Pub Date : 2024-10-07DOI: 10.1021/acsomega.4c0661710.1021/acsomega.4c06617
Justas Rodarte, Carly Baehr, Dustin Hicks, Morgan McGovern, Yue Zhang, Pedro Silva-Ortiz, Bryan Hannon, Sowmya Duddu, Marie Pancera* and Marco Pravetoni*,
The opioid overdose epidemic is a growing and evolving public health crisis fueled by the widespread presence of fentanyl and fentanyl analogues (F/FAs) in both street mixtures and counterfeit pills. To expand current treatment options, drug-targeting monoclonal antibodies (mAbs) offer a viable therapeutic for both pre- and postexposure clinical scenarios. This study reports the isolation, in vitro characterization, and in vivo efficacy of two murine mAb families targeting fentanyl, carfentanil, or both. Because humanization of the mAbs by CDR grafting negatively impacted affinity for both fentanyl and carfentanil, crystal structures of mAbs in complex with fentanyl or carfentanil were analyzed to identify key residues involved in ligand binding in murine versus humanized structures, and site-directed mutagenesis was used to verify their functional importance. The structural analysis identified a framework residue, Tyr36, present in the murine germline sequence of two mAbs, which was critical for binding to fentanyl and carfentanil. These studies emphasize the importance of structural considerations in mAb engineering to optimize mAbs targeting small molecules including opioids and other drugs of public health interest.
由于芬太尼和芬太尼类似物(Fentanyl and fentanyl analogues, F/FAs)在街头混合物和假药中的广泛存在,阿片类药物过量疫情是一个不断增长和演变的公共卫生危机。为了扩大现有的治疗方案,药物靶向单克隆抗体(mAbs)为暴露前和暴露后的临床治疗提供了一种可行的疗法。本研究报告了针对芬太尼、卡芬太尼或两者的两个小鼠 mAb 家族的分离、体外表征和体内疗效。由于通过 CDR 嫁接使 mAb 人源化会对芬太尼和卡芬太尼的亲和力产生负面影响,因此对 mAb 与芬太尼或卡芬太尼复合物的晶体结构进行了分析,以确定在小鼠结构与人源化结构中参与配体结合的关键残基,并使用定点突变来验证它们的功能重要性。结构分析确定了存在于两种 mAbs 的小鼠种系序列中的一个框架残基 Tyr36,它对与芬太尼和卡芬太尼的结合至关重要。这些研究强调了结构因素在 mAb 工程中的重要性,以优化靶向小分子(包括阿片类药物和其他关系到公众健康的药物)的 mAb。
{"title":"Structure-Based Engineering of Monoclonal Antibodies for Improved Binding to Counteract the Effects of Fentanyl and Carfentanil","authors":"Justas Rodarte, Carly Baehr, Dustin Hicks, Morgan McGovern, Yue Zhang, Pedro Silva-Ortiz, Bryan Hannon, Sowmya Duddu, Marie Pancera* and Marco Pravetoni*, ","doi":"10.1021/acsomega.4c0661710.1021/acsomega.4c06617","DOIUrl":"https://doi.org/10.1021/acsomega.4c06617https://doi.org/10.1021/acsomega.4c06617","url":null,"abstract":"<p >The opioid overdose epidemic is a growing and evolving public health crisis fueled by the widespread presence of fentanyl and fentanyl analogues (F/FAs) in both street mixtures and counterfeit pills. To expand current treatment options, drug-targeting monoclonal antibodies (mAbs) offer a viable therapeutic for both pre- and postexposure clinical scenarios. This study reports the isolation, <i>in vitro</i> characterization, and <i>in vivo</i> efficacy of two murine mAb families targeting fentanyl, carfentanil, or both. Because humanization of the mAbs by CDR grafting negatively impacted affinity for both fentanyl and carfentanil, crystal structures of mAbs in complex with fentanyl or carfentanil were analyzed to identify key residues involved in ligand binding in murine versus humanized structures, and site-directed mutagenesis was used to verify their functional importance. The structural analysis identified a framework residue, Tyr36, present in the murine germline sequence of two mAbs, which was critical for binding to fentanyl and carfentanil. These studies emphasize the importance of structural considerations in mAb engineering to optimize mAbs targeting small molecules including opioids and other drugs of public health interest.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c06617","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142437222","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-07eCollection Date: 2024-10-15DOI: 10.1021/acsomega.4c06031
Benjamin Schmuck, Gabriele Greco, Olga Shilkova, Anna Rising
Spiders can produce up to seven different types of silk, each with unique mechanical properties that stem from variations in the repetitive regions of spider silk proteins (spidroins). Artificial spider silk can be made from mini-spidroins in an all-aqueous-based spinning process, but the strongest fibers seldom reach more than 25% of the strength of native silk fibers. With the aim to improve the mechanical properties of silk fibers made from mini-spidroins and to understand the relationship between the protein design and the mechanical properties of the fibers, we designed 16 new spidroins, ranging from 31.7 to 59.5 kDa, that feature the globular spidroin N- and C-terminal domains, but harbor different repetitive sequences. We found that more than 50% of these constructs could be spun by extruding them into low-pH aqueous buffer and that the best fibers were produced from proteins whose repeat regions were derived from major ampullate spidroin 4 (MaSp4) and elastin. The mechanical properties differed between fiber types but did not correlate with the expected properties based on the origin of the repeats, suggesting that additional factors beyond protein design impact the properties of the fibers.
蜘蛛可以生产多达七种不同类型的丝,每种丝都具有独特的机械特性,这些特性源于蛛丝蛋白(spidroins)重复区域的变化。人工蛛丝可通过全水基纺丝工艺由小蜘蛛丝蛋白制成,但最强的纤维强度很少超过原生丝纤维的 25%。为了改善用迷你蜘蛛蛋白制成的蚕丝纤维的机械性能,并了解蛋白质设计与纤维机械性能之间的关系,我们设计了 16 种新的蜘蛛蛋白,它们的分子量从 31.7 到 59.5 kDa 不等,具有球状蜘蛛蛋白 N 端和 C 端结构域,但含有不同的重复序列。我们发现,将这些构建体挤入低pH值的水缓冲液中,50%以上的构建体可以纺成纤维,而重复区域来自主要安普拉蝶呤4(MaSp4)和弹性蛋白的蛋白质所制成的纤维最好。不同类型纤维的机械性能各不相同,但与基于重复区来源的预期性能并不相关,这表明除蛋白质设计外,还有其他因素影响着纤维的性能。
{"title":"Effects of Mini-Spidroin Repeat Region on the Mechanical Properties of Artificial Spider Silk Fibers.","authors":"Benjamin Schmuck, Gabriele Greco, Olga Shilkova, Anna Rising","doi":"10.1021/acsomega.4c06031","DOIUrl":"https://doi.org/10.1021/acsomega.4c06031","url":null,"abstract":"<p><p>Spiders can produce up to seven different types of silk, each with unique mechanical properties that stem from variations in the repetitive regions of spider silk proteins (spidroins). Artificial spider silk can be made from mini-spidroins in an all-aqueous-based spinning process, but the strongest fibers seldom reach more than 25% of the strength of native silk fibers. With the aim to improve the mechanical properties of silk fibers made from mini-spidroins and to understand the relationship between the protein design and the mechanical properties of the fibers, we designed 16 new spidroins, ranging from 31.7 to 59.5 kDa, that feature the globular spidroin N- and C-terminal domains, but harbor different repetitive sequences. We found that more than 50% of these constructs could be spun by extruding them into low-pH aqueous buffer and that the best fibers were produced from proteins whose repeat regions were derived from major ampullate spidroin 4 (MaSp4) and elastin. The mechanical properties differed between fiber types but did not correlate with the expected properties based on the origin of the repeats, suggesting that additional factors beyond protein design impact the properties of the fibers.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11483375/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453323","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-07eCollection Date: 2024-10-15DOI: 10.1021/acsomega.4c06617
Justas Rodarte, Carly Baehr, Dustin Hicks, Morgan McGovern, Yue Zhang, Pedro Silva-Ortiz, Bryan Hannon, Sowmya Duddu, Marie Pancera, Marco Pravetoni
The opioid overdose epidemic is a growing and evolving public health crisis fueled by the widespread presence of fentanyl and fentanyl analogues (F/FAs) in both street mixtures and counterfeit pills. To expand current treatment options, drug-targeting monoclonal antibodies (mAbs) offer a viable therapeutic for both pre- and postexposure clinical scenarios. This study reports the isolation, in vitro characterization, and in vivo efficacy of two murine mAb families targeting fentanyl, carfentanil, or both. Because humanization of the mAbs by CDR grafting negatively impacted affinity for both fentanyl and carfentanil, crystal structures of mAbs in complex with fentanyl or carfentanil were analyzed to identify key residues involved in ligand binding in murine versus humanized structures, and site-directed mutagenesis was used to verify their functional importance. The structural analysis identified a framework residue, Tyr36, present in the murine germline sequence of two mAbs, which was critical for binding to fentanyl and carfentanil. These studies emphasize the importance of structural considerations in mAb engineering to optimize mAbs targeting small molecules including opioids and other drugs of public health interest.
由于芬太尼和芬太尼类似物(Fentanyl and fentanyl analogues,F/FAs)在街头混合物和假药中的广泛存在,阿片类药物过量疫情是一个不断增长和演变的公共卫生危机。为了扩大现有的治疗方案,药物靶向单克隆抗体(mAbs)为暴露前和暴露后的临床治疗提供了一种可行的疗法。本研究报告了针对芬太尼、卡芬太尼或两者的两个小鼠 mAb 家族的分离、体外表征和体内疗效。由于通过 CDR 嫁接使 mAb 人源化会对芬太尼和卡芬太尼的亲和力产生负面影响,因此对 mAb 与芬太尼或卡芬太尼复合物的晶体结构进行了分析,以确定在小鼠结构与人源化结构中参与配体结合的关键残基,并使用定点突变来验证它们的功能重要性。结构分析确定了存在于两种 mAbs 的小鼠种系序列中的一个框架残基 Tyr36,它对与芬太尼和卡芬太尼的结合至关重要。这些研究强调了结构因素在 mAb 工程中的重要性,以优化靶向小分子(包括阿片类药物和其他关系到公众健康的药物)的 mAb。
{"title":"Structure-Based Engineering of Monoclonal Antibodies for Improved Binding to Counteract the Effects of Fentanyl and Carfentanil.","authors":"Justas Rodarte, Carly Baehr, Dustin Hicks, Morgan McGovern, Yue Zhang, Pedro Silva-Ortiz, Bryan Hannon, Sowmya Duddu, Marie Pancera, Marco Pravetoni","doi":"10.1021/acsomega.4c06617","DOIUrl":"https://doi.org/10.1021/acsomega.4c06617","url":null,"abstract":"<p><p>The opioid overdose epidemic is a growing and evolving public health crisis fueled by the widespread presence of fentanyl and fentanyl analogues (F/FAs) in both street mixtures and counterfeit pills. To expand current treatment options, drug-targeting monoclonal antibodies (mAbs) offer a viable therapeutic for both pre- and postexposure clinical scenarios. This study reports the isolation, <i>in vitro</i> characterization, and <i>in vivo</i> efficacy of two murine mAb families targeting fentanyl, carfentanil, or both. Because humanization of the mAbs by CDR grafting negatively impacted affinity for both fentanyl and carfentanil, crystal structures of mAbs in complex with fentanyl or carfentanil were analyzed to identify key residues involved in ligand binding in murine versus humanized structures, and site-directed mutagenesis was used to verify their functional importance. The structural analysis identified a framework residue, Tyr36, present in the murine germline sequence of two mAbs, which was critical for binding to fentanyl and carfentanil. These studies emphasize the importance of structural considerations in mAb engineering to optimize mAbs targeting small molecules including opioids and other drugs of public health interest.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11483391/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zinc hydroxide nitrate (Zn5) is one of the layered metal hydroxide materials, which has been extensively reported as an effective bifunctional catalyst for biodiesel production from acidic oils. This report gives a comprehensive summary of the reactivity of Zn5 in the methanolysis of various oil feedstocks, plant oils, free fatty acids, and other acidic oils. Notably, as evidenced by this work, Zn5 is highly effective in converting acidic oils [palmitic acid/palm oil (PO)] to fatty acid methyl ester (FAME or biodiesel) at high yields ranging from 80 to 95%, withstanding acid content up to 10% without soap formation. The high FAME yields result from complex methanolysis and hydrolysis processes, e.g., transesterification of triglycerides in the PO, esterification of palmitic acid, and hydrolysis of the triglycerides. Despite this, Zn5 is nonrecyclable because it is unstable in the reaction media and transforms into zinc hydroxide nitrate/zinc palmitate (Zn5/ZnP) composites. The Zn5/ZnP composites were suitable for use in FAME production from PO at 100 °C for 2 h by using a methanol-to-oil molar ratio of 30:1, yielding high FAME yields of 97 and 70.7% in the first and fourth cycles, respectively. This study added better insight into how to effectively produce FAME from oil feedstocks of varying acidity by using zinc layered hydroxide- or zinc carboxylate-based materials.
{"title":"Recyclability of Zinc Palmitate-Based Composites in Fatty Acid Methyl Ester Production from Oil Feedstocks at Varied Acidity.","authors":"Charoen Posa, Palmpapat Junpuek, Warisara Woranuch, Kittichai Chaiseeda, Kornkanya Pratumyot, Nongnuch Sungayuth, Siwaporn Meejoo Smith","doi":"10.1021/acsomega.4c02740","DOIUrl":"https://doi.org/10.1021/acsomega.4c02740","url":null,"abstract":"<p><p>Zinc hydroxide nitrate (Zn5) is one of the layered metal hydroxide materials, which has been extensively reported as an effective bifunctional catalyst for biodiesel production from acidic oils. This report gives a comprehensive summary of the reactivity of Zn5 in the methanolysis of various oil feedstocks, plant oils, free fatty acids, and other acidic oils. Notably, as evidenced by this work, Zn5 is highly effective in converting acidic oils [palmitic acid/palm oil (PO)] to fatty acid methyl ester (FAME or biodiesel) at high yields ranging from 80 to 95%, withstanding acid content up to 10% without soap formation. The high FAME yields result from complex methanolysis and hydrolysis processes, e.g., transesterification of triglycerides in the PO, esterification of palmitic acid, and hydrolysis of the triglycerides. Despite this, Zn5 is nonrecyclable because it is unstable in the reaction media and transforms into zinc hydroxide nitrate/zinc palmitate (Zn5/ZnP) composites. The Zn5/ZnP composites were suitable for use in FAME production from PO at 100 °C for 2 h by using a methanol-to-oil molar ratio of 30:1, yielding high FAME yields of 97 and 70.7% in the first and fourth cycles, respectively. This study added better insight into how to effectively produce FAME from oil feedstocks of varying acidity by using zinc layered hydroxide- or zinc carboxylate-based materials.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11483390/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453334","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-07DOI: 10.1021/acsomega.4c0603110.1021/acsomega.4c06031
Benjamin Schmuck*, Gabriele Greco, Olga Shilkova and Anna Rising*,
Spiders can produce up to seven different types of silk, each with unique mechanical properties that stem from variations in the repetitive regions of spider silk proteins (spidroins). Artificial spider silk can be made from mini-spidroins in an all-aqueous-based spinning process, but the strongest fibers seldom reach more than 25% of the strength of native silk fibers. With the aim to improve the mechanical properties of silk fibers made from mini-spidroins and to understand the relationship between the protein design and the mechanical properties of the fibers, we designed 16 new spidroins, ranging from 31.7 to 59.5 kDa, that feature the globular spidroin N- and C-terminal domains, but harbor different repetitive sequences. We found that more than 50% of these constructs could be spun by extruding them into low-pH aqueous buffer and that the best fibers were produced from proteins whose repeat regions were derived from major ampullate spidroin 4 (MaSp4) and elastin. The mechanical properties differed between fiber types but did not correlate with the expected properties based on the origin of the repeats, suggesting that additional factors beyond protein design impact the properties of the fibers.
蜘蛛可以生产多达七种不同类型的丝,每种丝都具有独特的机械特性,这些特性源于蛛丝蛋白(spidroins)重复区域的变化。人工蛛丝可通过全水基纺丝工艺由小蜘蛛丝蛋白制成,但最强的纤维强度很少超过原生丝纤维的 25%。为了改善用迷你蜘蛛蛋白制成的蚕丝纤维的机械性能,并了解蛋白质设计与纤维机械性能之间的关系,我们设计了 16 种新的蜘蛛蛋白,它们的分子量从 31.7 到 59.5 kDa 不等,具有球状蜘蛛蛋白 N 端和 C 端结构域,但含有不同的重复序列。我们发现,将这些构建体挤入低pH值的水缓冲液中,50%以上的构建体可以纺成纤维,而重复区域来自主要安普拉蝶呤4(MaSp4)和弹性蛋白的蛋白质所制成的纤维最好。不同类型纤维的机械性能各不相同,但与基于重复区来源的预期性能并不相关,这表明除蛋白质设计外,还有其他因素影响着纤维的性能。
{"title":"Effects of Mini-Spidroin Repeat Region on the Mechanical Properties of Artificial Spider Silk Fibers","authors":"Benjamin Schmuck*, Gabriele Greco, Olga Shilkova and Anna Rising*, ","doi":"10.1021/acsomega.4c0603110.1021/acsomega.4c06031","DOIUrl":"https://doi.org/10.1021/acsomega.4c06031https://doi.org/10.1021/acsomega.4c06031","url":null,"abstract":"<p >Spiders can produce up to seven different types of silk, each with unique mechanical properties that stem from variations in the repetitive regions of spider silk proteins (spidroins). Artificial spider silk can be made from mini-spidroins in an all-aqueous-based spinning process, but the strongest fibers seldom reach more than 25% of the strength of native silk fibers. With the aim to improve the mechanical properties of silk fibers made from mini-spidroins and to understand the relationship between the protein design and the mechanical properties of the fibers, we designed 16 new spidroins, ranging from 31.7 to 59.5 kDa, that feature the globular spidroin N- and C-terminal domains, but harbor different repetitive sequences. We found that more than 50% of these constructs could be spun by extruding them into low-pH aqueous buffer and that the best fibers were produced from proteins whose repeat regions were derived from major ampullate spidroin 4 (MaSp4) and elastin. The mechanical properties differed between fiber types but did not correlate with the expected properties based on the origin of the repeats, suggesting that additional factors beyond protein design impact the properties of the fibers.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c06031","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142437134","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-06DOI: 10.1021/acsomega.4c0477410.1021/acsomega.4c04774
Shogo Himori*, Riku Takahashi, Aya Tanaka and Masumi Yamaguchi,
Composites of hydrogels and metals are gaining interest because of each material’s unique properties. However, the stable adhesion of metals on hydrogels is challenging due to the mechanical mismatch at the soft–hard interface and the liquidity of the water components in hydrogels. We propose a facile physical-adhesion method that involves the dehydration process of hydrogels to transfer metals from a glass substrate. This method is based on the hydrophobic interaction between polymer chains and metals and is stable, even in water. Continuous metal wiring was achieved on a swollen hydrogel, and electrical conduction was effective for a soft electronic device. Therefore, our method could be a versatile method for integrating hydrogels and metals.
{"title":"Direct Metal Transfer on Swellable Hydrogel with Dehydration-Induced Physical Adhesion","authors":"Shogo Himori*, Riku Takahashi, Aya Tanaka and Masumi Yamaguchi, ","doi":"10.1021/acsomega.4c0477410.1021/acsomega.4c04774","DOIUrl":"https://doi.org/10.1021/acsomega.4c04774https://doi.org/10.1021/acsomega.4c04774","url":null,"abstract":"<p >Composites of hydrogels and metals are gaining interest because of each material’s unique properties. However, the stable adhesion of metals on hydrogels is challenging due to the mechanical mismatch at the soft–hard interface and the liquidity of the water components in hydrogels. We propose a facile physical-adhesion method that involves the dehydration process of hydrogels to transfer metals from a glass substrate. This method is based on the hydrophobic interaction between polymer chains and metals and is stable, even in water. Continuous metal wiring was achieved on a swollen hydrogel, and electrical conduction was effective for a soft electronic device. Therefore, our method could be a versatile method for integrating hydrogels and metals.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c04774","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436592","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-06eCollection Date: 2024-10-15DOI: 10.1021/acsomega.4c04774
Shogo Himori, Riku Takahashi, Aya Tanaka, Masumi Yamaguchi
Composites of hydrogels and metals are gaining interest because of each material's unique properties. However, the stable adhesion of metals on hydrogels is challenging due to the mechanical mismatch at the soft-hard interface and the liquidity of the water components in hydrogels. We propose a facile physical-adhesion method that involves the dehydration process of hydrogels to transfer metals from a glass substrate. This method is based on the hydrophobic interaction between polymer chains and metals and is stable, even in water. Continuous metal wiring was achieved on a swollen hydrogel, and electrical conduction was effective for a soft electronic device. Therefore, our method could be a versatile method for integrating hydrogels and metals.
{"title":"Direct Metal Transfer on Swellable Hydrogel with Dehydration-Induced Physical Adhesion.","authors":"Shogo Himori, Riku Takahashi, Aya Tanaka, Masumi Yamaguchi","doi":"10.1021/acsomega.4c04774","DOIUrl":"https://doi.org/10.1021/acsomega.4c04774","url":null,"abstract":"<p><p>Composites of hydrogels and metals are gaining interest because of each material's unique properties. However, the stable adhesion of metals on hydrogels is challenging due to the mechanical mismatch at the soft-hard interface and the liquidity of the water components in hydrogels. We propose a facile physical-adhesion method that involves the dehydration process of hydrogels to transfer metals from a glass substrate. This method is based on the hydrophobic interaction between polymer chains and metals and is stable, even in water. Continuous metal wiring was achieved on a swollen hydrogel, and electrical conduction was effective for a soft electronic device. Therefore, our method could be a versatile method for integrating hydrogels and metals.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11483376/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453322","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-06eCollection Date: 2024-10-15DOI: 10.1021/acsomega.4c07724
Ruixiao Li, Yunhe Zheng, Xuelian Li, Ruiping Su, Jiangchuan He, Song Xue, Ke Wang, Yanyao Gao, Jianxin Ni
Bacterial prostatitis is a common disease of the male genitourinary system, which seriously affects the normal life and health of male patients. Antibiotics are commonly used in the clinical treatment of bacterial prostatitis, but the efficacy of fluoroquinolones is gradually declining due to the increasing drug resistance of bacteria. Hence, it is necessary to find new antibacterial drugs to treat bacterial prostatitis. Luteolin is a natural flavonoid compound with many pharmacological activities such as antibacterial and anti-inflammatory activities, but its poor water solubility and low structural stability seriously limit its clinical application. In this study, we designed a targeting drug delivery system via a luteolin-copper complex grafted with hyaluronic acid. The results of the characterization proved the successful synthesis of the system. The results of the in vitro performance test show that the system has a good antibacterial effect and excellent blood compatibility and can be effectively released under different pH conditions. The prepared nanodrug delivery system not only provides a new idea for the treatment of bacterial prostatitis but also lays a theoretical and practical foundation for the wide application of luteolin in clinical practice.
{"title":"Hyaluronic Acid-Modified Luteolin-Copper Complex Nanodelivery System for Bacterial Prostatitis.","authors":"Ruixiao Li, Yunhe Zheng, Xuelian Li, Ruiping Su, Jiangchuan He, Song Xue, Ke Wang, Yanyao Gao, Jianxin Ni","doi":"10.1021/acsomega.4c07724","DOIUrl":"https://doi.org/10.1021/acsomega.4c07724","url":null,"abstract":"<p><p>Bacterial prostatitis is a common disease of the male genitourinary system, which seriously affects the normal life and health of male patients. Antibiotics are commonly used in the clinical treatment of bacterial prostatitis, but the efficacy of fluoroquinolones is gradually declining due to the increasing drug resistance of bacteria. Hence, it is necessary to find new antibacterial drugs to treat bacterial prostatitis. Luteolin is a natural flavonoid compound with many pharmacological activities such as antibacterial and anti-inflammatory activities, but its poor water solubility and low structural stability seriously limit its clinical application. In this study, we designed a targeting drug delivery system via a luteolin-copper complex grafted with hyaluronic acid. The results of the characterization proved the successful synthesis of the system. The results of the in vitro performance test show that the system has a good antibacterial effect and excellent blood compatibility and can be effectively released under different pH conditions. The prepared nanodrug delivery system not only provides a new idea for the treatment of bacterial prostatitis but also lays a theoretical and practical foundation for the wide application of luteolin in clinical practice.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11483909/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453233","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zinc hydroxide nitrate (Zn5) is one of the layered metal hydroxide materials, which has been extensively reported as an effective bifunctional catalyst for biodiesel production from acidic oils. This report gives a comprehensive summary of the reactivity of Zn5 in the methanolysis of various oil feedstocks, plant oils, free fatty acids, and other acidic oils. Notably, as evidenced by this work, Zn5 is highly effective in converting acidic oils [palmitic acid/palm oil (PO)] to fatty acid methyl ester (FAME or biodiesel) at high yields ranging from 80 to 95%, withstanding acid content up to 10% without soap formation. The high FAME yields result from complex methanolysis and hydrolysis processes, e.g., transesterification of triglycerides in the PO, esterification of palmitic acid, and hydrolysis of the triglycerides. Despite this, Zn5 is nonrecyclable because it is unstable in the reaction media and transforms into zinc hydroxide nitrate/zinc palmitate (Zn5/ZnP) composites. The Zn5/ZnP composites were suitable for use in FAME production from PO at 100 °C for 2 h by using a methanol-to-oil molar ratio of 30:1, yielding high FAME yields of 97 and 70.7% in the first and fourth cycles, respectively. This study added better insight into how to effectively produce FAME from oil feedstocks of varying acidity by using zinc layered hydroxide- or zinc carboxylate-based materials.
{"title":"Recyclability of Zinc Palmitate-Based Composites in Fatty Acid Methyl Ester Production from Oil Feedstocks at Varied Acidity","authors":"Charoen Posa, Palmpapat Junpuek, Warisara Woranuch, Kittichai Chaiseeda, Kornkanya Pratumyot, Nongnuch Sungayuth and Siwaporn Meejoo Smith*, ","doi":"10.1021/acsomega.4c0274010.1021/acsomega.4c02740","DOIUrl":"https://doi.org/10.1021/acsomega.4c02740https://doi.org/10.1021/acsomega.4c02740","url":null,"abstract":"<p >Zinc hydroxide nitrate (Zn5) is one of the layered metal hydroxide materials, which has been extensively reported as an effective bifunctional catalyst for biodiesel production from acidic oils. This report gives a comprehensive summary of the reactivity of Zn5 in the methanolysis of various oil feedstocks, plant oils, free fatty acids, and other acidic oils. Notably, as evidenced by this work, Zn5 is highly effective in converting acidic oils [palmitic acid/palm oil (PO)] to fatty acid methyl ester (FAME or biodiesel) at high yields ranging from 80 to 95%, withstanding acid content up to 10% without soap formation. The high FAME yields result from complex methanolysis and hydrolysis processes, e.g., transesterification of triglycerides in the PO, esterification of palmitic acid, and hydrolysis of the triglycerides. Despite this, Zn5 is nonrecyclable because it is unstable in the reaction media and transforms into zinc hydroxide nitrate/zinc palmitate (Zn5/ZnP) composites. The Zn5/ZnP composites were suitable for use in FAME production from PO at 100 °C for 2 h by using a methanol-to-oil molar ratio of 30:1, yielding high FAME yields of 97 and 70.7% in the first and fourth cycles, respectively. This study added better insight into how to effectively produce FAME from oil feedstocks of varying acidity by using zinc layered hydroxide- or zinc carboxylate-based materials.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c02740","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142437036","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-06DOI: 10.1021/acsomega.4c0772410.1021/acsomega.4c07724
Ruixiao Li, Yunhe Zheng, Xuelian Li, Ruiping Su, Jiangchuan He, Song Xue, Ke Wang*, Yanyao Gao* and Jianxin Ni*,
Bacterial prostatitis is a common disease of the male genitourinary system, which seriously affects the normal life and health of male patients. Antibiotics are commonly used in the clinical treatment of bacterial prostatitis, but the efficacy of fluoroquinolones is gradually declining due to the increasing drug resistance of bacteria. Hence, it is necessary to find new antibacterial drugs to treat bacterial prostatitis. Luteolin is a natural flavonoid compound with many pharmacological activities such as antibacterial and anti-inflammatory activities, but its poor water solubility and low structural stability seriously limit its clinical application. In this study, we designed a targeting drug delivery system via a luteolin–copper complex grafted with hyaluronic acid. The results of the characterization proved the successful synthesis of the system. The results of the in vitro performance test show that the system has a good antibacterial effect and excellent blood compatibility and can be effectively released under different pH conditions. The prepared nanodrug delivery system not only provides a new idea for the treatment of bacterial prostatitis but also lays a theoretical and practical foundation for the wide application of luteolin in clinical practice.
{"title":"Hyaluronic Acid-Modified Luteolin–Copper Complex Nanodelivery System for Bacterial Prostatitis","authors":"Ruixiao Li, Yunhe Zheng, Xuelian Li, Ruiping Su, Jiangchuan He, Song Xue, Ke Wang*, Yanyao Gao* and Jianxin Ni*, ","doi":"10.1021/acsomega.4c0772410.1021/acsomega.4c07724","DOIUrl":"https://doi.org/10.1021/acsomega.4c07724https://doi.org/10.1021/acsomega.4c07724","url":null,"abstract":"<p >Bacterial prostatitis is a common disease of the male genitourinary system, which seriously affects the normal life and health of male patients. Antibiotics are commonly used in the clinical treatment of bacterial prostatitis, but the efficacy of fluoroquinolones is gradually declining due to the increasing drug resistance of bacteria. Hence, it is necessary to find new antibacterial drugs to treat bacterial prostatitis. Luteolin is a natural flavonoid compound with many pharmacological activities such as antibacterial and anti-inflammatory activities, but its poor water solubility and low structural stability seriously limit its clinical application. In this study, we designed a targeting drug delivery system via a luteolin–copper complex grafted with hyaluronic acid. The results of the characterization proved the successful synthesis of the system. The results of the in vitro performance test show that the system has a good antibacterial effect and excellent blood compatibility and can be effectively released under different pH conditions. The prepared nanodrug delivery system not only provides a new idea for the treatment of bacterial prostatitis but also lays a theoretical and practical foundation for the wide application of luteolin in clinical practice.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c07724","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142437037","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}