首页 > 最新文献

ACS polymers Au最新文献

英文 中文
Design of Highly Conductive PILs by Simple Modification of Poly(epichlorohydrin-co-ethylene oxide) with Monosubstituted Imidazoles 用单取代咪唑对聚(环氧氯丙烷-环氧乙烷)进行简单改性设计高导电性 PIL
Q1 POLYMER SCIENCE Pub Date : 2024-09-12 DOI: 10.1021/acspolymersau.4c00051
Daniil R. Nosov, Elena I. Lozinskaya, Dmitrii Y. Antonov, Denis O. Ponkratov, Andrey A. Tyutyunov, Malak Alaa Eddine, Cédric Plesse, Daniel F. Schmidt, Alexander S. Shaplov
High ionic conductivity poly(ionic liquid)s (PILs) are of growing interest for their thermal and electrochemical stability, processability, and potential in safe, flexible all-solid-state electrochemical devices. While various approaches to enhance the ionic conductivity are reported, the influence of cation substituents is rarely addressed. Moreover, some of the asymmetric anions recently developed for high-conductivity ionic liquids were never tested in PILs. We report the design and synthesis of twelve novel cationic PILs prepared via quaternization of N-substituted imidazoles by commercially available poly(epichlorohydrin-co-ethylene oxide) (poly(EPCH-r-EO)) with subsequent ion metathesis. They differ by imidazolium side chain length (C1–C6 alkyl) and presence of heteroatoms (silyl, siloxane, and fluoroalkyl) and by anion type (bis(trifluoromethylsulfonyl)imide (TFSI), 2,2,2-trifluoromethylsulfonyl-N-cyanoamide (TFSAM), tetrafluoroborate (BF4), trifluoro(trifluoromethyl)borate (BF3CF3), and tricyanofluoroborate (BF(CN)3)). TFSI-based PILs with alkyl side chains gave lower glass transition temperatures (Tg) and higher ionic conductivities than those bearing heteroatomic substituents, with n-butyl side chains providing a conductivity of 4.7 × 10–6 S cm–1 at 25 °C under anhydrous conditions. This increased to 1.0 × 10–5 and 4.5 × 10–4 S cm–1 at 25 and 70 °C, respectively, when the TFSI anion was replaced with BF(CN)3. All PILs showed good electrochemical (>3.2 V vs Ag+/Ag) and thermal (>185 °C) stability, making them excellent candidates for solid-state electrolytes in electrochemical devices.
高离子电导率聚(离子液体)因其热稳定性和电化学稳定性、可加工性以及在安全、灵活的全固态电化学装置中的应用潜力而日益受到关注。虽然提高离子电导率的方法层出不穷,但阳离子取代基的影响却鲜有报道。此外,最近开发的一些用于高电导率离子液体的不对称阴离子从未在 PIL 中进行过测试。我们报告了十二种新型阳离子 PIL 的设计与合成,这些 PIL 是通过市售的聚环氧氯丙烷-环氧乙烷(poly(EPCH-r-EO))对 N-取代咪唑进行季铵化并随后进行离子偏聚而制备的。它们因咪唑侧链长度(C1-C6 烷基)、杂原子(硅烷基、硅氧烷基和氟烷基)的存在以及阴离子类型(双(三氟甲基磺酰基)亚胺(TFSI))而有所不同、2,2,2-三氟甲磺酰-N-氰酰胺(TFSAM)、四氟硼酸盐(BF4)、三氟(三氟甲基)硼酸盐(BF3CF3)和三氰氟硼酸盐(BF(CN)3))。与含有杂原子取代基的 PIL 相比,带有烷基侧链的 TFSI 基 PIL 具有更低的玻璃化转变温度(Tg)和更高的离子电导率,其中正丁基侧链在 25 °C 无水条件下的电导率为 4.7 × 10-6 S cm-1。当 TFSI 阴离子被 BF(CN)3 取代时,25 ℃ 和 70 ℃ 下的电导率分别增至 1.0 × 10-5 和 4.5 × 10-4 S cm-1。所有 PIL 都表现出良好的电化学稳定性(3.2 V vs Ag+/Ag)和热稳定性(185 °C),是电化学设备中固态电解质的理想候选材料。
{"title":"Design of Highly Conductive PILs by Simple Modification of Poly(epichlorohydrin-co-ethylene oxide) with Monosubstituted Imidazoles","authors":"Daniil R. Nosov, Elena I. Lozinskaya, Dmitrii Y. Antonov, Denis O. Ponkratov, Andrey A. Tyutyunov, Malak Alaa Eddine, Cédric Plesse, Daniel F. Schmidt, Alexander S. Shaplov","doi":"10.1021/acspolymersau.4c00051","DOIUrl":"https://doi.org/10.1021/acspolymersau.4c00051","url":null,"abstract":"High ionic conductivity poly(ionic liquid)s (PILs) are of growing interest for their thermal and electrochemical stability, processability, and potential in safe, flexible all-solid-state electrochemical devices. While various approaches to enhance the ionic conductivity are reported, the influence of cation substituents is rarely addressed. Moreover, some of the asymmetric anions recently developed for high-conductivity ionic liquids were never tested in PILs. We report the design and synthesis of twelve novel cationic PILs prepared via quaternization of N-substituted imidazoles by commercially available poly(epichlorohydrin-<i>co</i>-ethylene oxide) (poly(EPCH-<i>r</i>-EO)) with subsequent ion metathesis. They differ by imidazolium side chain length (C<sub>1</sub>–C<sub>6</sub> alkyl) and presence of heteroatoms (silyl, siloxane, and fluoroalkyl) and by anion type (bis(trifluoromethylsulfonyl)imide (TFSI), 2,2,2-trifluoromethylsulfonyl-<i>N</i>-cyanoamide (TFSAM), tetrafluoroborate (BF<sub>4</sub>), trifluoro(trifluoromethyl)borate (BF<sub>3</sub>CF<sub>3</sub>), and tricyanofluoroborate (BF(CN)<sub>3</sub>)). TFSI-based PILs with alkyl side chains gave lower glass transition temperatures (<i>T</i><sub>g</sub>) and higher ionic conductivities than those bearing heteroatomic substituents, with <i>n</i>-butyl side chains providing a conductivity of 4.7 × 10<sup>–6</sup> S cm<sup>–1</sup> at 25 °C under anhydrous conditions. This increased to 1.0 × 10<sup>–5</sup> and 4.5 × 10<sup>–4</sup> S cm<sup>–1</sup> at 25 and 70 °C, respectively, when the TFSI anion was replaced with BF(CN)<sub>3</sub>. All PILs showed good electrochemical (&gt;3.2 V vs Ag<sup>+</sup>/Ag) and thermal (&gt;185 °C) stability, making them excellent candidates for solid-state electrolytes in electrochemical devices.","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"14 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142211002","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Design of Highly Conductive PILs by Simple Modification of Poly(epichlorohydrin-co-ethylene oxide) with Monosubstituted Imidazoles 单取代咪唑对聚环氧氯丙烷-环氧乙烷的简单改性设计高导电性药粒
IF 4.7 Q1 POLYMER SCIENCE Pub Date : 2024-09-12 DOI: 10.1021/acspolymersau.4c0005110.1021/acspolymersau.4c00051
Daniil R. Nosov, Elena I. Lozinskaya, Dmitrii Y. Antonov, Denis O. Ponkratov, Andrey A. Tyutyunov, Malak Alaa Eddine, Cédric Plesse, Daniel F. Schmidt* and Alexander S. Shaplov*, 

High ionic conductivity poly(ionic liquid)s (PILs) are of growing interest for their thermal and electrochemical stability, processability, and potential in safe, flexible all-solid-state electrochemical devices. While various approaches to enhance the ionic conductivity are reported, the influence of cation substituents is rarely addressed. Moreover, some of the asymmetric anions recently developed for high-conductivity ionic liquids were never tested in PILs. We report the design and synthesis of twelve novel cationic PILs prepared via quaternization of N-substituted imidazoles by commercially available poly(epichlorohydrin-co-ethylene oxide) (poly(EPCH-r-EO)) with subsequent ion metathesis. They differ by imidazolium side chain length (C1–C6 alkyl) and presence of heteroatoms (silyl, siloxane, and fluoroalkyl) and by anion type (bis(trifluoromethylsulfonyl)imide (TFSI), 2,2,2-trifluoromethylsulfonyl-N-cyanoamide (TFSAM), tetrafluoroborate (BF4), trifluoro(trifluoromethyl)borate (BF3CF3), and tricyanofluoroborate (BF(CN)3)). TFSI-based PILs with alkyl side chains gave lower glass transition temperatures (Tg) and higher ionic conductivities than those bearing heteroatomic substituents, with n-butyl side chains providing a conductivity of 4.7 × 10–6 S cm–1 at 25 °C under anhydrous conditions. This increased to 1.0 × 10–5 and 4.5 × 10–4 S cm–1 at 25 and 70 °C, respectively, when the TFSI anion was replaced with BF(CN)3. All PILs showed good electrochemical (>3.2 V vs Ag+/Ag) and thermal (>185 °C) stability, making them excellent candidates for solid-state electrolytes in electrochemical devices.

高离子电导率的聚离子液体(pil)因其热稳定性、电化学稳定性、可加工性以及在安全、柔性全固态电化学器件中的潜力而日益受到人们的关注。虽然有各种提高离子电导率的方法被报道,但阳离子取代基的影响很少得到解决。此外,最近开发的一些用于高导电性离子液体的不对称阴离子从未在pil中进行过测试。本文报道了用市售聚(环氧氯丙烷-环氧乙烷)(聚(EPCH-r-EO))对n-取代咪唑进行季铵盐化制备的12种新型阳离子吡啶醇的设计和合成。它们的区别在于咪唑侧链长度(C1-C6烷基)和是否存在杂原子(硅氧烷、硅氧烷和氟烷基)以及阴离子类型(二(三氟甲基磺酰基)亚胺(TFSI)、2,2,2-三氟甲基磺酰基- n -氰酰胺(TFSAM)、四氟硼酸盐(BF4)、三氟(三氟甲基)硼酸盐(BF3CF3)和三氰氟硼酸盐(BF(CN)3)))。与杂原子取代基相比,带有烷基侧链的tfsi基pls具有更低的玻璃化转变温度(Tg)和更高的离子电导率,其中正丁基侧链在25℃无水条件下的电导率为4.7 × 10-6 S cm-1。用BF(CN)3代替TFSI阴离子后,在25°C和70°C温度下,分别增加到1.0 × 10-5和4.5 × 10-4 S cm-1。所有pil均表现出良好的电化学稳定性(>3.2 V vs Ag+/Ag)和热稳定性(>185℃),使其成为电化学器件中固态电解质的优秀候选者。
{"title":"Design of Highly Conductive PILs by Simple Modification of Poly(epichlorohydrin-co-ethylene oxide) with Monosubstituted Imidazoles","authors":"Daniil R. Nosov,&nbsp;Elena I. Lozinskaya,&nbsp;Dmitrii Y. Antonov,&nbsp;Denis O. Ponkratov,&nbsp;Andrey A. Tyutyunov,&nbsp;Malak Alaa Eddine,&nbsp;Cédric Plesse,&nbsp;Daniel F. Schmidt* and Alexander S. Shaplov*,&nbsp;","doi":"10.1021/acspolymersau.4c0005110.1021/acspolymersau.4c00051","DOIUrl":"https://doi.org/10.1021/acspolymersau.4c00051https://doi.org/10.1021/acspolymersau.4c00051","url":null,"abstract":"<p >High ionic conductivity poly(ionic liquid)s (PILs) are of growing interest for their thermal and electrochemical stability, processability, and potential in safe, flexible all-solid-state electrochemical devices. While various approaches to enhance the ionic conductivity are reported, the influence of cation substituents is rarely addressed. Moreover, some of the asymmetric anions recently developed for high-conductivity ionic liquids were never tested in PILs. We report the design and synthesis of twelve novel cationic PILs prepared via quaternization of N-substituted imidazoles by commercially available poly(epichlorohydrin-<i>co</i>-ethylene oxide) (poly(EPCH-<i>r</i>-EO)) with subsequent ion metathesis. They differ by imidazolium side chain length (C<sub>1</sub>–C<sub>6</sub> alkyl) and presence of heteroatoms (silyl, siloxane, and fluoroalkyl) and by anion type (bis(trifluoromethylsulfonyl)imide (TFSI), 2,2,2-trifluoromethylsulfonyl-<i>N</i>-cyanoamide (TFSAM), tetrafluoroborate (BF<sub>4</sub>), trifluoro(trifluoromethyl)borate (BF<sub>3</sub>CF<sub>3</sub>), and tricyanofluoroborate (BF(CN)<sub>3</sub>)). TFSI-based PILs with alkyl side chains gave lower glass transition temperatures (<i>T</i><sub>g</sub>) and higher ionic conductivities than those bearing heteroatomic substituents, with <i>n</i>-butyl side chains providing a conductivity of 4.7 × 10<sup>–6</sup> S cm<sup>–1</sup> at 25 °C under anhydrous conditions. This increased to 1.0 × 10<sup>–5</sup> and 4.5 × 10<sup>–4</sup> S cm<sup>–1</sup> at 25 and 70 °C, respectively, when the TFSI anion was replaced with BF(CN)<sub>3</sub>. All PILs showed good electrochemical (&gt;3.2 V vs Ag<sup>+</sup>/Ag) and thermal (&gt;185 °C) stability, making them excellent candidates for solid-state electrolytes in electrochemical devices.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"4 6","pages":"512–526 512–526"},"PeriodicalIF":4.7,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acspolymersau.4c00051","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142844030","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Investigation of Antibacterial Coatings Based on Chitosan/Polyacrylic Acid/Chlorhexidine for Orthopedic Implants. 基于壳聚糖/聚丙烯酸/洗必泰的骨科植入物抗菌涂层研究
IF 4.7 Q1 POLYMER SCIENCE Pub Date : 2024-08-22 eCollection Date: 2024-12-11 DOI: 10.1021/acspolymersau.4c00049
Balzhan Savdenbekova, Ayazhan Seidulayeva, Aruzhan Sailau, Zhanar Bekissanova, Dilafruz Rakhmatullayeva, Ardak Jumagaziyeva

Antibacterial coatings on model silicon wafers and implants, based on chitosan (CHI), poly(acrylic acid) (PAA), and the antibacterial agent chlorhexidine digluconate (CHX), were obtained using a layer-by-layer assembly method. The surface roughness and 2D and 3D images of the surfaces of CHI/PAA/CHX coatings obtained from different pH assemblies were investigated by atomic force microscopy, revealing that pH 6 enabled optimal inclusion of CHX in the multilayer film. The structure and elemental composition before and after implementation of CHX into the coating were investigated via scanning electron microscopy and energy-dispersive X-ray spectroscopy. The obtained films exhibited antimicrobial efficacy against Staphylococcus aureus and Staphylococcus epidermidis. The effects of CHX concentration and duration of contact with the coating on bacterial activity were investigated, and the quantitative release of CHX from coated implants in phosphate buffer was determined as a function of the incubation time. The biocompatibility of the PAA/CHI/CHX coatings was investigated using human mononuclear cells (HMNCs) and quantified using an MTT assay. HMNCs demonstrated high viability in eluted solutions obtained from implants coated with PAA/CHI/CHX (0.025%) and PAA/CHI/CHX (0.0125%), while the extract of implants coated with PAA/CHI/CHX (0.05%) induced slight cytotoxicity.

采用逐层组装法在模型硅晶片和植入物上获得了基于壳聚糖(CHI)、聚丙烯酸(PAA)和抗菌剂二葡萄糖酸氯己定(CHX)的抗菌涂层。原子力显微镜研究了不同 pH 值组装得到的 CHI/PAA/CHX 涂层的表面粗糙度以及二维和三维图像,结果表明,pH 值为 6 时,CHX 在多层膜中的加入效果最佳。通过扫描电子显微镜和能量色散 X 射线光谱研究了在涂层中加入 CHX 前后的结构和元素组成。获得的薄膜对金黄色葡萄球菌和表皮葡萄球菌具有抗菌效果。研究了 CHX 浓度和与涂层接触时间对细菌活性的影响,并测定了磷酸盐缓冲液中涂层植入物中 CHX 的定量释放与培养时间的函数关系。利用人体单核细胞(HMNCs)研究了 PAA/CHI/CHX 涂层的生物相容性,并使用 MTT 分析法进行了定量。在涂有 PAA/CHI/CHX (0.025%) 和 PAA/CHI/CHX (0.0125%) 的植入物的洗脱溶液中,HMNCs 表现出很高的存活率,而涂有 PAA/CHI/CHX (0.05%) 的植入物提取物会引起轻微的细胞毒性。
{"title":"Investigation of Antibacterial Coatings Based on Chitosan/Polyacrylic Acid/Chlorhexidine for Orthopedic Implants.","authors":"Balzhan Savdenbekova, Ayazhan Seidulayeva, Aruzhan Sailau, Zhanar Bekissanova, Dilafruz Rakhmatullayeva, Ardak Jumagaziyeva","doi":"10.1021/acspolymersau.4c00049","DOIUrl":"10.1021/acspolymersau.4c00049","url":null,"abstract":"<p><p>Antibacterial coatings on model silicon wafers and implants, based on chitosan (CHI), poly(acrylic acid) (PAA), and the antibacterial agent chlorhexidine digluconate (CHX), were obtained using a layer-by-layer assembly method. The surface roughness and 2D and 3D images of the surfaces of CHI/PAA/CHX coatings obtained from different pH assemblies were investigated by atomic force microscopy, revealing that pH 6 enabled optimal inclusion of CHX in the multilayer film. The structure and elemental composition before and after implementation of CHX into the coating were investigated via scanning electron microscopy and energy-dispersive X-ray spectroscopy. The obtained films exhibited antimicrobial efficacy against <i>Staphylococcus aureus</i> and <i>Staphylococcus epidermidis</i>. The effects of CHX concentration and duration of contact with the coating on bacterial activity were investigated, and the quantitative release of CHX from coated implants in phosphate buffer was determined as a function of the incubation time. The biocompatibility of the PAA/CHI/CHX coatings was investigated using human mononuclear cells (HMNCs) and quantified using an MTT assay. HMNCs demonstrated high viability in eluted solutions obtained from implants coated with PAA/CHI/CHX (0.025%) and PAA/CHI/CHX (0.0125%), while the extract of implants coated with PAA/CHI/CHX (0.05%) induced slight cytotoxicity.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"4 6","pages":"498-511"},"PeriodicalIF":4.7,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11638784/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142831095","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Investigation of Antibacterial Coatings Based on Chitosan/Polyacrylic Acid/Chlorhexidine for Orthopedic Implants 壳聚糖/聚丙烯酸/氯己定骨科植入物抗菌涂层的研究
IF 4.7 Q1 POLYMER SCIENCE Pub Date : 2024-08-22 DOI: 10.1021/acspolymersau.4c0004910.1021/acspolymersau.4c00049
Balzhan Savdenbekova*, Ayazhan Seidulayeva, Aruzhan Sailau, Zhanar Bekissanova, Dilafruz Rakhmatullayeva and Ardak Jumagaziyeva, 

Antibacterial coatings on model silicon wafers and implants, based on chitosan (CHI), poly(acrylic acid) (PAA), and the antibacterial agent chlorhexidine digluconate (CHX), were obtained using a layer-by-layer assembly method. The surface roughness and 2D and 3D images of the surfaces of CHI/PAA/CHX coatings obtained from different pH assemblies were investigated by atomic force microscopy, revealing that pH 6 enabled optimal inclusion of CHX in the multilayer film. The structure and elemental composition before and after implementation of CHX into the coating were investigated via scanning electron microscopy and energy-dispersive X-ray spectroscopy. The obtained films exhibited antimicrobial efficacy against Staphylococcus aureus and Staphylococcus epidermidis. The effects of CHX concentration and duration of contact with the coating on bacterial activity were investigated, and the quantitative release of CHX from coated implants in phosphate buffer was determined as a function of the incubation time. The biocompatibility of the PAA/CHI/CHX coatings was investigated using human mononuclear cells (HMNCs) and quantified using an MTT assay. HMNCs demonstrated high viability in eluted solutions obtained from implants coated with PAA/CHI/CHX (0.025%) and PAA/CHI/CHX (0.0125%), while the extract of implants coated with PAA/CHI/CHX (0.05%) induced slight cytotoxicity.

以壳聚糖(CHI)、聚丙烯酸(PAA)和双光酸氯己定(CHX)为基料,采用逐层组装的方法在模型硅片和植入物上制备了抗菌涂层。通过原子力显微镜研究了不同pH组合得到的CHI/PAA/CHX涂层的表面粗糙度和表面二维和三维图像,结果表明pH为6时CHX在多层膜中的包合效果最佳。通过扫描电镜和x射线能谱分析研究了CHX注入前后涂层的结构和元素组成。所得薄膜对金黄色葡萄球菌和表皮葡萄球菌具有抗菌作用。研究了CHX浓度和与包被接触时间对细菌活性的影响,并测定了包被植入物在磷酸盐缓冲液中CHX的定量释放与孵育时间的关系。采用人单核细胞(hmnc)研究PAA/CHI/CHX涂层的生物相容性,并采用MTT法定量。PAA/CHI/CHX包被液(0.025%)和PAA/CHI/CHX包被液(0.0125%)洗脱后,HMNCs具有较高的细胞活力,而PAA/CHI/CHX包被液(0.05%)对HMNCs有轻微的细胞毒性。
{"title":"Investigation of Antibacterial Coatings Based on Chitosan/Polyacrylic Acid/Chlorhexidine for Orthopedic Implants","authors":"Balzhan Savdenbekova*,&nbsp;Ayazhan Seidulayeva,&nbsp;Aruzhan Sailau,&nbsp;Zhanar Bekissanova,&nbsp;Dilafruz Rakhmatullayeva and Ardak Jumagaziyeva,&nbsp;","doi":"10.1021/acspolymersau.4c0004910.1021/acspolymersau.4c00049","DOIUrl":"https://doi.org/10.1021/acspolymersau.4c00049https://doi.org/10.1021/acspolymersau.4c00049","url":null,"abstract":"<p >Antibacterial coatings on model silicon wafers and implants, based on chitosan (CHI), poly(acrylic acid) (PAA), and the antibacterial agent chlorhexidine digluconate (CHX), were obtained using a layer-by-layer assembly method. The surface roughness and 2D and 3D images of the surfaces of CHI/PAA/CHX coatings obtained from different pH assemblies were investigated by atomic force microscopy, revealing that pH 6 enabled optimal inclusion of CHX in the multilayer film. The structure and elemental composition before and after implementation of CHX into the coating were investigated via scanning electron microscopy and energy-dispersive X-ray spectroscopy. The obtained films exhibited antimicrobial efficacy against <i>Staphylococcus aureus</i> and <i>Staphylococcus epidermidis</i>. The effects of CHX concentration and duration of contact with the coating on bacterial activity were investigated, and the quantitative release of CHX from coated implants in phosphate buffer was determined as a function of the incubation time. The biocompatibility of the PAA/CHI/CHX coatings was investigated using human mononuclear cells (HMNCs) and quantified using an MTT assay. HMNCs demonstrated high viability in eluted solutions obtained from implants coated with PAA/CHI/CHX (0.025%) and PAA/CHI/CHX (0.0125%), while the extract of implants coated with PAA/CHI/CHX (0.05%) induced slight cytotoxicity.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"4 6","pages":"498–511 498–511"},"PeriodicalIF":4.7,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acspolymersau.4c00049","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849862","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Polysaccharide-Based Hydrogels for Advanced Biomedical Engineering Applications 高级生物医学工程应用的多糖基水凝胶
IF 4.7 Q1 POLYMER SCIENCE Pub Date : 2024-08-20 DOI: 10.1021/acspolymersau.4c0002810.1021/acspolymersau.4c00028
Md. Mahamudul Hasan Rumon, Anwarul Azim Akib, Stephen Don Sarkar, Md. Abu Rayhan Khan, Md. Mosfeq Uddin, Dina Nasrin and Chanchal Kumar Roy*, 

In recent years, numerous applications of hydrogels using polysaccharides have evolved, benefiting from their widespread availability, excellent biodegradability, biocompatibility, and nonpoisonous nature. These natural polymers are typically sourced from renewable materials or from manufacturing processes, contributing collaboratively to waste management and demonstrating the potential for enhanced and enduring sustainability. In the field of novel bioactive molecule carriers for biotherapeutics, natural polymers are attracting attention due to their inherent properties and adaptable chemical structures. These polymers offer versatile matrices with a range of architectures and mechanical properties, while retaining the bioactivity of incorporated biomolecules. However, conventional polysaccharide-based hydrogels suffer from inadequate mechanical toughness with large swelling properties, which prohibit their efficacy in real-world applications. This review offers insights into the latest advancements in the development of diverse polysaccharide-based hydrogels for biotherapeutic administrations, either standalone or in conjunction with other polymers or drug delivery systems, in the pharmaceutical and biomedical fields.

近年来,由于多糖的广泛可用性、良好的生物可降解性、生物相容性和无毒性质,许多水凝胶的应用已经发展起来。这些天然聚合物通常来自可再生材料或制造过程,有助于废物管理,并展示了增强和持久可持续性的潜力。在新型生物活性分子载体领域,天然聚合物以其固有的特性和适应性强的化学结构而备受关注。这些聚合物提供了具有一系列结构和机械性能的多功能基质,同时保留了纳入的生物分子的生物活性。然而,传统的基于多糖的水凝胶存在机械韧性不足和较大的膨胀特性,这阻碍了它们在实际应用中的有效性。本文综述了在制药和生物医学领域中用于生物治疗的各种多糖基水凝胶的最新进展,无论是单独使用还是与其他聚合物或药物输送系统结合使用。
{"title":"Polysaccharide-Based Hydrogels for Advanced Biomedical Engineering Applications","authors":"Md. Mahamudul Hasan Rumon,&nbsp;Anwarul Azim Akib,&nbsp;Stephen Don Sarkar,&nbsp;Md. Abu Rayhan Khan,&nbsp;Md. Mosfeq Uddin,&nbsp;Dina Nasrin and Chanchal Kumar Roy*,&nbsp;","doi":"10.1021/acspolymersau.4c0002810.1021/acspolymersau.4c00028","DOIUrl":"https://doi.org/10.1021/acspolymersau.4c00028https://doi.org/10.1021/acspolymersau.4c00028","url":null,"abstract":"<p >In recent years, numerous applications of hydrogels using polysaccharides have evolved, benefiting from their widespread availability, excellent biodegradability, biocompatibility, and nonpoisonous nature. These natural polymers are typically sourced from renewable materials or from manufacturing processes, contributing collaboratively to waste management and demonstrating the potential for enhanced and enduring sustainability. In the field of novel bioactive molecule carriers for biotherapeutics, natural polymers are attracting attention due to their inherent properties and adaptable chemical structures. These polymers offer versatile matrices with a range of architectures and mechanical properties, while retaining the bioactivity of incorporated biomolecules. However, conventional polysaccharide-based hydrogels suffer from inadequate mechanical toughness with large swelling properties, which prohibit their efficacy in real-world applications. This review offers insights into the latest advancements in the development of diverse polysaccharide-based hydrogels for biotherapeutic administrations, either standalone or in conjunction with other polymers or drug delivery systems, in the pharmaceutical and biomedical fields.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"4 6","pages":"463–486 463–486"},"PeriodicalIF":4.7,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acspolymersau.4c00028","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849861","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Polysaccharide-Based Hydrogels for Advanced Biomedical Engineering Applications. 用于先进生物医学工程应用的多糖基水凝胶。
IF 4.7 Q1 POLYMER SCIENCE Pub Date : 2024-08-20 eCollection Date: 2024-12-11 DOI: 10.1021/acspolymersau.4c00028
Md Mahamudul Hasan Rumon, Anwarul Azim Akib, Stephen Don Sarkar, Md Abu Rayhan Khan, Md Mosfeq Uddin, Dina Nasrin, Chanchal Kumar Roy

In recent years, numerous applications of hydrogels using polysaccharides have evolved, benefiting from their widespread availability, excellent biodegradability, biocompatibility, and nonpoisonous nature. These natural polymers are typically sourced from renewable materials or from manufacturing processes, contributing collaboratively to waste management and demonstrating the potential for enhanced and enduring sustainability. In the field of novel bioactive molecule carriers for biotherapeutics, natural polymers are attracting attention due to their inherent properties and adaptable chemical structures. These polymers offer versatile matrices with a range of architectures and mechanical properties, while retaining the bioactivity of incorporated biomolecules. However, conventional polysaccharide-based hydrogels suffer from inadequate mechanical toughness with large swelling properties, which prohibit their efficacy in real-world applications. This review offers insights into the latest advancements in the development of diverse polysaccharide-based hydrogels for biotherapeutic administrations, either standalone or in conjunction with other polymers or drug delivery systems, in the pharmaceutical and biomedical fields.

近年来,利用多糖制成的水凝胶得到了广泛应用,这得益于它们的广泛可用性、良好的生物降解性、生物相容性和无毒性。这些天然聚合物通常来自可再生材料或生产工艺,有助于废物管理,并展示了增强和持久可持续性的潜力。在用于生物治疗的新型生物活性分子载体领域,天然聚合物因其固有特性和可适应的化学结构而备受关注。这些聚合物提供了具有各种结构和机械性能的多功能基质,同时还能保持所含生物分子的生物活性。然而,传统的多糖基水凝胶存在机械韧性不足、溶胀性大的问题,这阻碍了它们在实际应用中的功效。本综述深入探讨了在制药和生物医学领域开发用于生物治疗的各种多糖基水凝胶的最新进展,这些水凝胶可以单独使用,也可以与其他聚合物或给药系统结合使用。
{"title":"Polysaccharide-Based Hydrogels for Advanced Biomedical Engineering Applications.","authors":"Md Mahamudul Hasan Rumon, Anwarul Azim Akib, Stephen Don Sarkar, Md Abu Rayhan Khan, Md Mosfeq Uddin, Dina Nasrin, Chanchal Kumar Roy","doi":"10.1021/acspolymersau.4c00028","DOIUrl":"10.1021/acspolymersau.4c00028","url":null,"abstract":"<p><p>In recent years, numerous applications of hydrogels using polysaccharides have evolved, benefiting from their widespread availability, excellent biodegradability, biocompatibility, and nonpoisonous nature. These natural polymers are typically sourced from renewable materials or from manufacturing processes, contributing collaboratively to waste management and demonstrating the potential for enhanced and enduring sustainability. In the field of novel bioactive molecule carriers for biotherapeutics, natural polymers are attracting attention due to their inherent properties and adaptable chemical structures. These polymers offer versatile matrices with a range of architectures and mechanical properties, while retaining the bioactivity of incorporated biomolecules. However, conventional polysaccharide-based hydrogels suffer from inadequate mechanical toughness with large swelling properties, which prohibit their efficacy in real-world applications. This review offers insights into the latest advancements in the development of diverse polysaccharide-based hydrogels for biotherapeutic administrations, either standalone or in conjunction with other polymers or drug delivery systems, in the pharmaceutical and biomedical fields.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"4 6","pages":"463-486"},"PeriodicalIF":4.7,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11638789/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142831114","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Advancements in Novel Mechano-Rheological Probes for Studying Glassy Dynamics in Nanoconfined Thin Polymer Films 用于研究纳米约束薄聚合物薄膜玻璃态动力学的新型机械流变探针的研究进展
IF 4.7 Q1 POLYMER SCIENCE Pub Date : 2024-07-18 DOI: 10.1021/acspolymersau.4c0002210.1021/acspolymersau.4c00022
Mithun Madhusudanan,  and , Mithun Chowdhury*, 

The nanoconfinement effects of glassy polymer thin films on their thermal and mechanical properties have been investigated thoroughly, especially with an emphasis on its altered glass transition behavior compared to bulk polymer, which has been known for almost three decades. While research in this direction is still evolving, reaching new heights to unravel the underlying physics of phenomena observed in confined thin polymer films, we have a much clearer picture now. This, in turn, has promoted their application in miniaturized and functional applications. To extract the full potential of such confined films, starting from their fabrication, function, and various applications, we must realize the necessity to have an understanding and availability of robust characterization protocols that specifically target thin film thermo-mechanical stability. Being nanometer-sized in thickness, often atop a solid substrate, direct mechanical testing on such films becomes extremely challenging and often encounters serious complexity from the dominating effect of the substrate. In this review, we have compiled together a few important novel and promising techniques for mechano-rheological characterization of glassy polymer thin films. The conceptual background involved in each technique, constitutive equations, methodology, and current status of research are touched upon following a pedagogical tutorial approach. Further, we discussed each technique’s success and limitations, carefully covering the puzzling or contradicting observations reported within the broad nexus of glass transition temperature–viscosity–modulus–molecular mobility (including diffusion and relaxation).

人们已经深入研究了玻璃态聚合物薄膜的纳米致密效应对其热性能和机械性能的影响,特别是与块状聚合物相比其玻璃转变行为的改变。虽然这方面的研究仍在不断发展,并达到了新的高度,以揭示在密闭聚合物薄膜中观察到的现象的基本物理原理,但我们现在已经有了更清晰的认识。这反过来又促进了它们在微型化和功能性应用中的应用。为了充分挖掘这种封闭薄膜的潜力,从它们的制造、功能和各种应用入手,我们必须认识到有必要了解和掌握专门针对薄膜热机械稳定性的可靠表征规程。由于薄膜厚度仅为纳米级,通常位于固体基底之上,因此对此类薄膜进行直接机械测试极具挑战性,而且往往会因基底的主导效应而遭遇严重的复杂性。在本综述中,我们汇集了几种重要的、新颖的、有前途的玻璃聚合物薄膜机械流变学表征技术。每种技术所涉及的概念背景、构成方程、方法和研究现状都以教学教程的方式进行了阐述。此外,我们还讨论了每种技术的成功之处和局限性,仔细研究了在玻璃化温度-粘度-模量-分子流动性(包括扩散和弛豫)这一广泛联系中报告的令人费解或相互矛盾的观察结果。
{"title":"Advancements in Novel Mechano-Rheological Probes for Studying Glassy Dynamics in Nanoconfined Thin Polymer Films","authors":"Mithun Madhusudanan,&nbsp; and ,&nbsp;Mithun Chowdhury*,&nbsp;","doi":"10.1021/acspolymersau.4c0002210.1021/acspolymersau.4c00022","DOIUrl":"https://doi.org/10.1021/acspolymersau.4c00022https://doi.org/10.1021/acspolymersau.4c00022","url":null,"abstract":"<p >The nanoconfinement effects of glassy polymer thin films on their thermal and mechanical properties have been investigated thoroughly, especially with an emphasis on its altered glass transition behavior compared to bulk polymer, which has been known for almost three decades. While research in this direction is still evolving, reaching new heights to unravel the underlying physics of phenomena observed in confined thin polymer films, we have a much clearer picture now. This, in turn, has promoted their application in miniaturized and functional applications. To extract the full potential of such confined films, starting from their fabrication, function, and various applications, we must realize the necessity to have an understanding and availability of robust characterization protocols that specifically target thin film thermo-mechanical stability. Being nanometer-sized in thickness, often atop a solid substrate, direct mechanical testing on such films becomes extremely challenging and often encounters serious complexity from the dominating effect of the substrate. In this review, we have compiled together a few important novel and promising techniques for mechano-rheological characterization of glassy polymer thin films. The conceptual background involved in each technique, constitutive equations, methodology, and current status of research are touched upon following a pedagogical tutorial approach. Further, we discussed each technique’s success and limitations, carefully covering the puzzling or contradicting observations reported within the broad nexus of glass transition temperature–viscosity–modulus–molecular mobility (including diffusion and relaxation).</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"4 5","pages":"342–391 342–391"},"PeriodicalIF":4.7,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acspolymersau.4c00022","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142403040","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Advancements in Novel Mechano-Rheological Probes for Studying Glassy Dynamics in Nanoconfined Thin Polymer Films 用于研究纳米约束薄聚合物薄膜玻璃态动力学的新型机械流变探针的研究进展
Q1 POLYMER SCIENCE Pub Date : 2024-07-18 DOI: 10.1021/acspolymersau.4c00022
Mithun Madhusudanan, Mithun Chowdhury
The nanoconfinement effects of glassy polymer thin films on their thermal and mechanical properties have been investigated thoroughly, especially with an emphasis on its altered glass transition behavior compared to bulk polymer, which has been known for almost three decades. While research in this direction is still evolving, reaching new heights to unravel the underlying physics of phenomena observed in confined thin polymer films, we have a much clearer picture now. This, in turn, has promoted their application in miniaturized and functional applications. To extract the full potential of such confined films, starting from their fabrication, function, and various applications, we must realize the necessity to have an understanding and availability of robust characterization protocols that specifically target thin film thermo-mechanical stability. Being nanometer-sized in thickness, often atop a solid substrate, direct mechanical testing on such films becomes extremely challenging and often encounters serious complexity from the dominating effect of the substrate. In this review, we have compiled together a few important novel and promising techniques for mechano-rheological characterization of glassy polymer thin films. The conceptual background involved in each technique, constitutive equations, methodology, and current status of research are touched upon following a pedagogical tutorial approach. Further, we discussed each technique’s success and limitations, carefully covering the puzzling or contradicting observations reported within the broad nexus of glass transition temperature–viscosity–modulus–molecular mobility (including diffusion and relaxation).
人们已经深入研究了玻璃态聚合物薄膜的纳米致密效应对其热性能和机械性能的影响,特别是与块状聚合物相比其玻璃转变行为的改变。虽然这方面的研究仍在不断发展,并达到了新的高度,以揭示在密闭聚合物薄膜中观察到的现象的基本物理原理,但我们现在已经有了更清晰的认识。这反过来又促进了它们在微型化和功能性应用中的应用。为了充分挖掘这种封闭薄膜的潜力,从它们的制造、功能和各种应用入手,我们必须认识到有必要了解和掌握专门针对薄膜热机械稳定性的可靠表征规程。由于薄膜厚度仅为纳米级,通常位于固体基底之上,因此对此类薄膜进行直接机械测试极具挑战性,而且往往会因基底的主导效应而遭遇严重的复杂性。在本综述中,我们汇集了几种重要的、新颖的、有前途的玻璃聚合物薄膜机械流变学表征技术。每种技术所涉及的概念背景、构成方程、方法和研究现状都以教学教程的方式进行了阐述。此外,我们还讨论了每种技术的成功之处和局限性,仔细研究了在玻璃化温度-粘度-模量-分子流动性(包括扩散和弛豫)这一广泛联系中报告的令人费解或相互矛盾的观察结果。
{"title":"Advancements in Novel Mechano-Rheological Probes for Studying Glassy Dynamics in Nanoconfined Thin Polymer Films","authors":"Mithun Madhusudanan, Mithun Chowdhury","doi":"10.1021/acspolymersau.4c00022","DOIUrl":"https://doi.org/10.1021/acspolymersau.4c00022","url":null,"abstract":"The nanoconfinement effects of glassy polymer thin films on their thermal and mechanical properties have been investigated thoroughly, especially with an emphasis on its altered glass transition behavior compared to bulk polymer, which has been known for almost three decades. While research in this direction is still evolving, reaching new heights to unravel the underlying physics of phenomena observed in confined thin polymer films, we have a much clearer picture now. This, in turn, has promoted their application in miniaturized and functional applications. To extract the full potential of such confined films, starting from their fabrication, function, and various applications, we must realize the necessity to have an understanding and availability of robust characterization protocols that specifically target thin film thermo-mechanical stability. Being nanometer-sized in thickness, often atop a solid substrate, direct mechanical testing on such films becomes extremely challenging and often encounters serious complexity from the dominating effect of the substrate. In this review, we have compiled together a few important novel and promising techniques for mechano-rheological characterization of glassy polymer thin films. The conceptual background involved in each technique, constitutive equations, methodology, and current status of research are touched upon following a pedagogical tutorial approach. Further, we discussed each technique’s success and limitations, carefully covering the puzzling or contradicting observations reported within the broad nexus of glass transition temperature–viscosity–modulus–molecular mobility (including diffusion and relaxation).","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"339 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141743165","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Structural Engineering of l-Aspartic Amphiphilic Polyesters for Enzyme-Responsive Drug Delivery and Bioimaging in Cancer Cells 用于癌细胞酶反应性给药和生物成像的 l-天冬氨酸两性聚酯的结构工程学研究
Q1 POLYMER SCIENCE Pub Date : 2024-07-17 DOI: 10.1021/acspolymersau.4c00013
Mohammed Khuddus, Utreshwar Arjun Gavhane, Manickam Jayakannan
Design and development of amphiphilic polyesters based on bioresources are very important to cater to the ever-growing need for biodegradable polymers in biomedical applications. Here, we report structural engineering of enzyme-responsive amphiphilic polyesters based on l-amino acid bioresources and study their drug delivery aspects in the cancer cell line. For this purpose, an l-aspartic acid-based polyester platform is chosen, and two noncovalent forces such as hydrogen bonding and side-chain hydrophobic interactions are introduced to study their effect on the aqueous self-assembly of nanoparticles. The synthetic strategy involves the development of l-aspartic acid-based dimethyl ester monomers with acetal and stearate side chains and subjecting them to solvent-free melt polycondensation reactions to produce side-chain-functionalized polyesters in the entire composition range. Postpolymerization acid catalyst deprotection of acetal yielded hydroxyl-functionalized polyesters. Amphiphilicity of the polymer is carefully fine-tuned by varying the composition of the stearate and hydroxyl units in the polymer chains to produce self-assembly in water. Various drugs such as camptothecin (CPT), curcumin (CUR), and doxorubicin (DOX) and biomarkers like 8-hydroxypyrene-1,3,6-trisulfonic acid trisodium salt (HPTS), rose bengal (RB), and Nile red (NR) are successfully encapsulated in the polymer nanoparticles. Cytotoxicity of biodegradable polymer nanoparticles is tested in normal and breast cancer cell lines. The polymer nanoparticles are found to be highly biocompatible and delivered the anticancer drugs in the intracellular compartments of the cells.
基于生物资源的两亲性聚酯的设计和开发对于满足生物医学应用中对可生物降解聚合物日益增长的需求非常重要。在此,我们报告了基于 l- 氨基酸生物资源的酶响应性两亲性聚酯的结构工程,并研究了它们在癌细胞系中的药物输送方面。为此,我们选择了一种基于 l-天冬氨酸的聚酯平台,并引入了两种非共价作用力,如氢键和侧链疏水相互作用,以研究它们对纳米粒子水性自组装的影响。合成策略包括开发具有缩醛和硬脂酸侧链的 l-天冬氨酸基二甲酯单体,并将其进行无溶剂熔融缩聚反应,以生产整个组成范围内的侧链官能化聚酯。聚合后酸催化剂对缩醛进行脱保护,得到羟基官能化聚酯。通过改变聚合物链中硬脂酸单元和羟基单元的组成,可对聚合物的亲水性进行细致的微调,从而在水中产生自组装。喜树碱 (CPT)、姜黄素 (CUR) 和多柔比星 (DOX) 等多种药物以及 8-羟基芘-1,3,6-三磺酸三钠盐 (HPTS)、玫瑰红 (RB) 和尼罗红 (NR) 等生物标记物被成功封装在聚合物纳米颗粒中。在正常细胞系和乳腺癌细胞系中测试了生物可降解聚合物纳米粒子的细胞毒性。结果发现,这种聚合物纳米粒子具有很高的生物相容性,能将抗癌药物输送到细胞内。
{"title":"Structural Engineering of l-Aspartic Amphiphilic Polyesters for Enzyme-Responsive Drug Delivery and Bioimaging in Cancer Cells","authors":"Mohammed Khuddus, Utreshwar Arjun Gavhane, Manickam Jayakannan","doi":"10.1021/acspolymersau.4c00013","DOIUrl":"https://doi.org/10.1021/acspolymersau.4c00013","url":null,"abstract":"Design and development of amphiphilic polyesters based on bioresources are very important to cater to the ever-growing need for biodegradable polymers in biomedical applications. Here, we report structural engineering of enzyme-responsive amphiphilic polyesters based on <span>l</span>-amino acid bioresources and study their drug delivery aspects in the cancer cell line. For this purpose, an <span>l</span>-aspartic acid-based polyester platform is chosen, and two noncovalent forces such as hydrogen bonding and side-chain hydrophobic interactions are introduced to study their effect on the aqueous self-assembly of nanoparticles. The synthetic strategy involves the development of <span>l</span>-aspartic acid-based dimethyl ester monomers with acetal and stearate side chains and subjecting them to solvent-free melt polycondensation reactions to produce side-chain-functionalized polyesters in the entire composition range. Postpolymerization acid catalyst deprotection of acetal yielded hydroxyl-functionalized polyesters. Amphiphilicity of the polymer is carefully fine-tuned by varying the composition of the stearate and hydroxyl units in the polymer chains to produce self-assembly in water. Various drugs such as camptothecin (CPT), curcumin (CUR), and doxorubicin (DOX) and biomarkers like 8-hydroxypyrene-1,3,6-trisulfonic acid trisodium salt (HPTS), rose bengal (RB), and Nile red (NR) are successfully encapsulated in the polymer nanoparticles. Cytotoxicity of biodegradable polymer nanoparticles is tested in normal and breast cancer cell lines. The polymer nanoparticles are found to be highly biocompatible and delivered the anticancer drugs in the intracellular compartments of the cells.","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"23 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141721166","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Rational Monomer Design for the Synthesis of Conjugated Polymers by Direct Heteroarylation Polymerization 通过直接异芳基化聚合合成共轭聚合物的合理单体设计
IF 4.7 Q1 POLYMER SCIENCE Pub Date : 2024-07-05 DOI: 10.1021/acspolymersau.4c0005010.1021/acspolymersau.4c00050
Navnath R. Kakde, Himanshu Sharma, Nitin V. Dalvi, Kumar Vanka and Asha S.K*, 

This study focuses on the design concepts that contribute to the C–H activation in bithiophene-flanked monomers incorporating naphthalene diimide (NDI), perylene diimide (PDI), and fluorene (FLU) and their polymerization by direct heteroarylation. Density functional theory (DFT) calculations reveal distinct energy requirements for C–H bond abstraction, which is dictated by the electron-withdrawing strength of the central aromatic core flanked by bithiophene. These provide insights into the reactivity of each monomer for C–H bond activation. Proton NMR spectroscopic experimental results confirm the favorable energetic profiles predicted by DFT, with NDI- and PDI-flanked monomers exhibiting lower energy requirements than fluorene-flanked monomers. Successful polymer synthesis is demonstrated for NDI and PDI, while the fluorene-flanked monomer shows challenges due to its higher energy demands.

本研究的重点是掺入了萘二亚胺(NDI)、苝二亚胺(PDI)和芴(FLU)的双噻吩侧翼单体中有助于 C-H 活化的设计理念,以及它们通过直接杂芳基化的聚合反应。密度泛函理论(DFT)计算揭示了 C-H 键抽离所需的独特能量要求,而这取决于中央芳香核心两侧噻吩的电子抽离强度。这有助于深入了解每种单体对 C-H 键活化的反应性。质子核磁共振光谱实验结果证实了 DFT 预测的有利能量曲线,NDI 和 PDI 侧翼单体的能量需求低于芴侧翼单体。NDI 和 PDI 的聚合物合成获得了成功,而芴侧翼单体由于能量需求较高而面临挑战。
{"title":"Rational Monomer Design for the Synthesis of Conjugated Polymers by Direct Heteroarylation Polymerization","authors":"Navnath R. Kakde,&nbsp;Himanshu Sharma,&nbsp;Nitin V. Dalvi,&nbsp;Kumar Vanka and Asha S.K*,&nbsp;","doi":"10.1021/acspolymersau.4c0005010.1021/acspolymersau.4c00050","DOIUrl":"https://doi.org/10.1021/acspolymersau.4c00050https://doi.org/10.1021/acspolymersau.4c00050","url":null,"abstract":"<p >This study focuses on the design concepts that contribute to the C–H activation in bithiophene-flanked monomers incorporating naphthalene diimide (NDI), perylene diimide (PDI), and fluorene (FLU) and their polymerization by direct heteroarylation. Density functional theory (DFT) calculations reveal distinct energy requirements for C–H bond abstraction, which is dictated by the electron-withdrawing strength of the central aromatic core flanked by bithiophene. These provide insights into the reactivity of each monomer for C–H bond activation. Proton NMR spectroscopic experimental results confirm the favorable energetic profiles predicted by DFT, with NDI- and PDI-flanked monomers exhibiting lower energy requirements than fluorene-flanked monomers. Successful polymer synthesis is demonstrated for NDI and PDI, while the fluorene-flanked monomer shows challenges due to its higher energy demands.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"4 5","pages":"449–459 449–459"},"PeriodicalIF":4.7,"publicationDate":"2024-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acspolymersau.4c00050","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142402892","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
期刊
ACS polymers Au
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1