A cobalt redox switch driving alcohol dehydrogenation by redox coupled molecular swing |
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| Affiliation: | 1. CAS Key Laboratory of Design and Assembly of Functional Nanostructures, and Fujian Provincial Key Laboratory of Nanomaterials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Xiamen 361021, China;2. Xiamen Institute of Rare Earth Materials, Haixi Institute, Chinese Academy of Sciences, Xiamen 361021, China;3. Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou 350108, China;1. College of Chemistry and Environmental Science, Chemical Biology Key Laboratory of Hebei Province, Key Laboratory of Medicinal Chemistry and Molecular Diagnosis of the Ministry of Education, Hebei University, Baoding 071002, China;2. CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology of China, Beijing 100190, China;3. Department of Chemistry, The University of Manchester, Manchester M13 9PL, United Kingdom;1. Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou 215123, China;2. Macao Institute of Materials Science and Engineering, Macau University of Science and Technology, Taipa 999078, Macau SAR, China;1. Department of Biomaterials, Higher Educational Key Laboratory for Biomedical Engineering of Fujian Province, Research Center of Biomedical Engineering of Xiamen, College of Materials, Xiamen University, Xiamen 361005, China;2. Zhejiang Provincial Key Laboratory of Silkworm Bioreactor and Biomedicine, College of Life Science and Medicine, Zhejiang Sci-Tech University, Hangzhou 310018, China;3. School of Pharmaceutical Sciences, Xiamen University, Xiamen 361102, China;4. State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;1. School of Biomedical Engineering, Sun Yat-sen University, Shenzhen 518107, China;2. Department of Cardiology, The Affiliated TCM Hospital of Guangzhou Medical University, Guangzhou 510120, China;3. Bioscience and Biomedical Engineering Thrust, The Hong Kong University of Science and Technology (Guangzhou), Guangzhou 511400, China;4. Division of Life Science, Hong Kong University of Science and Technology, Hong Kong 999077, China |
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| Abstract: | 
Developing redox switches that not only perform specific mechanical movements but also drive important chemical reactions is important but a great challenge. Herein, we report a redox pair of cobalt species (CoIII/CoII) that switches through photo-dehydrogenation of alcohol and hydrogenation of azo-ligand. The cobalt species is equipped with a flexible azo-ligand containing two bulky planar substituents. A planar oxidated sate (CoIII species) can be photo-reduced to a saddle-like reduced state (CoII) with alcohol molecules as electron donors, and in turn the CoIII species can be recovered with azo-ligand as oxidant under acidic surrounding. Both the redox states of the pair are isolated and characterized by single crystal X-ray diffraction. In the switching cycle, alcohol is oxidized to aldehyde by azo-ligand through proton coupled electron transfer and the cobalt complex acts as a redox catalyst. These results provide important insights into alcohol dehydrogenation catalyzed by redox complexes. |
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