ChemistryEurope最新文献_第8页

Water Chemistry at the Nanoscale: Clues for Resolving the “Water Paradox” Underlying the Emergence of Life 纳米尺度的水化学：解决生命出现所依据的 "水悖论 "的线索

ChemistryEurope Pub Date : 2024-10-10 DOI: 10.1002/ceur.202400038

Dr. Hye-Eun Lee, Dr. Michael Russell, Prof. Ryuhei Nakamura

{"title":"Water Chemistry at the Nanoscale: Clues for Resolving the “Water Paradox” Underlying the Emergence of Life","authors":"Dr. Hye-Eun Lee, Dr. Michael Russell, Prof. Ryuhei Nakamura","doi":"10.1002/ceur.202400038","DOIUrl":"https://doi.org/10.1002/ceur.202400038","url":null,"abstract":"Water is the most common, yet highly peculiar, liquid on Earth. Biological systems manipulate the properties of water to perform reactions that are extremely difficult in synthetic chemistry. One such example is polymerization, which is essential for life and requires the removal of water; however, the removal of water adversely affects the redox reactions that harness the free energy to sustain life. This dichotomy in the water chemistry of life is referred to as the “water paradox”, which remains an unsolved puzzle in the origins of life research. In the present concept paper, we propose that the water paradox may be resolved if anomalous water behavior, including the extremely low dielectric constant and modulation of the enthalpy-entropy compensation relationship arising from nanoscale confinement, are considered. The unique properties of confined water allow for polymerization reactions to proceed even in water-rich hydrothermal vent (HV) environments due to the structurally aligned nanopores within HV walls. Studies of how structural changes in water networks in nano-spaces affect catalysis and free energy exchange represent the next frontier in the field of origins of life research and synthetic chemistry.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202400038","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142664849","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Total Synthesis of the Humulene-Derived Sesquiterpenoid (-)-Integrifolian-1,5-dione 葎草素衍生倍半萜类化合物 (-)-Integrifolian-1,5-dione 的全合成

ChemistryEurope Pub Date : 2024-10-10 DOI: 10.1002/ceur.202400064

Anne Zimmer, Prof. Alois Fürstner

引用次数: 0

Steering Photoinduced Electron Transfer in Intramolecular Photocatalysts by Peripheral Ligand Control 通过外围配体控制引导分子内光催化剂中的光诱导电子转移

ChemistryEurope Pub Date : 2024-10-10 DOI: 10.1002/ceur.202300084

Benedikt Bagemihl, Prof. Carolin Müller, Dr. Georgina E. Shillito, Marco Hartkorn, Dr. Alexander K. Mengele, Dr. Stephan Kupfer, Prof. Benjamin Dietzek-Ivanšić, Prof. Sven Rau

{"title":"Steering Photoinduced Electron Transfer in Intramolecular Photocatalysts by Peripheral Ligand Control","authors":"Benedikt Bagemihl, Prof. Carolin Müller, Dr. Georgina E. Shillito, Marco Hartkorn, Dr. Alexander K. Mengele, Dr. Stephan Kupfer, Prof. Benjamin Dietzek-Ivanšić, Prof. Sven Rau","doi":"10.1002/ceur.202300084","DOIUrl":"https://doi.org/10.1002/ceur.202300084","url":null,"abstract":"Bridged photosensitizer-catalyst systems are promising models to study photocatalytic hydrogen evolution. However, the systems in the literature structurally diverse and therefore hard to compare. Many systems show highly complex photophysics including several accepting orbitals for the excited state, as a result catalytic activity is hard to predict. Here we present a bimetallic Ru−Pt photocatalyst bearing peripheral spectator ligands at the ruthenium(II) photocenter as a member of the Ru-tpphz-Pt family. Consequently, it features a single acceptor tpphz ligand and so-called unidirectional electron transfer, i. e., electron transfer without co-occurring transfer to peripheral ligands, from the excited state. Thus – and in contrast to recently used peripheral ligands – the new spectator ligands do not disrupt electron transfer towards the catalytic center. By comparison to known systems, this facilitates unprecedented insight into the importance of electron transfer from the bridge to the catalytic center moving towards more rational design of oligonuclear photocatalysts.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300084","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142664823","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Glucose-based Ionic Liquid Organocatalysts for Asymmetric aza-Diels-Alder Reactions 用于不对称偶氮-狄尔斯-阿尔德反应的葡萄糖基离子液体有机催化剂

ChemistryEurope Pub Date : 2024-10-10 DOI: 10.1002/ceur.202400052

Mirai Komabayashi, Dr. Stefan Jopp

引用次数: 0

Pd-Catalyzed Thiotritylation Cross-Coupling of Aryl Bromides and Iodides to Access Sulfur Functional Groups Pd 催化溴化芳基和碘化芳基的硫代三苯甲基化交叉偶联以获得硫官能团

ChemistryEurope Pub Date : 2024-10-10 DOI: 10.1002/ceur.202400053

Yue Liu, Dr. Takashi Okazoe, Dr. Tim Gatzenmeier, Prof. Dr. Kyoko Nozaki

{"title":"Pd-Catalyzed Thiotritylation Cross-Coupling of Aryl Bromides and Iodides to Access Sulfur Functional Groups","authors":"Yue Liu, Dr. Takashi Okazoe, Dr. Tim Gatzenmeier, Prof. Dr. Kyoko Nozaki","doi":"10.1002/ceur.202400053","DOIUrl":"https://doi.org/10.1002/ceur.202400053","url":null,"abstract":"Sulfur-containing functional groups (SFGs) are increasingly important for modern medicinal chemistry and their large structural diversity provides many opportunities for lead optimization. In an effort to simplify the access to the full set of SFGs, we report herein a versatile strategy utilizing (hetero)aryl trityl sulfides (ArSCPh3) as the common precursors. We developed a mild and high yielding Pd-catalyzed thiotritylation cross-coupling methodology to afford ArSCPh3 compounds from (hetero)aryl bromides and iodides. Efficient chemoselective derivatizations provided access to eight different SFGs and sulfur(VI) fluorine exchange (SuFEx) hubs, which open up further downstream derivatizations towards the full set of SFGs. Thereby obtainable sulfur motifs include aryl sulfur pentafluorides (ArSF5), aryl tetrafluoro-λ6-sulfanyl chlorides (ArSF4Cl), aryl sulfonimidoyl fluorides (ArS(O)(NR)F), aryl sulfonyl fluorides (ArSO2F), aryl sulfonic acids (ArSO3H), and aryl sulfinyl fluorides (ArSOF), which are all valuable functional groups in modern drug discovery.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202400053","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142664851","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A Water-Soluble Cycloparaphenylene: Supramolecular Receptor with Visible Fluorescence 水溶性环联苯：具有可见荧光的超分子受体

ChemistryEurope Pub Date : 2024-10-08 DOI: 10.1002/ceur.202400025

Ryo Morito, Takayuki Kataoka, Kunio Saito, Prof. Dr. Kohtaro Osakada, Dr. Tomohito Ide, Dr. Yoshitaka Tsuchido, Prof. Dr. Hidetoshi Kawai

引用次数: 0

Front Cover: What a Difference an Electron Makes: Structural Response of Saddle-Shaped Tetraphenylene to One and Two Electron Uptake (ChemistryEurope 5/2024) 封面电子带来的变化：马鞍形四亚苯基对一个和两个电子吸收的结构响应（欧洲化学 5/2024 期）

ChemistryEurope Pub Date : 2024-09-26 DOI: 10.1002/ceur.202480501

Dr. Yikun Zhu, Dr. Zheng Zhou, Dr. Zheng Wei, Dr. Alexandra Tsybizova, Prof. Dr. Renana Gershoni-Poranne, Prof. Dr. Marina A. Petrukhina

{"title":"Front Cover: What a Difference an Electron Makes: Structural Response of Saddle-Shaped Tetraphenylene to One and Two Electron Uptake (ChemistryEurope 5/2024)","authors":"Dr. Yikun Zhu, Dr. Zheng Zhou, Dr. Zheng Wei, Dr. Alexandra Tsybizova, Prof. Dr. Renana Gershoni-Poranne, Prof. Dr. Marina A. Petrukhina","doi":"10.1002/ceur.202480501","DOIUrl":"https://doi.org/10.1002/ceur.202480501","url":null,"abstract":"The Front Cover highlights the core transformation that occurs in a polycyclic aromatic hydrocarbon with a central eight-membered ring (tetrabenzocyclooctatetraene) upon chemical reduction. The dial at the bottom illustrates the controlled addition of charge to the system. In the charge states—neutral, anionic, and dianionic—the eight-membered ring core is highlighted in red, yellow, or green, respectively. These “stoplight” colors emphasize the experimental observations described in the paper, whereby going from the neutral to the monoanionic form results in only a small structural perturbation of the carbon framework, whereas the addition of the second electron triggers the formation of an energetically favorable “butterfly” dianion with a new C−C bond. Thus, the central eight-membered ring is transformed into two fused five-membered rings. More information can be found in the Research Article by R. Gershoni-Poranne, M. A. Petrukhina and co-workers (DOI: 10.1002/ceur.202400055).\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture>\u0000 </div>\u0000 </figure>\u0000 ","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202480501","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324722","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

What a Difference an Electron Makes: Structural Response of Saddle-Shaped Tetraphenylene to One and Two Electron Uptake 电子带来的变化：马鞍形四亚苯基对一个和两个电子吸收的结构响应

ChemistryEurope Pub Date : 2024-09-19 DOI: 10.1002/ceur.202400055

Dr. Yikun Zhu, Dr. Zheng Zhou, Dr. Zheng Wei, Dr. Alexandra Tsybizova, Prof. Dr. Renana Gershoni-Poranne, Prof. Dr. Marina A. Petrukhina

{"title":"What a Difference an Electron Makes: Structural Response of Saddle-Shaped Tetraphenylene to One and Two Electron Uptake","authors":"Dr. Yikun Zhu, Dr. Zheng Zhou, Dr. Zheng Wei, Dr. Alexandra Tsybizova, Prof. Dr. Renana Gershoni-Poranne, Prof. Dr. Marina A. Petrukhina","doi":"10.1002/ceur.202400055","DOIUrl":"https://doi.org/10.1002/ceur.202400055","url":null,"abstract":"Cyclooctatetraene (COT) and COT2− dianion are well-known as archetypical non-aromatic and aromatic systems, respectively. However, despite a wealth of studies the effect of one electron addition to the eight-membered ring remains equivocal. Herein, we report the first stepwise electron addition to tetrabenzo[a,c,e,g]cyclooctatetraene (TBCOT or tetraphenylene), accompanied by isolation and structural characterization of the mono- and doubly-reduced anions. The X-ray crystallographic study reveals only a small asymmetric distortion of the saddle-shaped core upon one electron uptake. In contrast, the doubly-reduced product exhibits a severely twisted conformation, with a new C−C bond separating the COT ring into two fused 5-membered rings. The reversibility of the two-fold reduction and bond rearrangement is demonstrated by NMR spectroscopy. In agreement with experimental results, computational analysis confirms that the reduction-induced core rearrangement requires the addition of the second electron.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202400055","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324418","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Regulate the Uniform Deposition of Lithium Through MgF2/Hydroxypropyl Modified Polyethylene Separator Applied to Lithium Metal Batteries 通过应用于锂金属电池的 MgF2/羟丙基改性聚乙烯隔膜调节锂的均匀沉积

ChemistryEurope Pub Date : 2024-08-30 DOI: 10.1002/ceur.202400035

Qilu Zhu, Zhuoying Su, Xinyu Li, Jiaqi Ding, Longkai Zhang, Xin Xiao, Ronghua Zeng, Prof. Junming Nan, Prof. Xiaoxi Zuo

{"title":"Regulate the Uniform Deposition of Lithium Through MgF2/Hydroxypropyl Modified Polyethylene Separator Applied to Lithium Metal Batteries","authors":"Qilu Zhu, Zhuoying Su, Xinyu Li, Jiaqi Ding, Longkai Zhang, Xin Xiao, Ronghua Zeng, Prof. Junming Nan, Prof. Xiaoxi Zuo","doi":"10.1002/ceur.202400035","DOIUrl":"https://doi.org/10.1002/ceur.202400035","url":null,"abstract":"The uneven growth of lithium dendrites not only compromise the performance of lithium metal batteries, but also has security risks. In this sutudy, double coating with MgF2 and hydroxypropyl methylcellulose was synthesized on the surface of polyethylene separator through a simple soaking and in-situ chemical precipitation method, achieve the purpose of protecting lithium metal anode. Utilizing the MgF2/HPMC@PE separator, the Li||Li symmetric cell was capable of cycling for over 1000 hours with a voltage hysteresis of only 11.4 mV, comparing the voltage hysteresis based on the cell use of PE separator increases rapidly after 200 h. Furthermore, the initial discharge capacity of Li||LiNi0.6Co0.2Mn0.2O2(NCM622) is 144.6 mAh g−1 and the capacity retention is 87.2 % after 200 cycles at 1 C, which is higher than that of the PE separator (135.3 mAh g−1, with retention of 74.9 %). All improvements can be credited with the formation of stable solid electrolyte interphase(SEI) film induced by HPMC/MgF2 double coating, which is reduced the Li nucleation overpotential and ultimately promoted uniform Li deposition. This study provides a simple and effective strategy for improving the cycling performance and safety of lithium metal batteries.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202400035","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324682","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Rh-Catalyzed Hydroamination of Allenes: Asymmetric N-Allylation of Amino Acids and Peptides Rh催化的烯烃氢化反应：氨基酸和肽的不对称 N-烯丙基化

ChemistryEurope Pub Date : 2024-08-20 DOI: 10.1002/ceur.202400037

Edward Damer, Prof. Dr. Bernhard Breit

引用次数: 0