐stereogenic silanols. This review summarized the progress in the catalyzed synthesis of silanols via hydroxylation of hydrosilanes in the last decade, with a particular emphasis on the latest elegant developments in the desymmetrization strategy for the enantioselective synthesis of silicon‐stereogenic silanols from dihydrosilanes.

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Selective oxidation of silanes into silanols with water using [MnBr(CO)₅] as a precatalyst

Abstract: This study presents the use of MnBr(CO)5 for the selective conversion of silanes to silanols with water as an oxidant generating valuable hydrogen as the only by-product.

Cited by 13 publications

References 64 publications

Development of hybrid bioactive nanofibers composed of star Poly(lactic acid) and gelatin by sol–gel crosslinking during the electrospinning process

Development of hybrid bioactive nanofibers composed of star Poly(lactic acid) and gelatin by sol–gel crosslinking during the electrospinning process

Auto-VTNA: An Automatic VTNA platform for Determination of Global Rate Equations

Catalytic Synthesis of Silanols by Hydroxylation of Hydrosilanes: From Chemoselectivity to Enantioselectivity

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Selective oxidation of silanes into silanols with water using [MnBr(CO)5] as a precatalyst

Abstract: This study presents the use of MnBr(CO)5 for the selective conversion of silanes to silanols with water as an oxidant generating valuable hydrogen as the only by-product.

Cited by 13 publications

References 64 publications

Development of hybrid bioactive nanofibers composed of star Poly(lactic acid) and gelatin by sol–gel crosslinking during the electrospinning process

Development of hybrid bioactive nanofibers composed of star Poly(lactic acid) and gelatin by sol–gel crosslinking during the electrospinning process

Auto-VTNA: An Automatic VTNA platform for Determination of Global Rate Equations

Catalytic Synthesis of Silanols by Hydroxylation of Hydrosilanes: From Chemoselectivity to Enantioselectivity

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Selective oxidation of silanes into silanols with water using [MnBr(CO)₅] as a precatalyst