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Atomically resolved dealloying of structurally ordered Pt nanoalloy as an oxygen reduction reaction electrocatalyst
Andraž Pavlišič, Primož Jovanovič, Vid Simon Šelih, Martin Šala, Marjan Bele, Goran Dražić, Iztok Arčon, Samo B. Hočevar, Anton Kokalj, Nejc Hodnik, Miran Gaberšček, izvirni znanstveni članek

Opis: The positive effect of intermetallic ordering of platinum alloy nanoparticles on oxygen reduction reaction (ORR) activity has been well established. What is still missing is an understanding of selective leaching of the less noble metal from the ordered structure and its correlation to longterm ORR performance. Using a combination of kinetic Monte Carlo simulations and advanced characterization techniques, we provide unprecedented insight into dealloying of intermetallic PtCu3 nanoparticles a well-known binary alloy. Comparison of ordered and disordered samples with identical initial compositions and particle size distributions reveals an unexpected correlation: whereas the copper dealloying rates in the ordered and disordered counterparts are almost the same, in the ordered structure Pt atoms are surrounded by 15−30% more Cu atoms throughout all the stages of acid leaching. This more convenient Pt−Cu coordination explains the statistically significant increase of 23−37% in ORR activity of the ordered structure at all stages of alloy degradation.
Najdeno v: osebi
Ključne besede: ORR activity, fuel cells, platinum alloy, nanoparticle stability, intermetallic ordering, kinetic Monte Carlo, dealloying, in situ ICP-MS
Objavljeno: 27.09.2016; Ogledov: 2151; Prenosov: 0
.pdf Polno besedilo (3,27 MB)

3.
Electrochemical dissolution of iridium and iridium oxide particles in acidic media
Miran Gaberšček, Samo B. Hočevar, Vid Simon Šelih, Martin Šala, Marjan Bele, Milena Zorko, Barbara Jozinović, Iztok Arčon, Francisco Ruiz-Zepeda, Nejc Hodnik, Primož Jovanovič, 2017, izvirni znanstveni članek

Opis: Iridium based particles as the most promising proton exchange membrane electrolyser electrocatalysts were investigated by transmission electron microscopy (TEM), and by coupling of electrochemical flow cell (EFC) with online inductively coupled plasma mass spectrometer (ICP-MS). Additionally, a thin-film rotating disc electrode (RDE), an identical location transmission and scanning electron microscopy (IL-TEM and IL-SEM) as well as an X-ray absorption spectroscopy (XAS) studies have been performed. Extremely sensitive online time-and potential-resolved electrochemical dissolution profiles revealed that iridium particles dissolved already well below oxygen evolution reaction (OER) potentials, presumably induced by iridium surface oxidation and reduction processes, also referred to as transient dissolution. Overall, thermally prepared rutile type IrO2 particles (T-IrO2) are substantially more stable and less active in comparison to as prepared metallic (A-Ir) and electrochemically pretreated (E-Ir) analogues. Interestingly, under OER relevant conditions E-Ir particles exhibit superior stability and activity owing to the altered corrosion mechanism where the formation of unstable Ir(>IV) species is hindered. Due to the enhanced and lasting OER performance, electrochemically pre-oxidized E-Ir particles may be considered as the electrocatalyst of choice for an improved low temperature electrochemical hydrogen production device, namely a proton exchange membrane electrolyser.
Najdeno v: osebi
Ključne besede: Iridium Oxide Par-ticles, Electrochemical Dissolution of Iridium, Ir L3-edge XANES
Objavljeno: 23.08.2017; Ogledov: 1157; Prenosov: 0
.pdf Polno besedilo (1,43 MB)

4.
Staranje nitrogvajakola pod vplivom sončne svetlobe
Ajda Delić, 2020, magistrsko delo

Opis: Nitrogvajakoli so rumeno obarvane spojine, ki prispevajo k absorpciji rjavega ogljika v ozračju. Na podnebje vplivajo z absorbiranjem svetlobe v bližnjem UV in vidnem delu spektra, saj po absorpciji sproščajo toploto, kar vodi v ogrevanje ozračja. Poleg tega imajo škodljiv vpliv tudi na ekosistem. Prisotnost v ozračju in njihovi mehanizmi nastanka so že raziskani, mehanizmi razpadanja v vodni fazi ozračja pa so malo znani. V tem delu smo raziskali, kako sončna svetloba vpliva na staranje nitrogvajakolov v ozračju. Z uporabo fotospektroskopije smo najprej proučili spektroskopske lastnosti vodnih raztopin gvajakola, 4-nitrogvajakola, 5-nitrogvajakola in dinitrogvajakola ter kako nanje vpliva pH. Preiskovani nitrogvajakoli v vidnem delu spektra močno absorbirajo le pri visokih pH, dinitrogvajakol pa zaradi nekoliko nižjega pKa absorbira tudi že pri rahlo kislih pH vrednostih. pH raztopin 4-nitrogvajakola in 5-nitrogvajakola različnih koncentracij smo pred fotolizo prilagodili na vrednost atmosferskih vod (pH okoli 5), nato pa smo jih izpostavili sončnemu simulatorju z močjo enega sonca. Produkte fotorazgradnje smo ločili in identificirali s tekočinsko kromatografijo sklopljeno s pretočnim spektrometrom in tandemskim masnim spektrometrom (LC-UV/Vis-MS/MS). Fotorazgradnja nitrogvajakolov poteka zelo počasi. Najdeni produkti imajo ohranjen aromatski obroč in eno ali več nitro skupin (dinitrogvajakol, 4-nitrokatehol). Zaključimo lahko, da so nitrogvajakoli v vodni fazi ozračja obstojni, absorbirajo v širokem območju pH vrednosti in s svojimi absorpcijskimi lastnostmi skupaj s produkti fotorazgradnje prispevajo k vplivu rjavega ogljika na podnebje.
Najdeno v: osebi
Ključne besede: Rjavi ogljik, nitrogvajakol, fotorazpad, spektroskopske lastnosti, vpliv pH, identifikacija produktov, LC-UV/Vis-MS/MS
Objavljeno: 03.06.2020; Ogledov: 238; Prenosov: 14
.pdf Polno besedilo (1,62 MB)

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