Adiabatic electrochemical electron-transfer reactions involving frequency changes of inner-sphere modes |
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| Institution: | 1. Abteilung Elektrochemie, Universität Ulm, D-89069 Ulm, Germany;2. Schuit Institute of Catalysis, Laboratory of Inorganic Chemistry and Catalysis, Eindhoven University of Technology, 5600 MB Eindhoven, Netherlands;1. School of Management Science and Engineering, Shandong University of Finance and Economics, Jinan 250014, China;2. PolyU Business School, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong;3. Department of Industrial and Systems Engineering, University of Tennessee, Knoxville, TN 37996, USA;1. Institute of Rehabilitation Engineering, Binzhou Medical University, Yantai 264003, China;2. Department of Physics, Binzhou Medical Ccollege, Yantai 264003, China;3. Ningbo Innoshines New Material Co., Ltd., Ningbo 315800, China;4. School of pharmacy (School of Enology), Binzhou Medical University, Yantai 264003, China;5. China Yantai Intellectual Property Protect Ctr, Yantai 264005, China;6. College of Chemical Engineering, Shijiazhuang University, Shijiazhuang 050035, China;7. College of Physics Science & Technology, Hebei University, Baoding 071002, China;8. College of Chemistry & Chemical Engineering, Yantai University, Yantai 264005, China;1. Key Laboratory of Rubber-Plastics of the Ministry of Education, School of Polymer Science & Engineering, Qingdao University of Science and Technology, 53-Zhengzhou Road, Qingdao, 266042, PR China;2. State Key Laboratory of Supramolecular Structure and Materials, Institute of Theoretical Chemistry, College of Chemistry, Jilin University, Changchun, 130012, PR China;3. School of Petrochemical Engineering, Shenyang University of Technology, 30 Guanghua Street, Liaoyang, 111003, PR China;1. Biological and Chemical Research Centre, Faculty of Chemistry, University of Warsaw, ul. Żwirki i Wigury 101, 02-089 Warsaw, Poland |
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| Abstract: | A Hamiltonian model is formulated for electrochemical electron-transfer reactions involving frequency changes of the inner-sphere modes. The adiabatic free energy surface is calculated and it is shown that this nonlinear coupling leads to a transfer coefficient different from 1/2, and that the transfer coefficient can no longer be identified with the electron occupation probability in the transition state saddle point, as in the linear coupling case. |
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