Strujni elektrohemijski oscilator
Current electrochemical oscillator
2016
Аутори
Potkonjak, Nebojša I.Остала ауторства
Minić, Dragica M.Anić, Slobodan
Stanisavljev, Dragomir
Vukelić, Nikola
Nikolić, Zoran M.
Докторска теза
Метаподаци
Приказ свих података о документуАпстракт
Ova doktorska disertacija se bavi potenciodinamičkim ispitivanjem ponašanja struje pri anodnoj polarizaciji bakarne elektrode, u prisistvu 1M CF3COOH (trifluorosirćetna kiselina). Poseban naglasak je dat na ispitivanje strujnih oscilacija koje se generišu u odreĎenoj oblasti potencijala (oscilatorna oblast, oblast OsS). Pojava strujnih oscilacija ukazuje da se elektrohemijski sistem Cu|1M CF3COOH moţe okarakterisati kao strujni elektrohemijski oscilator. Uočena oscilatorna oblast na struja-potencijal polarizacionim krivama se nalazi izmeĎu dve oblasti stabilnih stacionarnih stanja, naime izmeĎu oblasti aktivnog rastvaranja bakarne elektrode (oblast SSS1) i oblasti njene pasivacije (oblast SSS2).Primenom ciklične voltametrije ustanovljeno je da se strujne oscilacije javljaju pri oba smera polarizacije, anodnom i katodnom smeru. Prelaz SSS1OsS karakteriše zanemarljivo mali histerezis (5 mV), dok je širina histerezisa na prelazu OsSSSS2 značajno veća (34 mV). Bifurkaciona analiza je pok...azala da se prelaz SSS1OsS odvija preko superkritične Hopfove bifurkacije, dok je prelaz OsSSSS2 okarakterisan homokliničnom bifurkacijom.Tafelova analiza je pokazala da se anodno rastvaranje bakarne elektrode odvija preko mehanizma jednoelektronskog prenosa naelektrisanja. Rendgeno-difrakcionom analizom ustanovljeno je da oksidi bakra (CuO i Cu2O) ne ulaze u sastav pasivnog sloja. Difrakciona refleksija na 2 = 7,95, koja nije mogla biti indeksirana, ulazuje da se u sastavu pasivnog sloja nalazi faza velike elementarne ćelije, najverovatnije so koju čine Cu(I) i/ili Cu(II) trifluoroacetat. Dobijena mikro-porozna struktura površine bakarne elektrode koja je bila izloţena potencijalima unutar oscilatorne oblasti je detektovana primenom mikroskopije atomskih sila, što ukazuje na tačkastu (piting) koroziju.Na osnovu ispitivanja uticaja temperature elektrolitičke ćelije na oscilatorno ponašanje struje, naĎeno je da se unutar temperaturskog intervala 5 – 52 C strujne oscilacije javljaju na polarizacionim krivama; strujne oscilacije nisu bile opaţene kadaje temperatura elektrolitičke ćelije iznosila 55 C...
This doctoral dissertation deals with potentiodynamic examination of current response during the anodic polarization of copper electrode in the presence of 1M CF3COOH (trifluoroacetic acid). Particular focus is given on investigation of the current oscillations that are generated in certain potential region (oscillatory region, region OsS). Appearance of the current oscillations indicates that the electrochemical system Cu|1M CF3COOH can be classified as a current electrochemical oscillator. The observed oscillatory region at the current-potential polarization curve is situated between two regions of stable steady states, namely between the region of active dissolution of copper electrode (region SSS1) and the region of its passivation (region SSS2).It was determined that the current oscillations occur in anodic and cathodic direction of polarization, by applying of cyclic voltammetry. The transition SSS1OsS is characterized by negligible hysteresis (5 mV), while the width of hysteres...is at the transition OsSSSS2 is significantly higher (34 mV). Bifurcation analysis showed that the transition SSS1OsS goes via supercritical Hopf bifurcation, while the transition OsSSSS2 is characterize by homoclinic bifurcation.The Tafel analysis showed that the anodic dissolution of copper electrode immersed in 1M CF3COOH goes via one-electron charge transfer step. X-ray diffraction analysis showed absence of copper oxides (Cu2O and CuO) in passive layer. Diffraction reflections at 2 = 7.95, which could not be indexed, indicates presence of phase with large unit cell in passive layer, most probably salt composed of Cu(I) or/and Cu(II) trifluoroacetate. Obtained micro-porous structure of the copper electrode surface, which was exposed to potentials within oscillatory region was detected by using atomic force microscopy, this indicates a pitting corrosion.Based on the investigation of the temperature effect on current oscillatory behavior, it was found that within temperature interval ranged from 5 °C to 52 °C,current oscillations occur on polarization curves...
Кључне речи:
bakar / copper / trifluorosirćetna kiselina / anodno rastvaranje / elektrokorozija / pasivacija / strujne oscilacije / elektrohemijski oscilator / prividna energija aktivacije / omski pad potencijala / strujno-prekidna metoda / trifluoroacetic acid / anodic dissolution / electrocorrosion / passivation / current oscillations / electrochemical oscillator / apparent energy of activation / ohmic potential drop / current interrupt methodИзвор:
Универзитет у Београду, 2016Издавач:
- Универзитет у Београду, Факултет за физичку хемију
Финансирање / пројекти:
- Динамика нелинеарних физичкохемијских и биохемијских система са моделирањем и предвиђањем њихових понашања под неравнотежним условима (RS-MESTD-Basic Research (BR or ON)-172015)
URI
http://eteze.bg.ac.rs/application/showtheses?thesesId=3886https://fedorabg.bg.ac.rs/fedora/get/o:13049/bdef:Content/download
http://vbs.rs/scripts/cobiss?command=DISPLAY&base=70036&RID=47780879
http://nardus.mpn.gov.rs/123456789/6761
https://vinar.vin.bg.ac.rs/handle/123456789/7308
Колекције
Институција/група
VinčaTY - THES AU - Potkonjak, Nebojša I. PY - 2016 UR - http://eteze.bg.ac.rs/application/showtheses?thesesId=3886 UR - https://fedorabg.bg.ac.rs/fedora/get/o:13049/bdef:Content/download UR - http://vbs.rs/scripts/cobiss?command=DISPLAY&base=70036&RID=47780879 UR - http://nardus.mpn.gov.rs/123456789/6761 UR - https://vinar.vin.bg.ac.rs/handle/123456789/7308 AB - Ova doktorska disertacija se bavi potenciodinamičkim ispitivanjem ponašanja struje pri anodnoj polarizaciji bakarne elektrode, u prisistvu 1M CF3COOH (trifluorosirćetna kiselina). Poseban naglasak je dat na ispitivanje strujnih oscilacija koje se generišu u odreĎenoj oblasti potencijala (oscilatorna oblast, oblast OsS). Pojava strujnih oscilacija ukazuje da se elektrohemijski sistem Cu|1M CF3COOH moţe okarakterisati kao strujni elektrohemijski oscilator. Uočena oscilatorna oblast na struja-potencijal polarizacionim krivama se nalazi izmeĎu dve oblasti stabilnih stacionarnih stanja, naime izmeĎu oblasti aktivnog rastvaranja bakarne elektrode (oblast SSS1) i oblasti njene pasivacije (oblast SSS2).Primenom ciklične voltametrije ustanovljeno je da se strujne oscilacije javljaju pri oba smera polarizacije, anodnom i katodnom smeru. Prelaz SSS1OsS karakteriše zanemarljivo mali histerezis (5 mV), dok je širina histerezisa na prelazu OsSSSS2 značajno veća (34 mV). Bifurkaciona analiza je pokazala da se prelaz SSS1OsS odvija preko superkritične Hopfove bifurkacije, dok je prelaz OsSSSS2 okarakterisan homokliničnom bifurkacijom.Tafelova analiza je pokazala da se anodno rastvaranje bakarne elektrode odvija preko mehanizma jednoelektronskog prenosa naelektrisanja. Rendgeno-difrakcionom analizom ustanovljeno je da oksidi bakra (CuO i Cu2O) ne ulaze u sastav pasivnog sloja. Difrakciona refleksija na 2 = 7,95, koja nije mogla biti indeksirana, ulazuje da se u sastavu pasivnog sloja nalazi faza velike elementarne ćelije, najverovatnije so koju čine Cu(I) i/ili Cu(II) trifluoroacetat. Dobijena mikro-porozna struktura površine bakarne elektrode koja je bila izloţena potencijalima unutar oscilatorne oblasti je detektovana primenom mikroskopije atomskih sila, što ukazuje na tačkastu (piting) koroziju.Na osnovu ispitivanja uticaja temperature elektrolitičke ćelije na oscilatorno ponašanje struje, naĎeno je da se unutar temperaturskog intervala 5 – 52 C strujne oscilacije javljaju na polarizacionim krivama; strujne oscilacije nisu bile opaţene kadaje temperatura elektrolitičke ćelije iznosila 55 C... AB - This doctoral dissertation deals with potentiodynamic examination of current response during the anodic polarization of copper electrode in the presence of 1M CF3COOH (trifluoroacetic acid). Particular focus is given on investigation of the current oscillations that are generated in certain potential region (oscillatory region, region OsS). Appearance of the current oscillations indicates that the electrochemical system Cu|1M CF3COOH can be classified as a current electrochemical oscillator. The observed oscillatory region at the current-potential polarization curve is situated between two regions of stable steady states, namely between the region of active dissolution of copper electrode (region SSS1) and the region of its passivation (region SSS2).It was determined that the current oscillations occur in anodic and cathodic direction of polarization, by applying of cyclic voltammetry. The transition SSS1OsS is characterized by negligible hysteresis (5 mV), while the width of hysteresis at the transition OsSSSS2 is significantly higher (34 mV). Bifurcation analysis showed that the transition SSS1OsS goes via supercritical Hopf bifurcation, while the transition OsSSSS2 is characterize by homoclinic bifurcation.The Tafel analysis showed that the anodic dissolution of copper electrode immersed in 1M CF3COOH goes via one-electron charge transfer step. X-ray diffraction analysis showed absence of copper oxides (Cu2O and CuO) in passive layer. Diffraction reflections at 2 = 7.95, which could not be indexed, indicates presence of phase with large unit cell in passive layer, most probably salt composed of Cu(I) or/and Cu(II) trifluoroacetate. Obtained micro-porous structure of the copper electrode surface, which was exposed to potentials within oscillatory region was detected by using atomic force microscopy, this indicates a pitting corrosion.Based on the investigation of the temperature effect on current oscillatory behavior, it was found that within temperature interval ranged from 5 °C to 52 °C,current oscillations occur on polarization curves... PB - Универзитет у Београду, Факултет за физичку хемију T2 - Универзитет у Београду T1 - Strujni elektrohemijski oscilator T1 - Current electrochemical oscillator UR - https://hdl.handle.net/21.15107/rcub_nardus_6761 ER -
@phdthesis{ author = "Potkonjak, Nebojša I.", year = "2016", abstract = "Ova doktorska disertacija se bavi potenciodinamičkim ispitivanjem ponašanja struje pri anodnoj polarizaciji bakarne elektrode, u prisistvu 1M CF3COOH (trifluorosirćetna kiselina). Poseban naglasak je dat na ispitivanje strujnih oscilacija koje se generišu u odreĎenoj oblasti potencijala (oscilatorna oblast, oblast OsS). Pojava strujnih oscilacija ukazuje da se elektrohemijski sistem Cu|1M CF3COOH moţe okarakterisati kao strujni elektrohemijski oscilator. Uočena oscilatorna oblast na struja-potencijal polarizacionim krivama se nalazi izmeĎu dve oblasti stabilnih stacionarnih stanja, naime izmeĎu oblasti aktivnog rastvaranja bakarne elektrode (oblast SSS1) i oblasti njene pasivacije (oblast SSS2).Primenom ciklične voltametrije ustanovljeno je da se strujne oscilacije javljaju pri oba smera polarizacije, anodnom i katodnom smeru. Prelaz SSS1OsS karakteriše zanemarljivo mali histerezis (5 mV), dok je širina histerezisa na prelazu OsSSSS2 značajno veća (34 mV). Bifurkaciona analiza je pokazala da se prelaz SSS1OsS odvija preko superkritične Hopfove bifurkacije, dok je prelaz OsSSSS2 okarakterisan homokliničnom bifurkacijom.Tafelova analiza je pokazala da se anodno rastvaranje bakarne elektrode odvija preko mehanizma jednoelektronskog prenosa naelektrisanja. Rendgeno-difrakcionom analizom ustanovljeno je da oksidi bakra (CuO i Cu2O) ne ulaze u sastav pasivnog sloja. Difrakciona refleksija na 2 = 7,95, koja nije mogla biti indeksirana, ulazuje da se u sastavu pasivnog sloja nalazi faza velike elementarne ćelije, najverovatnije so koju čine Cu(I) i/ili Cu(II) trifluoroacetat. Dobijena mikro-porozna struktura površine bakarne elektrode koja je bila izloţena potencijalima unutar oscilatorne oblasti je detektovana primenom mikroskopije atomskih sila, što ukazuje na tačkastu (piting) koroziju.Na osnovu ispitivanja uticaja temperature elektrolitičke ćelije na oscilatorno ponašanje struje, naĎeno je da se unutar temperaturskog intervala 5 – 52 C strujne oscilacije javljaju na polarizacionim krivama; strujne oscilacije nisu bile opaţene kadaje temperatura elektrolitičke ćelije iznosila 55 C..., This doctoral dissertation deals with potentiodynamic examination of current response during the anodic polarization of copper electrode in the presence of 1M CF3COOH (trifluoroacetic acid). Particular focus is given on investigation of the current oscillations that are generated in certain potential region (oscillatory region, region OsS). Appearance of the current oscillations indicates that the electrochemical system Cu|1M CF3COOH can be classified as a current electrochemical oscillator. The observed oscillatory region at the current-potential polarization curve is situated between two regions of stable steady states, namely between the region of active dissolution of copper electrode (region SSS1) and the region of its passivation (region SSS2).It was determined that the current oscillations occur in anodic and cathodic direction of polarization, by applying of cyclic voltammetry. The transition SSS1OsS is characterized by negligible hysteresis (5 mV), while the width of hysteresis at the transition OsSSSS2 is significantly higher (34 mV). Bifurcation analysis showed that the transition SSS1OsS goes via supercritical Hopf bifurcation, while the transition OsSSSS2 is characterize by homoclinic bifurcation.The Tafel analysis showed that the anodic dissolution of copper electrode immersed in 1M CF3COOH goes via one-electron charge transfer step. X-ray diffraction analysis showed absence of copper oxides (Cu2O and CuO) in passive layer. Diffraction reflections at 2 = 7.95, which could not be indexed, indicates presence of phase with large unit cell in passive layer, most probably salt composed of Cu(I) or/and Cu(II) trifluoroacetate. Obtained micro-porous structure of the copper electrode surface, which was exposed to potentials within oscillatory region was detected by using atomic force microscopy, this indicates a pitting corrosion.Based on the investigation of the temperature effect on current oscillatory behavior, it was found that within temperature interval ranged from 5 °C to 52 °C,current oscillations occur on polarization curves...", publisher = "Универзитет у Београду, Факултет за физичку хемију", journal = "Универзитет у Београду", title = "Strujni elektrohemijski oscilator, Current electrochemical oscillator", url = "https://hdl.handle.net/21.15107/rcub_nardus_6761" }
Potkonjak, N. I.. (2016). Strujni elektrohemijski oscilator. in Универзитет у Београду Универзитет у Београду, Факултет за физичку хемију.. https://hdl.handle.net/21.15107/rcub_nardus_6761
Potkonjak NI. Strujni elektrohemijski oscilator. in Универзитет у Београду. 2016;. https://hdl.handle.net/21.15107/rcub_nardus_6761 .
Potkonjak, Nebojša I., "Strujni elektrohemijski oscilator" in Универзитет у Београду (2016), https://hdl.handle.net/21.15107/rcub_nardus_6761 .
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