Pub Date : 2024-10-18DOI: 10.1016/j.carbpol.2024.122865
Ye Wang , Chong Chen , Changyuan He , Wentao Dong , Xuekun Yang , Qingquan Kong , Bin Yan , Jin He
Management of chronic diabetic wounds is challenging due to excess reactive oxygen species (ROS), hypoxia, persistent inflammation, and bacterial infection within the wound microenvironment. For addressing the aforementioned concern, we have developed a multifunctional hydrogel dressing (PMT-C@PhM) based on chitosan with self-healing, adhesive, antibacterial, and antioxidant capacities for therapeutic diabetic wounds. The hydrogel dressing consisted of quaternary ammonium salt- and catechol- modified chitosan (CQCS), thioctic acid-functionalized poly(ethylene glycol)s (PEGs), and polydopamine-coated honeycomb manganese dioxide nanoparticles (hMnO2@PDA NPs). The nanozyme-modified hydrogel exhibits superoxide dismutase (SOD) and catalase (CAT) activities to scavenge ROS while generating oxygen to alleviate oxidative stress and hypoxic environment in wounds, and to attenuate the inflammatory response through modulating macrophage polarization. The PMT-C@PhM hydrogel is effective in the treatment of diabetic wound infections caused by Staphylococcus aureus, and relieves oxidative stress, inhibits inflammation, and promotes neovascularization and dermal collagen synthesis thus providing favorable conditions for accelerated wound healing. In conclusion, the aforementioned approach offers a biosafe, straightforward, and efficient strategy for the management of diabetic wounds.
{"title":"Quaternized chitosan-based biomimetic nanozyme hydrogels with ROS scavenging, oxygen generating, and antibacterial capabilities for diabetic wound repair","authors":"Ye Wang , Chong Chen , Changyuan He , Wentao Dong , Xuekun Yang , Qingquan Kong , Bin Yan , Jin He","doi":"10.1016/j.carbpol.2024.122865","DOIUrl":"10.1016/j.carbpol.2024.122865","url":null,"abstract":"<div><div>Management of chronic diabetic wounds is challenging due to excess reactive oxygen species (ROS), hypoxia, persistent inflammation, and bacterial infection within the wound microenvironment. For addressing the aforementioned concern, we have developed a multifunctional hydrogel dressing (PMT-C@PhM) based on chitosan with self-healing, adhesive, antibacterial, and antioxidant capacities for therapeutic diabetic wounds. The hydrogel dressing consisted of quaternary ammonium salt- and catechol- modified chitosan (CQCS), thioctic acid-functionalized poly(ethylene glycol)s (PEGs), and polydopamine-coated honeycomb manganese dioxide nanoparticles (hMnO<sub>2</sub>@PDA NPs). The nanozyme-modified hydrogel exhibits superoxide dismutase (SOD) and catalase (CAT) activities to scavenge ROS while generating oxygen to alleviate oxidative stress and hypoxic environment in wounds, and to attenuate the inflammatory response through modulating macrophage polarization. The PMT-C@PhM hydrogel is effective in the treatment of diabetic wound infections caused by <em>Staphylococcus aureus</em>, and relieves oxidative stress, inhibits inflammation, and promotes neovascularization and dermal collagen synthesis thus providing favorable conditions for accelerated wound healing. In conclusion, the aforementioned approach offers a biosafe, straightforward, and efficient strategy for the management of diabetic wounds.</div></div>","PeriodicalId":261,"journal":{"name":"Carbohydrate Polymers","volume":"348 ","pages":"Article 122865"},"PeriodicalIF":10.7,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142528406","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chitin nanocrystals (ChNCs), prepared from a down-sizing process from chitin, have recently captured great attention to access sustainable nanomaterials. The surface modification of ChNCs is crucial to regulate the surface physicochemical properties and introduce specific functions, thus satisfying their diverse applications. In this study, aldehyde-functionalized ChNCs (ChNCs-PVMA) with enhanced hydrophobicity were developed via surface-initiated activators regenerated by electron transfer for atom transfer radical polymerization (SI-ARGET ATRP) of a lignin-derived polymerizable aldehyde monomer, vanillin methacrylate (VMA). The monomer conversion was determined by 1H NMR spectroscopy of the reaction mixture based on the change of the relative ratio of VMA and solvent signals. The prepared ChNCs-PVMA were systematically characterized by FTIR, CP/MAS 13C NMR, XPS, XRD, DSC, TGA, and TEM. The dispersibility of ChNCs and ChNCs-PVMA in water and DMF was evaluated by dynamic light scattering and visual observation, indicating good dispersion of ChNCs-PVMA in organic solvents. Furthermore, based on the available aldehyde groups, the ChNCs-PVMA was reacted with amino acids via Schiff base reaction, demonstrating a rich follow-up chemistry towards diverse functions by the reactive aldehyde groups.
{"title":"Aldehyde-functionalization of chitin nanocrystals via SI-ARGET ATRP of lignin-derived monomers","authors":"Tongjun Yang, Rongli Li, Mingtao Ding, Hong Yu, Lihua Zhang, Haibo Xie","doi":"10.1016/j.carbpol.2024.122892","DOIUrl":"10.1016/j.carbpol.2024.122892","url":null,"abstract":"<div><div>Chitin nanocrystals (ChNCs), prepared from a down-sizing process from chitin, have recently captured great attention to access sustainable nanomaterials. The surface modification of ChNCs is crucial to regulate the surface physicochemical properties and introduce specific functions, thus satisfying their diverse applications. In this study, aldehyde-functionalized ChNCs (ChNCs-PVMA) with enhanced hydrophobicity were developed <em>via</em> surface-initiated activators regenerated by electron transfer for atom transfer radical polymerization (SI-ARGET ATRP) of a lignin-derived polymerizable aldehyde monomer, vanillin methacrylate (VMA). The monomer conversion was determined by <sup>1</sup>H NMR spectroscopy of the reaction mixture based on the change of the relative ratio of VMA and solvent signals. The prepared ChNCs-PVMA were systematically characterized by FTIR, CP/MAS <sup>13</sup>C NMR, XPS, XRD, DSC, TGA, and TEM. The dispersibility of ChNCs and ChNCs-PVMA in water and DMF was evaluated by dynamic light scattering and visual observation, indicating good dispersion of ChNCs-PVMA in organic solvents. Furthermore, based on the available aldehyde groups, the ChNCs-PVMA was reacted with amino acids <em>via</em> Schiff base reaction, demonstrating a rich follow-up chemistry towards diverse functions by the reactive aldehyde groups.</div></div>","PeriodicalId":261,"journal":{"name":"Carbohydrate Polymers","volume":"348 ","pages":"Article 122892"},"PeriodicalIF":10.7,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142528411","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-18DOI: 10.1016/j.carbpol.2024.122893
Abolfazl Heydari , Nassim Borazjani , Fereshteh Kazemi-Aghdam , Juraj Filo , Igor Lacík
DMTMM-mediated amidation of sodium alginate is one of the methods used for the chemical modification of alginate with amines. However, there is a limited understanding of how the reaction conditions, particularly the pH value, influence the conjugation efficiency (CE) and the resulting degree of substitution (DS). In this study, we investigated the effect of the pH during the reaction, focusing on both neutral and weakly basic conditions, using water and buffer as solvents. Two model amines with high pKaH values were selected, furfurylamine (FFA, pKaH = 9.12) and 4-(2-aminoethyl)morpholine (AEM, pKaH = 9.93). Sodium alginate with a high mannuronate content (60 mol%) and molar mass of 168 kg·mol−1 was used for amidation. Our results show that both FFA and AEM effectively conjugate to sodium alginate under the selected reaction conditions. We found that pH significantly affects both CE and DS, which varied between 2 % to 40 % and 3 % to 53 %, respectively, depending on the specific reaction conditions. Optimal conditions were observed at neutral pH in water, whereas weak basic pH led to lower CE. Our findings thus offer a recommendation for optimizing the DMTMM-mediated amidation of sodium alginate, emphasizing the importance of pH values during the reaction.
{"title":"DMTMM-mediated amidation of sodium alginate in aqueous solutions: pH-dependent efficiency of conjugation","authors":"Abolfazl Heydari , Nassim Borazjani , Fereshteh Kazemi-Aghdam , Juraj Filo , Igor Lacík","doi":"10.1016/j.carbpol.2024.122893","DOIUrl":"10.1016/j.carbpol.2024.122893","url":null,"abstract":"<div><div>DMTMM-mediated amidation of sodium alginate is one of the methods used for the chemical modification of alginate with amines. However, there is a limited understanding of how the reaction conditions, particularly the pH value, influence the conjugation efficiency (CE) and the resulting degree of substitution (DS). In this study, we investigated the effect of the pH during the reaction, focusing on both neutral and weakly basic conditions, using water and buffer as solvents. Two model amines with high p<em>K</em><sub>a</sub>H values were selected, furfurylamine (FFA, p<em>K</em><sub>a</sub>H = 9.12) and 4-(2-aminoethyl)morpholine (AEM, p<em>K</em><sub>a</sub>H = 9.93). Sodium alginate with a high mannuronate content (60 mol%) and molar mass of 168 kg·mol<sup>−1</sup> was used for amidation. Our results show that both FFA and AEM effectively conjugate to sodium alginate under the selected reaction conditions. We found that pH significantly affects both CE and DS, which varied between 2 % to 40 % and 3 % to 53 %, respectively, depending on the specific reaction conditions. Optimal conditions were observed at neutral pH in water, whereas weak basic pH led to lower CE. Our findings thus offer a recommendation for optimizing the DMTMM-mediated amidation of sodium alginate, emphasizing the importance of pH values during the reaction.</div></div>","PeriodicalId":261,"journal":{"name":"Carbohydrate Polymers","volume":"348 ","pages":"Article 122893"},"PeriodicalIF":10.7,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142528409","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-18DOI: 10.1016/j.carbpol.2024.122870
Xiaojie Lu , Yue Jing , Naisheng Zhang , Lei Chen , Jiandong Tai , Yongguo Cao
Obesity is a serious public health challenge worldwide, the present study is aimed to investigate the structural characteristic and anti-obesity effect of a water-soluble galactomannan (PEC) extracted from Eurotium cristatum (E. cristatum). Detailed analysis of the PEC structure showed a weight-average molecular weight of 32,305 Da and a composition of mainly mannose, galactose and small amounts of glucose. Nuclear magnetic resonance spectroscopy combined with methylation analysis indicated that the main chain of PEC is →5)-β-D-Galf-(1 → 6)-α-D-Manp-(1 → glycosidic bond, and the branched chain →2)-α-D-Manp-(1 → through →2,6)-α-D-Manp-(1 → is connected to the main chain by an O-2 bond. Furthermore, PEC was found to ameliorate body weight gain, metabolic disorders, and to modulate the gut microbiota in HFD-fed mice. Fecal microbiota transplantation trial confirmed that PEC prevented obesity development and metabolic disorders by reversing gut dysbiosis in HFD-fed mice. This is the first report of the isolation of PEC from E. cristatum, and the findings suggested that PEC exerted its antiobesity and related beneficial effects by regulating the gut microbiota. In conclusion, as a polysaccharide, PEC could reduce obesity by modulating the gut microbiota and has potential been a prophylactic agent for obesity and related metabolic diseases.
{"title":"Structural characterization and anti-obesity effect of a novel water-soluble galactomannan isolated from Eurotium cristatum","authors":"Xiaojie Lu , Yue Jing , Naisheng Zhang , Lei Chen , Jiandong Tai , Yongguo Cao","doi":"10.1016/j.carbpol.2024.122870","DOIUrl":"10.1016/j.carbpol.2024.122870","url":null,"abstract":"<div><div>Obesity is a serious public health challenge worldwide, the present study is aimed to investigate the structural characteristic and anti-obesity effect of a water-soluble galactomannan (PEC) extracted from <em>Eurotium cristatum</em> (<em>E. cristatum</em>). Detailed analysis of the PEC structure showed a weight-average molecular weight of 32,305 Da and a composition of mainly mannose, galactose and small amounts of glucose. Nuclear magnetic resonance spectroscopy combined with methylation analysis indicated that the main chain of PEC is →5)-β-D-Galf-(1 → 6)-α-D-Manp-(1 → glycosidic bond, and the branched chain →2)-α-D-Manp-(1 → through →2,6)-α-D-Manp-(1 → is connected to the main chain by an O-2 bond. Furthermore, PEC was found to ameliorate body weight gain, metabolic disorders, and to modulate the gut microbiota in HFD-fed mice. Fecal microbiota transplantation trial confirmed that PEC prevented obesity development and metabolic disorders by reversing gut dysbiosis in HFD-fed mice. This is the first report of the isolation of PEC from <em>E. cristatum</em>, and the findings suggested that PEC exerted its antiobesity and related beneficial effects by regulating the gut microbiota. In conclusion, as a polysaccharide, PEC could reduce obesity by modulating the gut microbiota and has potential been a prophylactic agent for obesity and related metabolic diseases.</div></div>","PeriodicalId":261,"journal":{"name":"Carbohydrate Polymers","volume":"348 ","pages":"Article 122870"},"PeriodicalIF":10.7,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142561292","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-18DOI: 10.1016/j.carbpol.2024.122889
Qianqian Wang , Lin Zhong , Yang Zhou , Shixuan Feng , Jun Liu , Huan Liu , Qianqian Zhu
Cellulose nanomaterials (CNMs) with their remarkable properties and abundant natural sources have emerged as a versatile platform for material science. However, their widespread adoption to develop novel applications often hinges on precise control over their surface chemistry. Regioselective functionalization, i.e., the ability to modify specific hydroxy groups on the cellulose backbone or aldehyde reducing end group (REG), offers unparalleled control on their surface chemistry. This review highlights the exciting developments in regioselective functionalization of CNMs and their impacts on structure-property relationships. Key factors that influence regioselectivity are examined and exciting applications of regioselectively functionalized CNMs are reviewed. This review also highlights the need for efficient, large-scale regioselective functionalization techniques and identifies key areas for future research.
{"title":"Regioselective functionalization of cellulose nanomaterial for advanced application","authors":"Qianqian Wang , Lin Zhong , Yang Zhou , Shixuan Feng , Jun Liu , Huan Liu , Qianqian Zhu","doi":"10.1016/j.carbpol.2024.122889","DOIUrl":"10.1016/j.carbpol.2024.122889","url":null,"abstract":"<div><div>Cellulose nanomaterials (CNMs) with their remarkable properties and abundant natural sources have emerged as a versatile platform for material science. However, their widespread adoption to develop novel applications often hinges on precise control over their surface chemistry. Regioselective functionalization, i.e., the ability to modify specific hydroxy groups on the cellulose backbone or aldehyde reducing end group (REG), offers unparalleled control on their surface chemistry. This review highlights the exciting developments in regioselective functionalization of CNMs and their impacts on structure-property relationships. Key factors that influence regioselectivity are examined and exciting applications of regioselectively functionalized CNMs are reviewed. This review also highlights the need for efficient, large-scale regioselective functionalization techniques and identifies key areas for future research.</div></div>","PeriodicalId":261,"journal":{"name":"Carbohydrate Polymers","volume":"348 ","pages":"Article 122889"},"PeriodicalIF":10.7,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142552186","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-17DOI: 10.1016/j.carbpol.2024.122888
Chang Tian , Anthony Chun Yin Yuen , Jinlong Zhao , Timothy Bo Yuan Chen , Qian Chen , Ivan Miguel De Cachinho Cordeiro
A biomass fire suppression gel foam (FSGF) with outstanding thermal stability and fire resistance performance was synthesised to improve the flame retardancy of foam agents on liquid fuel fires. The foam comprehensive index, microstructure, thermal stability, fire resistance and extinguishing properties of the FSGF were benchmarked against aqueous film-forming foam (AFFF). Subsequently, reactive forcefield (ReaxFF) molecular dynamics (MD) simulations were performed on the FSGF to study the thermokinetic properties. Based on the experimental results, a porosity layer was found on the external film of FSGF, which enhanced the thermal stability of the foam. The gelling mechanism of the foam is the formation of an O–Ca–O bond. Through MD simulations it was discovered that the remained calcium oxide/hydroxide species when deposited on fuel surfaces would promote char formation as they capture H/O atoms via dehydration. Alternatively, the foam showed better thermal stability than that of AFFF due to a lower weight loss rate and longer collapse time. The extinguishing performance tests demonstrated that the fire extinguishing time and resistance time of FSGF respectively are 72 s and 801 s, showing a significant potential to suppress the re-ignition of tank fires.
{"title":"A facile sunflower pectin gel foam for liquid fuel fire suppression with ReaxFF characterisation on its char-enhancing ability","authors":"Chang Tian , Anthony Chun Yin Yuen , Jinlong Zhao , Timothy Bo Yuan Chen , Qian Chen , Ivan Miguel De Cachinho Cordeiro","doi":"10.1016/j.carbpol.2024.122888","DOIUrl":"10.1016/j.carbpol.2024.122888","url":null,"abstract":"<div><div>A biomass fire suppression gel foam (FSGF) with outstanding thermal stability and fire resistance performance was synthesised to improve the flame retardancy of foam agents on liquid fuel fires. The foam comprehensive index, microstructure, thermal stability, fire resistance and extinguishing properties of the FSGF were benchmarked against aqueous film-forming foam (AFFF). Subsequently, reactive forcefield (ReaxFF) molecular dynamics (MD) simulations were performed on the FSGF to study the thermokinetic properties. Based on the experimental results, a porosity layer was found on the external film of FSGF, which enhanced the thermal stability of the foam. The gelling mechanism of the foam is the formation of an O–Ca–O bond. Through MD simulations it was discovered that the remained calcium oxide/hydroxide species when deposited on fuel surfaces would promote char formation as they capture H/O atoms via dehydration. Alternatively, the foam showed better thermal stability than that of AFFF due to a lower weight loss rate and longer collapse time. The extinguishing performance tests demonstrated that the fire extinguishing time and resistance time of FSGF respectively are 72 s and 801 s, showing a significant potential to suppress the re-ignition of tank fires.</div></div>","PeriodicalId":261,"journal":{"name":"Carbohydrate Polymers","volume":"348 ","pages":"Article 122888"},"PeriodicalIF":10.7,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142528400","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-17DOI: 10.1016/j.carbpol.2024.122866
Xianghua Wu , Zhiheng Zhang , Haiying Lin , Qingge Feng , Bin Xue , Mingen Li , Zixuan Chen , Jiatong Lv , Lianghong Li
The use of chitosan-based sponge materials for Hg(II) removal has gained attention recently due to their effectiveness. However, the complex preparation, limited performance, and poor acid resistance remained major drawbacks. Herein, a nitrogen‑sulfur functionalized macroporous chitosan sponge was successfully synthesized via two mild amidation reactions and exhibited abundant interconnected mesopores. These features endowed the functionalized chitosan-based sponge with high adsorption capacity (1227.15 mg g−1), fast reaction rate (8.27 × 10−3 g mg−1·min−1), broad pH adaptability (1–7), and high selectivity, even in the artificial chlor-alkali wastewater. Furthermore, the impressive saturation capacity of 1329.24 mg g−1 was achieved in various heights and injection rates in the fixed-bed column test, and the good removal efficiency (>85 %) was maintained after six dynamic regeneration cycles. The excellent performance was primarily attributed to the chemisorption of CS groups. Among the three machine learning models, the ANFIS algorithm owned the best results of the smallest RMSE (0.00315) and highest R2 (0.9752) for predicting dynamic adsorptive behaviors. Overall, this research provided a reference for preparing a promising mesoporous sponge as an alternative recyclable and efficient candidate for industrial wastewater treatment and offered a machine learning model to predict the dynamic adsorptive performance.
{"title":"The static and dynamic adsorptive performance of a nitrogen and sulfur functionalized 3D chitosan sponge for mercury and its machine learning evaluation","authors":"Xianghua Wu , Zhiheng Zhang , Haiying Lin , Qingge Feng , Bin Xue , Mingen Li , Zixuan Chen , Jiatong Lv , Lianghong Li","doi":"10.1016/j.carbpol.2024.122866","DOIUrl":"10.1016/j.carbpol.2024.122866","url":null,"abstract":"<div><div>The use of chitosan-based sponge materials for Hg(II) removal has gained attention recently due to their effectiveness. However, the complex preparation, limited performance, and poor acid resistance remained major drawbacks. Herein, a nitrogen‑sulfur functionalized macroporous chitosan sponge was successfully synthesized via two mild amidation reactions and exhibited abundant interconnected mesopores. These features endowed the functionalized chitosan-based sponge with high adsorption capacity (1227.15 mg g<sup>−1</sup>), fast reaction rate (8.27 × 10<sup>−3</sup> g mg<sup>−1</sup>·min<sup>−1</sup>), broad pH adaptability (1–7), and high selectivity, even in the artificial chlor-alkali wastewater. Furthermore, the impressive saturation capacity of 1329.24 mg g<sup>−1</sup> was achieved in various heights and injection rates in the fixed-bed column test, and the good removal efficiency (>85 %) was maintained after six dynamic regeneration cycles. The excellent performance was primarily attributed to the chemisorption of C<img>S groups. Among the three machine learning models, the ANFIS algorithm owned the best results of the smallest RMSE (0.00315) and highest R<sup>2</sup> (0.9752) for predicting dynamic adsorptive behaviors. Overall, this research provided a reference for preparing a promising mesoporous sponge as an alternative recyclable and efficient candidate for industrial wastewater treatment and offered a machine learning model to predict the dynamic adsorptive performance.</div></div>","PeriodicalId":261,"journal":{"name":"Carbohydrate Polymers","volume":"348 ","pages":"Article 122866"},"PeriodicalIF":10.7,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142539080","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-17DOI: 10.1016/j.carbpol.2024.122863
Lars Passauer
Investigations on the pyrolysis and potential flame retardancy imparted by solvent-free and semi-dry phosphorylation of different starches using sodium orthophosphates were conducted. The samples – low-substituted starch phosphates (SP) with degrees of substitution DSP < 0.5 - were subjected to differential scanning calorimetry, thermogravimetry coupled with evolved gas analysis and pyrolysis – gas chromatography – mass spectrometry. The data obtained as well as features of charring residues examined using microscopic and spectroscopic methods were related to structural aspects of SP – analysed by means of various spectroscopic techniques - and compared with those of native starches. It was found that charring and polyphosphate formation and the thermal resistance of the solid SP residues increased significantly if the DSP was at least 0.1. Accordingly, the exothermal decomposition, the temperature-induced loss of mass and the decomposition rates of SP decreased distinctly compared to native starch. The activation temperatures of SP and the formation of low-molecular pyrolysis products including aliphatic, cyclic, and aromatic aldehydes and ketones as well as anhydrosugars decreased markedly, even at DSP < 0.1. The results confirm the potential flame-retardancy of SP achieved by flame-inhibiting effects, despite low phosphorylation degrees, in both the gas and condensed phases.
{"title":"Studies on the pyrolysis and potential flame retardancy of low-substituted starch phosphates","authors":"Lars Passauer","doi":"10.1016/j.carbpol.2024.122863","DOIUrl":"10.1016/j.carbpol.2024.122863","url":null,"abstract":"<div><div>Investigations on the pyrolysis and potential flame retardancy imparted by solvent-free and semi-dry phosphorylation of different starches using sodium orthophosphates were conducted. The samples – low-substituted starch phosphates (SP) with degrees of substitution DS<sub>P</sub> < 0.5 - were subjected to differential scanning calorimetry, thermogravimetry coupled with evolved gas analysis and pyrolysis – gas chromatography – mass spectrometry. The data obtained as well as features of charring residues examined using microscopic and spectroscopic methods were related to structural aspects of SP – analysed by means of various spectroscopic techniques - and compared with those of native starches. It was found that charring and polyphosphate formation and the thermal resistance of the solid SP residues increased significantly if the DS<sub>P</sub> was at least 0.1. Accordingly, the exothermal decomposition, the temperature-induced loss of mass and the decomposition rates of SP decreased distinctly compared to native starch. The activation temperatures of SP and the formation of low-molecular pyrolysis products including aliphatic, cyclic, and aromatic aldehydes and ketones as well as anhydrosugars decreased markedly, even at DS<sub>P</sub> < 0.1. The results confirm the potential flame-retardancy of SP achieved by flame-inhibiting effects, despite low phosphorylation degrees, in both the gas and condensed phases.</div></div>","PeriodicalId":261,"journal":{"name":"Carbohydrate Polymers","volume":"348 ","pages":"Article 122863"},"PeriodicalIF":10.7,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142552187","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-17DOI: 10.1016/j.carbpol.2024.122885
Yu Wang , Haojie Yu , Li Wang , Lei Zhang , Jinyi Liu , Dingning Chen , Jian Yang , Chenguang Ouyang , Jian Hu , Jingyi Feng , Chengjiang Li
Severely diabetic patients need insulin input to maintain the body's glycemic balance. However, traditional injection methods are often associated with poor adherence and an increased risk of hypoglycemia. Microneedle technology offers a promising solution by minimizing pain and trauma during insulin administration. Nonetheless, achieving prolonged glycemic control by microneedle with high insulin loading remains a significant challenge. Herein, we introduce an innovative microneedle patch that draws inspiration from the elegant light-induced blooming of water lily petals. The patch features a glucose-responsive hydrogel network crafted from two modified polysaccharide polymers, which enables the delivery of long-acting insulin without depending on glucose oxidase. By incorporating phenylboronic acid-modified sodium alginate, quaternary ammonium chitosan, and polyvinyl alcohol into a hydrogel matrix, we have created a microneedle system that harbors dynamic borate ester linkages and electrostatic attractions, resulting in heightened sensitivity to blood glucose levels. The electrostatic interaction acts as a relatively stable crosslinking point, balancing the dynamic reproducibility response based on the borate ester bond. This self-adaptive hydrogel can regulate insulin-controlled release by responding to changes in glucose concentration. Herein, we achieved massive insulin loading (20 IU) with long lasting glycaemic control (48 h) in a single treatment of diabetic SD rats.
{"title":"Intelligent microneedle patch based on functionalized alginate and chitosan for long-term self-regulated insulin delivery","authors":"Yu Wang , Haojie Yu , Li Wang , Lei Zhang , Jinyi Liu , Dingning Chen , Jian Yang , Chenguang Ouyang , Jian Hu , Jingyi Feng , Chengjiang Li","doi":"10.1016/j.carbpol.2024.122885","DOIUrl":"10.1016/j.carbpol.2024.122885","url":null,"abstract":"<div><div>Severely diabetic patients need insulin input to maintain the body's glycemic balance. However, traditional injection methods are often associated with poor adherence and an increased risk of hypoglycemia. Microneedle technology offers a promising solution by minimizing pain and trauma during insulin administration. Nonetheless, achieving prolonged glycemic control by microneedle with high insulin loading remains a significant challenge. Herein, we introduce an innovative microneedle patch that draws inspiration from the elegant light-induced blooming of water lily petals. The patch features a glucose-responsive hydrogel network crafted from two modified polysaccharide polymers, which enables the delivery of long-acting insulin without depending on glucose oxidase. By incorporating phenylboronic acid-modified sodium alginate, quaternary ammonium chitosan, and polyvinyl alcohol into a hydrogel matrix, we have created a microneedle system that harbors dynamic borate ester linkages and electrostatic attractions, resulting in heightened sensitivity to blood glucose levels. The electrostatic interaction acts as a relatively stable crosslinking point, balancing the dynamic reproducibility response based on the borate ester bond. This self-adaptive hydrogel can regulate insulin-controlled release by responding to changes in glucose concentration. Herein, we achieved massive insulin loading (20 IU) with long lasting glycaemic control (48 h) in a single treatment of diabetic SD rats.</div></div>","PeriodicalId":261,"journal":{"name":"Carbohydrate Polymers","volume":"348 ","pages":"Article 122885"},"PeriodicalIF":10.7,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142528402","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-16DOI: 10.1016/j.carbpol.2024.122880
Shumaila Arshad , Syed Atif Raza , Alamgeer , Syed Nasir Abbas Bukhari , Nasser F. Alotaibi , Naveed Ahmad , Hafiz Muhammad Irfan , Arshad Mahmood , Mulazim Hussain Asim
The current study aimed to generate a sulfhydryl-modified β-cyclodextrin-silymarin complex (sulfhydryl-modified β-CD-SMN complex) and to evaluate the enchantment in solubility, permeability, and bioavailability of a model BCS Class IV drug silymarin (SMN). For this purpose, sulfhydryl-modified β-CD was synthesized by replacing all primary and secondary –OH groups at the β-CD backbone with sulfhydryl groups via a novel microwave-assisted technique. Afterward, sulfhydryl-modified β-CD was complexed with silymarin and characterized by FTIR and 1H NMR spectroscopy. Moreover, no. of sulfhydryl groups and their oxidative stability, solubility, safety, mucoadhesion, release, diffusion, and rheological studies were performed. Furthermore, in-vivo studies were conducted to confirm enhanced pharmacokinetic properties of silymarin. Sulfhydryl-modified β-CD showed 8291 ± 418 μmol/g sulfhydryl groups that were prone to oxidation at pH ≥ 5, however, most of the sulfhydryl groups were found stable at pH 4 having a pKa value of 8.3. Modified β-CD oligomer showed improved solubility of SMN, significantly enhanced drug transport across goat intestinal mucosa, 78-fold improved mucoadhesion, improved drug dissolution and 4.4-fold enhanced dynamic viscosity. No toxic effects were reported to Caco-2 cells at 0.5% (m/v) concentration of sulfhydryl-modified β-CD for 24 h. The apparent permeability coefficient (Papp) of SMN was 6.9-fold enhanced on goat intestinal mucosa. Moreover, in-vivo studies confirmed a significantly enhanced oral bioavailability of SMN due to combination with sulfhydryl-modified β-CD. Based on these findings, the sulfhydryl-modified β-CD-silymarin inclusion complex can be a promising technique to enhance the bioavailability of BCS Class IV drugs via enhanced solubility, mucoadhesion, and permeability triple action.
{"title":"Microwave-assisted, sulfhydryl-modified β-cyclodextrin-silymarin inclusion complex: A diverse approach to improve oral drug bioavailability via enhanced mucoadhesion and permeation","authors":"Shumaila Arshad , Syed Atif Raza , Alamgeer , Syed Nasir Abbas Bukhari , Nasser F. Alotaibi , Naveed Ahmad , Hafiz Muhammad Irfan , Arshad Mahmood , Mulazim Hussain Asim","doi":"10.1016/j.carbpol.2024.122880","DOIUrl":"10.1016/j.carbpol.2024.122880","url":null,"abstract":"<div><div>The current study aimed to generate a sulfhydryl-modified β-cyclodextrin-silymarin complex (sulfhydryl-modified β-CD-SMN complex) and to evaluate the enchantment in solubility, permeability, and bioavailability of a model BCS Class IV drug silymarin (SMN). For this purpose, sulfhydryl-modified β-CD was synthesized by replacing all primary and secondary –OH groups at the β-CD backbone with sulfhydryl groups via a novel microwave-assisted technique. Afterward, sulfhydryl-modified β-CD was complexed with silymarin and characterized by FTIR and <sup>1</sup>H NMR spectroscopy. Moreover, no. of sulfhydryl groups and their oxidative stability, solubility, safety, mucoadhesion, release, diffusion, and rheological studies were performed. Furthermore, <em>in-vivo</em> studies were conducted to confirm enhanced pharmacokinetic properties of silymarin. Sulfhydryl-modified β-CD showed 8291 ± 418 μmol/g sulfhydryl groups that were prone to oxidation at pH ≥ 5, however, most of the sulfhydryl groups were found stable at pH 4 having a pKa value of 8.3. Modified β-CD oligomer showed improved solubility of SMN, significantly enhanced drug transport across goat intestinal mucosa, 78-fold improved mucoadhesion, improved drug dissolution and 4.4-fold enhanced dynamic viscosity. No toxic effects were reported to Caco-2 cells at 0.5% (m/v) concentration of sulfhydryl-modified β-CD for 24 h. The apparent permeability coefficient (P<sub>app</sub>) of SMN was 6.9-fold enhanced on goat intestinal mucosa. Moreover, <em>in-vivo</em> studies confirmed a significantly enhanced oral bioavailability of SMN due to combination with sulfhydryl-modified β-CD. Based on these findings, the sulfhydryl-modified β-CD-silymarin inclusion complex can be a promising technique to enhance the bioavailability of BCS Class IV drugs via enhanced solubility, mucoadhesion, and permeability triple action.</div></div>","PeriodicalId":261,"journal":{"name":"Carbohydrate Polymers","volume":"348 ","pages":"Article 122880"},"PeriodicalIF":10.7,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142528403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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