Abstract
Solid acids are desirable heterogeneous catalysts for green chemistry, with zirconia and its sulfated analogues offering tunable Lewis/Brønsted character. A new route to sulfated ZrO2, and Al-substituted ZrO2 (SO4/AlxZrO2), via carbonization and calcination of metal citrate gels and their subsequent sulfation by (NH4)2SO4 is reported. Structural and acidic properties of these materials were characterized by XRD, Raman, XPS, TGA-MS, N2 porosimetry, and propylamine and pyridine titration. Parent and sulfated materials all adopted the tetragonal zirconia phase, with Al-substitution (evidenced by contraction of the zirconia lattice parameter) at between 0.38–3.50wt% increasing the surface area but decreasing acid strength, accompanied by an overall increase in total acid site loading and Lewis character. Low Al concentrations enhance α-pinene isomerization activity by up to 50% due to the increased acid site loading, however the Turnover Frequency (TOF) remained constant indicating a common active site. The TOF decreased for Al concentrations >3.5wt% due to a further fall in acid strength, manifest as higher selectivity to polycyclic versus monocyclic products.
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Disclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.