Electrochemical oxidation of methanol on Pt/(RuxSn1-x)O2 nanocatalyst
Elektrohemijska oksidacija metanola na katalizatoru Pt/(RuxSn1-x)O2
Аутори
Krstajić, MilaObradović, Maja
Babić, Biljana M.
Radmilović, Velimir R.
Lačnjevac, Uroš
Krstajić, Nedeljko V.
Gojković, Snežana Lj.
Чланак у часопису (Објављена верзија)
Метаподаци
Приказ свих података о документуАпстракт
Ru-doped SnO2 powder, (RuxSn1-x)O2, with a Sn:Ru atomic ratio of 9:1 was synthesized and used as a support for Pt nanoparticles (30 mass % loading). The (RuxSn1-x)O2 support and the Pt/(RuxSn1-x)O2 catalyst were characterized by X-ray diffraction measurements, energy dispersive X-ray spectroscopy and transmission electron microscopy (TEM). The (RuxSn1-x)O2 was found to be a two-phase material consisting of probably a solid solution of RuO2 in SnO2 and pure RuO2. The average Pt particle size determined by TEM was 5.3 nm. Cyclic voltammetry of Pt/(RuxSn1-x)O2 indicated good conductivity of the support and displayed the usual features of Pt. The results of the electrochemical oxidation of COads and methanol on Pt/(RuxSn1-x)O2 were compared with those on commercial Pt/C and PtRu/C catalysts. Oxidation of COads on Pt/(RuxSn1-x)O2 starts at lower positive potentials than on PtRu/C and Pt/C. Potentiodynamic polarization curves and chronoamperometric curves of methanol oxidation indicated high...er initial activity of the Pt/(RuxSn1-x)O2 catalyst compared to PtRu/C, but also a greater loss in current density over time. A potentiodynamic stability test of the catalysts revealed that deactivation of Pt/(RuxSn1-x)O2 and Pt/C was primarily caused by poisoning of the Pt surface by residues of methanol oxidation, which mostly occurred during the first potential cycle. In the case of PtRu/C, the poisoning of the surface was minor and deactivation was caused by surface area loss of the PtRu.
Sintetizovan je prah SnO2 dopovan rutenijumom, (RuxSn1-x)O2, sa atomskim odnosom Sn:Ru od 9:1, i korišćen kao nosač nanočestica platine. Udeo Pt u dobijenom katalizatoru, Pt/(RuxSn1-x)O2, bio je 30 mas. %. Nosač i katalizator su karakterisani difrakcijom X-zraka, energetski disperzivnom spektroskopijom X-zraka i transmisionom elektronskom mikroskopijom (TEM). Pokazano je da je (RuxSn1-x)O2 dvofazni materijal koji verovatno sadrži čvrst rastvor RuO2 u SnO2 i čist RuO2. Prosečna veličina zrna Pt, određena TEM analizom, iznosi 5,3 nm. Ciklična voltametrija Pt/(RuxSn1-x)O2 ukazala je na dobru provodnost nosača katalizatora i na uobičajene karakteristike Pt. Upoređeni su rezultati elektrohemijske oksidacije COads na Pt/(RuxSn1-x)O2, Pt/C i PtRu/C. Oksidacija COads na Pt/(RuxSn1-x)O2 počinje na negativnijim potencijalima u odnosu na PtRu/C i Pt/C. Potenciodinamičke polarizacione krive i hronoamperometrijske krive za oksidaciju metanola ukazuju na veću početnu aktivnost katalizatora Pt/(RuxSn...1-x)O2 u odnosu na PtRu/C, ali i na veće smanjenje gustine struje tokom vremena. Test potenciodinamičke stabilnosti katalizatora je ukazao da je smanjenje aktivnosti Pt/(RuxSn1-x)O2 i Pt/C prvenstveno prouzrokovano trovanjem površine Pt proizvodima nepotpune oksidacije metanola, koje se uglavnom odigrava tokom prvog ciklusa. Kod PtRu/C trovanje površine je minimalno, a smanjenje aktivnosti je prouzrokovano smanjenjem elektrohemijski aktivne površine PtRu.
Кључне речи:
methanol oxidation / CO oxidation / platinum / Ru-doped SnO2 / electrocatalysis / fuel cellИзвор:
Journal of the Serbian Chemical Society, 2013, 78, 11, 1703-1716Издавач:
- Serbian Chemical Society, Belgrade
Финансирање / пројекти:
Институција/група
Tehnološko-metalurški fakultetTY - JOUR AU - Krstajić, Mila AU - Obradović, Maja AU - Babić, Biljana M. AU - Radmilović, Velimir R. AU - Lačnjevac, Uroš AU - Krstajić, Nedeljko V. AU - Gojković, Snežana Lj. PY - 2013 UR - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/2353 AB - Ru-doped SnO2 powder, (RuxSn1-x)O2, with a Sn:Ru atomic ratio of 9:1 was synthesized and used as a support for Pt nanoparticles (30 mass % loading). The (RuxSn1-x)O2 support and the Pt/(RuxSn1-x)O2 catalyst were characterized by X-ray diffraction measurements, energy dispersive X-ray spectroscopy and transmission electron microscopy (TEM). The (RuxSn1-x)O2 was found to be a two-phase material consisting of probably a solid solution of RuO2 in SnO2 and pure RuO2. The average Pt particle size determined by TEM was 5.3 nm. Cyclic voltammetry of Pt/(RuxSn1-x)O2 indicated good conductivity of the support and displayed the usual features of Pt. The results of the electrochemical oxidation of COads and methanol on Pt/(RuxSn1-x)O2 were compared with those on commercial Pt/C and PtRu/C catalysts. Oxidation of COads on Pt/(RuxSn1-x)O2 starts at lower positive potentials than on PtRu/C and Pt/C. Potentiodynamic polarization curves and chronoamperometric curves of methanol oxidation indicated higher initial activity of the Pt/(RuxSn1-x)O2 catalyst compared to PtRu/C, but also a greater loss in current density over time. A potentiodynamic stability test of the catalysts revealed that deactivation of Pt/(RuxSn1-x)O2 and Pt/C was primarily caused by poisoning of the Pt surface by residues of methanol oxidation, which mostly occurred during the first potential cycle. In the case of PtRu/C, the poisoning of the surface was minor and deactivation was caused by surface area loss of the PtRu. AB - Sintetizovan je prah SnO2 dopovan rutenijumom, (RuxSn1-x)O2, sa atomskim odnosom Sn:Ru od 9:1, i korišćen kao nosač nanočestica platine. Udeo Pt u dobijenom katalizatoru, Pt/(RuxSn1-x)O2, bio je 30 mas. %. Nosač i katalizator su karakterisani difrakcijom X-zraka, energetski disperzivnom spektroskopijom X-zraka i transmisionom elektronskom mikroskopijom (TEM). Pokazano je da je (RuxSn1-x)O2 dvofazni materijal koji verovatno sadrži čvrst rastvor RuO2 u SnO2 i čist RuO2. Prosečna veličina zrna Pt, određena TEM analizom, iznosi 5,3 nm. Ciklična voltametrija Pt/(RuxSn1-x)O2 ukazala je na dobru provodnost nosača katalizatora i na uobičajene karakteristike Pt. Upoređeni su rezultati elektrohemijske oksidacije COads na Pt/(RuxSn1-x)O2, Pt/C i PtRu/C. Oksidacija COads na Pt/(RuxSn1-x)O2 počinje na negativnijim potencijalima u odnosu na PtRu/C i Pt/C. Potenciodinamičke polarizacione krive i hronoamperometrijske krive za oksidaciju metanola ukazuju na veću početnu aktivnost katalizatora Pt/(RuxSn1-x)O2 u odnosu na PtRu/C, ali i na veće smanjenje gustine struje tokom vremena. Test potenciodinamičke stabilnosti katalizatora je ukazao da je smanjenje aktivnosti Pt/(RuxSn1-x)O2 i Pt/C prvenstveno prouzrokovano trovanjem površine Pt proizvodima nepotpune oksidacije metanola, koje se uglavnom odigrava tokom prvog ciklusa. Kod PtRu/C trovanje površine je minimalno, a smanjenje aktivnosti je prouzrokovano smanjenjem elektrohemijski aktivne površine PtRu. PB - Serbian Chemical Society, Belgrade T2 - Journal of the Serbian Chemical Society T1 - Electrochemical oxidation of methanol on Pt/(RuxSn1-x)O2 nanocatalyst T1 - Elektrohemijska oksidacija metanola na katalizatoru Pt/(RuxSn1-x)O2 EP - 1716 IS - 11 SP - 1703 VL - 78 UR - https://hdl.handle.net/21.15107/rcub_technorep_2353 ER -
@article{ author = "Krstajić, Mila and Obradović, Maja and Babić, Biljana M. and Radmilović, Velimir R. and Lačnjevac, Uroš and Krstajić, Nedeljko V. and Gojković, Snežana Lj.", year = "2013", abstract = "Ru-doped SnO2 powder, (RuxSn1-x)O2, with a Sn:Ru atomic ratio of 9:1 was synthesized and used as a support for Pt nanoparticles (30 mass % loading). The (RuxSn1-x)O2 support and the Pt/(RuxSn1-x)O2 catalyst were characterized by X-ray diffraction measurements, energy dispersive X-ray spectroscopy and transmission electron microscopy (TEM). The (RuxSn1-x)O2 was found to be a two-phase material consisting of probably a solid solution of RuO2 in SnO2 and pure RuO2. The average Pt particle size determined by TEM was 5.3 nm. Cyclic voltammetry of Pt/(RuxSn1-x)O2 indicated good conductivity of the support and displayed the usual features of Pt. The results of the electrochemical oxidation of COads and methanol on Pt/(RuxSn1-x)O2 were compared with those on commercial Pt/C and PtRu/C catalysts. Oxidation of COads on Pt/(RuxSn1-x)O2 starts at lower positive potentials than on PtRu/C and Pt/C. Potentiodynamic polarization curves and chronoamperometric curves of methanol oxidation indicated higher initial activity of the Pt/(RuxSn1-x)O2 catalyst compared to PtRu/C, but also a greater loss in current density over time. A potentiodynamic stability test of the catalysts revealed that deactivation of Pt/(RuxSn1-x)O2 and Pt/C was primarily caused by poisoning of the Pt surface by residues of methanol oxidation, which mostly occurred during the first potential cycle. In the case of PtRu/C, the poisoning of the surface was minor and deactivation was caused by surface area loss of the PtRu., Sintetizovan je prah SnO2 dopovan rutenijumom, (RuxSn1-x)O2, sa atomskim odnosom Sn:Ru od 9:1, i korišćen kao nosač nanočestica platine. Udeo Pt u dobijenom katalizatoru, Pt/(RuxSn1-x)O2, bio je 30 mas. %. Nosač i katalizator su karakterisani difrakcijom X-zraka, energetski disperzivnom spektroskopijom X-zraka i transmisionom elektronskom mikroskopijom (TEM). Pokazano je da je (RuxSn1-x)O2 dvofazni materijal koji verovatno sadrži čvrst rastvor RuO2 u SnO2 i čist RuO2. Prosečna veličina zrna Pt, određena TEM analizom, iznosi 5,3 nm. Ciklična voltametrija Pt/(RuxSn1-x)O2 ukazala je na dobru provodnost nosača katalizatora i na uobičajene karakteristike Pt. Upoređeni su rezultati elektrohemijske oksidacije COads na Pt/(RuxSn1-x)O2, Pt/C i PtRu/C. Oksidacija COads na Pt/(RuxSn1-x)O2 počinje na negativnijim potencijalima u odnosu na PtRu/C i Pt/C. Potenciodinamičke polarizacione krive i hronoamperometrijske krive za oksidaciju metanola ukazuju na veću početnu aktivnost katalizatora Pt/(RuxSn1-x)O2 u odnosu na PtRu/C, ali i na veće smanjenje gustine struje tokom vremena. Test potenciodinamičke stabilnosti katalizatora je ukazao da je smanjenje aktivnosti Pt/(RuxSn1-x)O2 i Pt/C prvenstveno prouzrokovano trovanjem površine Pt proizvodima nepotpune oksidacije metanola, koje se uglavnom odigrava tokom prvog ciklusa. Kod PtRu/C trovanje površine je minimalno, a smanjenje aktivnosti je prouzrokovano smanjenjem elektrohemijski aktivne površine PtRu.", publisher = "Serbian Chemical Society, Belgrade", journal = "Journal of the Serbian Chemical Society", title = "Electrochemical oxidation of methanol on Pt/(RuxSn1-x)O2 nanocatalyst, Elektrohemijska oksidacija metanola na katalizatoru Pt/(RuxSn1-x)O2", pages = "1716-1703", number = "11", volume = "78", url = "https://hdl.handle.net/21.15107/rcub_technorep_2353" }
Krstajić, M., Obradović, M., Babić, B. M., Radmilović, V. R., Lačnjevac, U., Krstajić, N. V.,& Gojković, S. Lj.. (2013). Electrochemical oxidation of methanol on Pt/(RuxSn1-x)O2 nanocatalyst. in Journal of the Serbian Chemical Society Serbian Chemical Society, Belgrade., 78(11), 1703-1716. https://hdl.handle.net/21.15107/rcub_technorep_2353
Krstajić M, Obradović M, Babić BM, Radmilović VR, Lačnjevac U, Krstajić NV, Gojković SL. Electrochemical oxidation of methanol on Pt/(RuxSn1-x)O2 nanocatalyst. in Journal of the Serbian Chemical Society. 2013;78(11):1703-1716. https://hdl.handle.net/21.15107/rcub_technorep_2353 .
Krstajić, Mila, Obradović, Maja, Babić, Biljana M., Radmilović, Velimir R., Lačnjevac, Uroš, Krstajić, Nedeljko V., Gojković, Snežana Lj., "Electrochemical oxidation of methanol on Pt/(RuxSn1-x)O2 nanocatalyst" in Journal of the Serbian Chemical Society, 78, no. 11 (2013):1703-1716, https://hdl.handle.net/21.15107/rcub_technorep_2353 .