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Anhydrous proton-conducting imidazole triflate-SiO₂ composite.

ABSTRACT: ImidazoleTriflate (ITF)-SiO₂ composites xITF-(100-x)SiO₂ were prepared by planetary ball-milling method. The structure of the composites was studied by TG-DTA, XRD and FT-IR methods. The ionic conductivity was assessed by alternative current (AC) electrochemical impedance measurement. From XRD results, the crystal size of imidazole triflate became smaller as its loading in xITF-(100-x)SiO₂ decreased. With x = 40 weight percent, the calculated crystal size was about 7.3 nm. FT-IR spectra showed the existence of CF₃SO₃ ^-···H⁺ ion aggregates and imidazole-proton bonds. The electrical conductivity of sample x = 50 was about 6.3 × 10^-3 Scm^-1 at 130 °C under anhydrous condition and about 30 times higher than that of sample x = 100.

SUBMITTER: Tu TA

PROVIDER: S-EPMC9803831 | biostudies-literature | 2022 Dec

REPOSITORIES: biostudies-literature

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Anhydrous proton-conducting imidazole triflate-SiO2 composite.

Tu Tran Anh TA Huy Phuc Nguyen Huu NH

Heliyon 20221222 12

ImidazoleTriflate (ITF)-SiO2 composites xITF-(100-x)SiO2 were prepared by planetary ball-milling method. The structure of the composites was studied by TG-DTA, XRD and FT-IR methods. The ionic conductivity was assessed by alternative current (AC) electrochemical impedance measurement. From XRD results, the crystal size of imidazole triflate became smaller as its loading in xITF-(100-x)SiO2 decreased. With x = 40 weight percent, ...[more]

PMID: 36593837

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Project description:Three imidazole-based hybrid materials, coded as IGOPS, IPS and impyridine@SiO2 nanohybrids, were prepared via the covalent immobilization of N-ligands onto a mesoporous nano-SiO2 matrix for H2 generation from formic acid (FA). BET and HRTEM demonstrated that the immobilization of the imidazole derivative onto SiO2 has a significant effect on the SSA, average pore volume, and particle size distribution. In the context of FA dehydrogenation, their catalytic activity (TONs, TOFs), stability, and reusability were assessed. Additionally, the homologous homogeneous counterparts were evaluated for comparison purposes. Mapping the redox potential of solution Eh vs. SHE revealed that poly-phosphine PP3 plays an essential role in FA dehydrogenation. On the basis of performance and stability, [Fe2+/IGOPS/PP3] demonstrated superior activity compared to other heterogeneous catalysts, producing 9.82 L of gases (VH2 + CO2) with TONs = 31,778, albeit with low recyclability. In contrast, [Fe2+/IPS/PP3] showed the highest stability, retaining considerable performance after three consecutive uses. With VH2 + CO2 = 7.8 L, [Fe2+/impyridine@SiO2/PP3] activity decreased, and it was no longer recyclable. However, the homogeneous equivalent of [Fe2+/impyridine/PP3] was completely inactive. Raman, FT/IR, and UV/Vis spectroscopy demonstrated that the reduced recyclability of [Fe2+/IGOPS/PP3] and [Fe2+/impyridine@SiO2/PP3] nanohybrids is due to the reductive cleavage of their C-O-C bonds during catalysis. An alternative grafting procedure is proposed, applying here to the grafting of IPS, resulting in its higher stability. The accumulation of water derived from substrate's feeding causes the inhibition of catalysis. In the case of [Fe2+-imidazole@SiO2] nanohybrids, simple washing and drying result in their re-activation, overcoming the water inhibition. Thus, the low-cost imidazole-based nanohybrids IGOPS and IPS are capable of forming [Fe2+/IGOPS/PP3] and [Fe2+/IPS/PP3] heterogeneous catalytic systems with high stability and performance for FA dehydrogenation.

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Anhydrous proton-conducting imidazole triflate-SiO₂ composite.

Publications

Anhydrous proton-conducting imidazole triflate-SiO<sub>2</sub> composite.

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