A new experimental method to distinguish two different mechanisms for a category of oscillators involving mass transfer |
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| Affiliation: | 1. Department of Chemistry, Hunan Normal University, Changsha 410081, China;2. State Key Laboratory for Physical Chemistry of Solid Surfaces and Department of Chemistry, Xiamen University, Xiamen 361005, China;3. Institute of Physical Chemistry and Department of Chemistry, Zhejiang Normal University, Jinhua 321004, China;1. School of Pharmacy, University of Camerino, via Sant’ Agostino 1, 62032 Camerino, Italy;2. Department of Pharmacognosy, Faculty of Pharmacy, Zagazig University, Zagazig 44519, Egypt;3. RICH – Research and Innovation Coffee Hub, Via E. Betti 1, 62020 Belforte del Chienti, MC, Italy;4. Faculty of Food Science and Technology, University of Vigo, Spain;1. Center for Quality and Productivity Improvement and Department of Industrial and Systems Engineering, University of Wisconsin–Madison, USA;2. Armstrong Institute for Patient Safety and Quality, Johns Hopkins University, USA;3. Oracle, USA;1. Clinical Immunology Service, Institute of Immunology and Immunotherapy, University of Birmingham, Birmingham, United Kingdom;2. Institute of Immunity and Transplantation, University College London, London, United Kingdom;3. Department of Immunology, Royal Free London NHS Foundation Trust, London, United Kingdom;4. Department of Clinical Immunology and Allergy, St James’s University Hospital, Leeds Teaching Hospitals NHS Trust, Leeds, United Kingdom;5. Department of Immunology, Lancashire Teaching Hospitals NHS Foundation Trust, Preston, United Kingdom;6. Department of Clinical Immunology, The Leeds Teaching Hospital NHS Foundation Trust, Leeds, United Kingdom;7. Newcastle University Translational and Clinical Research Institute, Newcastle, United Kingdom;8. NIHR Newcastle Biomedical Research Centre at Newcastle Hospitals NHS Foundation Trust, Newcastle, United Kingdom;9. Department of Rheumatology, Newcastle Upon Tyne Hospitals NHS Foundation Trust, Newcastle, United Kingdom;10. West Midlands Immunodeficiency Centre, University Hospitals Birmingham NHS Foundation Trust, Birmingham, United Kingdom;11. Walsall Healthcare NHS Trust, Walsall, United Kingdom;12. Department of Clinical Immunology, Nottingham University Hospitals NHS Foundation Trust, Nottingham, United Kingdom;13. North Bristol NHS Trust, Bristol, United Kingdom;14. Regional Immunology Service, Royal Victoria Hospital, Belfast, United Kingdom;15. Department of Immunology, Great Ormond Street Hospital for Children NHS Foundation Trust, London, United Kingdom;p. Developmental Immunology, Weatherall Institute of Molecular Medicine, University of Oxford, Oxford, United Kingdom;q. Department of Infection and Tropical Medicine, Newcastle Upon Tyne Hospitals NHS Foundation Trust, Newcastle, United Kingdom;r. Department of Immunology, Salford Royal NHS Foundation Trust, Manchester, United Kingdom;s. Faculty of Biology, Medicine and Health, University of Manchester, Manchester, United Kingdom;t. Department of Immunology, University Hospital North Midlands, Stoke, United Kingdom;u. Department of Immunology, Royal London Hospital, Barts Health NHS Trust, London, United Kingdom;v. Department of Immunology, Epsom and St Helier NHS Trust, Epsom, United Kingdom;w. Institute of Immunology and Immunotherapy, University of Birmingham, Birmingham, United Kingdom;x. Department of Clinical Immunology, Oxford University Hospitals NHS Foundation Trust, Oxford, United Kingdom;y. Immunodeficiency Centre for Wales, Cardiff, United Kingdom;z. Eden Unit, University Hospitals Plymouth NHS Foundation Trust, Plymouth, United Kingdom;11. Department of Immunology, University Hospitals Leicester NHS Trust, Leicester, United Kingdom;22. Department of Immunology, Sandwell and West Birmingham NHS Trust, Birmingham, United Kingdom;33. Department of Immunology, Frimley Health NHS Foundation Trust, Frimley, United Kingdom;44. NIHR Oxford Biomedical Research Centre, Oxford, United Kingdom;55. Clinical Immunology and Allergy Unit, Sheffield Teaching Hospitals NHS Foundation Trust, Sheffield, United Kingdom;66. Department of Immunology, Newcastle Upon Tyne Hospitals NHS Foundation Trust, Newcastle, United Kingdom;77. Department of Allergy and Clinical Immunology, University College London Hospitals NHS Foundation Trust, London, United Kingdom;1. Clinical Immunology Service, Institute of Immunology and Immunotherapy, University of Birmingham, Birmingham, United Kingdom;2. Institute of Immunity and Transplantation, University College London, London, United Kingdom;3. Department of Immunology, Royal Free London NHS Foundation Trust, London, United Kingdom;4. Department of Clinical Immunology and Allergy, St James’s University Hospital, Leeds Teaching Hospitals NHS Trust, Leeds, United Kingdom;1. State Key Laboratory of Biotherapy and Cancer Center/Collaborative Innovation Center for Biotherapy, West China Hospital, West China Medical School, Sichuan University, Chengdu, 610041, China;2. Key Laboratory of Drug Targeting and Drug Delivery System, Ministry of Education, West China School of Pharmacy, Sichuan University, Chengdu, Sichuan, 610041, China;3. Laboratory of Human Diseases and Immunotherapies, West China Hospital, Sichuan University, Chengdu, 610041, China;1. Department of Chemical Sciences, University of Naples Federico II, Via Cintia 4, I-80126 Naples, Italy;2. Department of Metabolism and Nutrition, ICTAN, CSIC, José Antonio Novais 10, 28040 Madrid, Spain;3. Department of Environmental Science and Policy, via Celoria 2, University of Milan, 20133 Milano, Italy |
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| Abstract: | We present new experimental evidence that further confirms that a combination of electrochemical reactions and diffusion–convection (ERDC) mass transfer accounts for the potential oscillations that appear under conditions of transport limited current. A typical example is given for the reduction of Fe(CN)63− in alkaline solution accompanying periodic hydrogen evolution. No potential oscillations occur by simply replacing the hydrogen evolution with IO3− reduction as the second current carrier. That replacement removes only the convection mass transfer induced by the hydrogen evolution, and retains the negative differential resistance (NDR) from the Frumkin repulsive effect. The key role of hydrogen evolution is thus to restore the Fe(CN)63− surface concentration after its depleting to zero by diffusion-limited reduction, rather than purely a second current carrier. Therefore, the other mechanism, which emphasizes the NDR from the Frumkin interaction due to electrostatic repulsion, is excluded because it does not have a direct connection with the oscillations. Moreover, a crossing cycle in cyclic voltammograms is a more convincible criterion for this category of electrochemical oscillators than the negative impedance. |
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