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Triphenylphosphine-functionalized hyper-crosslinked polymers for efficient hydrogen generation via sodium borohydride methanolysis   
Yazarlar (6)
Dr. Öğr. Üyesi Kutalmış GÖKKUŞ Dr. Öğr. Üyesi Kutalmış GÖKKUŞ
Kastamonu Üniversitesi, Türkiye
Aysegul Ozbal
Eskişehir Osmangazi Üniversitesi, Türkiye
Prof. Dr. Mahmut GÜR Prof. Dr. Mahmut GÜR
Kastamonu Üniversitesi, Türkiye
Salih Alper Akalin
Dokuz Eylül Üniversitesi, Türkiye
Hazal Sebli
Kastamonu Üniversitesi, Türkiye
Vural Bütün
Eskişehir Osmangazi Üniversitesi, Türkiye
Devamını Göster
Özet
Four novel hyper-crosslinked polymers (HCP-1 to HCP-4) were synthesized via Friedel–Crafts alkylation using 4,4′-bis(chloromethyl)-1,1′-biphenyl as the crosslinker and various aromatic monomers including triphenylphosphine (TPP). These polymers were designed as metal-free catalysts for hydrogen generation via sodium borohydride methanolysis. Comprehensive characterization using FT-IR, XPS, BET, TGA, SEM, and zeta potential analyses confirmed that the materials possess thermally stable, porous networks with irregular morphologies and distinct surface charges. Under practical conditions, HCP-3 exhibited the highest catalytic activity with a hydrogen generation rate of 9857 mL H2 min−1 g−1 at 303.15 K and the lowest activation energy (Ea = 32.0 kJ mol−1). At elevated temperature (333.15 K), HCP-2 achieved the highest activity (37,200 mL H2 min−1 g−1), reflecting the strong influence of temperature on performance trends. Despite not having the highest surface area or pore volume, the superior activity of HCP-3 at 303.15 K highlights the decisive roles of microporous architecture, electrostatic surface characteristics, and heteroatom functionality. Zeta potential analysis revealed significant reductions in surface charge after reaction, particularly for HCP-3, suggesting strong electrostatic interactions with BH₄ ions. XPS data further confirmed the successful incorporation of TPP and heteroaromatic units, correlating with enhanced catalytic efficiency. Overall, the findings underscore a surface-mediated mechanism where both charge-assisted hydride attraction and structural topology govern hydrogen evolution. The metal-free and reusable nature of these catalysts supports their potential in sustainable hydrogen technologies.
Anahtar Kelimeler
Hydrogen generation | Hyper-crosslinked polymers | NaBH4 methanolysis | Triphenylphosphine | Zeta potential
Makale Türü Özgün Makale
Makale Alt Türü SSCI, AHCI, SCI, SCI-Exp dergilerinde yayınlanan tam makale
Dergi Adı Reactive and Functional Polymers
Dergi ISSN 1381-5148 Wos Dergi Scopus Dergi
Dergi Grubu Q1
Makale Dili İngilizce
Basım Tarihi 12-2025
Cilt No 217
Sayı 1
Doi Numarası 10.1016/j.reactfunctpolym.2025.106480