Jisoo Park, Danbee Lee, Kyojung Hwang, Jimin Lee, Tai-Ju Lee, Youngsu Kim, Jung Hyeun Kim, Jieun Lee, Won-Jae Youe, Sang-Jin Chun and Jaegyoung Gwon
In traditional TEMPO oxidation systems, the high cost of TEMPO catalysts has been a significant barrier to the industrialization of oxidized CNF. From an economic perspective, presenting the characteristics of various CNFs produced with the oxidation systems with reduced catalyst usage could facilitate the industrial application of CNF across a wide range of fields. In this study, it was demonstrated that reducing the amount of TEMPO catalyst used (from 0.1 to 0.05 mmol g−1) in a conventional oxidation system increased the carboxylate content by approximately 6.3%. Furthermore, the activation of hydroxyl amine TEMPO, which is generated after the oxidation reaction of cellulose, was enhanced by adjusting the dosage of the inexpensive oxidant NaClO, leading to a 20% improvement in carboxylate content. This suggests that controlling the amount of NaClO as an oxidant can be a key parameter in adjusting the dosage of TEMPO to achieve the targeted degree of surface substitution. Results from the dispersion stability, UV-transmittance, and morphological properties of TEMPO-oxidized CNF using microfluidizing treatment showed that high carboxylate content plays a crucial role in producing high-purity CNF suspensions, which are small, uniform, and free from microfibers. Additionally, by varying the number of mechanical treatments applied to the oxidized cellulose, various types of CNF suspensions with different mean widths were obtained. We expect that these findings offer meaningful insights to end-users seeking a breakthrough in the performance limitations of final applications using cellulose nanomaterials.
在传统的 TEMPO 氧化系统中,TEMPO 催化剂的高成本一直是氧化 CNF 产业化的一大障碍。从经济角度来看,介绍使用减少催化剂用量的氧化系统生产的各种 CNF 的特性,可促进 CNF 在广泛领域的工业应用。本研究表明,在传统氧化体系中减少 TEMPO 催化剂用量(从 0.1 mmol g-1 减少到 0.05 mmol g-1)可使羧酸盐含量增加约 6.3%。此外,通过调整廉价氧化剂 NaClO 的用量,纤维素氧化反应后生成的羟胺 TEMPO 的活化也得到了增强,从而使羧酸盐含量提高了 20%。这表明,控制作为氧化剂的 NaClO 的用量可以作为调整 TEMPO 用量的关键参数,从而达到目标的表面取代度。利用微流化处理技术研究 TEMPO 氧化 CNF 的分散稳定性、紫外线透过率和形貌特性的结果表明,高羧酸盐含量在制备高纯度 CNF 悬浮液中起着关键作用,这种悬浮液细小、均匀、无微纤维。此外,通过改变对氧化纤维素进行机械处理的次数,还可获得平均宽度不同的各类 CNF 悬浮液。我们希望这些发现能为最终用户提供有意义的见解,帮助他们突破使用纤维素纳米材料的最终应用的性能限制。
{"title":"Effect of catalyst and oxidant concentrations in a TEMPO oxidation system on the production of cellulose nanofibers†","authors":"Jisoo Park, Danbee Lee, Kyojung Hwang, Jimin Lee, Tai-Ju Lee, Youngsu Kim, Jung Hyeun Kim, Jieun Lee, Won-Jae Youe, Sang-Jin Chun and Jaegyoung Gwon","doi":"10.1039/D4RA04948A","DOIUrl":"https://doi.org/10.1039/D4RA04948A","url":null,"abstract":"<p >In traditional TEMPO oxidation systems, the high cost of TEMPO catalysts has been a significant barrier to the industrialization of oxidized CNF. From an economic perspective, presenting the characteristics of various CNFs produced with the oxidation systems with reduced catalyst usage could facilitate the industrial application of CNF across a wide range of fields. In this study, it was demonstrated that reducing the amount of TEMPO catalyst used (from 0.1 to 0.05 mmol g<small><sup>−1</sup></small>) in a conventional oxidation system increased the carboxylate content by approximately 6.3%. Furthermore, the activation of hydroxyl amine TEMPO, which is generated after the oxidation reaction of cellulose, was enhanced by adjusting the dosage of the inexpensive oxidant NaClO, leading to a 20% improvement in carboxylate content. This suggests that controlling the amount of NaClO as an oxidant can be a key parameter in adjusting the dosage of TEMPO to achieve the targeted degree of surface substitution. Results from the dispersion stability, UV-transmittance, and morphological properties of TEMPO-oxidized CNF using microfluidizing treatment showed that high carboxylate content plays a crucial role in producing high-purity CNF suspensions, which are small, uniform, and free from microfibers. Additionally, by varying the number of mechanical treatments applied to the oxidized cellulose, various types of CNF suspensions with different mean widths were obtained. We expect that these findings offer meaningful insights to end-users seeking a breakthrough in the performance limitations of final applications using cellulose nanomaterials.</p>","PeriodicalId":102,"journal":{"name":"RSC Advances","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ra/d4ra04948a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142447278","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}
Superhydrophobic coatings with remarkable water repellence have emerged as an increasingly prominent field of research with the growth of the material engineering and coating industries. Superhydrophobic coatings address the requirements of several application areas with characteristics including corrosion resistance, drag reduction, anti-icing, anti-fogging, and self-cleaning properties. Furthermore, the range of applications for superhydrophobic coatings has been substantially broadened by the inclusion of key performance features such as flame retardancy, thermal insulation, resistance to water penetration, UV resistance, transparency, anti-reflection, and many more. Numerous research endeavours have been focused on biomimetic superhydrophobic materials because of their distinct surface wettability. To develop superhydrophobic coatings with a long lifespan, scientists have refined the processes of material preparation and selection. To accomplish water repellency, superhydrophobic coatings are usually fabricated using harmful fluorinated chemicals or synthetic polymers. Utilising materials derived from biomass offers a sustainable alternative that uses renewable resources in order to eliminate the consumption of these hazardous substances. This paper provides an insight of several researches reported on the construction of superhydrophobic coatings using biomass materials such as lignin, cellulose, chitosan and starch along with the techniques used for the constructing superhydrophobic coatings. This study is a useful resource that offers guidance on the selection of various biobased polymers for superhydrophobic coatings tailored to specific applications. The further part of the paper put a light on different application of superhydrophobic coatings employed in various disciplines and the future perspectives of the superhydrophobic coatings.
{"title":"A review on recent progress and techniques used for fabricating superhydrophobic coatings derived from biobased materials","authors":"Mugdha Shigrekar and Vaijayanti Amdoskar","doi":"10.1039/D4RA04767B","DOIUrl":"https://doi.org/10.1039/D4RA04767B","url":null,"abstract":"<p >Superhydrophobic coatings with remarkable water repellence have emerged as an increasingly prominent field of research with the growth of the material engineering and coating industries. Superhydrophobic coatings address the requirements of several application areas with characteristics including corrosion resistance, drag reduction, anti-icing, anti-fogging, and self-cleaning properties. Furthermore, the range of applications for superhydrophobic coatings has been substantially broadened by the inclusion of key performance features such as flame retardancy, thermal insulation, resistance to water penetration, UV resistance, transparency, anti-reflection, and many more. Numerous research endeavours have been focused on biomimetic superhydrophobic materials because of their distinct surface wettability. To develop superhydrophobic coatings with a long lifespan, scientists have refined the processes of material preparation and selection. To accomplish water repellency, superhydrophobic coatings are usually fabricated using harmful fluorinated chemicals or synthetic polymers. Utilising materials derived from biomass offers a sustainable alternative that uses renewable resources in order to eliminate the consumption of these hazardous substances. This paper provides an insight of several researches reported on the construction of superhydrophobic coatings using biomass materials such as lignin, cellulose, chitosan and starch along with the techniques used for the constructing superhydrophobic coatings. This study is a useful resource that offers guidance on the selection of various biobased polymers for superhydrophobic coatings tailored to specific applications. The further part of the paper put a light on different application of superhydrophobic coatings employed in various disciplines and the future perspectives of the superhydrophobic coatings.</p>","PeriodicalId":102,"journal":{"name":"RSC Advances","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ra/d4ra04767b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443199","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}
Retraction of ‘Short polyethylene glycol chains densely bound to soft nanotube channels for inhibition of protein aggregation’ by N. Kameta et al., RSC Adv., 2016, 6, 36744–36750, https://doi.org/10.1039/C6RA06793J.
撤回 N. Kameta 等人的论文 "Short polyethylene glycol chains densely bound to soft nanotube channels for inhibition of protein aggregation",RSC Adv., 2016, 6, 36744-36750, https://doi.org/10.1039/C6RA06793J。
{"title":"Retraction: Short polyethylene glycol chains densely bound to soft nanotube channels for inhibition of protein aggregation","authors":"N. Kameta, T. Matsuzawa, K. Yaoi and M. Masuda","doi":"10.1039/D4RA90125H","DOIUrl":"https://doi.org/10.1039/D4RA90125H","url":null,"abstract":"<p >Retraction of ‘Short polyethylene glycol chains densely bound to soft nanotube channels for inhibition of protein aggregation’ by N. Kameta <em>et al.</em>, <em>RSC Adv.</em>, 2016, <strong>6</strong>, 36744–36750, https://doi.org/10.1039/C6RA06793J.</p>","PeriodicalId":102,"journal":{"name":"RSC Advances","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ra/d4ra90125h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443204","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}
Nakul S., Bhagavathish R., Naveen V. Kulkarni, Ajeetkumar Patil, Suresh B. Arakera and Sam John
Two novel uranyl complexes were synthesized using bis-pyrazolyl methane ligands. The complexes were characterized by several spectroscopic techniques, including UV-Vis, IR, NMR, mass spectrometry, fluorescence, electrochemical, and thermogravimetric analysis. The solid-state structure of the complex C1 was determined with the help of single-crystal X-ray diffraction studies. The complexes C1 and C2 efficiently catalyse the oxidation of 3,5-di-tert-butyl catechol and 2-aminophenol in the atmospheric air, imitating the catalytic activity of the catechol oxidase and phenoxazinone synthase enzymes. The kinetic parameters and the catalytic efficiency (Kcat/KM) of the reactions were calculated. Formation of organic free radicals in the catalytic reactions was confirmed by EPR spectroscopy. The interaction of these complexes with the protein, bovine serum albumin, was investigated by using UV-Vis and fluorescence spectral analysis. The cytotoxicity of the complexes against MDAMB-231 and A549 cell lines was investigated, and IC50 values were determined.
{"title":"Synthesis and characterization of novel uranyl clusters supported by bis(pyrazolyl) methane ligands: biomimetic catalytic oxidation, BSA protein interaction and cytotoxicity studies†","authors":"Nakul S., Bhagavathish R., Naveen V. Kulkarni, Ajeetkumar Patil, Suresh B. Arakera and Sam John","doi":"10.1039/D4RA06347C","DOIUrl":"https://doi.org/10.1039/D4RA06347C","url":null,"abstract":"<p >Two novel uranyl complexes were synthesized using bis-pyrazolyl methane ligands. The complexes were characterized by several spectroscopic techniques, including UV-Vis, IR, NMR, mass spectrometry, fluorescence, electrochemical, and thermogravimetric analysis. The solid-state structure of the complex <strong>C1</strong> was determined with the help of single-crystal X-ray diffraction studies. The complexes <strong>C1</strong> and <strong>C2</strong> efficiently catalyse the oxidation of 3,5-di-<em>tert</em>-butyl catechol and 2-aminophenol in the atmospheric air, imitating the catalytic activity of the catechol oxidase and phenoxazinone synthase enzymes. The kinetic parameters and the catalytic efficiency (<em>K</em><small><sub>cat</sub></small>/<em>K</em><small><sub>M</sub></small>) of the reactions were calculated. Formation of organic free radicals in the catalytic reactions was confirmed by EPR spectroscopy. The interaction of these complexes with the protein, bovine serum albumin, was investigated by using UV-Vis and fluorescence spectral analysis. The cytotoxicity of the complexes against MDAMB-231 and A549 cell lines was investigated, and IC<small><sub>50</sub></small> values were determined.</p>","PeriodicalId":102,"journal":{"name":"RSC Advances","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ra/d4ra06347c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443207","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}
Herein, we report the synthesis, characterization, supramolecular gelation and multiple applications of 6-aminocoumarin-derived Schiff bases 1 and 2. Both Schiff bases underwent gelation in DMF–H2O (2 : 1, v/v), DMSO–H2O (2 : 1, v/v) and dioxane–H2O (2 : 1, v/v) involving weak forces. Furthermore, the gels were stable and exhibited good viscoelastic properties. The storage modulus (G′) of each gel was considerably higher than its loss modulus (G′′). The higher value of the crossover point and lower value of tan δ for the gel of Schiff base 2 compared to the gel of Schiff base 1 demonstrated the better gelation behaviour of 2 than that of 1 in DMF–H2O (2 : 1, v/v). Further, iodo-analogue 2 exhibited cross-linked helical morphology, whereas non-iodo analogue 1 exhibited long chain fibrous morphology, as observed via FESEM. These differences in morphology and viscoelastic behaviors were attributed to the iodo group present in 2, which influenced its aggregation involving halogen bonding. To demonstrate their application, the DMF–H2O (2 : 1, v/v) gels of both 1 and 2 recognized CN− over a series of other anions by exhibiting a gel-to-sol phase change. Besides anion sensing, gels 1 and 2 selectively detected Fe3+ and Cu2+ ions over other metal ions via a gel-to-gel colour change. Finally, CN−-treated solutions of 1 and 2 allowed the successful detection of CO2 by the naked eye. Moreover, the detection was possible using a test-kit method.
{"title":"6-Aminocoumarin-derived Schiff base gelators: aggregation and sensing of CN−, Fe3+, Cu2+ and CO2 under different conditions†","authors":"Eshani Paul, Rameez Raza, Subrata Ranjan Dhara, Nabajyoti Baildya and Kumaresh Ghosh","doi":"10.1039/D4RA05503A","DOIUrl":"https://doi.org/10.1039/D4RA05503A","url":null,"abstract":"<p >Herein, we report the synthesis, characterization, supramolecular gelation and multiple applications of 6-aminocoumarin-derived Schiff bases <strong>1</strong> and <strong>2</strong>. Both Schiff bases underwent gelation in DMF–H<small><sub>2</sub></small>O (2 : 1, v/v), DMSO–H<small><sub>2</sub></small>O (2 : 1, v/v) and dioxane–H<small><sub>2</sub></small>O (2 : 1, v/v) involving weak forces. Furthermore, the gels were stable and exhibited good viscoelastic properties. The storage modulus (<em>G</em>′) of each gel was considerably higher than its loss modulus (<em>G</em>′′). The higher value of the crossover point and lower value of tan <em>δ</em> for the gel of Schiff base <strong>2</strong> compared to the gel of Schiff base <strong>1</strong> demonstrated the better gelation behaviour of <strong>2</strong> than that of <strong>1</strong> in DMF–H<small><sub>2</sub></small>O (2 : 1, v/v). Further, iodo-analogue <strong>2</strong> exhibited cross-linked helical morphology, whereas non-iodo analogue <strong>1</strong> exhibited long chain fibrous morphology, as observed <em>via</em> FESEM. These differences in morphology and viscoelastic behaviors were attributed to the iodo group present in <strong>2</strong>, which influenced its aggregation involving halogen bonding. To demonstrate their application, the DMF–H<small><sub>2</sub></small>O (2 : 1, v/v) gels of both <strong>1</strong> and <strong>2</strong> recognized CN<small><sup>−</sup></small> over a series of other anions by exhibiting a gel-to-sol phase change. Besides anion sensing, gels <strong>1</strong> and <strong>2</strong> selectively detected Fe<small><sup>3+</sup></small> and Cu<small><sup>2+</sup></small> ions over other metal ions <em>via</em> a gel-to-gel colour change. Finally, CN<small><sup>−</sup></small>-treated solutions of <strong>1</strong> and <strong>2</strong> allowed the successful detection of CO<small><sub>2</sub></small> by the naked eye. Moreover, the detection was possible using a test-kit method.</p>","PeriodicalId":102,"journal":{"name":"RSC Advances","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ra/d4ra05503a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443203","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}
W. Kamal, Abeer Enaiet Allah, Rehab Mahmoud, Ahmed A. Farghali, Amna A. Kotp and Abdalla Abdelwahab
The energy crisis is the most urgent issue facing contemporary society and needs to be given top priority. As energy consumption rises, environmental pollution is becoming a serious issue. Direct methanol fuel cells (DMFCs) have emerged as the most promising energy source for a variety of applications such as electric vehicles and portable devices. Unfortunately, the kinetics of methanol oxidation is slow and needs an electrocatalyst to improve the reaction kinetics and the overall fuel cell efficiency. Herein, a straightforward hydrothermal procedure was utilized to prepare copper, nickel, and cobalt-based MOF composites by altering the elemental molar ratios. Cu-MOF (MOFP1), Cu/Ni-MOF (MOFP2), and Cu/Ni/Co-MOF (MOFP3) were prepared after carbonization and characterized using several key techniques such as FTIR, XRD, SEM, and EDX. The SEM analysis reveals that the morphology of MOFP1 is spherical aggregated particles, while that of MOFP2 or MOFP3 is in the form of nanoflakes and nanoflowers. Moreover, upon application of these composites as electrocatalysts for methanol electro-oxidation in an alkaline medium of 1 M NaOH using cyclic voltammetry (CV) and chronoamperometry (CA) tests, the electrochemical performance of MOFP2 in 1 M methanol exhibits the best performance for methanol oxidation with a current density reaching 38.77 mA cm−2 at a scan rate of 60 mV s−1. This can be attributed to the unique porous open flower structure and the synergistic effect between copper, nickel, and 2-aminoterephthalic acid which develop its catalytic activity.
能源危机是当代社会面临的最紧迫问题,必须予以高度重视。随着能源消耗的增加,环境污染正成为一个严重的问题。直接甲醇燃料电池(DMFC)已成为电动汽车和便携式设备等各种应用中最有前途的能源。遗憾的是,甲醇氧化的动力学过程比较缓慢,需要一种电催化剂来改善反应动力学和燃料电池的整体效率。在此,通过改变元素摩尔比,利用简单的水热法制备了铜、镍和钴基 MOF 复合材料。碳化后制备出了铜-MOF(MOFP1)、铜/镍-MOF(MOFP2)和铜/镍/钴-MOF(MOFP3),并利用傅立叶变换红外光谱、XRD、扫描电镜和 EDX 等几种关键技术对其进行了表征。扫描电镜分析表明,MOFP1 的形态为球形聚集颗粒,而 MOFP2 或 MOFP3 的形态为纳米片和纳米花。此外,利用循环伏安法(CV)和计时比拟法(CA)测试将这些复合材料作为电催化剂在 1 M NaOH 的碱性介质中进行甲醇电氧化时,MOFP2 在 1 M 甲醇中的电化学性能最佳,在 60 mV s-1 的扫描速率下电流密度达到 38.77 mA cm-2。这归功于其独特的多孔开放花结构以及铜、镍和 2-氨基对苯二甲酸之间的协同效应,从而提高了其催化活性。
{"title":"Metal–organic framework-derived nanoflower and nanoflake metal oxides as electrocatalysts for methanol oxidation†","authors":"W. Kamal, Abeer Enaiet Allah, Rehab Mahmoud, Ahmed A. Farghali, Amna A. Kotp and Abdalla Abdelwahab","doi":"10.1039/D4RA04902K","DOIUrl":"https://doi.org/10.1039/D4RA04902K","url":null,"abstract":"<p >The energy crisis is the most urgent issue facing contemporary society and needs to be given top priority. As energy consumption rises, environmental pollution is becoming a serious issue. Direct methanol fuel cells (DMFCs) have emerged as the most promising energy source for a variety of applications such as electric vehicles and portable devices. Unfortunately, the kinetics of methanol oxidation is slow and needs an electrocatalyst to improve the reaction kinetics and the overall fuel cell efficiency. Herein, a straightforward hydrothermal procedure was utilized to prepare copper, nickel, and cobalt-based MOF composites by altering the elemental molar ratios. Cu-MOF (MOFP1), Cu/Ni-MOF (MOFP2), and Cu/Ni/Co-MOF (MOFP3) were prepared after carbonization and characterized using several key techniques such as FTIR, XRD, SEM, and EDX. The SEM analysis reveals that the morphology of MOFP1 is spherical aggregated particles, while that of MOFP2 or MOFP3 is in the form of nanoflakes and nanoflowers. Moreover, upon application of these composites as electrocatalysts for methanol electro-oxidation in an alkaline medium of 1 M NaOH using cyclic voltammetry (CV) and chronoamperometry (CA) tests, the electrochemical performance of MOFP2 in 1 M methanol exhibits the best performance for methanol oxidation with a current density reaching 38.77 mA cm<small><sup>−2</sup></small> at a scan rate of 60 mV s<small><sup>−1</sup></small>. This can be attributed to the unique porous open flower structure and the synergistic effect between copper, nickel, and 2-aminoterephthalic acid which develop its catalytic activity.</p>","PeriodicalId":102,"journal":{"name":"RSC Advances","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ra/d4ra04902k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142447277","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}
Marwa Elewa, Mohamed Shehda, Pierre A. Hanna, Mohamed M. Said, Sherif Ramadan, Assem Barakat and Yasmine M. Abdel Aziz
Non-steroidal anti-inflammatory drugs NSAIDs are widely used for managing various conditions including pain, inflammation, arthritis and many musculoskeletal disorders. NSAIDs exert their biological effects by inhibiting the cyclooxygenase (COX) enzyme, which has two main isoforms COX-1 and COX-2. The COX-2 isoform is believed to be directly related to inflammation. Based on structure–activity relationship (SAR) studies of known selective COX-2 inhibitors, our aim is to design and synthesize a novel series of 2-benzamido-N-(4-substituted phenyl)thiophene-3-carboxamide derivatives. These derivatives are intended to be selective COX-2 inhibitors through structural modification of diclofenac and celecoxib. The compound 2-benzamido-5-ethyl-N-(4-fluorophenyl)thiophene-3-carboxamide VIIa demonstrated selective COX-2 inhibition with an IC50 value of 0.29 μM and a selectivity index 67.24. This is compared to celecoxib, which has an IC50 value of 0.42 μM and a selectivity index 33.8. Molecular docking studies for compound VIIa displayed high binding affinity toward COX-2. Additionally, the suppression of protein denaturation with respect to albumin was performed as an indicative measure of the potential anti-inflammatory efficacy of the novel compounds. Compound VIIa showed potent anti-inflammatory activity with 93% inhibition and an IC50 value 0.54 μM. In comparison, celecoxib achieved 94% inhibition with an IC50 value 0.89 μM. Although molecule VIIa demonstrated significant in vitro anti-inflammatory activity, adhered to Lipinski's “five rules” (RO5) and exhibited promising drug-like properties, it showed indications of poor in vivo activity. This limitation is likely due to poor aqueous solubility, which impacts its bioavailability. This issue could be addressed by incorporating the drug in niosomal nanocarrier. Niosomes were prepared using the thin-film hydration technique. These niosomes exhibited a particle size of less than 200 nm, high entrapment efficiency, and an appropriate drug loading percentage. Transmission electron microscopy (TEM) and differential scanning calorimetry (DSC) studies revealed that the niosomes were spherical and demonstrated compatibility of all of its components. The drug release study indicated that the pure drug had limited practicality for in vivo use. However, incorporating the drug into niosomes significantly improved its release profile, making it more suitable for practical use.
{"title":"Development of a selective COX-2 inhibitor: from synthesis to enhanced efficacy via nano-formulation†","authors":"Marwa Elewa, Mohamed Shehda, Pierre A. Hanna, Mohamed M. Said, Sherif Ramadan, Assem Barakat and Yasmine M. Abdel Aziz","doi":"10.1039/D4RA06295G","DOIUrl":"https://doi.org/10.1039/D4RA06295G","url":null,"abstract":"<p >Non-steroidal anti-inflammatory drugs NSAIDs are widely used for managing various conditions including pain, inflammation, arthritis and many musculoskeletal disorders. NSAIDs exert their biological effects by inhibiting the cyclooxygenase (COX) enzyme, which has two main isoforms COX-1 and COX-2. The COX-2 isoform is believed to be directly related to inflammation. Based on structure–activity relationship (SAR) studies of known selective COX-2 inhibitors, our aim is to design and synthesize a novel series of 2-benzamido-<em>N</em>-(4-substituted phenyl)thiophene-3-carboxamide derivatives. These derivatives are intended to be selective COX-2 inhibitors through structural modification of diclofenac and celecoxib. The compound 2-benzamido-5-ethyl-<em>N</em>-(4-fluorophenyl)thiophene-3-carboxamide <strong>VIIa</strong> demonstrated selective COX-2 inhibition with an IC<small><sub>50</sub></small> value of 0.29 μM and a selectivity index 67.24. This is compared to celecoxib, which has an IC<small><sub>50</sub></small> value of 0.42 μM and a selectivity index 33.8. Molecular docking studies for compound <strong>VIIa</strong> displayed high binding affinity toward COX-2. Additionally, the suppression of protein denaturation with respect to albumin was performed as an indicative measure of the potential anti-inflammatory efficacy of the novel compounds. Compound <strong>VIIa</strong> showed potent anti-inflammatory activity with 93% inhibition and an IC<small><sub>50</sub></small> value 0.54 μM. In comparison, celecoxib achieved 94% inhibition with an IC<small><sub>50</sub></small> value 0.89 μM. Although molecule <strong>VIIa</strong> demonstrated significant <em>in vitro</em> anti-inflammatory activity, adhered to Lipinski's “five rules” (RO5) and exhibited promising drug-like properties, it showed indications of poor <em>in vivo</em> activity. This limitation is likely due to poor aqueous solubility, which impacts its bioavailability. This issue could be addressed by incorporating the drug in niosomal nanocarrier. Niosomes were prepared using the thin-film hydration technique. These niosomes exhibited a particle size of less than 200 nm, high entrapment efficiency, and an appropriate drug loading percentage. Transmission electron microscopy (TEM) and differential scanning calorimetry (DSC) studies revealed that the niosomes were spherical and demonstrated compatibility of all of its components. The drug release study indicated that the pure drug had limited practicality for <em>in vivo</em> use. However, incorporating the drug into niosomes significantly improved its release profile, making it more suitable for practical use.</p>","PeriodicalId":102,"journal":{"name":"RSC Advances","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ra/d4ra06295g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443201","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}
Vaishali Amrute, Monika, K. K. Supin, M. Vasundhara and Anupama Chanda
Nanotechnology is the platform with the greatest promise for scientific advancements. One of the advancement is improvement in photocatalytic and antibacterial performance. This work was undertaken to synthesize un-doped and silver (Ag) doped zinc oxide (ZnO) nanoparticles (NPs) using an inexpensive wet chemical method and to investigate the structural and optical properties, photocatalytic and antibacterial activity. The structural analysis from X-ray diffraction (XRD) pattern of un-doped and Ag-doped ZnO NPs displayed hexagonal wurtzite crystal structure and shifting in the peak position confirms the incorporation of Ag in ZnO lattice. Morphological study done by scanning electron microscope reveals spherical shaped NPs and an increase in grain size with Ag doping, the HRTEM images showed the nanocrystalline nature of particle. The Raman spectra showed variation in vibrational characteristics of the nanoparticles with Ag doping. The functional groups were analyzed using Fourier transform-infrared spectroscopy (FTIR). The optical properties were investigated by UV-visible and photoluminescence (PL) spectroscopic techniques. The Ag-doped ZnO NPs have a notably lower band gap than that of un-doped ZnO NPs, i.e. from 3.04 eV to 2.81 eV as studied by UV-visible spectra. The PL study showed decrease in intensity at near band edge emission with increase in Ag doping concentration indicating reduction in the free charge carrier recombination. These variations in the properties play major role in the enhancement of photocatalytic and antibacterial activity with increase in Ag doping concentration as compared to un-doped zinc oxide nanoparticles. The photo degradation efficiency of 99.12 ± 1% against Methylene Blue dye was achieved in the shortest period of 45 minutes ever reported when irradiated under the solar light and efficiency of 97.33 ± 1% was achieved in 15 min under Xenon Short Arc lamp. The antibacterial study was conducted using the Agar well diffusion method where the diameter of the zone of inhibition (ZOI) was increased from 14 mm to 20 mm and 13 mm to 18 mm against the bacteria Escherchia coli and Bacillus subtilis respectively, rendering this material suitable for photocatalytic degradation and antibacterial applications.
{"title":"Observation of excellent photocatalytic and antibacterial activity of Ag doped ZnO nanoparticles","authors":"Vaishali Amrute, Monika, K. K. Supin, M. Vasundhara and Anupama Chanda","doi":"10.1039/D4RA05197A","DOIUrl":"https://doi.org/10.1039/D4RA05197A","url":null,"abstract":"<p >Nanotechnology is the platform with the greatest promise for scientific advancements. One of the advancement is improvement in photocatalytic and antibacterial performance. This work was undertaken to synthesize un-doped and silver (Ag) doped zinc oxide (ZnO) nanoparticles (NPs) using an inexpensive wet chemical method and to investigate the structural and optical properties, photocatalytic and antibacterial activity. The structural analysis from X-ray diffraction (XRD) pattern of un-doped and Ag-doped ZnO NPs displayed hexagonal wurtzite crystal structure and shifting in the peak position confirms the incorporation of Ag in ZnO lattice. Morphological study done by scanning electron microscope reveals spherical shaped NPs and an increase in grain size with Ag doping, the HRTEM images showed the nanocrystalline nature of particle. The Raman spectra showed variation in vibrational characteristics of the nanoparticles with Ag doping. The functional groups were analyzed using Fourier transform-infrared spectroscopy (FTIR). The optical properties were investigated by UV-visible and photoluminescence (PL) spectroscopic techniques. The Ag-doped ZnO NPs have a notably lower band gap than that of un-doped ZnO NPs, <em>i.e.</em> from 3.04 eV to 2.81 eV as studied by UV-visible spectra. The PL study showed decrease in intensity at near band edge emission with increase in Ag doping concentration indicating reduction in the free charge carrier recombination. These variations in the properties play major role in the enhancement of photocatalytic and antibacterial activity with increase in Ag doping concentration as compared to un-doped zinc oxide nanoparticles. The photo degradation efficiency of 99.12 ± 1% against Methylene Blue dye was achieved in the shortest period of 45 minutes ever reported when irradiated under the solar light and efficiency of 97.33 ± 1% was achieved in 15 min under Xenon Short Arc lamp. The antibacterial study was conducted using the Agar well diffusion method where the diameter of the zone of inhibition (ZOI) was increased from 14 mm to 20 mm and 13 mm to 18 mm against the bacteria <em>Escherchia coli</em> and <em>Bacillus subtilis</em> respectively, rendering this material suitable for photocatalytic degradation and antibacterial applications.</p>","PeriodicalId":102,"journal":{"name":"RSC Advances","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ra/d4ra05197a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443206","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}
Puneet Kumar, Sapna Saini, Anjali Gangwar, Rashmi Sharma and Jasha Momo H. Anal
Isobavachalcone (IBC) is a natural prenylated flavonoid containing chalcone and prenyl chain moieties with a wide range of biological and pharmacological properties. In this work, we synthesized structurally diversified derivatives (IBC-2 to IBC-10) from the natural prenylated chalcone IBC isolated from Psoralea corylifolia and assessed their antibacterial potency against the Gram-positive and Gram-negative bacterial strains S. aureus ATCC 29213, MRSA ATCC 15187, E. coli ATCC25922 and P. aeruginosa ATCC 27853. IBC and IBC-2 exhibited a minimum inhibition concentration (MIC) of 5.0 μM against S. aureus ATCC 29213, whereas IBC-3 exhibited a broad-spectrum activity against Gram-positive and Gram-negative pathogens. Cytotoxicity assessments on the murine RAW 264.7 macrophage cell line revealed minimal to moderate cytotoxicity for IBC-2 and IBC-3 with a favorable selectivity index (>10). Time- and concentration-dependent studies further supported the bactericidal nature of the compounds, as IBC, IBC-2, and IBC-3 exhibited concentration-dependent killing of S. aureus in a time-dependent manner. Furthermore, combination studies, SEM analysis, and PI staining suggest that IBC-3's mechanism of action targets the bacteria's cytoplasmic membrane or cell wall. The bioactive compounds displayed promising drug-like characteristics and a favorable pharmacokinetic profile (ADME-Tox), indicating a projected high oral bioavailability. Structure–activity relationships (SARs) drawn from this study reveal that a prenyl chain at the A-ring and hydroxy functional groups attached to the aromatic rings of chalcone scaffolds are responsible for this antibacterial potential, which will be helpful in the future discovery and development of antibiotics from natural products to overcome the antibiotic resistance crisis.
{"title":"Antibacterial activity of structurally diverse natural prenylated isobavachalcone derivatives†","authors":"Puneet Kumar, Sapna Saini, Anjali Gangwar, Rashmi Sharma and Jasha Momo H. Anal","doi":"10.1039/D4RA05370B","DOIUrl":"https://doi.org/10.1039/D4RA05370B","url":null,"abstract":"<p >Isobavachalcone (<strong>IBC</strong>) is a natural prenylated flavonoid containing chalcone and prenyl chain moieties with a wide range of biological and pharmacological properties. In this work, we synthesized structurally diversified derivatives (<strong>IBC-2</strong> to <strong>IBC-10</strong>) from the natural prenylated chalcone <strong>IBC</strong> isolated from <em>Psoralea corylifolia</em> and assessed their antibacterial potency against the Gram-positive and Gram-negative bacterial strains <em>S. aureus</em> ATCC 29213, <em>MRSA</em> ATCC 15187, <em>E. coli</em> ATCC25922 and <em>P. aeruginosa</em> ATCC 27853. <strong>IBC</strong> and <strong>IBC-2</strong> exhibited a minimum inhibition concentration (MIC) of 5.0 μM against <em>S. aureus</em> ATCC 29213, whereas <strong>IBC-3</strong> exhibited a broad-spectrum activity against Gram-positive and Gram-negative pathogens. Cytotoxicity assessments on the murine RAW 264.7 macrophage cell line revealed minimal to moderate cytotoxicity for <strong>IBC-2</strong> and <strong>IBC-3</strong> with a favorable selectivity index (>10). Time- and concentration-dependent studies further supported the bactericidal nature of the compounds, as <strong>IBC</strong>, <strong>IBC-2</strong>, and <strong>IBC-3</strong> exhibited concentration-dependent killing of <em>S. aureus</em> in a time-dependent manner. Furthermore, combination studies, SEM analysis, and PI staining suggest that <strong>IBC-3</strong>'s mechanism of action targets the bacteria's cytoplasmic membrane or cell wall. The bioactive compounds displayed promising drug-like characteristics and a favorable pharmacokinetic profile (ADME-Tox), indicating a projected high oral bioavailability. Structure–activity relationships (SARs) drawn from this study reveal that a prenyl chain at the A-ring and hydroxy functional groups attached to the aromatic rings of chalcone scaffolds are responsible for this antibacterial potential, which will be helpful in the future discovery and development of antibiotics from natural products to overcome the antibiotic resistance crisis.</p>","PeriodicalId":102,"journal":{"name":"RSC Advances","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ra/d4ra05370b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443205","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}
Anika Höppel, Olivia Bahr, Regina Ebert, Annette Wittmer, Michael Seidenstuecker, M. Carolina Lanzino, Uwe Gbureck and Sofia Dembski
Calcium phosphate (CaP) minerals have shown great promise as bone replacement materials due to their similarity to the mineral phase of natural bone. In addition to biocompatibility and osseointegration, the prevention of infection is crucial, especially due to the high concern of antibiotic resistance. In this context, a controlled drug release as well as biodegradation are important features which depend on the porosity of CaP. An increase in porosity can be achieved by using nanoparticles (NPs), which can be processed to supraparticles, combining the properties of nano- and micromaterials. In this study, Cu-doped CaP supraparticles were prepared to improve the bone substitute properties while providing antibacterial effects. In this context, a modified sol–gel process was used for the synthesis of CaP NPs, where a Ca/P molar ratio of 1.10 resulted in the formation of crystalline β-tricalcium phosphate (β-TCP) after calcination at 1000 °C. In the next step, CaP NPs with Cu2+ (0.5–15.0 wt%) were processed into supraparticles by a spray drying method. Cu release experiments of the different Cu-doped CaP supraparticles demonstrated a long-term sustained release over 14 days. The antibacterial properties of the supraparticles were determined against Gram-positive (Bacillus subtilis and Staphylococcus aureus) and Gram-negative (Escherichia coli) bacteria, where complete antibacterial inhibition was achieved using a Cu concentration of 5.0 wt%. In addition, cell viability assays of the different CaP supraparticles with human telomerase-immortalized mesenchymal stromal cells (hMSC-TERT) exhibited high biocompatibility with particle concentrations of 0.01 mg mL−1 over 72 hours.
磷酸钙(CaP)矿物质由于与天然骨的矿物质相类似,因此作为骨替代材料大有可为。除了生物相容性和骨结合性之外,预防感染也至关重要,尤其是在抗生素耐药性问题备受关注的情况下。因此,控制药物释放和生物降解是 CaP 的重要特征,而这取决于 CaP 的孔隙率。使用纳米颗粒(NPs)可以增加孔隙率,纳米颗粒可以加工成超颗粒,结合纳米和微米材料的特性。本研究制备了掺铜的 CaP 超微粒,以改善骨替代物的性能,同时提供抗菌效果。在此背景下,采用了改良的溶胶-凝胶工艺合成 CaP NPs,其中 Ca/P 摩尔比为 1.10,在 1000 °C 煅烧后形成结晶的 β-磷酸三钙(β-TCP)。下一步,采用喷雾干燥法将含 Cu2+ (0.5-15.0 wt%)的 CaP NPs 加工成超微粒。不同掺铜 CaP 超微粒的铜释放实验表明,它们能在 14 天内长期持续释放铜。实验还测定了超微粒对革兰氏阳性菌(枯草杆菌和金黄色葡萄球菌)和革兰氏阴性菌(大肠杆菌)的抗菌特性。此外,对不同的 CaP 超微粒与人类端粒酶蜕变间充质基质细胞(hMSC-TERT)进行的细胞存活率测试表明,在微粒浓度为 0.01 mg mL-1 的情况下,72 小时内具有很高的生物相容性。
{"title":"Cu-doped calcium phosphate supraparticles for bone tissue regeneration†","authors":"Anika Höppel, Olivia Bahr, Regina Ebert, Annette Wittmer, Michael Seidenstuecker, M. Carolina Lanzino, Uwe Gbureck and Sofia Dembski","doi":"10.1039/D4RA04769A","DOIUrl":"https://doi.org/10.1039/D4RA04769A","url":null,"abstract":"<p >Calcium phosphate (CaP) minerals have shown great promise as bone replacement materials due to their similarity to the mineral phase of natural bone. In addition to biocompatibility and osseointegration, the prevention of infection is crucial, especially due to the high concern of antibiotic resistance. In this context, a controlled drug release as well as biodegradation are important features which depend on the porosity of CaP. An increase in porosity can be achieved by using nanoparticles (NPs), which can be processed to supraparticles, combining the properties of nano- and micromaterials. In this study, Cu-doped CaP supraparticles were prepared to improve the bone substitute properties while providing antibacterial effects. In this context, a modified sol–gel process was used for the synthesis of CaP NPs, where a Ca/P molar ratio of 1.10 resulted in the formation of crystalline β-tricalcium phosphate (β-TCP) after calcination at 1000 °C. In the next step, CaP NPs with Cu<small><sup>2+</sup></small> (0.5–15.0 wt%) were processed into supraparticles by a spray drying method. Cu release experiments of the different Cu-doped CaP supraparticles demonstrated a long-term sustained release over 14 days. The antibacterial properties of the supraparticles were determined against Gram-positive (<em>Bacillus subtilis</em> and <em>Staphylococcus aureus</em>) and Gram-negative (<em>Escherichia coli</em>) bacteria, where complete antibacterial inhibition was achieved using a Cu concentration of 5.0 wt%. In addition, cell viability assays of the different CaP supraparticles with human telomerase-immortalized mesenchymal stromal cells (hMSC-TERT) exhibited high biocompatibility with particle concentrations of 0.01 mg mL<small><sup>−1</sup></small> over 72 hours.</p>","PeriodicalId":102,"journal":{"name":"RSC Advances","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ra/d4ra04769a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443209","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}