Improved Pt/C electrocatalysts for methanol oxidation prepared by different reducing agents and surfactants and DFT studies on it

Autor: Gülsün Gökağaç, Aysu Çokangın, Metin Aydin
Přispěvatelé: Ondokuz Mayıs Üniversitesi
Rok vydání: 2017
Předmět:
Zdroj: Journal of Nanoparticle Research. 19
ISSN: 1572-896X
1388-0764
DOI: 10.1007/s11051-017-4044-y
Popis: AYDIN, METIN/0000-0003-3767-946X WOS: 000412935700002 In this work, PtCl4 as precursor; sodium borohydride (Cat I), hydrazinium hydroxide (Cat II), and formaldehyde (Cat III) as reducing agents; and 1-heptanamine (a), N-methyl-1-heptanamine (b), and N, N-dimethyl-1-heptanamine (c) as surfactants were used to prepare platinum nanoparticles which were then dispersed on carbon XC-72 for use as catalysts in the methanol oxidation reaction. XRD and TEM results indicate that the platinum has a face-centered cubic structure and is found as small and agglomerated particles in different shapes, sizes, and densities. Cat I comprises small (similar to 5 nm) cubic and formless agglomerated (similar to 20-similar to 300 nm) particles, Cat II is composed of small (similar to 5 nm) and a significant number of quite dense spherical agglomerated (similar to 20-similar to 150 nm) particles, and Cat III contains large number of small (similar to 5 nm) and a small number of spherical, less dense, and agglomerated (similar to 20-similar to 200 nm) particles. XPS data shows that the platinum exists in two different oxidation states Pt(0) (similar to 64.5-similar to 69.6%) and Pt(IV) (similar to 35.5-similar to 30.4%), and platinum surface also contains OH, H2O, C-O, C=O, and carbon. DFT and FTIR show that the surfactants decompose to form partially crystalline carbon. Electrochemical studies reveal that performance order of the catalysts towards the methanol oxidation reaction is Cat II < Cat I < Cat III, and that Cat IIIc has the highest performance, which is 2.23 times larger than E-TEK catalysts. It was found that the performance of the catalysts depends on the kind of surfactant, reducing agent, electrochemical surface area, percent platinum utility, roughness factor, and If/(I)r ratio. Turkiye Bilimsel ve Teknolojik Arastirma KurumuTurkiye Bilimsel ve Teknolojik Arastirma Kurumu (TUBITAK) [TUBITAK-111T162] This study was funded by Turkiye Bilimsel ve Teknolojik Arastirma Kurumu (TUBITAK-111T162).
Databáze: OpenAIRE