Hiroyuki Tamura, Takahiro Nakama, A. Rossen, Hiroshi Ishikita, Makoto Fujita
We investigate the molecular mechanism of acetonitrile-induced structural changes in a cutinase-like enzyme in a giant coordination cage using molecular dynamics (MD) simulations. As the acetonitrile content within the cage increases, significant conformational changes of the caged protein occur due to acetonitrile binding to the specific sites, in line with protein denaturation events observed in previous nuclear magnetic resonance (NMR) studies. Accordingly, employing MD simulations on caged proteins represents an effective strategy for investigating the dynamics of unstable protein structures.
{"title":"Organic Solvent-Induced Structural Changes in a Protein Confined in a Giant Coordination Cage","authors":"Hiroyuki Tamura, Takahiro Nakama, A. Rossen, Hiroshi Ishikita, Makoto Fujita","doi":"10.1093/chemle/upae101","DOIUrl":"https://doi.org/10.1093/chemle/upae101","url":null,"abstract":"\u0000 We investigate the molecular mechanism of acetonitrile-induced structural changes in a cutinase-like enzyme in a giant coordination cage using molecular dynamics (MD) simulations. As the acetonitrile content within the cage increases, significant conformational changes of the caged protein occur due to acetonitrile binding to the specific sites, in line with protein denaturation events observed in previous nuclear magnetic resonance (NMR) studies. Accordingly, employing MD simulations on caged proteins represents an effective strategy for investigating the dynamics of unstable protein structures.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141122521","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}
Hiromasa Niinomi, Hiroshi Y Yoshikawa, Ryuzo Kawamura, T. Yamazaki, Tomoya Oshikiri, Masaru Nakagawa
Nucleation from an aqueous solution is an important step in crystallization which controls the physicochemical properties of crystalline materials. Although dense liquid droplets are considered as a precursor of a crystal in the two-step nucleation model, their actual role is unclear. Our in-situ microscopic observations of the crystallization of DL-alanine from a dense liquid droplet trapped by laser tweezers show that the liquid droplets play the role of a substrate facilitating heterogeneous nucleation rather than a precursor of a crystal.
{"title":"In-Situ Observation of DL-Alanine Crystallization from a Laser-Trapped Dense Liquid Droplet as a Heterogeneous Nucleation Site","authors":"Hiromasa Niinomi, Hiroshi Y Yoshikawa, Ryuzo Kawamura, T. Yamazaki, Tomoya Oshikiri, Masaru Nakagawa","doi":"10.1093/chemle/upae100","DOIUrl":"https://doi.org/10.1093/chemle/upae100","url":null,"abstract":"\u0000 Nucleation from an aqueous solution is an important step in crystallization which controls the physicochemical properties of crystalline materials. Although dense liquid droplets are considered as a precursor of a crystal in the two-step nucleation model, their actual role is unclear. Our in-situ microscopic observations of the crystallization of DL-alanine from a dense liquid droplet trapped by laser tweezers show that the liquid droplets play the role of a substrate facilitating heterogeneous nucleation rather than a precursor of a crystal.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141120756","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 Pd/Fe bimetallic catalyst in the presence of the Xantphos ligand promoted the cross-coupling reaction of alcohols and nitroarenes via a hydrogen-transfer redox system. The consecutive formation of aldimines from benzyl alcohols and nitroarenes proceeded in three steps in a single manipulation: oxidation of alcohols, reduction of nitroarenes, and dehydrative condensation of aldehydes and aminoarenes.
{"title":"Palladium-Iron Bimetallic-Catalyzed Cross-Coupling Reaction of Alcohols and Nitroarenes Using a Hydrogen-Transfer Redox System","authors":"Rikiya Horikawa, Shoma Ishii, Urara Shinozaki, Reika Midorikawa, Takamichi Mori, Masanari Kimura","doi":"10.1093/chemle/upae094","DOIUrl":"https://doi.org/10.1093/chemle/upae094","url":null,"abstract":"\u0000 A Pd/Fe bimetallic catalyst in the presence of the Xantphos ligand promoted the cross-coupling reaction of alcohols and nitroarenes via a hydrogen-transfer redox system. The consecutive formation of aldimines from benzyl alcohols and nitroarenes proceeded in three steps in a single manipulation: oxidation of alcohols, reduction of nitroarenes, and dehydrative condensation of aldehydes and aminoarenes.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140962226","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}
Yu Zhang, Peng Guo, Yonghua Tang, Hongxing Li, R. Mo
Slow oxygen evolution kinetics and severe corrosion limit the further application of BiVO4 photoelectrodes in photoelectrochemical water splitting. Here, BiVO4/Co-Pi/Ni(OH)2 photoanodes were synthetized aiming at improving its photoelectric conversion efficiency and stability. Compared with pure BiVO4 photoanode, the BiVO4/Co-Pi/Ni(OH)2 photoanode enhanced the photocurrent from 1.1 mA/cm2 to 4.5 mA/cm2 at 1.23 V versus reversible hydrogen electrode. In addition, Ni(OH)2 acted as a corrosion protection layer on the surface of the photoanode, allowing the BiVO4/Co-Pi/Ni(OH)2 photoanode to exhibit excellent stability.
{"title":"Dual-layer cocatalysts of Co-Pi and Ni(OH)2 on BiVO4 photoanodes for efficient water oxidation","authors":"Yu Zhang, Peng Guo, Yonghua Tang, Hongxing Li, R. Mo","doi":"10.1093/chemle/upae096","DOIUrl":"https://doi.org/10.1093/chemle/upae096","url":null,"abstract":"\u0000 Slow oxygen evolution kinetics and severe corrosion limit the further application of BiVO4 photoelectrodes in photoelectrochemical water splitting. Here, BiVO4/Co-Pi/Ni(OH)2 photoanodes were synthetized aiming at improving its photoelectric conversion efficiency and stability. Compared with pure BiVO4 photoanode, the BiVO4/Co-Pi/Ni(OH)2 photoanode enhanced the photocurrent from 1.1 mA/cm2 to 4.5 mA/cm2 at 1.23 V versus reversible hydrogen electrode. In addition, Ni(OH)2 acted as a corrosion protection layer on the surface of the photoanode, allowing the BiVO4/Co-Pi/Ni(OH)2 photoanode to exhibit excellent stability.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140970345","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}
Minori Abe, C. Kachi‐Terajima, Masahiro Toyoda, Yasushi Ohga, Takunori Harada
To demonstrate chiral induction and amplification in the solid state, we investigated co-crystals prepared from (S)- or (R)-1-phenylethylamine and achiral biphenyl-4-carboxylic acid by solvent-free crystallization. The chiroptical and optical properties of the co-crystals were characterized by circular dichroism spectroscopy, Fourier transform infrared spectroscopy, and time-dependent density functional theory calculations, revealing chiral induction and amplification in the solid phase.
{"title":"Chiral induction and amplification of achiral molecules induced by chiral compounds in solid matrices","authors":"Minori Abe, C. Kachi‐Terajima, Masahiro Toyoda, Yasushi Ohga, Takunori Harada","doi":"10.1093/chemle/upae097","DOIUrl":"https://doi.org/10.1093/chemle/upae097","url":null,"abstract":"\u0000 To demonstrate chiral induction and amplification in the solid state, we investigated co-crystals prepared from (S)- or (R)-1-phenylethylamine and achiral biphenyl-4-carboxylic acid by solvent-free crystallization. The chiroptical and optical properties of the co-crystals were characterized by circular dichroism spectroscopy, Fourier transform infrared spectroscopy, and time-dependent density functional theory calculations, revealing chiral induction and amplification in the solid phase.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140976636","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}
With recent advances in photoredox chemistry, a variety of methods for generating carbon radicals have emerged. This review highlights recent approaches for radical generation utilizing zirconocene(III), a species infrequently employed in organic syntheses. Of particular interest are methods employing visible light irradiation, which induce C–Zr bond homolysis of alkyl zirconium species or activate a photoredox catalyst to reduce zirconocene(IV).
{"title":"Harnessing Zirconocene (III) for Photoinduced Carbon Radical Generation","authors":"Eisuke Ota, Kazuhiro Aida, Junichiro Yamaguchi","doi":"10.1093/chemle/upae095","DOIUrl":"https://doi.org/10.1093/chemle/upae095","url":null,"abstract":"\u0000 With recent advances in photoredox chemistry, a variety of methods for generating carbon radicals have emerged. This review highlights recent approaches for radical generation utilizing zirconocene(III), a species infrequently employed in organic syntheses. Of particular interest are methods employing visible light irradiation, which induce C–Zr bond homolysis of alkyl zirconium species or activate a photoredox catalyst to reduce zirconocene(IV).","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140976977","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}
Poly(triazine imide) synthesized by the molten salt route with incorporation of Li+ and Cl‒ ions (PTI/Li + Cl-) was prepared by rational controlling the washing extent. The surface transformation of the phase-pure PTI framework incurred by thorough washing has been confirmed by a systematic analysis based on XRD, UV Raman, AFM and XPS measurements. Uranyl ion adsorption experiments further support the surface structural transformation from triazine-unit PTI to heptazine-based graphitic carbon nitride. Efforts on the exploration of PTI material application should be mainly directed to the waterless fields to give good repeatability.
{"title":"Surface structural transformation and adsorption performance of Poly(triazine imide)","authors":"Gege Yu, Yubao Zhao","doi":"10.1093/chemle/upae089","DOIUrl":"https://doi.org/10.1093/chemle/upae089","url":null,"abstract":"\u0000 Poly(triazine imide) synthesized by the molten salt route with incorporation of Li+ and Cl‒ ions (PTI/Li + Cl-) was prepared by rational controlling the washing extent. The surface transformation of the phase-pure PTI framework incurred by thorough washing has been confirmed by a systematic analysis based on XRD, UV Raman, AFM and XPS measurements. Uranyl ion adsorption experiments further support the surface structural transformation from triazine-unit PTI to heptazine-based graphitic carbon nitride. Efforts on the exploration of PTI material application should be mainly directed to the waterless fields to give good repeatability.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140980193","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 title complex was newly synthesized by straightforward ligand substitution of a parent complex having a N2P2 set. The present complex had a deformed rhomboidal {Cu2I2} core with shortened Cu···Cu and prolonged I···I diagonals compared to those of the parent complex and formed one-dimensional channels filled with solvent molecules in crystals. The complex exhibited unusual red shift in solid-state photoluminescence assigned to halogen/metal-to-ligand charge transfer, indicating association of the unique crystal packing containing intramolecular electronic coupling between benzothienobenzothiophene moieties.
{"title":"Iodo-Bridged Dicopper(I) Complex Containing a Benzothienobenzothiophene (BTBT) Unit: Structure, Characterization, and Crystal Packing Effects on Solid-State Photoluminescence","authors":"Takashi Ikeda, Keishiro Tahara, Tomofumi Kadoya, Yoshiki Ozawa, Masaaki Abe","doi":"10.1093/chemle/upae092","DOIUrl":"https://doi.org/10.1093/chemle/upae092","url":null,"abstract":"\u0000 The title complex was newly synthesized by straightforward ligand substitution of a parent complex having a N2P2 set. The present complex had a deformed rhomboidal {Cu2I2} core with shortened Cu···Cu and prolonged I···I diagonals compared to those of the parent complex and formed one-dimensional channels filled with solvent molecules in crystals. The complex exhibited unusual red shift in solid-state photoluminescence assigned to halogen/metal-to-ligand charge transfer, indicating association of the unique crystal packing containing intramolecular electronic coupling between benzothienobenzothiophene moieties.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140993127","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}
Chihiro Maeda, Ren Kumemoto, Rio Tanaka, Tadashi Ema
Light-driven ring-opening carboxylation of epoxides with CO2 provided β-hydroxy acids via the sequential single electron transfer (SET), followed by the reaction with CO2. This reaction condition was applicable to aryl epoxides and oxetanes with (hetero)polycyclic aromatics to give the corresponding β- and γ-hydroxy acids, respectively, with the high chemoselectivity.
{"title":"Synthesis of Hydroxy Acids via the Light-Driven Carboxylation of Epoxides with CO2","authors":"Chihiro Maeda, Ren Kumemoto, Rio Tanaka, Tadashi Ema","doi":"10.1093/chemle/upae086","DOIUrl":"https://doi.org/10.1093/chemle/upae086","url":null,"abstract":"\u0000 Light-driven ring-opening carboxylation of epoxides with CO2 provided β-hydroxy acids via the sequential single electron transfer (SET), followed by the reaction with CO2. This reaction condition was applicable to aryl epoxides and oxetanes with (hetero)polycyclic aromatics to give the corresponding β- and γ-hydroxy acids, respectively, with the high chemoselectivity.","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":"141006174","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}
Adsorption is crucial for the performance of photocatalysts in degrading new pollutants. Here, we report a magnetic molecularly imprinted material Fe3O4@SiO2@TiO2@MIPs with a semiconductor/insulator/semiconductor structure, which achieved up to 81% preferential degradation of berberine hydrochloride (BH). The significant enhancement of catalytic performance can be attributed to the interaction between BH and the imprinted cavity, as well as size matching, which proposes new solutions to address the current problem of difficult degradation of new pollutants.
{"title":"Study on the specific photodegradation performance of Fe3O4@SiO2@TiO2@MIPs for berberine hydrochloride","authors":"Junfu Xiong, Hao Tian, Xicheng Li, Changzheng Wang, Shoufang Xu","doi":"10.1093/chemle/upae080","DOIUrl":"https://doi.org/10.1093/chemle/upae080","url":null,"abstract":"\u0000 Adsorption is crucial for the performance of photocatalysts in degrading new pollutants. Here, we report a magnetic molecularly imprinted material Fe3O4@SiO2@TiO2@MIPs with a semiconductor/insulator/semiconductor structure, which achieved up to 81% preferential degradation of berberine hydrochloride (BH). The significant enhancement of catalytic performance can be attributed to the interaction between BH and the imprinted cavity, as well as size matching, which proposes new solutions to address the current problem of difficult degradation of new pollutants.","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":"141008395","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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