Amphiphilic halloysite nanotube enclosing molybdenum oxide as nanoreactor for efficient desulfurization of model fuels

Hollow nanomaterials are regarded as the outstanding supports due to their confinement effect and stable carries, which can enhance the performance of the supported catalysts and even simplify the process. In this work, halloysite nanotubes (HNT) are chosen as the support due to their monoclinic tubular structures with two different surface compositions and charges. By a simple impregnation-calcination approach, MoOx is immobilized in the internal surface of HNT, then modify with organosilanes on the external surface of HNT to yield the amphiphilic Mo/HNT/S nanoreactor. The catalyst exhibits prominent activity for oxidative desulfurization in solvent-free system, the desulfurization rate of dibenzothiophene (DBT) reaches 100 % and the turnover frequency (TOF) value reaches 67.5 h(-1) at 60 degrees C with 15 min, which is higher than most reported Mo-based catalysts. The hydrophobic surface enables the nanoreactor to be well dispersed in oil phase, and H2O2 solution in the hydrophilic cavity can extract DBT to form a concentrated microenvironment of the reactants and reactive oxygen species. The confinement function of the HNT nanoreactor can enhance the activity and stability of active ingredients (MoOx) over at least 5 cycles. Additionally, oxidation products can be retained in the hydrophilic lumen and completely separated from the model fuel. This amphiphilic catalytic system eliminates the following solvent extraction step in the ODS procedure. Thus, the catalyst is a promising candidate for large-scale industrial application.

Automated summary

In this study, an amphiphilic Mo/HNT/S nanoreactor was developed by immobilizing MoOx on the internal surface of halloysite nanotubes (HNT) and modifying the external surface with organosilanes. The catalyst exhibited high activity for oxidative desulfurization and showed improved stability over multiple cycles. The amphiphilic nature of the nanoreactor allowed for enhanced dispersion in the oil phase and formation of a concentrated microenvironment for the reactants and reactive oxygen species. This catalytic system eliminates the need for solvent extraction in the desulfurization process, making it a promising candidate for large-scale industrial applications.