N. Kitamura, Ryo Noritake, Chiaki Ishibashi, Y. Idemoto
To improve electrode properties of MgMn2O4 (MMO), which has attracted attention as a positive electrode material for magnesium rechargeable batteries, we performed modification of MMO with a Mo compound and investigated particularly effects of heat-treatment temperature (600-800 °C) in the modification process on the electrode properties and crystal structures. The Mo-modified MMO were successfully synthesized by immersing MMO in an aqueous solution containing Mo ion, followed by the heat treatment. Discharge/charge cycle tests revealed that Mo-modified MMO heat-treated at 700 °C exhibited the highest discharge capacity and cycle characteristics. Crystal-structure analyses using synchrotron X-ray diffraction data showed that the heat treatment at higher temperature could relax the distortion of the crystal structure although it increased an amount of Mg and Mn cation mixing. The crystal-structure change and surface modification with a Mo compound are considered to be the factors for improved positive-electrode properties of MMO.
镁锰氧化物（MMO）作为镁充电电池的正极材料备受关注，为了改善其电极性能，我们用钼化合物对 MMO 进行了改性，并研究了改性过程中热处理温度（600-800 ℃）对电极性能和晶体结构的影响。将 MMO 浸入含 Mo 离子的水溶液中，然后进行热处理，成功合成了 Mo 改性 MMO。放电/充电循环测试表明，在 700 °C 下热处理的钼改性 MMO 具有最高的放电容量和循环特性。利用同步辐射 X 射线衍射数据进行的晶体结构分析表明，高温热处理虽然增加了镁和锰阳离子的混合量，但却能减缓晶体结构的畸变。晶体结构的变化和钼化合物的表面改性被认为是改善 MMO 正电极性能的因素。
{"title":"Effect of heat treatment on positive electrode properties and crystal structures of Mo-modified MgMn2O4","authors":"N. Kitamura, Ryo Noritake, Chiaki Ishibashi, Y. Idemoto","doi":"10.1093/chemle/upae117","DOIUrl":"https://doi.org/10.1093/chemle/upae117","url":null,"abstract":"\u0000 To improve electrode properties of MgMn2O4 (MMO), which has attracted attention as a positive electrode material for magnesium rechargeable batteries, we performed modification of MMO with a Mo compound and investigated particularly effects of heat-treatment temperature (600-800 °C) in the modification process on the electrode properties and crystal structures. The Mo-modified MMO were successfully synthesized by immersing MMO in an aqueous solution containing Mo ion, followed by the heat treatment. Discharge/charge cycle tests revealed that Mo-modified MMO heat-treated at 700 °C exhibited the highest discharge capacity and cycle characteristics. Crystal-structure analyses using synchrotron X-ray diffraction data showed that the heat treatment at higher temperature could relax the distortion of the crystal structure although it increased an amount of Mg and Mn cation mixing. The crystal-structure change and surface modification with a Mo compound are considered to be the factors for improved positive-electrode properties of MMO.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141352857","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}
Lacunary polyoxometalates represent a distinctive category of inorganic multidentate ligands that serve as precursors for building organic-inorganic hybrid materials and multinuclear metal oxo clusters. In this study, we successfully synthesized and characterized the organic-inorganic hybrid, [P2W12O44(C6H5PO3)2]10–. Two phenylphosphonato ligands were introduced at both ends of the vacant site to form the unique organic-inorganic-organic structure.
{"title":"Synthesis and Characterization of Ligand-introduced [P2W12O44(C6H5PO3)2]10–","authors":"Shumpei Take, T. Minato, M. Sadakane","doi":"10.1093/chemle/upae118","DOIUrl":"https://doi.org/10.1093/chemle/upae118","url":null,"abstract":"\u0000 Lacunary polyoxometalates represent a distinctive category of inorganic multidentate ligands that serve as precursors for building organic-inorganic hybrid materials and multinuclear metal oxo clusters. In this study, we successfully synthesized and characterized the organic-inorganic hybrid, [P2W12O44(C6H5PO3)2]10–. Two phenylphosphonato ligands were introduced at both ends of the vacant site to form the unique organic-inorganic-organic structure.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141350871","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}
Zhengyu Su, Haruka Kinoshita, Makoto Ogaito, Yoichi Takeda, Y. Toyotake, Mamoru Wakayama
In this research, we prepared novel hydrogels from enzymatically synthesized α-1,3-glucan and its carboxymethyl derivative by crosslinking with ethylene glycol diglycidyl ether. The resulting hydrogels were highly swellable and pH-sensitive with an enhanced highly developed structure and showed excellent protein/dye adsorption performances. Furthermore, the hydrogels had good biodegradability and could be degraded in soil extract solution. Herein, the prepared hydrogels have potential applications as a green and environmentally friendly adsorbent for the effective removal of organic dyes in printing and dyeing wastewater.
{"title":"Preparation and degradability of novel cross-linked functional hydrogels from enzymatic synthesized α-1,3-glucan and its carboxymethyl derivative","authors":"Zhengyu Su, Haruka Kinoshita, Makoto Ogaito, Yoichi Takeda, Y. Toyotake, Mamoru Wakayama","doi":"10.1093/chemle/upae120","DOIUrl":"https://doi.org/10.1093/chemle/upae120","url":null,"abstract":"\u0000 In this research, we prepared novel hydrogels from enzymatically synthesized α-1,3-glucan and its carboxymethyl derivative by crosslinking with ethylene glycol diglycidyl ether. The resulting hydrogels were highly swellable and pH-sensitive with an enhanced highly developed structure and showed excellent protein/dye adsorption performances. Furthermore, the hydrogels had good biodegradability and could be degraded in soil extract solution. Herein, the prepared hydrogels have potential applications as a green and environmentally friendly adsorbent for the effective removal of organic dyes in printing and dyeing wastewater.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141350451","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}
Herein, we describe a direct radical addition reaction of aryl aldehyde and N, N-dimethylaniline using iridium complex as photocatalysts to form amino alcohols under mild conditions, which exhibit an excellent convenient and sustainable methodology. The reaction could be easily scale up through continuous flow with high yield. Mechanism studies with the assistance of DFT calculations indicated such a reaction undertaking a radical pathway.
{"title":"Visible-light-catalyzed Synthesis of Amino Alcohols from N,N-dimethylaniline and Aryl Aldehyde","authors":"Jia-Hui Jin, Yi-Jian Ma, Yu-Yun Yin, Fu-Gang Zhao, Cheng-Shuo Shen, Cheng-Miao Xu, Yong-Miao Shen","doi":"10.1093/chemle/upae112","DOIUrl":"https://doi.org/10.1093/chemle/upae112","url":null,"abstract":"\u0000 Herein, we describe a direct radical addition reaction of aryl aldehyde and N, N-dimethylaniline using iridium complex as photocatalysts to form amino alcohols under mild conditions, which exhibit an excellent convenient and sustainable methodology. The reaction could be easily scale up through continuous flow with high yield. Mechanism studies with the assistance of DFT calculations indicated such a reaction undertaking a radical pathway.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141270423","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}
Shape-forming technology is essential for the widespread utilization of metal-organic frameworks. We developed a one-pot synthesis method for HKUST-1 monolith. HKUST-1 monolith was successfully prepared by the hydrothermal treatment of a Cu monolith in an aqueous solution of 1,3,5-benzenetricarboxylic acid, ethanol, and nitric acid without the addition of a metal source. The prepared HKUST-1 monolith showed CO2 adsorption properties comparable to those of commercially available HKUST-1 powdery crystals.
{"title":"One-pot synthesis of HKUST-1 monolith for CO2 adsorption","authors":"Motomu Sakai, Ayaka Ito, Takaya Matsumoto, Masahiko Matsukata","doi":"10.1093/chemle/upae109","DOIUrl":"https://doi.org/10.1093/chemle/upae109","url":null,"abstract":"\u0000 Shape-forming technology is essential for the widespread utilization of metal-organic frameworks. We developed a one-pot synthesis method for HKUST-1 monolith. HKUST-1 monolith was successfully prepared by the hydrothermal treatment of a Cu monolith in an aqueous solution of 1,3,5-benzenetricarboxylic acid, ethanol, and nitric acid without the addition of a metal source. The prepared HKUST-1 monolith showed CO2 adsorption properties comparable to those of commercially available HKUST-1 powdery crystals.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141271114","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}
K6M10.8O30 (M = Ta, Nb) with partially filled C sites in a tetragonal tungsten bronze structure represented as the general formula (A1)4(A2)2C4M10O30 shows photocatalytic activity for water splitting under UV light irradiation upon loading with suitable cocatalysts. An apparent quantum yield of the optimized NiO(0.2 wt%)-loaded K6Ta10.8O30 for water splitting is 13% at 248 nm.
{"title":"Photocatalytic water splitting over K6M10.8O30 (M = Ta, Nb) with a partially filled tetragonal tungsten bronze structure","authors":"Misa Moriya, Hideki Kato, Akihide Iwase","doi":"10.1093/chemle/upae110","DOIUrl":"https://doi.org/10.1093/chemle/upae110","url":null,"abstract":"\u0000 K6M10.8O30 (M = Ta, Nb) with partially filled C sites in a tetragonal tungsten bronze structure represented as the general formula (A1)4(A2)2C4M10O30 shows photocatalytic activity for water splitting under UV light irradiation upon loading with suitable cocatalysts. An apparent quantum yield of the optimized NiO(0.2 wt%)-loaded K6Ta10.8O30 for water splitting is 13% at 248 nm.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141271606","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}
In peptide drug discovery, the C-terminal structure of peptide compounds is crucial for enhancing the affinity with target proteins and for optimizing the compound's dynamics and physical properties. In conventional solid-phase synthesis, two steps are necessary to modify the C-terminal structure: cleavage from the resin and subsequent amidation involving activation of the resulting carboxylic acid. This process can potentially lead to racemization of the C-terminal amino acid side chain. To address this issue, we developed a novel method that, in the presence of a Ta catalyst, directly allows amines to react with amino acid-loaded resins, thereby accomplishing both resin cleavage and amidation in a single step.
在多肽药物研发中，多肽化合物的 C 端结构对于提高与目标蛋白质的亲和力以及优化化合物的动力学和物理性质至关重要。在传统的固相合成过程中，需要两个步骤来改变 C 端结构：从树脂中裂解，然后对产生的羧酸进行活化酰胺化。这一过程有可能导致 C 端氨基酸侧链的消旋化。为了解决这个问题，我们开发了一种新方法，在 Ta 催化剂的作用下，直接让胺与负载氨基酸的树脂发生反应，从而一步完成树脂裂解和酰胺化。
{"title":"Substrate-directed novel direct amidation of resin-bound amino acids","authors":"Hiroki Ozasa, H. Mikamiyama, Hisashi Yamamoto","doi":"10.1093/chemle/upae107","DOIUrl":"https://doi.org/10.1093/chemle/upae107","url":null,"abstract":"\u0000 In peptide drug discovery, the C-terminal structure of peptide compounds is crucial for enhancing the affinity with target proteins and for optimizing the compound's dynamics and physical properties. In conventional solid-phase synthesis, two steps are necessary to modify the C-terminal structure: cleavage from the resin and subsequent amidation involving activation of the resulting carboxylic acid. This process can potentially lead to racemization of the C-terminal amino acid side chain. To address this issue, we developed a novel method that, in the presence of a Ta catalyst, directly allows amines to react with amino acid-loaded resins, thereby accomplishing both resin cleavage and amidation in a single step.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141393140","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 reaction mechanisms of C3H8 dehydrogenation and subsequent metathesis on a TiH2 surface were investigated using an automated reaction path search method. The predicted pathway suggests that dehydrogenation could occur at the H vacancies present on the TiH2 surface. The propylidene species formed by the initial dehydrogenation reaction are crucial intermediates in butane formation; this compound is in turn required by the subsequent metathesis reaction on the surface of the metal hydrides.
利用自动反应路径搜索法研究了 C3H8 在 TiH2 表面脱氢和随后偏合成的反应机理。预测的路径表明，脱氢反应可能发生在 TiH2 表面的 H 空位处。初始脱氢反应形成的亚丙基物种是丁烷形成的关键中间体；而金属氢化物表面上的后续偏合成反应又需要这种化合物。
{"title":"Reaction path search for propane dehydrogenation and metathesis on titanium hydride","authors":"Takumi Miyakage, Shunsaku Yasumura, Mengwen Huang, Takashi Toyao, Z. Maeno, Ken-ichi Shimizu","doi":"10.1093/chemle/upae083","DOIUrl":"https://doi.org/10.1093/chemle/upae083","url":null,"abstract":"\u0000 The reaction mechanisms of C3H8 dehydrogenation and subsequent metathesis on a TiH2 surface were investigated using an automated reaction path search method. The predicted pathway suggests that dehydrogenation could occur at the H vacancies present on the TiH2 surface. The propylidene species formed by the initial dehydrogenation reaction are crucial intermediates in butane formation; this compound is in turn required by the subsequent metathesis reaction on the surface of the metal hydrides.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141404968","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 wish to report a new synthetic approach for diphenylacetylene in which tetrachloroethylene was reacted with phenylboronic acid in the presence of Pd catalyst, followed by a workup procedure to provide the crude product, which was then allowed to react with n-butyllithium via the halogen lithium exchange of Cl atom and loss of Li and Cl atoms to afford the desired diphenylacetylene in good yield.
{"title":"Concise synthetic routes for diphenylacetylene from tetrachloroethylene using Suzuki coupling reaction followed by treatment with n-butyllithium","authors":"Yuta Fujiki, Hiyono Suzuki, Junya Kikuzawa, Keiji Nishiwaki, N. Kawashita, Junpei Matsuoka, Akira Nakamura, Tomohiro Maegawa, Akiko Kuwabara, Masafumi Kobayashi, Kouichi Matsumoto","doi":"10.1093/chemle/upae043","DOIUrl":"https://doi.org/10.1093/chemle/upae043","url":null,"abstract":"\u0000 We wish to report a new synthetic approach for diphenylacetylene in which tetrachloroethylene was reacted with phenylboronic acid in the presence of Pd catalyst, followed by a workup procedure to provide the crude product, which was then allowed to react with n-butyllithium via the halogen lithium exchange of Cl atom and loss of Li and Cl atoms to afford the desired diphenylacetylene in good yield.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141409504","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}
Yudai Ichikawa, Kanami Sugiyama, Masahiro Higashi, Shuichi Hiraoka, Hirofumi Sato
We propose a coarse-grained analysis to understand coordination self-assembly. The developed model reduced the system into the assembling components that interact mainly electrostatically. The modeled energies sufficiently reproduced the energy changes to produce a caged di-nuclear palladium complex obtained by the density functional theory. The model made it possible to clarify the physicochemical background of the assembly process.
{"title":"A coarse-grained analysis on coordination self-assembly of a caged dinuclear palladium complex","authors":"Yudai Ichikawa, Kanami Sugiyama, Masahiro Higashi, Shuichi Hiraoka, Hirofumi Sato","doi":"10.1093/chemle/upae099","DOIUrl":"https://doi.org/10.1093/chemle/upae099","url":null,"abstract":"\u0000 We propose a coarse-grained analysis to understand coordination self-assembly. The developed model reduced the system into the assembling components that interact mainly electrostatically. The modeled energies sufficiently reproduced the energy changes to produce a caged di-nuclear palladium complex obtained by the density functional theory. The model made it possible to clarify the physicochemical background of the assembly process.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":1.6,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141410226","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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