Yasuomi Yamazaki, Riku Maruyama, H. Kumagai, Kazuhiko Maeda, Taro Tsubomura
Hybrid photocatalysts prepared by the adsorption of metal complexes on semiconductors via anchoring groups are among notable photocatalysts for selective CO2 reduction using abundant electron donors. However, their photocatalytic activities are limited by their low adsorption amounts and strength. In this study, we demonstrate the reductive polymerization of vinyl groups in metal complexes triggered by excited electrons on semiconductors as a new immobilization method. This approach significantly enhanced the adsorption amount and durability, thus increasing the photocatalytic performance.
{"title":"Hybrid Photocatalyst Constructed Using Polymerized Metal Complexes and Semiconductor Powders for Photocatalytic Carbon Dioxide Reduction","authors":"Yasuomi Yamazaki, Riku Maruyama, H. Kumagai, Kazuhiko Maeda, Taro Tsubomura","doi":"10.1093/chemle/upae085","DOIUrl":"https://doi.org/10.1093/chemle/upae085","url":null,"abstract":"\u0000 Hybrid photocatalysts prepared by the adsorption of metal complexes on semiconductors via anchoring groups are among notable photocatalysts for selective CO2 reduction using abundant electron donors. However, their photocatalytic activities are limited by their low adsorption amounts and strength. In this study, we demonstrate the reductive polymerization of vinyl groups in metal complexes triggered by excited electrons on semiconductors as a new immobilization method. This approach significantly enhanced the adsorption amount and durability, thus increasing the photocatalytic performance.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141007737","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
We have developed a transfer hydrogenation of aldehydes and ketones with B2(OH)4 as a reductant and amphiphilic resin-dispersed palladium nanoparticles as a catalyst system in an aqueous medium, where water also serves as a hydrogen donor. A variety of aldehydes and ketones, including aliphatic carbonyl compounds, reacted to give the corresponding primary and secondary alcohols, respectively. The catalyst was recovered by filtration and reused nine times without a significant loss of its catalytic activity.
{"title":"Transfer-Hydrogenation of Aldehydes and Ketones with Tetrahydroxydiboran in Water","authors":"Kaili Zhang, S. Okumura, Yasuhiro Uozumi","doi":"10.1093/chemle/upae082","DOIUrl":"https://doi.org/10.1093/chemle/upae082","url":null,"abstract":"\u0000 We have developed a transfer hydrogenation of aldehydes and ketones with B2(OH)4 as a reductant and amphiphilic resin-dispersed palladium nanoparticles as a catalyst system in an aqueous medium, where water also serves as a hydrogen donor. A variety of aldehydes and ketones, including aliphatic carbonyl compounds, reacted to give the corresponding primary and secondary alcohols, respectively. The catalyst was recovered by filtration and reused nine times without a significant loss of its catalytic activity.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141009985","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A metal-organic framework (MOF) composed of a zirconium cluster with a bis(hydroxyphenyl)anthracene linker, Zr6O4(OH)4(adhb)6 (adhb: 4,4′-(anthracene-9,10-diyl)bis(2-hydroxybenzoic acid), was designed to achieve methane storage up to 300 g and batch synthesized without using an autoclave. This MOF can adsorb 65.4 cm3STP/cm3 and 4.7w% of methane at 294 K and 9.8 bar due to its large specific surface area of 1,818 m2/g and void fraction of 0.78 cm3/g. Furthermore, an octahedral cage model indicated that the anthracene ring provides a suitable pore entrance and steric hindrance for methane inclusion.
{"title":"Zirconium-based metal-organic framework with bis(hydroxyphenyl)anthracene derivative: molecular design, synthesis, crystal structures, and methane adsorption","authors":"T. Ohmura, Yoichi Hosokawa, Hirofumi Motegi, Yusuke Mukae, Shunsuke Senda, Tsuyoshi Matsumoto, Kazuyuki Tatsumi, Akira Shichi, Hiroshi Nakamura, Arimitsu Usuki","doi":"10.1093/chemle/upae091","DOIUrl":"https://doi.org/10.1093/chemle/upae091","url":null,"abstract":"\u0000 A metal-organic framework (MOF) composed of a zirconium cluster with a bis(hydroxyphenyl)anthracene linker, Zr6O4(OH)4(adhb)6 (adhb: 4,4′-(anthracene-9,10-diyl)bis(2-hydroxybenzoic acid), was designed to achieve methane storage up to 300 g and batch synthesized without using an autoclave. This MOF can adsorb 65.4 cm3STP/cm3 and 4.7w% of methane at 294 K and 9.8 bar due to its large specific surface area of 1,818 m2/g and void fraction of 0.78 cm3/g. Furthermore, an octahedral cage model indicated that the anthracene ring provides a suitable pore entrance and steric hindrance for methane inclusion.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141131986","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The deformation of transfersomes (TFs) dispersed in deep eutectic solvents and applied to the stratum corneum (SC) was evaluated by small-angle X-ray scattering. We found that TFs permeated the SC, while the regularity and period of the multilayer structure of TFs deformed significantly, depending on the SC location and the time after application.
我们通过小角 X 射线散射评估了分散在深共晶溶剂中并涂抹在角质层（SC）上的转移体（TFs）的变形情况。我们发现 TFs 可渗透角质层，而 TFs 多层结构的规则性和周期则随角质层位置和涂抹时间的不同而发生显著变形。
{"title":"Deformation of transfersomes dispersed in hydrated deep eutectic solvent in stratum corneum","authors":"Amika Takada, Misato Matsuoka, Mina Sakuragi","doi":"10.1093/chemle/upae074","DOIUrl":"https://doi.org/10.1093/chemle/upae074","url":null,"abstract":"\u0000 The deformation of transfersomes (TFs) dispersed in deep eutectic solvents and applied to the stratum corneum (SC) was evaluated by small-angle X-ray scattering. We found that TFs permeated the SC, while the regularity and period of the multilayer structure of TFs deformed significantly, depending on the SC location and the time after application.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141038810","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A. Goto, Y. Anraku, Shigeto Fukushima, Akihiro Kishimura
Polyion complex vesicles (PICsomes) possess several features that render them as suitable for drug delivery systems. However, retaining water-soluble low-molecular-weight compounds (WLMWCs) remains challenging because of the high permeability of their vesicular membranes. Herein, we propose a new approach for prolonged retention and sustained release of WLMWCs from PICsomes by loading hydroxypropyl methylcellulose to increase the viscosity of the inner aqueous phase. The PICsomes retained 2% to 4% of the WLMWCs, and 100% of the WLMWCs were released within 96 h according to first-order kinetics.
{"title":"Polyion complex vesicles containing viscosity enhancer for sustained release of water-soluble low-molecular-weight drugs","authors":"A. Goto, Y. Anraku, Shigeto Fukushima, Akihiro Kishimura","doi":"10.1093/chemle/upae070","DOIUrl":"https://doi.org/10.1093/chemle/upae070","url":null,"abstract":"\u0000 Polyion complex vesicles (PICsomes) possess several features that render them as suitable for drug delivery systems. However, retaining water-soluble low-molecular-weight compounds (WLMWCs) remains challenging because of the high permeability of their vesicular membranes. Herein, we propose a new approach for prolonged retention and sustained release of WLMWCs from PICsomes by loading hydroxypropyl methylcellulose to increase the viscosity of the inner aqueous phase. The PICsomes retained 2% to 4% of the WLMWCs, and 100% of the WLMWCs were released within 96 h according to first-order kinetics.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141050868","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
This paper, for the first time, reports on an alternative method for measuring the free radical-scavenging properties of phenolic compounds, specifically against superoxide anion radicals (O2•−) by sonochemiluminescence (SCL) of lucigenin (Luc2+). A miniaturized sonochemical reactor is developed for the SCL observation under pulsed 450 kHz ultrasound irradiation.
{"title":"Measurement of Antioxidant Activity Against Superoxide Radical Anions by Sonochemiluminescence","authors":"Hikari Kuriya, Qilan Zhang, Shusuke Sasahara, Masanori Wakamiya, Junichiro Soejima, Jiye Jin","doi":"10.1093/chemle/upae081","DOIUrl":"https://doi.org/10.1093/chemle/upae081","url":null,"abstract":"\u0000 This paper, for the first time, reports on an alternative method for measuring the free radical-scavenging properties of phenolic compounds, specifically against superoxide anion radicals (O2•−) by sonochemiluminescence (SCL) of lucigenin (Luc2+). A miniaturized sonochemical reactor is developed for the SCL observation under pulsed 450 kHz ultrasound irradiation.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141032745","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Abstract A very powerful organic structure-directing agent (OSDA) for the synthesis of MSE-type zeolite was designed and successfully prepared. When using conventional OSDA, more than 10 d of crystallization time was necessary, whereas the use of the new type of OSDA gave a highly crystalline MSE-type zeolite using only 32 h of crystallization time.
{"title":"Remarkably facilitated crystallization of MSE-type zeolite by using an efficient organic structure-directing agent","authors":"Kaisei Nakamura, Kai Okubo, Fumiya Takaoka, Shengxiang Zhang, Satoshi Inagaki, Yoshihiro Kubota","doi":"10.1093/chemle/upae077","DOIUrl":"https://doi.org/10.1093/chemle/upae077","url":null,"abstract":"<jats:title>Abstract</jats:title> A very powerful organic structure-directing agent (OSDA) for the synthesis of MSE-type zeolite was designed and successfully prepared. When using conventional OSDA, more than 10 d of crystallization time was necessary, whereas the use of the new type of OSDA gave a highly crystalline MSE-type zeolite using only 32 h of crystallization time.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141255163","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Abstract Self-assembled hyaluronic acid (HA) microspheres are utilized for memorable optical humidity sensing. Because of the extremely high hygroscopic property of HA, the microsphere deforms in a highly humid atmosphere and the shape change is irreversible, thereby memorizing the history of the humidity change. The optically memorable humidity sensor can notify whether the humidity exceeds the upper limit of 50%.
{"title":"Hyaluronic acid microresonators for memorable humidity sensing","authors":"Hsin-Yen Liao, Wey Yih Heah, Hiroshi Yamagishi, Yohei Yamamoto","doi":"10.1093/chemle/upae078","DOIUrl":"https://doi.org/10.1093/chemle/upae078","url":null,"abstract":"<jats:title>Abstract</jats:title> Self-assembled hyaluronic acid (HA) microspheres are utilized for memorable optical humidity sensing. Because of the extremely high hygroscopic property of HA, the microsphere deforms in a highly humid atmosphere and the shape change is irreversible, thereby memorizing the history of the humidity change. The optically memorable humidity sensor can notify whether the humidity exceeds the upper limit of 50%.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141255319","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The synthesis of 2,2-difluoro-1,4-diazaboroles was achieved through the condensation of aliphatic acyltrifluoroborates and amino-N-heteroarenes under acidic conditions. Various N-heteroarenes, including pyridine, pyrimidine, pyridazine, thiazole, and isoquinoline, were successfully employed in the reaction. Among the synthesized 2,2-difluoro-1,4-diazaboroles, the one with an isoquinoline structure exhibited the most intense light blue emission.
{"title":"Synthesis and Property of 2,2-Difluoro-1,4-diazaborole","authors":"Masataka Nakahara, Yuki Wada, Masaki Kawano, Kengo Hanaya, Takeshi Sugai, Shuhei Higashibayashi","doi":"10.1093/chemle/upae069","DOIUrl":"https://doi.org/10.1093/chemle/upae069","url":null,"abstract":"\u0000 The synthesis of 2,2-difluoro-1,4-diazaboroles was achieved through the condensation of aliphatic acyltrifluoroborates and amino-N-heteroarenes under acidic conditions. Various N-heteroarenes, including pyridine, pyrimidine, pyridazine, thiazole, and isoquinoline, were successfully employed in the reaction. Among the synthesized 2,2-difluoro-1,4-diazaboroles, the one with an isoquinoline structure exhibited the most intense light blue emission.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140670163","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A synthetic method of SeCF3-substituted alkenes by a copper-mediated trifluoromethylselenolation of alkenyl iodides has been developed. In the presence of CuI and bpy, AgSeCF3 generated in-situ from Ag salt, TMSCF3, and commercially available Se powder, can be successfully coupled with alkenyl iodides to produce the trifluoromethylselenoalkenes with high chemoselectivity. The reaction shows a broad substrate scope including alkenyl iodides derived from biologically active molecules. Moreover, the feasibility of its scale-up synthesis has been demonstrated, thereby underscoring the practicality of the protocol.
通过铜介导的烯基碘化物三氟甲基硒化反应，开发了一种 SeCF3 取代烯的合成方法。在 CuI 和 bpy 的存在下，由 Ag 盐、TMSCF3 和市售 Se 粉末原位生成的 AgSeCF3 可以成功地与烯基碘化物偶联，以高化学选择性生成三氟甲基硒烯烃。该反应的底物范围很广，包括来自生物活性分子的烯基碘化物。此外，该反应还证明了放大合成的可行性，从而突出了该方案的实用性。
{"title":"Facile Preparation of SeCF3-substituted Alkenes from Alkenyl Iodides and Selenium Powder","authors":"Haruka Matsui, Yuki Kojima, Koji Hirano","doi":"10.1093/chemle/upae076","DOIUrl":"https://doi.org/10.1093/chemle/upae076","url":null,"abstract":"\u0000 A synthetic method of SeCF3-substituted alkenes by a copper-mediated trifluoromethylselenolation of alkenyl iodides has been developed. In the presence of CuI and bpy, AgSeCF3 generated in-situ from Ag salt, TMSCF3, and commercially available Se powder, can be successfully coupled with alkenyl iodides to produce the trifluoromethylselenoalkenes with high chemoselectivity. The reaction shows a broad substrate scope including alkenyl iodides derived from biologically active molecules. Moreover, the feasibility of its scale-up synthesis has been demonstrated, thereby underscoring the practicality of the protocol.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140682295","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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