Single entity electrochemistry and the electron transfer kinetics of hydrazine oxidation
The mechanism and kinetics of the electro-catalytic oxidation of hydrazine by graphene oxide platelets randomly decorated with palladium nanoparticles are deduced using single particle impact electrochemical measurements in buffered aqueous solutions across the pH range 2–11. Both hydrazine, N2H4, a...
| Main Authors: | , , |
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| 格式: | Journal article |
| 語言: | English |
| 出版: |
Springer
2021
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| _version_ | 1826300124112879616 |
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| author | Miao, R Shao, L Compton, R |
| author_facet | Miao, R Shao, L Compton, R |
| author_sort | Miao, R |
| collection | OXFORD |
| description | The mechanism and kinetics of the electro-catalytic oxidation of hydrazine by graphene oxide platelets randomly decorated with palladium nanoparticles are deduced using single particle impact electrochemical measurements in buffered aqueous solutions across the pH range 2–11. Both hydrazine, N2H4, and protonated hydrazine N2H5+ are shown to be electroactive following Butler-Volmer kinetics, of which the relative contribution is strongly pH-dependent. The negligible interconversion between N2H4 and N2H5+ due to the sufficiently short timescale of the impact voltammetry, allows the analysis of the two electron transfer rates from impact signals thus reflecting the composition of the bulk solution at the pH in question. In this way the rate determining step in the oxidation of each specie is deduced to be a one electron step in which no protons are released and so likely corresponds to the initial formation of a very short-lived radical cation either in solution or adsorbed on the platelet. Overall the work establishes a generic method for the elucidation of the rate determining electron transfer in a multistep process free from any complexity imposed by preceding or following chemical reactions which occur on the timescale of conventional voltammetry. |
| first_indexed | 2024-03-07T05:12:23Z |
| format | Journal article |
| id | oxford-uuid:dbfef64f-2d99-4a61-9f9b-f1ac9624d93e |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-07T05:12:23Z |
| publishDate | 2021 |
| publisher | Springer |
| record_format | dspace |
| spelling | oxford-uuid:dbfef64f-2d99-4a61-9f9b-f1ac9624d93e2022-03-27T09:14:44ZSingle entity electrochemistry and the electron transfer kinetics of hydrazine oxidationJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:dbfef64f-2d99-4a61-9f9b-f1ac9624d93eEnglishSymplectic ElementsSpringer2021Miao, RShao, LCompton, RThe mechanism and kinetics of the electro-catalytic oxidation of hydrazine by graphene oxide platelets randomly decorated with palladium nanoparticles are deduced using single particle impact electrochemical measurements in buffered aqueous solutions across the pH range 2–11. Both hydrazine, N2H4, and protonated hydrazine N2H5+ are shown to be electroactive following Butler-Volmer kinetics, of which the relative contribution is strongly pH-dependent. The negligible interconversion between N2H4 and N2H5+ due to the sufficiently short timescale of the impact voltammetry, allows the analysis of the two electron transfer rates from impact signals thus reflecting the composition of the bulk solution at the pH in question. In this way the rate determining step in the oxidation of each specie is deduced to be a one electron step in which no protons are released and so likely corresponds to the initial formation of a very short-lived radical cation either in solution or adsorbed on the platelet. Overall the work establishes a generic method for the elucidation of the rate determining electron transfer in a multistep process free from any complexity imposed by preceding or following chemical reactions which occur on the timescale of conventional voltammetry. |
| spellingShingle | Miao, R Shao, L Compton, R Single entity electrochemistry and the electron transfer kinetics of hydrazine oxidation |
| title | Single entity electrochemistry and the electron transfer kinetics of hydrazine oxidation |
| title_full | Single entity electrochemistry and the electron transfer kinetics of hydrazine oxidation |
| title_fullStr | Single entity electrochemistry and the electron transfer kinetics of hydrazine oxidation |
| title_full_unstemmed | Single entity electrochemistry and the electron transfer kinetics of hydrazine oxidation |
| title_short | Single entity electrochemistry and the electron transfer kinetics of hydrazine oxidation |
| title_sort | single entity electrochemistry and the electron transfer kinetics of hydrazine oxidation |
| work_keys_str_mv | AT miaor singleentityelectrochemistryandtheelectrontransferkineticsofhydrazineoxidation AT shaol singleentityelectrochemistryandtheelectrontransferkineticsofhydrazineoxidation AT comptonr singleentityelectrochemistryandtheelectrontransferkineticsofhydrazineoxidation |