双语化学辞典Chem Lexicon
反应 · 有机化学 · 烯烃合成 Organic chemistry · Alkene synthesis

霍纳尔-沃兹沃思-埃蒙斯反应Horner–Wadsworth–Emmons reaction

拼音Pinyin huò nà ěr wò zī wò sī āi méng sī fǎn yìng 别名Also HWE 反应;霍纳尔-埃蒙斯反应;HWE olefination; Horner–Emmons reaction

定义Definition

HWE 反应是稳定化的膦酸酯碳负离子(如 (EtO)₂P(O)CH⁻CO₂Et)与醛或酮反应,高选择性地生成 E-α,β-不饱和酯(或酮、腈)的烯化反应,副产物为水溶性磷酸二烷基酯盐。

The HWE reaction olefinates aldehydes or ketones with stabilised phosphonate carbanions such as (EtO)₂P(O)CH⁻CO₂Et, giving mainly E-α,β-unsaturated esters (or ketones, nitriles); the dialkyl phosphate by-product is water-soluble.

与维蒂希反应比较Compared with the Wittig reaction

膦酸酯负离子比磷叶立德亲核性更强、碱性更弱,能与位阻酮反应;E-选择性高;副产物易用水洗去,无三苯基氧膦分离难题。膦酸酯可由阿尔布佐夫反应方便制备。

Phosphonate anions are more nucleophilic and less basic than phosphorus ylides, react with hindered ketones and give high E-selectivity; the by-product washes out with water, avoiding Ph₃PO. Phosphonates are easily made by the Arbuzov reaction.

变体Variants

施蒂尔–根纳里(Still–Gennari)改良用双(三氟乙基)膦酸酯和 KHMDS/18-冠-6,得到 Z-烯烃;安藤(Ando)试剂也给出 Z-选择性。马萨穆内–鲁什条件(LiCl/DBU)适合碱敏感底物。

The Still–Gennari modification (bis(trifluoroethyl) phosphonates, KHMDS/18-crown-6) and Ando’s reagents give Z-alkenes; Masamune–Roush conditions (LiCl/DBU) suit base-sensitive substrates.

由来Origin

霍纳于 1958 年报道膦氧化物变体,沃兹沃思与埃蒙斯于 1961 年系统发展了膦酸酯版本。

Horner reported the phosphine-oxide variant in 1958; Wadsworth and Emmons developed the phosphonate version in 1961.

反应Reactions

(EtO)2P(O)CH2CO2Et + RCHO NaH⟶ (E)-RCH=CHCO2Et + (EtO)2PO2−Na+

NaH 或 DBU/LiCl,THF,0 °C 至室温

NaH or DBU/LiCl in THF at 0 °C to room temperature

  1. 碱夺取膦酸酯 α-H 生成碳负离子。

    Base removes the α-H of the phosphonate.

  2. 加成到醛羰基形成 β-氧负离子中间体。

    Addition to the aldehyde gives a β-alkoxide.

  3. 经氧磷杂环丁烷消除磷酸酯盐得 E-烯烃。

    Elimination through an oxaphosphetane gives the E-alkene.

PhCHO + (EtO)2P(O)CH2CO2Et ⟶ (E)-肉桂酸乙酯PhCHO + (EtO)2P(O)CH2CO2Et ⟶ (E)-

高 E 选择性。

High E selectivity.

反应机理图Mechanism

红色弯箭头表示一对电子的移动方向:从电子来源(孤对电子或化学键)指向电子去向。Red curly arrows show where an electron pair moves: from its source (lone pair or bond) to its destination.

1

膦酸酯碳负离子进攻醛羰基

The phosphonate carbanion attacks the aldehyde

2

烷氧负离子进攻磷,经四元环中间体消除

The alkoxide attacks P; a four-membered intermediate then fragments

3

(E)-α,β-不饱和酯;磷酸盐副产物溶于水,易分离

(E)-α,β-Unsaturated ester; the phosphate by-product washes out with water

年表Timeline

  • 1958

    霍纳报道

    Horner’s report

  • 1961

    沃兹沃思与埃蒙斯发展膦酸酯烯化

    Wadsworth and Emmons develop phosphonate olefination

  • 1983

    施蒂尔–根纳里 Z-选择性改良

    Still–Gennari Z-selective modification