Sustainable Plasma‐Assisted Oxidative Desulfurization of Dibenzothiophene Over Phosphotungstic Acid/ZIF‐8 Catalysts: Catalytic Performance, Kinetic Analysis, and Life Cycle Assessment

ABSTRACT In this study, phosphotungstic acid (PTA)‐ZIF‐8 catalysts were successfully synthesized and integrated with non‐thermal air plasma to establish a highly efficient plasma‐assisted oxidative desulfurization (ODS) system for the removal of dibenzothiophene (DBT). The structural, morphological, textural, and electrochemical properties of the synthesized catalysts were comprehensively characterized using XRD, FTIR, FESEM, EDX, BET, and cyclic voltammetry (CV). The results confirmed the successful immobilization of PTA onto the ZIF‐8 framework while preserving both the crystalline structure of ZIF‐8 and the Keggin structure of PTA. Among the prepared catalysts, 5%PTA‐ZIF‐8 exhibited the highest catalytic activity owing to its optimal balance between PTA dispersion, pore accessibility, and interfacial electron transfer capability. Under the operating conditions of 0.15‐g catalyst, 500‐ppm DBT, pH 7, a plasma voltage of 33 kV, an airflow rate of 49.7 L/min, and a reaction time of 5 min, the integrated plasma/PTA‐ZIF‐8 system achieved a maximum DBT oxidation efficiency of 87%. The synergistic interaction between plasma and the PTA‐ZIF‐8 catalyst was confirmed by a synergy index of 3.41, demonstrating the effective coupling of plasma‐generated reactive oxygen species with the redox‐active PTA‐ZIF‐8. Systematic optimization demonstrated that catalyst dosage, plasma voltage, airflow rate, and pH significantly affected the DBT oxidation efficiency. Radical scavenger experiments identified ozone as the dominant oxidizing species, whereas hydroxyl and superoxide radicals played secondary roles. Furthermore, a cradle‐to‐gate life cycle assessment (LCA) revealed that the 5%PTA‐ZIF‐8 catalyst provided the most favorable environmental performance by achieving the optimum balance between catalytic efficiency and material and energy consumption.