Oxidative desulfurization of heavy gas oil over Ti-TUD-1 supported Keggin-type molybdenum heteropolyacid

Sundaramurthy Vedachalam, Philip E. Boahene, Ajay K. Dalai

Research output: Contribution to journalArticlepeer-review

Abstract

Catalytic oxidative desulfurization (ODS) is emerging as a potential alternative to deep hydroprocessing due to its milder operating conditions and no hydrogen requirements. In this study, ODS catalysts based on mesoporous TUD-1 support were developed to overcome the diffusion limitation of zeolite-based catalysts in oxidizing large-size organosulfur compounds present in real petroleum feedstocks. Different mesoporous oxidation catalysts were formed by substituting Ti in the TUD-1 framework and impregnating Keggin molybdenum heteropoly acid (HPA) on TUD-1 support. The mesoporosity of TUD-1, and the presence of Ti (IV) and Mo Keggin units in the prepared catalysts were confirmed from the characterization results of XRD, XPS, XANES, and BET-N2. The ODS performance of catalysts was studied using a mild hydrotreated bitumen derived heavy gas oil feedstock. The HPA dispersed Ti-TUD-1 catalyst was found to be most active for desulfurizing the heavy gas oil feedstock due to a strong synergy effect of Ti and Mo Keggin ions on catalyzing oxygen transfer from an oxidant to a substrate. Oxidants such as hydrogen peroxide, cumene hydroperoxide, tert-butyl hydroperoxide, and molecular oxygen were screened in this study. The first two oxidants were better than others and equally efficient. The HPA /Ti-TUD-1 catalyst was found to be suitable for oxidative desulfurization and oxidative denitrogenation (ODN) both in the batch stirred tank reactor and continuous fixed-bed reactor systems.
Original languageEnglish (US)
JournalEnergy & Fuels
DOIs
StatePublished - Aug 20 2020
Externally publishedYes

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