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Poly(iminoborane)s with Aromatic Side Groups: Insights into the Microstructure from Monodisperse Model Oligomers 具有芳香族侧基的聚(亚氨基硼烷)：从单分散模型低聚物洞察微观结构

ChemistryEurope Pub Date : 2024-02-29 DOI: 10.1002/ceur.202400011

Matthias Maier, Dr. Alexandra Friedrich, Johannes S. Schneider, Dr. Jan A. P. Sprenger, Jonas Klopf, Dr. Lars Fritze, Prof. Dr. Maik Finze, Prof. Dr. Holger Helten

{"title":"Poly(iminoborane)s with Aromatic Side Groups: Insights into the Microstructure from Monodisperse Model Oligomers","authors":"Matthias Maier, Dr. Alexandra Friedrich, Johannes S. Schneider, Dr. Jan A. P. Sprenger, Jonas Klopf, Dr. Lars Fritze, Prof. Dr. Maik Finze, Prof. Dr. Holger Helten","doi":"10.1002/ceur.202400011","DOIUrl":"https://doi.org/10.1002/ceur.202400011","url":null,"abstract":"An oligo(iminoborane), depicted on the cover as the dinosaur, was synthesized as part of a series of monodisperse oligo(iminoborane)s with increasing number of B=N units in the chain. Herein, the number of backbone atoms could be extended to 7 boron and 8 nitrogen atoms. This oligomer represents the longest well-defined molecular [>B=N<]x chain reported so far. The structures of the oligomers were studied by X-ray diffractometry, also providing insight into the microstructure of poly(iminoborane)s (PIBs). In their Research Article, H. Helten and co-workers describe PIBs with increased aromatic content, including the PIB with the highest molecular weight known to date. The meteorite collision visualizes TGA measurements of the polymers which lead to the formation of boron nitride. The authors would like to thank Tina Schneider for creating the cover artwork.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture>\u0000 </div>\u0000 </figure>\u0000 ","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202400011","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140135469","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}

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Cover Feature: Nucleobase Stacking Sustained by Pt−Pt Interactions (ChemistryEurope 2/2024) 封面专题：铂-铂相互作用维持的核碱基堆叠（欧洲化学 2/2024 期）

ChemistryEurope Pub Date : 2024-02-29 DOI: 10.1002/ceur.202400010

Dr. Carmen Lorenzo-Aparicio, Prof. Dr. Pablo García-Álvarez, Prof. Dr. Javier A. Cabeza, Prof. Dr. Mar Gómez-Gallego, Prof. Dr. Miguel A. Sierra

引用次数: 0

Lemieux-Johnson oxidation with N,N-bidentate bisPYA ruthenium complexes: insights into reaction conditions and catalyst design 用 N,N-二叉双PYA 钌络合物进行莱米厄-约翰逊氧化反应：对反应条件和催化剂设计的见解

ChemistryEurope Pub Date : 2024-02-29 DOI: 10.1002/ceur.202300070

Dr. Kevin Salzmann, Dr. Candela Segarra, Dr. Aline Carrel, Prof. Dr. Martin Albrecht

{"title":"Lemieux-Johnson oxidation with N,N-bidentate bisPYA ruthenium complexes: insights into reaction conditions and catalyst design","authors":"Dr. Kevin Salzmann, Dr. Candela Segarra, Dr. Aline Carrel, Prof. Dr. Martin Albrecht","doi":"10.1002/ceur.202300070","DOIUrl":"https://doi.org/10.1002/ceur.202300070","url":null,"abstract":"The carbonyl group is arguably the most versatile functional group for synthetic purposes. Here, a series of N,N’-bis(pyridylideneamide) (bisPYA) complexes of ruthenium(II), [Ru(cym)(bisPYA)Cl]+ (cym=cymene), were synthesized and applied as catalysts for Lemieux-Johnson oxidation of alkenes to access carbonyl functionalities. Complexes bearing para- and ortho-bisPYA ligands induce higher activity and selectivity than their mesoionic meta-bisPYA analogues. The non-coordinating counterion of the cationic complexes affects the catalytic performance markedly, with PF6− enhancing the activity compared to trifluoromethanesulfonate, OTf−. Likewise, replacing the anionic ancillary chloride ligand by a neutral and more labile MeCN ligand led to increased activity. Electrochemical and solubility measurements revealed no direct correlation of ligand donor strength to catalytic performance. Variation of the solvent mixture and the ratio of its components provided access to high-performance catalysts. In H2O/MeCN/CH2Cl2 at 3 : 1:0.5 (v/v) ratio, turnover frequencies up to 10,000 h−1 were obtained for the Lemieux-Johnson oxidation of styrene with these Ru(bisPYA) complexes, allowing quantitative conversions within 30 min at 0.1 mol % catalyst loadings and corresponding to a 5 times faster reaction than the best catalyst known to date for this transformation.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300070","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140135471","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}

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A Photocatalytic Approach for the Synthesis of L-Shape Bicyclic NHC Ligands 合成 L 型双环 NHC 配体的光催化方法

ChemistryEurope Pub Date : 2024-02-13 DOI: 10.1002/ceur.202300083

Tanakorn Kittikool, Kunita Phakdeeyothin, Agustín Morales, Cécile Barthes, Dr. Laure Vendier, Prof. Sirilata Yotphan, Dr. Sébastien Bontemps, Stéphanie Bastin, Prof. Agustí Lledós, Dr. Olivier Baslé, Dr. Vincent César

{"title":"A Photocatalytic Approach for the Synthesis of L-Shape Bicyclic NHC Ligands","authors":"Tanakorn Kittikool, Kunita Phakdeeyothin, Agustín Morales, Cécile Barthes, Dr. Laure Vendier, Prof. Sirilata Yotphan, Dr. Sébastien Bontemps, Stéphanie Bastin, Prof. Agustí Lledós, Dr. Olivier Baslé, Dr. Vincent César","doi":"10.1002/ceur.202300083","DOIUrl":"https://doi.org/10.1002/ceur.202300083","url":null,"abstract":"L-shape N-Heterocyclic Carbenes (NHCs) based on the imidazo[1,5-a]pyridine (ImPy) scaffold have recently gained considerable interest as the true carbene ligand analogues of the popular dialkylbiarylphosphines, better known as Buchwald phosphines. Nevertheless, the substitution pattern of ImPy ligands is still rather limited due to synthetic access issues. We report herein an efficient and versatile visible light photocatalytic strategy to access L-shape bifunctional ImPy ligands laterally-functionalized by a phenol group. Mechanistic investigations supported by density functional theory (DFT) reveal that the excited state of the iridium photocatalyst undergoes either a reductive quenching (SET process) or an energy-transfer quenching (EnT process) depending on the nature of the counterion of the 5-bromoimidazo[1,5-a]pyridinium substrate salt. Moreover, the bifunctional character of these new family of L-shape ImPy ligands is demonstrated by the preparation of a gold(I) complex exhibiting a free OH function capable of intermolecular hydrogen bonding. This work highlights the advantage of visible light photocatalysis in the synthesis of advanced NHC ligand structures, a strategy that has not yet been considered despite its potential benefits in terms of versatility, diversity and practicability.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300083","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140135388","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

Poly(iminoborane)s with Aromatic Side Groups: Insights into the Microstructure from Monodisperse Model Oligomers 具有芳香族侧基的聚(亚氨基硼烷)：从单分散模型低聚物洞察微观结构

ChemistryEurope Pub Date : 2024-02-06 DOI: 10.1002/ceur.202300085

Matthias Maier, A. Friedrich, Johannes S Schneider, J. Sprenger, Jonas Klopf, Lars Fritze, Maik Finze, Holger Helten

{"title":"Poly(iminoborane)s with Aromatic Side Groups: Insights into the Microstructure from Monodisperse Model Oligomers","authors":"Matthias Maier, A. Friedrich, Johannes S Schneider, J. Sprenger, Jonas Klopf, Lars Fritze, Maik Finze, Holger Helten","doi":"10.1002/ceur.202300085","DOIUrl":"https://doi.org/10.1002/ceur.202300085","url":null,"abstract":"While certain inorganic main‐group polymers such as silicones (polysiloxanes) are ubiquitous in our everyday life, poly(iminoborane)s have been elusive for a long time. Incorporation of heterocyclic building blocks into their backbone has recently enabled access to the first derivatives of this inorganic‐polymer class, as this approach effectively prevents undesired side‐reactions to borazines. Information about the microstructure of these cyclolinear macromolecules, however, has been scarce. Herein, we present the synthesis of a series of monodisperse oligomers with up to 7 boron and 8 nitrogen atoms, representing the longest well‐defined molecular [>B=N<]x chain to date. We accomplished to characterize six of them structurally in the solid state by single‐crystal X‐ray diffraction, thus providing valuable insight into the microstructure of poly(iminoborane)s. In addition, we report on the synthesis of new poly(iminoborane) derivatives featuring aryl side groups, with an increased content of unsubstituted phenyl groups. The p‐(n‐butyl)phenyl‐substituted species 13 represents the highest‐molecular‐weight sample of this class of inorganic polymers to date.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"103 10","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139801425","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Poly(iminoborane)s with Aromatic Side Groups: Insights into the Microstructure from Monodisperse Model Oligomers 具有芳香族侧基的聚(亚氨基硼烷)：从单分散模型低聚物洞察微观结构

ChemistryEurope Pub Date : 2024-02-06 DOI: 10.1002/ceur.202300085

Matthias Maier, Dr. Alexandra Friedrich, Johannes S. Schneider, Dr. Jan A. P. Sprenger, Jonas Klopf, Dr. Lars Fritze, Prof. Dr. Maik Finze, Prof. Dr. Holger Helten

{"title":"Poly(iminoborane)s with Aromatic Side Groups: Insights into the Microstructure from Monodisperse Model Oligomers","authors":"Matthias Maier, Dr. Alexandra Friedrich, Johannes S. Schneider, Dr. Jan A. P. Sprenger, Jonas Klopf, Dr. Lars Fritze, Prof. Dr. Maik Finze, Prof. Dr. Holger Helten","doi":"10.1002/ceur.202300085","DOIUrl":"10.1002/ceur.202300085","url":null,"abstract":"While certain inorganic main-group polymers such as silicones (polysiloxanes) are ubiquitous in our everyday life, poly(iminoborane)s have been elusive for a long time. Incorporation of heterocyclic building blocks into their backbone has recently enabled access to the first derivatives of this inorganic-polymer class, as this approach effectively prevents undesired side-reactions to borazines. Information about the microstructure of these cyclolinear macromolecules, however, has been scarce. Herein, we present the synthesis of a series of monodisperse oligomers with up to 7 boron and 8 nitrogen atoms, representing the longest well-defined molecular [>B=N<]x chain to date. We accomplished to characterize six of them structurally in the solid state by single-crystal X-ray diffraction, thus providing valuable insight into the microstructure of poly(iminoborane)s. In addition, we report on the synthesis of new poly(iminoborane) derivatives featuring aryl side groups, with an increased content of unsubstituted phenyl groups. The p-(n-butyl)phenyl-substituted species 13 represents the highest-molecular-weight sample of this class of inorganic polymers to date.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300085","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139861108","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

Front Cover: Molecular Actuation of a Bistable Liquid-Crystalline [c2]Daisy Chain Rotaxane (ChemistryEurope 1/2024) 封面：双稳态液晶[c2]雏菊链旋烷的分子驱动（欧洲化学 1/2024）

ChemistryEurope Pub Date : 2024-01-28 DOI: 10.1002/ceur.202300090

Dr. Christian C. Carmona-Vargas, Dr. Lara Faour, Dr. Shoichi Tokunaga, Dr. Doru Constantin, Guillaume Fleith, Dr. Emilie Moulin, Prof. Dr. Nicolas Giuseppone

引用次数: 0

Cover Feature: Peroxo-Zr/Hf-Containing Wells-Dawson Polyoxometalates for H2O2-based Homogeneous, Heterogeneous, and Biphasic Oxidation Catalysis (ChemistryEurope 1/2024) 封面专题：用于基于 H2O2 的均相、异相和双相氧化催化的含过氧化 Zr/Hf 的 Wells-Dawson 聚氧化金属酸盐（欧洲化学 1/2024 期）

ChemistryEurope Pub Date : 2024-01-28 DOI: 10.1002/ceur.202300089

Dr. Anusree Sundar, Dr. Nataliya V. Maksimchuk, Dr. Irina D. Ivanchikova, Dr. Olga V. Zalomaeva, Dr. Danica Bajuk-Bogdanović, Prof. Oxana A. Kholdeeva, Prof. Gordana Ćirić-Marjanović, Dr. Bassem S. Bassil, Prof. Ulrich Kortz

{"title":"Cover Feature: Peroxo-Zr/Hf-Containing Wells-Dawson Polyoxometalates for H2O2-based Homogeneous, Heterogeneous, and Biphasic Oxidation Catalysis (ChemistryEurope 1/2024)","authors":"Dr. Anusree Sundar, Dr. Nataliya V. Maksimchuk, Dr. Irina D. Ivanchikova, Dr. Olga V. Zalomaeva, Dr. Danica Bajuk-Bogdanović, Prof. Oxana A. Kholdeeva, Prof. Gordana Ćirić-Marjanović, Dr. Bassem S. Bassil, Prof. Ulrich Kortz","doi":"10.1002/ceur.202300089","DOIUrl":"https://doi.org/10.1002/ceur.202300089","url":null,"abstract":"Peroxo-zirconium-/hafnium-containing polyoxometalates as 3-in-1 catalysts were prepared and studied for homogeneous, heterogeneous, and biphasic oxidation catalysis with H2O2 as oxidant. In their Research Article, U. Kortz and co-workers evaluate the catalysts in terms of activity and product selectivity and exhibited unique profiles. Most interestingly, the catalytic results proved to be highly relevant for applications in the chemical industry, possibly paving the way for green chemical processes. The authors would like to thank Mr. Adhiraj Sundar for creating the cover artwork.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture>\u0000 </div>\u0000 </figure>\u0000 ","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300089","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139655426","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

Cover Feature: Radical-Formation Management: Towards Aza-Analogues of the Benzothioxanthene Imide (ChemistryEurope 1/2024) 封面专题：自由基形成管理：迈向苯并噻吨酰亚胺的氮杂类似物（欧洲化学 1/2024）

ChemistryEurope Pub Date : 2024-01-28 DOI: 10.1002/ceur.202300091

Darío Puchán Sánchez, Dr. Pierre Josse, Dr. Monika G. Mutovska, Benjamin Siegler, Dr. Magali Allain, Korentin Morice, Dr. Philippe Blanchard, Prof. Frédéric Gohier, Prof. Tangui Le Bahers, Prof. Cyrille Monnereau, Prof. Yulian Zagranyarski, Prof. Dominik Lungerich, Prof. Dr. Clément Cabanetos

{"title":"Cover Feature: Radical-Formation Management: Towards Aza-Analogues of the Benzothioxanthene Imide (ChemistryEurope 1/2024)","authors":"Darío Puchán Sánchez, Dr. Pierre Josse, Dr. Monika G. Mutovska, Benjamin Siegler, Dr. Magali Allain, Korentin Morice, Dr. Philippe Blanchard, Prof. Frédéric Gohier, Prof. Tangui Le Bahers, Prof. Cyrille Monnereau, Prof. Yulian Zagranyarski, Prof. Dominik Lungerich, Prof. Dr. Clément Cabanetos","doi":"10.1002/ceur.202300091","DOIUrl":"https://doi.org/10.1002/ceur.202300091","url":null,"abstract":"Subtle chemical modifications of an intermediate can have significant impacts, since they usually considered to control the reactivity. In their Research Article, J. Zagranyarski, D. Lungerich, C. Cabanetos, and co-workers report the preparation of aza derivatives of the benzothixanthene imide. The intramolecular radical cyclization can be controlled by means of a simple methylation to either afford the thermodynamically favored six-membered or its kinetically favored five-membered ring regioisomers, exhibiting significant photophysical properties.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture>\u0000 </div>\u0000 </figure>\u0000 ","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300091","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139655266","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

Nucleobase Stacking Sustained by Pt−Pt Interactions 铂-铂相互作用维持的核碱基堆叠

ChemistryEurope Pub Date : 2024-01-11 DOI: 10.1002/ceur.202300065

Dr. Carmen Lorenzo-Aparicio, Prof. Dr. Pablo García-Álvarez, Prof. Dr. Javier A. Cabeza, Prof. Dr. Mar Gómez-Gallego, Prof. Dr. Miguel A. Sierra

{"title":"Nucleobase Stacking Sustained by Pt−Pt Interactions","authors":"Dr. Carmen Lorenzo-Aparicio, Prof. Dr. Pablo García-Álvarez, Prof. Dr. Javier A. Cabeza, Prof. Dr. Mar Gómez-Gallego, Prof. Dr. Miguel A. Sierra","doi":"10.1002/ceur.202300065","DOIUrl":"10.1002/ceur.202300065","url":null,"abstract":"This article reports the use of metal–metal interactions as a way to induce nucleobase stacking in a dinucleotide chain. We synthetized and study a series of C,N-cyclometallated platinum(II) binuclear complexes derived from 6-phenylpurine dinucleotide 1 as proligand, and β-diketonates, 2,2'-bipyridines and 1,10-phenanthroline as ancillary ligands. The X-ray diffraction analysis revealed that the diketonate derivatives 7 and 8 are chiral helixes sustained by Pt−Pt intramolecular interactions that allow the nucleobase stacking. The folded helical structures are maintained in solution, as demonstrated by the appearance of metal–metal-to-ligand charge-transfer (MMLCT) transitions in the UV-vis spectra. The influence of the ancillary ligand in the molecular structure was evidenced by the absence of bands derived from M−M interactions in the absorption spectra of 2,2’-bipyridine and and 1,10-phenanthroline derivatives 12–14. The existence of Pt−Pt in the complexes of this study can be also detected by electrochemistry.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300065","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139533328","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