Kutalmis Gokkus , Aysegul Ozbal , Mahmut Gür , Salih Alper Akalin , Hazal Sebli , Vural Bütün
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引用次数: 0
Abstract
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.
期刊介绍:
Reactive & Functional Polymers provides a forum to disseminate original ideas, concepts and developments in the science and technology of polymers with functional groups, which impart specific chemical reactivity or physical, chemical, structural, biological, and pharmacological functionality. The scope covers organic polymers, acting for instance as reagents, catalysts, templates, ion-exchangers, selective sorbents, chelating or antimicrobial agents, drug carriers, sensors, membranes, and hydrogels. This also includes reactive cross-linkable prepolymers and high-performance thermosetting polymers, natural or degradable polymers, conducting polymers, and porous polymers.
Original research articles must contain thorough molecular and material characterization data on synthesis of the above polymers in combination with their applications. Applications include but are not limited to catalysis, water or effluent treatment, separations and recovery, electronics and information storage, energy conversion, encapsulation, or adhesion.