Modification of Fe on hydrophobic ZSM-5 zeolite: Optimization of adsorption and catalytic performance for decomposition of VOCs at low-temperature

Abstract

The conjugation of high adsorption and excellent catalytic characteristics is desirable for the removal of volatile-organic-compounds (VOCs) at low-temperatures. In this study, ZSM-5 zeolites with varying Si/Al ratios (15, 30, 100, and 200) were synthesized using the hydrothermal-method to assess their adsorption capability for VOCs. Among them, the ZSM-5(30) sample exhibited a well-defined zeolite structure, exceptional hydrophobicity, a high surface area (SBET), and micropores, resulting in a higher toluene adsorption capacity of 135 mg/g compared to other adsorbents. Additionally, the ZSM-5(30) sample demonstrated excellent regenerative stability in both dry and humid environments. Consequently, ZSM-5(30), identified as the most effective adsorbent, was subjected to loading with various amounts of Fe metal for the catalytic-oxidation of toluene at low-temperatures. Due to its abundant oxygen-vacancies, adequate acid-sites, and various active oxygen-species, the Fe0.2/ZSM-5(30) catalyst (Fe/(Si + Al) = 0.2) not only exhibited a high adsorption capacity for toluene with good stability over five successive cycles but also demonstrated excellent performance in the catalytic oxidation of toluene. The complete conversion of toluene was attained at temperatures approximately 200 °C, with a gas hourly space velocity (GHSV) of 20,000 mL/(g∙h), and maintained stability for 40 h. Furthermore, in-situ diffuse-reflectance infrared-Fourier-transform-spectroscopy (DRIFTS) and gas chromatography-mass spectrometry (GC–MS) results, along with the Mars-Van-Krevelen model, were utilized to elucidate the adsorption and oxidation mechanism of toluene. The unique adsorption and oxidation capabilities of Fe0.2/ZSM-5(30) for toluene indicate its promising potential for the removal of VOCs in real industrial-environments. This study provides valuable insights for the design of high-performance bifunctional materials for the adsorption and catalytic-oxidation of VOCs.