Tungstate catalysis: pressure-switched 2- and 6-electron reductive functionalization of CO2 with amines and phenylsilane,Green Chemistry

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Tungstate catalysis: pressure-switched 2- and 6-electron reductive functionalization of CO2 with amines and phenylsilane
Green Chemistry ( IF 9.3 ) Pub Date : 2018-02-21 00:00:00 , DOI: 10.1039/c7gc03416d
Mei-Yan Wang _{1,

2,

3,

4,

5} , Ning Wang _{1,

2,

3,

4,

5} , Xiao-Fang Liu _{1,

2,

3,

4,

5} , Chang Qiao _{1,

2,

3,

4,

5} , Liang-Nian He _{1,

2,

3,

4,

5}

Affiliation

An efficient and environmentally benign tungstate catalyst for reductive functionalization of CO₂ with amines and phenylsilane was developed. By simply varying the pressure, 2-electron or 6-electron reduction of CO₂ was successfully achieved with simultaneous C–N bond formation, thus leading to the formation of formamides and methylamines, respectively. That is, secondary and primary amines furnished the corresponding methylamines or dimethylamines in excellent yields under atmospheric pressure of CO₂, while various formamides were formed in yields ranging from 52% to 98% when increasing the CO₂ pressure to 2 MPa. ¹H NMR studies and control experiments demonstrate that N-formylation proceeds through the formation of silyl formate, while N-methylation proceeds through an aminal intermediate generated by 4-electron reduction of CO₂.

中文翻译：

钨酸盐催化：用胺和苯基硅烷对CO ₂进行压力转换的2和6电子还原功能化

开发了一种有效的，对环境无害的钨酸盐催化剂，用于用胺和苯基硅烷对CO ₂进行还原功能化。通过简单地改变的压力，CO 2电子或6-电子还原₂被成功地与同时C-N键的形成来实现，由此导致的甲酰胺和甲胺的形成，分别。即，仲胺和伯胺在CO _2的大气压下以优异的产率提供了相应的甲胺或二甲基胺，而当将CO ₂压力提高至2 MPa时，形成了各种甲酰胺，产率为52％至98％。¹ H NMR研究和对照实验表明，N-甲酰化通过甲硅烷基甲酸酯的形成而进行，而N-甲基化则通过通过4电子还原CO ₂生成的氨基中间体来进行。

更新日期：2018-04-03

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