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Light-gated binding in double-motorized porphyrin cages 双动力卟啉笼的光门控结合
Natural sciences (Weinheim, Germany) Pub Date : 2021-08-09 DOI: 10.22541/au.162850019.93838101/v1
R. Nolte, Pieter J. Gilissen, N. Vanthuyne, B. Feringa, J. Elemans
{"title":"Light-gated binding in double-motorized porphyrin cages","authors":"R. Nolte, Pieter J. Gilissen, N. Vanthuyne, B. Feringa, J. Elemans","doi":"10.22541/au.162850019.93838101/v1","DOIUrl":"https://doi.org/10.22541/au.162850019.93838101/v1","url":null,"abstract":"Molecular motors change conformation under the influence of light and\u0000when attached to host molecules they may find applications as sensors\u0000and switchable catalysts. Here we present a porphyrin macrocyclic host\u0000functionalized with two motor appendages for future catalytic\u0000applications. The compound is formed as a mixture of six stereoisomers\u0000(three sets of enantiomers), which have been separated by (chiral)\u0000chromatography. 1H NMR and chiral spectroscopy revealed that in one set\u0000of diastereomers the two motors interact with the cavity of the host\u0000(bound-bound), whereas in a second set one interacts and the other one\u0000does not (bound-loose). In the third set both motors do not interact\u0000with the host compound (loose-loose). The motorized hosts bind guest\u0000molecules in the order: (loose-loose) > (bound-loose)\u0000> (bound-bound). They can be switched with light to\u0000pseudo-identical diastereomers, leading to orthogonal behavior in the\u0000light-gated binding of guest molecules. Whereas the photo-isomerization\u0000of the diastereomer set loose-loose significantly lowers the binding\u0000affinity for viologen guests, the opposite is true for the diastereomer\u0000set bound-bound, i.e. the binding affinity increases. For the\u0000diastereomer set bound-loose no influence on guest binding is observed\u0000as the effect of photoisomerization on the motors is cancelled out.","PeriodicalId":74244,"journal":{"name":"Natural sciences (Weinheim, Germany)","volume":"99 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-08-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"76983416","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
Decision letter for "Liberating photoinhibition through nongenetic drainage of electrons from photosynthesis" “通过光合作用中电子的非遗传排水来释放光抑制”的决定书
Natural sciences (Weinheim, Germany) Pub Date : 2021-08-05 DOI: 10.1002/ntls.20210038/v2/decision1
Wangyin Wang, Dingyi Li, Xupeng Cao, Song Xue, Can Li
{"title":"Decision letter for \"Liberating photoinhibition through nongenetic drainage of electrons from photosynthesis\"","authors":"Wangyin Wang, Dingyi Li, Xupeng Cao, Song Xue, Can Li","doi":"10.1002/ntls.20210038/v2/decision1","DOIUrl":"https://doi.org/10.1002/ntls.20210038/v2/decision1","url":null,"abstract":"","PeriodicalId":74244,"journal":{"name":"Natural sciences (Weinheim, Germany)","volume":"130 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"80261590","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: 7
One Hundred Years of Alfred Landé’s g-Factor 阿尔弗雷德·兰德的g因子百年
Natural sciences (Weinheim, Germany) Pub Date : 2021-08-02 DOI: 10.22541/au.162792174.46183015/v1
Bretislav Friedrich, G. Meijer, H. Schmidt-Böcking, G. Gruber
{"title":"One Hundred Years of Alfred Landé’s g-Factor","authors":"Bretislav Friedrich, G. Meijer, H. Schmidt-Böcking, G. Gruber","doi":"10.22541/au.162792174.46183015/v1","DOIUrl":"https://doi.org/10.22541/au.162792174.46183015/v1","url":null,"abstract":"Prompted by the centenary of Alfred Landé’s g-factor, we reconstruct\u0000Landé’s path to his discovery of half-integer angular momentum quantum\u0000numbers and of vector coupling of atomic angular momenta - both\u0000encapsulated in the g-factor - as well as point to reverberations of\u0000Landé’s breakthroughs in the work of other pioneers of quantum physics.","PeriodicalId":74244,"journal":{"name":"Natural sciences (Weinheim, Germany)","volume":"137 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"86397337","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: 2
Guest‐selective gate‐opening by pore engineering of two‐dimensional Kagomè lattice porous coordination polymers 通过二维Kagomè点阵多孔配位聚合物的孔工程进行客选门打开
Natural sciences (Weinheim, Germany) Pub Date : 2021-07-15 DOI: 10.1002/NTLS.10020
Mickaele Bonneau, K. Sugimoto, Ken‐ichi Otake, Y. Tsuji, N. Shimanaka, Christophe Lavenn, S. Kitagawa
{"title":"Guest‐selective gate‐opening by pore engineering of two‐dimensional Kagomè lattice porous coordination polymers","authors":"Mickaele Bonneau, K. Sugimoto, Ken‐ichi Otake, Y. Tsuji, N. Shimanaka, Christophe Lavenn, S. Kitagawa","doi":"10.1002/NTLS.10020","DOIUrl":"https://doi.org/10.1002/NTLS.10020","url":null,"abstract":"","PeriodicalId":74244,"journal":{"name":"Natural sciences (Weinheim, Germany)","volume":"10 1 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"83405832","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: 2
The Interface is a Tunable Dimension in Electricity-Driven Organic Synthesis 在电驱动有机合成中，界面是一个可调的维度
Natural sciences (Weinheim, Germany) Pub Date : 2021-07-07 DOI: 10.22541/AU.162569010.07717143/V1
Anna Wuttig, F. Toste
{"title":"The Interface is a Tunable Dimension in Electricity-Driven Organic Synthesis","authors":"Anna Wuttig, F. Toste","doi":"10.22541/AU.162569010.07717143/V1","DOIUrl":"https://doi.org/10.22541/AU.162569010.07717143/V1","url":null,"abstract":"Predictive control over the selectivity outcome of an organic synthetic\u0000method is an essential hallmark of reaction success. Electricity-driven\u0000synthesis offers a reemerging approach to facilitate the design of\u0000reaction sequences towards increased molecular complexity. In addition\u0000to the desirable sustainability features of electroorganic processes,\u0000the inherent interfacial nature of electrochemical systems present\u0000unique opportunities to tune reaction selectivity. To illustrate this\u0000feature, we outline examples of mechanism-guided interfacial control\u0000over CO2 electroreduction selectivity, a well-studied and instructive\u0000electrochemical process with multiple reduction products that are\u0000thermodynamically accessible. These studies reveal how controlled proton\u0000delivery to the electrode surface and substrate electroadsorption with\u0000the electrode dictate reaction selectivity. We describe and compare\u0000simple, yet salient, examples from the electroorganic literature, where\u0000we postulate that similar effects predominate the observed reactivity.\u0000This perspective highlights how the interface serves as a tunable\u0000dimension in electrochemical processes, delineating unique tools to\u0000study, manipulate, and achieve reaction selectivity in\u0000electricity-driven organic synthesis.","PeriodicalId":74244,"journal":{"name":"Natural sciences (Weinheim, Germany)","volume":"71 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"91201355","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: 2
Decision letter for "Asymmetric hydrogenation of γ ‐branched allylamines for the efficient synthesis of γ ‐chirogenic amines" “γ -支化烯丙胺的不对称氢化以高效合成γ -致氮胺”的决议书
Natural sciences (Weinheim, Germany) Pub Date : 2021-06-14 DOI: 10.1002/ntls.10021/v1/decision1
Jian Zhang, Tiantian Chen, Yuanhao Wang, F. Zhou, Zhenfeng Zhang, I. Gridnev, Wanbin Zhang
{"title":"Decision letter for \"Asymmetric hydrogenation of γ ‐branched allylamines for the efficient synthesis of γ ‐chirogenic amines\"","authors":"Jian Zhang, Tiantian Chen, Yuanhao Wang, F. Zhou, Zhenfeng Zhang, I. Gridnev, Wanbin Zhang","doi":"10.1002/ntls.10021/v1/decision1","DOIUrl":"https://doi.org/10.1002/ntls.10021/v1/decision1","url":null,"abstract":"The efficient construction of γ-chirogenic amines has been realized via\u0000asymmetric hydrogenation of γ-branched N-phthaloyl allylamines by using\u0000a bisphosphine-Rh catalyst bearing a large bite angle. The desired\u0000products possessing different types of γ-substituents were obtained in\u0000quantitative yields and with excellent enantioselectivities (up to\u0000>99.9% ee). This protocol provided a practical method for\u0000the preparation of γ-chirogenic amine derivatives such as the famous\u0000antidepressant drug Fluoxetine (up to 50000 S/C). The mechanism\u0000calculation shows a weak interaction-promoted activation mode which is\u0000completely different from the traditional coordination-promoted\u0000activation mode in the Rh-catalyzed hydrogenation.","PeriodicalId":74244,"journal":{"name":"Natural sciences (Weinheim, Germany)","volume":"52 9 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"91120270","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: 5
Decision letter for "Commentary: Chemical dynamics from the gas‐phase to surfaces" “评论:从气相到表面的化学动力学”的决定书
Natural sciences (Weinheim, Germany) Pub Date : 2021-06-01 DOI: 10.1002/NTLS.10007
D. Herschbach
{"title":"Decision letter for \"Commentary: Chemical dynamics from the gas‐phase to surfaces\"","authors":"D. Herschbach","doi":"10.1002/NTLS.10007","DOIUrl":"https://doi.org/10.1002/NTLS.10007","url":null,"abstract":"","PeriodicalId":74244,"journal":{"name":"Natural sciences (Weinheim, Germany)","volume":"1 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"82348418","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
Commentary: Chemical dynamics from the gas‐phase to surfaces 注释:从气相到表面的化学动力学
Natural sciences (Weinheim, Germany) Pub Date : 2021-06-01 DOI: 10.1002/NTLS.10006
G. Ertl
{"title":"Commentary: Chemical dynamics from the gas‐phase to surfaces","authors":"G. Ertl","doi":"10.1002/NTLS.10006","DOIUrl":"https://doi.org/10.1002/NTLS.10006","url":null,"abstract":"A trio of outstanding physical chemists, Daniel Auerbach, John Tully, andAlecWodtke, has produced a superb reviewof the field of chemical dynamics.1 They stress “linkages between gas phase and surface chemical dynamics . . . a fruitful interplay of theory and experiment . . . which may often seem impenetrably complex and challenging.” Their review offers a sparkling table of contents with 48 entries, along with references to congenial articles and books, totaling 493 items. They worked withmultifaceted exuberance, intrepid questing, and zestful spirit. Back in 1955, molecular beam study of chemical dynamics was “a lunatic fringe.” However, a precious gem by Simplicius of Cilicia (490– 560) dating to even earlier times provided its vivid anticipation2:","PeriodicalId":74244,"journal":{"name":"Natural sciences (Weinheim, Germany)","volume":"26 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"74764342","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: 1
Decision letter for "A breakthrough from 60 years ago: “General nature of the genetic code for proteins” (1961)" 60年前的重大突破:“蛋白质遗传密码的一般性质”(1961年)
Natural sciences (Weinheim, Germany) Pub Date : 2021-06-01 DOI: 10.1002/NTLS.10018
Matthew Cobb
{"title":"Decision letter for \"A breakthrough from 60 years ago: “General nature of the genetic code for proteins” (1961)\"","authors":"Matthew Cobb","doi":"10.1002/NTLS.10018","DOIUrl":"https://doi.org/10.1002/NTLS.10018","url":null,"abstract":"","PeriodicalId":74244,"journal":{"name":"Natural sciences (Weinheim, Germany)","volume":"124 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"80366417","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
Disclosed: quasiparticle properties and dynamics in real and momentum space 公开:实空间和动量空间中的准粒子性质和动力学
Natural sciences (Weinheim, Germany) Pub Date : 2021-05-17 DOI: 10.1002/NTLS.10017
U. Wurstbauer
{"title":"Disclosed: quasiparticle properties and dynamics in real and momentum space","authors":"U. Wurstbauer","doi":"10.1002/NTLS.10017","DOIUrl":"https://doi.org/10.1002/NTLS.10017","url":null,"abstract":"Disclosed: quasiparticle properties and dynamics in real and momentum spaceUrsula Wurstbauer","PeriodicalId":74244,"journal":{"name":"Natural sciences (Weinheim, Germany)","volume":"114 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"79008459","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: 1
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