• 文献检索
  • 文档翻译
  • 深度研究
  • 学术资讯
  • Suppr Zotero 插件Zotero 插件
  • 邀请有礼
  • 套餐&价格
  • 历史记录
应用&插件
Suppr Zotero 插件Zotero 插件浏览器插件Mac 客户端Windows 客户端微信小程序
定价
高级版会员购买积分包购买API积分包
服务
文献检索文档翻译深度研究API 文档MCP 服务
关于我们
关于 Suppr公司介绍联系我们用户协议隐私条款
关注我们

Suppr 超能文献

核心技术专利:CN118964589B侵权必究
粤ICP备2023148730 号-1Suppr @ 2026

文献检索

告别复杂PubMed语法,用中文像聊天一样搜索,搜遍4000万医学文献。AI智能推荐,让科研检索更轻松。

立即免费搜索

文件翻译

保留排版,准确专业,支持PDF/Word/PPT等文件格式,支持 12+语言互译。

免费翻译文档

深度研究

AI帮你快速写综述,25分钟生成高质量综述,智能提取关键信息,辅助科研写作。

立即免费体验

使用具有两个C(2)F(5)基团的新型双齿配体合成、结构及具有反亲顶键合模式的芳基磷烷的异构化

Synthesis, structure and isomerization of arylphosphoranes with anti-apicophilic bonding modes using a novel bidentate ligand with two C(2)F(5) groups.

作者信息

Jiang Xin-Dong, Matsukawa Shiro, Yamamoto Yohsuke

机构信息

Department of Chemistry, Graduate School of Science, Hiroshima University, 1-3-1 Kagamiyama, Higashi-Hiroshima, 739-8526, Japan.

出版信息

Dalton Trans. 2008 Jul 28(28):3678-87. doi: 10.1039/b802947d. Epub 2008 Jun 13.

DOI:10.1039/b802947d
PMID:18615213
Abstract

A series of anti-apicophilic pentacoordinate phosphoranes (with one chelating substituent in an O-equatorial, C-apical bonding mode at pentacoordinated phosphorus atom) bearing a para-substituted aryl group (-C(6)H(4)(p-X); X = H, CF(3), F, OMe) or a mesityl (2,4,6-trimethylphenyl) group were isolated using a novel bulky bidentate ligand with two C(2)F(5) groups. These phosphoranes were stable to isomerization at room temperature, and quantitatively converted into the corresponding more stable isomers (O-apical) at elevated temperatures in solution. On the basis of a kinetic study, the free energy of activation (DeltaG(double dagger)) of the stereomutation of the O-equatorial mesitylphosphorane to its O-apical isomer was higher than that of the CF(3) derivative by 2.6 kcal mol(-1), giving rise to a further example of the steric effect of the C(2)F(5) group to freeze the isomerization of the pentacoordinate phosphorus compounds. Kinetic measurements of the isomerization of the O-equatorial ortho-unsubstituted derivatives (-C(6)H(4)(p-X)) to the corresponding O-apical isomers suggested that the O-equatorial isomers were stabilized by the pi --> sigma*(P-O) interaction in the ground state.

摘要

使用一种带有两个五氟乙基基团的新型大位阻双齿配体,分离得到了一系列反亲顶五配位磷烷(在五配位磷原子上,一个螯合取代基以氧-赤道面、碳-顶点键合模式存在),其带有对取代芳基(-C(6)H(4)(p-X);X = H、CF(3)、F、OMe)或均三甲苯基(2,4,6-三甲基苯基)基团。这些磷烷在室温下对异构化稳定,并且在溶液中升高温度时定量转化为相应更稳定的异构体(氧-顶点)。基于动力学研究,氧-赤道面均三甲苯基磷烷向其氧-顶点异构体立体异构化的活化自由能(ΔG‡)比三氟甲基衍生物的高2.6 kcal mol(-1),这进一步例证了五氟乙基基团的空间效应可抑制五配位磷化合物的异构化。对氧-赤道面邻位未取代衍生物(-C(6)H(4)(p-X))向相应氧-顶点异构体异构化的动力学测量表明,氧-赤道面异构体在基态通过π→σ*(P-O)相互作用得以稳定。

相似文献

1
Synthesis, structure and isomerization of arylphosphoranes with anti-apicophilic bonding modes using a novel bidentate ligand with two C(2)F(5) groups.使用具有两个C(2)F(5)基团的新型双齿配体合成、结构及具有反亲顶键合模式的芳基磷烷的异构化
Dalton Trans. 2008 Jul 28(28):3678-87. doi: 10.1039/b802947d. Epub 2008 Jun 13.
2
Experimental determination of the nN --> sigma*P-O interaction energy of O-equatorial C-apical phosphoranes bearing a primary amino group.带有伯氨基的赤道面氧-顶端磷烷的nN→σ*P-O相互作用能的实验测定。
Inorg Chem. 2006 Sep 4;45(18):7269-77. doi: 10.1021/ic0609047.
3
Synthesis and application of a bidentate ligand based on decafluoro-3-phenyl-3-pentanol: steric effect of pentafluoroethyl groups on the stereomutation of O-equatorial C-apical spirophosphoranes.基于十氟-3-苯基-3-戊醇的双齿配体的合成与应用:五氟乙基对O-赤道面C-顶点螺磷烷立体异构化的空间效应
Chem Asian J. 2007 Feb 5;2(2):314-23. doi: 10.1002/asia.200600334.
4
Efficient synthesis of tetradecafluoro-4-phenylheptan-4-ol by a Cannizzaro-type reaction and application of the alcohol as a bulky Martin ligand variant for a new anti-apicophilic phosphorane.通过康尼扎罗型反应高效合成十四氟-4-苯基庚烷-4-醇,并将该醇用作新型反亲脂性膦叶立德的大位阻 Martin 配体变体。
Dalton Trans. 2010 Nov 7;39(41):9823-9. doi: 10.1039/c0dt00539h. Epub 2010 Sep 22.
5
Characteristic reactions and properties of C-apical O-equatorial (O-cis) spirophosphoranes: effect of the sigma(P)(-)(O) orbital in the equatorial plane and isolation of a hexacoordinate oxaphosphetane as an intermediate of the Wittig type reaction of 10-P-5 phosphoranes.C-顶端O-赤道面(O-顺式)螺磷烷的特征反应和性质:赤道面中σ(P)(-)(O)轨道的影响以及六配位氧杂磷环丁烷作为10-P-5磷烷Wittig型反应中间体的分离
J Am Chem Soc. 2002 Nov 6;124(44):13154-70. doi: 10.1021/ja026776c.
6
Intramolecular hydrogen bond-controlled prolyl amide isomerization in glucosyl 3'(S)-hydroxy-5'-hydroxymethylproline hybrids: influence of a C-5'-hydroxymethyl substituent on the thermodynamics and kinetics of prolyl amide cis/trans isomerization.葡萄糖基3'(S)-羟基-5'-羟甲基脯氨酸杂合物中分子内氢键控制的脯氨酰胺异构化:C-5'-羟甲基取代基对脯氨酰胺顺/反异构化热力学和动力学的影响
J Org Chem. 2009 May 15;74(10):3735-43. doi: 10.1021/jo9003458.
7
The first structural study on a cyclic tricoordinate phosphorochloridite and a pentacoordinate phosphorane based on 1,2,3,5-protected myo-inositol--a new conformation of 1,3,2-dioxaphosphorinane ring.基于1,2,3,5-保护的肌醇对环状三配位亚磷酰氯和五配位磷烷的首次结构研究——1,3,2-二氧磷杂环己烷环的一种新构象。
Carbohydr Res. 2007 Jul 2;342(9):1182-8. doi: 10.1016/j.carres.2007.02.031. Epub 2007 Mar 1.
8
Pseudorotation barriers of biological oxyphosphoranes: a challenge for simulations of ribozyme catalysis.生物氧膦烷的假旋转势垒:对核酶催化模拟的挑战。
Chemistry. 2005 Mar 18;11(7):2081-93. doi: 10.1002/chem.200400790.
9
Bulky N-substituted 1,3-benzazaphospholes: access via Pd-catalyzed C-N and C-P cross coupling, lithiation, and conversion to novel P=C-PtBu2 hybrid ligands.大分子N-取代的1,3-苯并氮杂磷环戊二烯:通过钯催化的C-N和C-P交叉偶联、锂化反应制备,并转化为新型P=C-PtBu2杂化配体。
Inorg Chem. 2008 Aug 4;47(15):6900-12. doi: 10.1021/ic800430f. Epub 2008 Jul 9.
10
Supramolecular structures in N-isonicotinoyl arylaldehydehydrazones: multiple hydrogen-bonding modes in series of geometric isomers.N-异烟酰芳醛腙中的超分子结构:一系列几何异构体中的多种氢键模式。
Acta Crystallogr B. 2007 Dec;63(Pt 6):879-95. doi: 10.1107/S0108768107036270. Epub 2007 Nov 9.

引用本文的文献

1
Chiral Hypervalent, Pentacoordinated Phosphoranes.手性高价五配位磷烷
Molecules. 2016 Nov 21;21(11):1573. doi: 10.3390/molecules21111573.