Pub Date : 2024-12-10eCollection Date: 2024-12-01DOI: 10.1093/chemle/upae234
Masanari Shibata, Osami Shoji, Yuichiro Aiba
We have successfully achieved efficient recognition of mismatched sites in double-stranded DNA through the formation of an invasion complex by using partially noncomplementary peptide nucleic acids (PNAs). Owing to mismatches between 2 PNAs used for invasion, the undesired PNA/PNA duplex, which inhibits invasion complex formation, was destabilized. This approach overcame an inherent challenge in PNA invasion, in particular, undesired PNA/PNA duplex formation resulting from PNA complementarity, thereby enhancing overall invasion efficiency.
{"title":"Recognition of mismatched sites in double-stranded DNA by a pair of partially noncomplementary peptide nucleic acids.","authors":"Masanari Shibata, Osami Shoji, Yuichiro Aiba","doi":"10.1093/chemle/upae234","DOIUrl":"10.1093/chemle/upae234","url":null,"abstract":"<p><p>We have successfully achieved efficient recognition of mismatched sites in double-stranded DNA through the formation of an invasion complex by using partially noncomplementary peptide nucleic acids (PNAs). Owing to mismatches between 2 PNAs used for invasion, the undesired PNA/PNA duplex, which inhibits invasion complex formation, was destabilized. This approach overcame an inherent challenge in PNA invasion, in particular, undesired PNA/PNA duplex formation resulting from PNA complementarity, thereby enhancing overall invasion efficiency.</p>","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"53 12","pages":"upae234"},"PeriodicalIF":1.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11640769/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142827352","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-30eCollection Date: 2024-11-01DOI: 10.1093/chemle/upae204
Goh Sennari, Hiroki Yamagishi, Richmond Sarpong
Camphor and related monoterpenoid natural products have served as versatile "chiral pool" materials in organic chemistry for over half a century. Historically, many researchers have used a variety of transformations involving orchestrated rearrangements of the bornane skeleton to functionalize the camphor framework, expanding the utility of this chiral building block. Recent developments in C-H functionalization methodologies provide myriad opportunities to derivatize the camphor framework in a selective and predictable fashion. In this review, a short summary of the methods for functionalization of the camphor scaffold using rearrangement chemistry is provided followed by a discussion of emerging methods for directed C-H functionalizations that provide diverse new ways to derivatize the camphor framework.
{"title":"C-H functionalization of camphor through emerging approaches.","authors":"Goh Sennari, Hiroki Yamagishi, Richmond Sarpong","doi":"10.1093/chemle/upae204","DOIUrl":"10.1093/chemle/upae204","url":null,"abstract":"<p><p>Camphor and related monoterpenoid natural products have served as versatile \"chiral pool\" materials in organic chemistry for over half a century. Historically, many researchers have used a variety of transformations involving orchestrated rearrangements of the bornane skeleton to functionalize the camphor framework, expanding the utility of this chiral building block. Recent developments in C-H functionalization methodologies provide myriad opportunities to derivatize the camphor framework in a selective and predictable fashion. In this review, a short summary of the methods for functionalization of the camphor scaffold using rearrangement chemistry is provided followed by a discussion of emerging methods for directed C-H functionalizations that provide diverse new ways to derivatize the camphor framework.</p>","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"53 11","pages":"upae204"},"PeriodicalIF":1.4,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11580201/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142709266","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
SnO as a negative electrode material for Mg-ion batteries exhibited a larger capacity of 540 mA h g−1 at the first cycle than that of pure Sn, despite the lower 88 wt.% Sn content. XRD patterns and XPS spectra revealed the alloying/de-alloying with Sn formed by the reduction during the first charging. The greater capacity is attributed to the shorter Mg diffusion length in the resulting fine Sn particles. MgO matrix played a role in maintaining the high capacity for more than 10 cycles by diminishing the Sn agglomeration.
作为镁离子电池负极材料的氧化锡尽管88 wt.%的锡含量较低，但与纯锡相比，在第一个循环中显示出更大的容量（540 mA h g-1）。XRD 图谱和 XPS 光谱显示，在第一次充电过程中，通过还原形成了与锡的合金化/脱合金化。由于生成的细小锡颗粒中的镁扩散长度更短，因此容量更大。氧化镁基质减少了锡的团聚，从而在 10 个以上的循环中保持了高容量。
{"title":"Tin Oxides as a Negative Electrode Material for Mg-Ion Batteries","authors":"Keito Yamamoto, Takuya Kawai, Masahiro Shimizu","doi":"10.1093/chemle/upae177","DOIUrl":"https://doi.org/10.1093/chemle/upae177","url":null,"abstract":"SnO as a negative electrode material for Mg-ion batteries exhibited a larger capacity of 540 mA h g−1 at the first cycle than that of pure Sn, despite the lower 88 wt.% Sn content. XRD patterns and XPS spectra revealed the alloying/de-alloying with Sn formed by the reduction during the first charging. The greater capacity is attributed to the shorter Mg diffusion length in the resulting fine Sn particles. MgO matrix played a role in maintaining the high capacity for more than 10 cycles by diminishing the Sn agglomeration.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"11 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142248893","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}
Chemometrics is a useful technique to analyze large amounts of data collected to generate insights and predict behaviors, being applied to boronate supramolecules. Boronic acid-based dynamic covalent bond with diols and catechols is a great advantage for multivariate analysis, involving calibration and prediction of the % ee of enantiomeric analytes using chiral boronates. Chemometrics-assisted quantitative structure-property relationship analysis has also been applied to room-temperature phosphorescence behavior of boronate assemblies. This review highlights the effectiveness of chemometrics in experimental material chemistry.
{"title":"Chemometrics-assisted functionalization of boronic acid-derived supramolecules","authors":"Yuji Kubo, Kaede Kawaguchi, Masato Ito","doi":"10.1093/chemle/upae181","DOIUrl":"https://doi.org/10.1093/chemle/upae181","url":null,"abstract":"Chemometrics is a useful technique to analyze large amounts of data collected to generate insights and predict behaviors, being applied to boronate supramolecules. Boronic acid-based dynamic covalent bond with diols and catechols is a great advantage for multivariate analysis, involving calibration and prediction of the % ee of enantiomeric analytes using chiral boronates. Chemometrics-assisted quantitative structure-property relationship analysis has also been applied to room-temperature phosphorescence behavior of boronate assemblies. This review highlights the effectiveness of chemometrics in experimental material chemistry.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"45 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142248892","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}
Constructing highly efficient and low-cost catalysts is crucial for the reduction reaction of 4-nitrophenol (4-NP). Herein, we provide a simple processing method, including vacuum storage, natural oxidation and heating oxidation, which effectively regulates the surface oxidation state of copper nanowires and obtains copper nanowires with different oxidation states (such as Cu, Cu2O, and CuO). Research has found that CuNW-N (Cu nanowires for vacuum stotage) catalysts with a surface composition of 67.9% Cu0, 20.6% Cu+, and 11.5% Cu2+exhibit the best catalytic performance for the reduction of 4-nitrophenol (4-NP), and their reaction rate constant reach 0.791 min-1. This work provides a feasible catalyst preparation strategy for the efficient catalytic reduction of 4-NP.
{"title":"Regulating oxidation states of Cu nanowires for enhanced catalytic reduction of 4-nitrophenol","authors":"Zhong Li, Yongchen Chao, Kaiyue Sun, Junyang Cao, Dan Sun, Dengfeng Wu","doi":"10.1093/chemle/upae176","DOIUrl":"https://doi.org/10.1093/chemle/upae176","url":null,"abstract":"Constructing highly efficient and low-cost catalysts is crucial for the reduction reaction of 4-nitrophenol (4-NP). Herein, we provide a simple processing method, including vacuum storage, natural oxidation and heating oxidation, which effectively regulates the surface oxidation state of copper nanowires and obtains copper nanowires with different oxidation states (such as Cu, Cu2O, and CuO). Research has found that CuNW-N (Cu nanowires for vacuum stotage) catalysts with a surface composition of 67.9% Cu0, 20.6% Cu+, and 11.5% Cu2+exhibit the best catalytic performance for the reduction of 4-nitrophenol (4-NP), and their reaction rate constant reach 0.791 min-1. This work provides a feasible catalyst preparation strategy for the efficient catalytic reduction of 4-NP.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"408 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208290","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}
Ion-pair extraction enables the recovery of anionic metal ions, such as pertechnetate and chlorinated rhodium ions, by protonated extractants with tertiary amino N atom in their structures. We expand this technique for other anionic species dissolved in different mineral acids. Extractions of Zr, Hf, Nb, and Ta, metal anions present in sulfuric and hydrofluoric acids (H2SO4 and HF), are examined. Zr and Hf in H2SO4, and Zr, Hf, Nb, and Ta in HF can be extracted by ion-pair extraction using NTAamide (nitrilotriacetamide), methylimino-N, N’-dioctylacetamide (MIDOA), and trioctylamine (TOA). Basic information about their extraction behavior was obtained through this study.
离子对萃取可以通过质子化萃取剂回收阴离子金属离子，例如过硫酸盐和氯化铑离子，质子化萃取剂的结构中含有三级氨基 N 原子。我们将这一技术扩展到溶解在不同矿物酸中的其他阴离子物种。我们研究了硫酸和氢氟酸（H2SO4 和 HF）中的金属阴离子 Zr、Hf、Nb 和 Ta 的萃取。H2SO4 中的 Zr 和 Hf 以及 HF 中的 Zr、Hf、Nb 和 Ta 可以通过使用 NTAamide（次氮基三乙酰胺）、Methylimino-N，N'-dioctylacetamide（MIDOA）和 trioctylamine（TOA）进行离子对萃取来提取。本研究获得了有关它们萃取行为的基本信息。
{"title":"Preliminary studies on ion-pair extractions of Zr, Hf, Nb, and Ta using extractants having tertiary N atom from H2SO4 and HF","authors":"Yuji Sasaki, Masashi Kaneko, Masahiko Matsumiya","doi":"10.1093/chemle/upae164","DOIUrl":"https://doi.org/10.1093/chemle/upae164","url":null,"abstract":"Ion-pair extraction enables the recovery of anionic metal ions, such as pertechnetate and chlorinated rhodium ions, by protonated extractants with tertiary amino N atom in their structures. We expand this technique for other anionic species dissolved in different mineral acids. Extractions of Zr, Hf, Nb, and Ta, metal anions present in sulfuric and hydrofluoric acids (H2SO4 and HF), are examined. Zr and Hf in H2SO4, and Zr, Hf, Nb, and Ta in HF can be extracted by ion-pair extraction using NTAamide (nitrilotriacetamide), methylimino-N, N’-dioctylacetamide (MIDOA), and trioctylamine (TOA). Basic information about their extraction behavior was obtained through this study.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"4 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208291","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 investigation on Pt-adsorbed melamine is important in elucidating the effect of molecular decoration on enhancement of catalytic performance for fuel cells, and is an interesting system where covalent stabilisation between the surface and molecule competes with resonance destabilisation by the coordination. The present work discussed whether graph neural network potentials can predict the adsorption structure with the competition. The most stable structure predicted by preferred potential was consistent with that by density functional theory but underestimated resonance destabilisation.
{"title":"Neural Network Potential Calculations for Melamine Adsorption onto Pt (111) Comparing with Density Functional Theory","authors":"Kohei Tada","doi":"10.1093/chemle/upae173","DOIUrl":"https://doi.org/10.1093/chemle/upae173","url":null,"abstract":"The investigation on Pt-adsorbed melamine is important in elucidating the effect of molecular decoration on enhancement of catalytic performance for fuel cells, and is an interesting system where covalent stabilisation between the surface and molecule competes with resonance destabilisation by the coordination. The present work discussed whether graph neural network potentials can predict the adsorption structure with the competition. The most stable structure predicted by preferred potential was consistent with that by density functional theory but underestimated resonance destabilisation.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"11 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208292","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}
Piyapatch Techasarintr, Liu Yin, Yong Wang, Peipei Xiao, Samya Bekhti, Junko N Kondo, Toshiyuki Yokoi
The effect of introducing oxalic acid into the mother gel of TS-1 zeolite on the crystallization behavior and physiochemical properties was investigated. The addition of oxalic acid with a buffering action significantly accelerated the crystallization process of TS-1, while simultaneously inhibiting the formation of anatase. The resultant TS-1 zeolites displayed enhanced performance in catalyzing the epoxidation of 1-hexene with H2O2 as an oxidant.
{"title":"Effective incorporation of Ti atom into TS-1 zeolite assisted with oxalic acid additive","authors":"Piyapatch Techasarintr, Liu Yin, Yong Wang, Peipei Xiao, Samya Bekhti, Junko N Kondo, Toshiyuki Yokoi","doi":"10.1093/chemle/upae170","DOIUrl":"https://doi.org/10.1093/chemle/upae170","url":null,"abstract":"The effect of introducing oxalic acid into the mother gel of TS-1 zeolite on the crystallization behavior and physiochemical properties was investigated. The addition of oxalic acid with a buffering action significantly accelerated the crystallization process of TS-1, while simultaneously inhibiting the formation of anatase. The resultant TS-1 zeolites displayed enhanced performance in catalyzing the epoxidation of 1-hexene with H2O2 as an oxidant.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"1 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142226438","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 production of hydrogen peroxide (H2O2) by photocatalytic reduction of oxygen (O2) has attracted considerable attention as a more efficient and cleaner method than traditional methods for synthesizing H2O2. Carbon nitride (C3N4) is a suitable photocatalyst for H2O2 production under solar light due to its band gap. The objective of this study was to achieve rapid production and high concentration of H2O2 over a C3N4 photocatalyst through the strategy of increasing the H2O2 production rate and decreasing the H2O2 decomposition rate. The results showed that 34 mM H2O2 was produced by photocatalytic reactions in an alcohol at slightly elevated temperatures under visible light irradiation. To gain a deeper understanding of the rapid production and high concentration of H2O2, various parameters were investigated.
{"title":"A simple approach to produce 34 mM hydrogen peroxide utilizing carbon nitride photocatalysts","authors":"Hiroshi Kominami, Ryuki Yamashita, Xiangru Liu, Atsuhiro Tanaka","doi":"10.1093/chemle/upae175","DOIUrl":"https://doi.org/10.1093/chemle/upae175","url":null,"abstract":"The production of hydrogen peroxide (H2O2) by photocatalytic reduction of oxygen (O2) has attracted considerable attention as a more efficient and cleaner method than traditional methods for synthesizing H2O2. Carbon nitride (C3N4) is a suitable photocatalyst for H2O2 production under solar light due to its band gap. The objective of this study was to achieve rapid production and high concentration of H2O2 over a C3N4 photocatalyst through the strategy of increasing the H2O2 production rate and decreasing the H2O2 decomposition rate. The results showed that 34 mM H2O2 was produced by photocatalytic reactions in an alcohol at slightly elevated temperatures under visible light irradiation. To gain a deeper understanding of the rapid production and high concentration of H2O2, various parameters were investigated.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"1 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208293","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 study presents an electrochemical permeability assay for drugs using an engineered gut model. Caco-2 cells (human colorectal adenocarcinoma cell line) were cultured on porous membranes for 21 days. Acetylsalicylic acid (aspirin), after hydrolysis, was introduced from either the apical or basal sides and incubated for 2 h. The solution from the acceptor side was collected, and cyclic voltammetry was conducted to measure the hydrolyzed acetylsalicylic acid. This electrochemical approach holds promise for drug screening applications in engineered gut models.
{"title":"Electrochemical permeability assays of hydrolyzed acetylsalicylic acid (aspirin) in engineered gut models","authors":"Chisato Ito, Kosuke Ino, Yoshinobu Utagawa, Kazuyuki Iwase, Yasuhiko Shinoda, Hiroya Abe, Hitoshi Shiku","doi":"10.1093/chemle/upae174","DOIUrl":"https://doi.org/10.1093/chemle/upae174","url":null,"abstract":"This study presents an electrochemical permeability assay for drugs using an engineered gut model. Caco-2 cells (human colorectal adenocarcinoma cell line) were cultured on porous membranes for 21 days. Acetylsalicylic acid (aspirin), after hydrolysis, was introduced from either the apical or basal sides and incubated for 2 h. The solution from the acceptor side was collected, and cyclic voltammetry was conducted to measure the hydrolyzed acetylsalicylic acid. This electrochemical approach holds promise for drug screening applications in engineered gut models.","PeriodicalId":9862,"journal":{"name":"Chemistry Letters","volume":"34 1","pages":""},"PeriodicalIF":1.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208294","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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