Develop New Reactions based on Heterocyclic C(sp3)–H Bond Activation

开发基于杂环C(sp3)的新反应

• 批准号: 18J20833
• 负责人: ZHANG DELIANG
• 金额: $ 1.41万
• 依托单位: Hokkaido University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for JSPS Fellows
• 财政年份: 2018
• 资助国家: 日本
• 起止时间: 2018-04-25 至 2021-03-31
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-18J20833/
• 关键词: heterogeneous catalyst; dehydrogenation; heterocycles; Iridium; Transfer hydrogenation; Heterogeneous catalyst; Dehydrogenation

The first project: In this research work, the polystyrene-cross-linking bisphosphine ligand PS-DPPBz was effective for the Ir-catalyzedreversible acceptorless dehydrogenation/hydrogenation of N-heterocycles. Notably, this protocol is applicable to the dehydrogenation of N-substituted indoline derivatives with various N-substituents with different electronic and steric natures. A reaction pathway involving oxidative addition of an N-adjacent C(sp3)-H bond to a bisphosphine-coordinated Ir(I) center is proposed for the dehydrogenation of N-substituted substrates. The second project: Design new material for hydrogen storage carriers.

第一个项目：在本研究工作中，聚苯乙烯-交联双膦配体PS-DPPBz对ir催化的n -杂环可逆无受体脱氢/加氢是有效的。值得注意的是，该方案适用于具有不同电子和空间性质的各种n取代基的n取代吲哚衍生物的脱氢。提出了一种反应途径，涉及将n相邻的C(sp3)-H键氧化加成到双膦配位的Ir(I)中心，用于n取代底物的脱氢。第二个项目：设计储氢载体新材料。

项目成果

Ir-Catalyzed Reversible Acceptorless Dehydrogenation/Hydrogenation of N-Substituted and Unsubstituted Heterocycles Enabled by a Polymer-Cross-Linking Bisphosphine

聚合物交联双膦实现 N-取代和未取代杂环的 Ir 催化可逆无受体脱氢/氢化

• DOI: 10.1021/acs.orglett.0c01905
• 发表时间: 2020
• 期刊: Organic Letters
• 影响因子: 5.2
• 作者: Zhang Deliang;Iwai Tomohiro;Sawamura Masaya
• 通讯作者: Sawamura Masaya

Acceptorless Dehydrogenation of N-Heterocycles with a Polystyrene-Cross-Linking Bisphosphine-Ir Catalyst

使用聚苯乙烯交联双膦-Ir 催化剂进行 N-杂环无受体脱氢

• 发表时间: 2019
• 作者: Zhang Deliang;Iwai Tomohiro;Sawamura Masaya;Deliang Zhang
• 通讯作者: Deliang Zhang

Iridium-Catalyzed Alkene-Selective Transfer Hydrogenation with 1,4-Dioxane as Hydrogen Donor

以 1,4-二恶烷为供氢体的铱催化烯烃选择性转移氢化

• DOI: 10.1021/acs.orglett.9b01989
• 发表时间: 2019
• 期刊: Organic Letters
• 影响因子: 5.2
• 作者: Zhang Deliang;Iwai Tomohiro;Sawamura Masaya
• 通讯作者: Sawamura Masaya

1,4-Dioxane-Enabled Chemoselective Transfer Hydrogenation of Alkenes with Iridium-Bisphosphine Catalysts

使用铱-双膦催化剂进行 1,4-二氧杂环己烷化学选择性转移氢化烯烃

• 发表时间: 2018
• 作者: Zhang Deliang;Iwai Tomohiro;Sawamura Masaya;Deliang Zhang;Deliang Zhang
• 通讯作者: Deliang Zhang