Pyrazino[2,3-b]pyrazine (PP), which is a naphthalene analogue with iminium nitrogen atoms at 1,4,5,8-positions instead of sp2-carbon atoms, is attractive as a building block for nitrogen-highly-contained π-conjugated systems. In this study, we synthesized PP-based linear and tripodal molecules, in which PP moieties are bonded with the central benzene ring at 1,4-positions and 1,3,5-positions, respectively, giving conformationally flexible and moderately π-conjugated molecules. It is noteworthy that the tripodal one forms unique interdigitated dimer with a small cavity in a crystalline state because of flexible tripodal molecular shape.
{"title":"Synthesis, Solid State Structures, and Properties of Linear and Tripodal Flexible Molecules with Pyrazinopyrazine Moieties","authors":"Yuto Ohmura, Ryusei Oketani, Akihito Konishi, Makoto Yasuda, Ichiro Hisaki","doi":"10.1093/chemle/upae140","DOIUrl":"https://doi.org/10.1093/chemle/upae140","url":null,"abstract":"Pyrazino[2,3-b]pyrazine (PP), which is a naphthalene analogue with iminium nitrogen atoms at 1,4,5,8-positions instead of sp2-carbon atoms, is attractive as a building block for nitrogen-highly-contained π-conjugated systems. In this study, we synthesized PP-based linear and tripodal molecules, in which PP moieties are bonded with the central benzene ring at 1,4-positions and 1,3,5-positions, respectively, giving conformationally flexible and moderately π-conjugated molecules. It is noteworthy that the tripodal one forms unique interdigitated dimer with a small cavity in a crystalline state because of flexible tripodal molecular shape.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"17 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141585692","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}
Fan Zhang, Yong-Hsin Wang, Cheng-Lin Wu, Tzu-Chau Lin, Manabu Abe
A series of coumarin-based quadrupolar and octupolar derivatives containing electron-donating substituents (carbazole or diphenylamine groups) were synthesized. Their photophysical properties were explored in different organic solvents (toluene, dichloromethane, and dimethyl sulfoxide). Each donor group was connected via cyclic stilbene based on coumarin, resulting in compounds with large two-photon absorption cross-sections.
{"title":"Molecular engineering of coumarins for enhanced two-photon absorption property","authors":"Fan Zhang, Yong-Hsin Wang, Cheng-Lin Wu, Tzu-Chau Lin, Manabu Abe","doi":"10.1093/chemle/upae131","DOIUrl":"https://doi.org/10.1093/chemle/upae131","url":null,"abstract":"A series of coumarin-based quadrupolar and octupolar derivatives containing electron-donating substituents (carbazole or diphenylamine groups) were synthesized. Their photophysical properties were explored in different organic solvents (toluene, dichloromethane, and dimethyl sulfoxide). Each donor group was connected via cyclic stilbene based on coumarin, resulting in compounds with large two-photon absorption cross-sections.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"37 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141567551","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}
CdS/ZnS core-shell semiconductor quantum dots (QDs) were hybridized with1-naphthalenecarboxylic acid, a triplet transmitter, by a ligand exchange method. UV emission peaked at 340 nm or longer was obtained by visible continuous-wave excitation at 405 nm in n-hexane solution by mixing the hybridized QD with 2,5-diphenyloxazole (PPO) as UV emitter, based on triplet-triplet annihilation upconversion (TTA-UC) mechanism. The same mixture but in tetrahydrofuran gave solid film by solution casting, and the solid showed upconversion emission in near UV spectral region (380-395 nm) by 405-nm excitation.
{"title":"Near UV photon upconversion in cast solid with quantum dot","authors":"Kenta Sawaguchi, Kazuki Inada, Daichi Eguchi, Kenji Kamada, Naoto Tamai","doi":"10.1093/chemle/upae137","DOIUrl":"https://doi.org/10.1093/chemle/upae137","url":null,"abstract":"CdS/ZnS core-shell semiconductor quantum dots (QDs) were hybridized with1-naphthalenecarboxylic acid, a triplet transmitter, by a ligand exchange method. UV emission peaked at 340 nm or longer was obtained by visible continuous-wave excitation at 405 nm in n-hexane solution by mixing the hybridized QD with 2,5-diphenyloxazole (PPO) as UV emitter, based on triplet-triplet annihilation upconversion (TTA-UC) mechanism. The same mixture but in tetrahydrofuran gave solid film by solution casting, and the solid showed upconversion emission in near UV spectral region (380-395 nm) by 405-nm excitation.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"14 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141567550","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}
Silicon nitride (Si3N4) exhibits low friction in aqueous environments due to a tribolayer that is formed through tribochemical reactions. However, the low friction state is not maintained in high contact pressure conditions, where surface-surface contact is dominant at the sliding interface, i.e. the load carrying capacity is low. Recently, it was reported that an ethylene glycol (EG) additive improves the load carrying capacity of Si3N4 in aqueous environments, though their mechanism is still in debate. In this study, we performed friction simulations to analyze the tribochemical reactions of water and an EG additive using a neural network molecular dynamics method which enables large-scale simulation with high accuracy comparable with ab initio molecular dynamics calculations. We found that tribochemical reactions of water produce SiO2 particles. On the other hand, tribochemical reactions of EG produce compounds which consist of carbon, nitrogen, and hydrogen atoms on the Si3N4 surface and the Si3N4 surface is covered by the compounds. Based on this finding, we propose that the compounds covering the Si3N4 surface can improve its load carrying capacity.
{"title":"Neural network molecular dynamics simulation on friction-induced chemical reactions of Si3N4 in water and ethylene glycol environments","authors":"Ryutaro Kudo, Yusuke Ootani, Shogo Fukushima, Nobuki Ozawa, Momoji Kubo","doi":"10.1093/chemle/upae114","DOIUrl":"https://doi.org/10.1093/chemle/upae114","url":null,"abstract":"Silicon nitride (Si3N4) exhibits low friction in aqueous environments due to a tribolayer that is formed through tribochemical reactions. However, the low friction state is not maintained in high contact pressure conditions, where surface-surface contact is dominant at the sliding interface, i.e. the load carrying capacity is low. Recently, it was reported that an ethylene glycol (EG) additive improves the load carrying capacity of Si3N4 in aqueous environments, though their mechanism is still in debate. In this study, we performed friction simulations to analyze the tribochemical reactions of water and an EG additive using a neural network molecular dynamics method which enables large-scale simulation with high accuracy comparable with ab initio molecular dynamics calculations. We found that tribochemical reactions of water produce SiO2 particles. On the other hand, tribochemical reactions of EG produce compounds which consist of carbon, nitrogen, and hydrogen atoms on the Si3N4 surface and the Si3N4 surface is covered by the compounds. Based on this finding, we propose that the compounds covering the Si3N4 surface can improve its load carrying capacity.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"116 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141567592","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}
There are only limited methods available to synthesize metastable olivine NaMnPO4, and these methods all involve a time-consuming process. Herein, we report a rapid synthesis of olivine NaMnPO4, and the results show that the formation of olivine NaMnPO4 highly depends on the Na/Mn/P ratio and the pH of the reaction system, and pure olivine NaMnPO4 can be hydrothermally synthesized for only 1 h under appropriate conditions. This communication provides an efficient process for synthesis of olivine NaMnPO4.
{"title":"Rapid synthesis of olivine NaMnPO4","authors":"Han Xiao, Haisheng Fang","doi":"10.1093/chemle/upae125","DOIUrl":"https://doi.org/10.1093/chemle/upae125","url":null,"abstract":"There are only limited methods available to synthesize metastable olivine NaMnPO4, and these methods all involve a time-consuming process. Herein, we report a rapid synthesis of olivine NaMnPO4, and the results show that the formation of olivine NaMnPO4 highly depends on the Na/Mn/P ratio and the pH of the reaction system, and pure olivine NaMnPO4 can be hydrothermally synthesized for only 1 h under appropriate conditions. This communication provides an efficient process for synthesis of olivine NaMnPO4.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"28 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141548445","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 new and effective method for the [3 + 2] annulation of β-oxo-acrylamides with diethyl 2-oxomalonate, catalyzed by NEt3, has been developed to be carried out under mild reaction conditions. This approach offers a direct route to synthesize oxazolidin-4-one derivatives with yields ranging from 58% to 76%. The process is notable for being highly atom-efficient and operationally simple.
{"title":"Et3N-catalyzed [3 + 2] annulation reaction of β-oxo-acrylamides with diethyl 2-oxomalonates: facile access to oxazolidin-4-one derivatives","authors":"Lingang Wu, Baochuan Guan, Zhaoxue Wang, Lei Xie","doi":"10.1093/chemle/upae116","DOIUrl":"https://doi.org/10.1093/chemle/upae116","url":null,"abstract":"A new and effective method for the [3 + 2] annulation of β-oxo-acrylamides with diethyl 2-oxomalonate, catalyzed by NEt3, has been developed to be carried out under mild reaction conditions. This approach offers a direct route to synthesize oxazolidin-4-one derivatives with yields ranging from 58% to 76%. The process is notable for being highly atom-efficient and operationally simple.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"17 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141518755","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}
Visible-light activation of photocatalysts is crucial for effectively utilizing solar energy in molecular conversions. This study demonstrates that modifying the bipyridine ligand with carbazole enables visible-light activation of a Ru(II) carbonyl complex catalyst, which is originally developed as an electrocatalyst for CO2 reduction but inactive as a photocatalyst on its own. The present study opens avenues for individually designing light-absorbing ligands and catalytic functions within one mononuclear complex.
{"title":"Visible-Light Activation of a Ru(II) Complex Catalyst via a Carbazole-Modified Donor–Acceptor Ligand for CO2 Reduction","authors":"Akinobu Nakada, Yuya Tomiura, Hajime Suzuki, Osamu Tomita, Ryu Abe","doi":"10.1093/chemle/upae127","DOIUrl":"https://doi.org/10.1093/chemle/upae127","url":null,"abstract":"Visible-light activation of photocatalysts is crucial for effectively utilizing solar energy in molecular conversions. This study demonstrates that modifying the bipyridine ligand with carbazole enables visible-light activation of a Ru(II) carbonyl complex catalyst, which is originally developed as an electrocatalyst for CO2 reduction but inactive as a photocatalyst on its own. The present study opens avenues for individually designing light-absorbing ligands and catalytic functions within one mononuclear complex.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"38 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141531212","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}
Realizing multiple metastable configurations in a single porous coordination polymer (PCP) has long been pursued to achieve switchable functionality. In this study, we reported multiple configurations in one PCP material via the design of the adjustable intraframework π-π stacking moieties. We demonstrated that the PCP can accommodate three different open pore phases depending on the type of solvent. Furthermore, this PCP exhibits three distinct closed pore phases depending on the activation approaches, demonstrating different CO2 sorption properties.
{"title":"Flexible Porous Coordination Polymer with Multiple Configurations for Guest Recognition and Switchable CO2 Sorption Properties","authors":"Ping Wang, Ken-ichi Otake, Shotaro Hiraide, Yoshiki Kubota, Shogo Kawaguchi, Susumu Kitagawa","doi":"10.1093/chemle/upae128","DOIUrl":"https://doi.org/10.1093/chemle/upae128","url":null,"abstract":"Realizing multiple metastable configurations in a single porous coordination polymer (PCP) has long been pursued to achieve switchable functionality. In this study, we reported multiple configurations in one PCP material via the design of the adjustable intraframework π-π stacking moieties. We demonstrated that the PCP can accommodate three different open pore phases depending on the type of solvent. Furthermore, this PCP exhibits three distinct closed pore phases depending on the activation approaches, demonstrating different CO2 sorption properties.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"2012 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141518756","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}
Sanhanut Kesornsit, Tsuyoshi Taniguchi, Mai Nozaki, Tatsuya Nishimura, Katsuhiro Maeda
A symmetrically meta-substituted poly(diphenylacetylene) bearing chiral amide groups was synthesized by reacting (R)-1-phenylethylamine with a carboxy-group-containing precursor polymer, which was obtained by polymerizing the corresponding ester-containing diphenylacetylene using a modified Mo(V)-based catalytic system followed by hydrolysis. The polymer formed a one-handed helical conformation when thermally annealed in a solvent. The chiral recognition ability of the polymer before and after thermal annealing was investigated when used as a chiral stationary phase for high-performance liquid chromatography.
{"title":"Synthesis of a Symmetrically meta-Substituted Poly(diphenylacetylene) Bearing Chiral Amide Groups and Its Application as a Chiral Stationary Phase for HPLC","authors":"Sanhanut Kesornsit, Tsuyoshi Taniguchi, Mai Nozaki, Tatsuya Nishimura, Katsuhiro Maeda","doi":"10.1093/chemle/upae129","DOIUrl":"https://doi.org/10.1093/chemle/upae129","url":null,"abstract":"A symmetrically meta-substituted poly(diphenylacetylene) bearing chiral amide groups was synthesized by reacting (R)-1-phenylethylamine with a carboxy-group-containing precursor polymer, which was obtained by polymerizing the corresponding ester-containing diphenylacetylene using a modified Mo(V)-based catalytic system followed by hydrolysis. The polymer formed a one-handed helical conformation when thermally annealed in a solvent. The chiral recognition ability of the polymer before and after thermal annealing was investigated when used as a chiral stationary phase for high-performance liquid chromatography.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"8 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141502675","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}
Solvated metal cations represent fundamental and crucial mononuclear species in various research fields, including chemical, physical, and biochemical studies. However, controlling their coordination geometry poses a significant challenge. In this study, we successfully synthesized and structurally characterized solvated Ba2+ complexes. The coordination geometry of [Ba(CH3CN)8]2+ was a thermodynamically stable square antiprism, while that of [Ba{(CH3)2CO}8]2+ exhibited a rare cubic structure, demonstrating a unique approach to controlling coordination geometry solely by altering crystallization solvents.
{"title":"Solvated Ba2+ with square antiprismatic and cubic coordination geometries","authors":"Ayano Umakoshi, Takuo Minato, Yusuke Kanematsu, Masahiro Sadakane","doi":"10.1093/chemle/upae126","DOIUrl":"https://doi.org/10.1093/chemle/upae126","url":null,"abstract":"Solvated metal cations represent fundamental and crucial mononuclear species in various research fields, including chemical, physical, and biochemical studies. However, controlling their coordination geometry poses a significant challenge. In this study, we successfully synthesized and structurally characterized solvated Ba2+ complexes. The coordination geometry of [Ba(CH3CN)8]2+ was a thermodynamically stable square antiprism, while that of [Ba{(CH3)2CO}8]2+ exhibited a rare cubic structure, demonstrating a unique approach to controlling coordination geometry solely by altering crystallization solvents.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"1 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141502677","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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