Hybrid Catalysis Enabling Room-Temperature Hydrogen Gas Release from N-Heterocycles and Tetrahydronaphthalenes
Hybrid Catalysis Enabling Room-Temperature Hydrogen Gas Release from N-Heterocycles and Tetrahydronaphthalenes
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DOI：
10.1021/jacs.7b00253
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发表时间：
2017-02-15
影响因子：
15
通讯作者：
Kanai, Motomu
中科院分区：
文献类型：
--
作者：
Kato, Shota;Saga, Yutaka;Kanai, Motomu
开发了用于实现N-杂环和四氢萘-液态有机氢载体的模型基质-的无受体脱氢的混合催化剂系统。包含吖啶鎓光氧化还原催化剂和Pd金属催化剂的二元混合催化对于N-杂环的脱氢是有效的，而包含吖啶鎓光氧化还原催化剂、Pd金属催化剂和硫代磷酰亚胺有机催化剂的三元混合催化实现了四氢萘的脱氢。这些混合催化剂体系允许在温和条件下从六元N-杂环和四氢萘释放2摩尔当量的H-2气体，两种或三种不同催化剂类型的组合使用对于催化活性是必不可少的。
Hybrid catalyst systems to achieve acceptorless dehydrogenation of N-heterocycles and tetrahydronaphthalenes-model substrates for liquid organic hydrogen carriers-were developed. A binary hybrid catalysis comprising an acridinium phototedox catalyst and a Pd metal catalyst was effective for the dehydrogenation of N-heterocycles, whereas a ternary hybrid catalysis comprising an acridinium photoredox catalyst, a Pd metal catalyst, and a thiophosphoric imide organocatalyst achieved dehydrogenation of tetrahydronaphthalenes. These hybrid catalyst systems allowed for 2 molar equiv of H-2 gas release from six-membered N-heterocycles and tetrahydronaphthalenes under mild conditions, i.e., visible light irradiation at rt. The combined use of two or three different catalyst types was essential for the catalytic activity.