Specific Enhancement of Catalytic Activity by a Dicopper Core: Selective Hydroxylation of Benzene to Phenol with Hydrogen Peroxide,Angewandte Chemie International Edition

当前位置： X-MOL 学术 › Angew. Chem. Int. Ed. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Specific Enhancement of Catalytic Activity by a Dicopper Core: Selective Hydroxylation of Benzene to Phenol with Hydrogen Peroxide
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2017-05-31 , DOI: 10.1002/anie.201702291
Tomokazu Tsuji ₁ , Antonius Andre Zaoputra ₁ , Yutaka Hitomi ₁ , Kaoru Mieda ₂ , Takashi Ogura ₂ , Yoshihito Shiota ₃ , Kazunari Yoshizawa ₃ , Hiroyasu Sato ₄ , Masahito Kodera ₁

Affiliation

A dicopper(II) complex, stabilized by the bis(tpa) ligand 1,2‐bis[2‐[bis(2‐pyridylmethyl)aminomethyl]‐6‐pyridyl]ethane (6‐hpa), [Cu₂(μ‐OH)(6‐hpa)]³⁺, was synthesized and structurally characterized. This complex catalyzed selective hydroxylation of benzene to phenol using H₂O₂, thus attaining large turnover numbers (TONs) and high H₂O₂ efficiency. The TON after 40 hours for the phenol production exceeded 12000 in MeCN at 50 °C under N₂, the highest value reported for benzene hydroxylation with H₂O₂ catalyzed by homogeneous complexes. At 22 % benzene conversion, phenol (95.2 %) and p‐benzoquinone (4.8 %) were produced. The mechanism of H₂O₂ activation and benzene hydroxylation is proposed.

中文翻译：

Dicopper核的催化活性的特定增强：过氧化氢将苯选择性地羟基化为苯酚

一种双铜（II）络合物，由双（tpa）配体1,2-双[2- [双（2-吡啶基甲基）氨基甲基] -6-吡啶基]乙烷（6-hpa）稳定，[Cu ₂（μ- OH）（6-hpa）] ³⁺，并进行结构表征。该络合物使用H ₂ O ₂催化苯选择性羟基化为苯酚，从而获得较大的周转数（TONs）和高H ₂ O ₂效率。在50℃，N ₂下的MeCN中，苯酚生产40小时后的TON超过12000 ，这是均相络合物催化H ₂ O ₂苯羟基化的最高值。苯转化率为22％时，苯酚（95.2％）和p产生了苯醌（4.8％）。提出了H ₂ O ₂活化和苯羟基化的机理。

更新日期：2017-05-31

点击分享查看原文

点击收藏

公开下载

阅读更多本刊新发论文本刊介绍/投稿指南