Liang Chu, Zhaokun Wang, Teng Zhao, Mu Yang, Ge Wang
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Defective hierarchical porous Ce-UiO-66 excites phosphotungstic acid for superior low-temperature oxidative desulfurization
Metal-organic frameworks (MOFs) as host-guest catalyst in oxidative desulfurization (ODS) face challenges due to limited access to active sites through their microporosity. Herein, hierarchical porous Ce-UiO-66 (HCU) was synthesized through a templating method in an aqueous environment to enhance host accessibility; phosphotungstic acid (PW) was uniformly loaded within the mesopores of HCU via post-impregnation; Ce sites were exposed by selective removing the coordinated acetate from the HCU with the acid post-treatment, these synergistically optimized the catalytic potential of the composite. The resulting HCU@5PW-H demonstrates outstanding desulfurization performance (1000 ppm sulfur removal) within 16 minutes under mild conditions (40 °C, O/S molar ratio = 5) and maintains high efficiency over at least eight cycles. The catalytic mechanism involves the decomposition of H2O2 to reactive oxygen species (ROS) and the formation of WVI-peroxo intermediates that determine the ODS activity. This synergistic mechanism offers a promising strategy to enhance the oxidation potential of hierarchical porous MOF-based host-guest catalysts under mild conditions.
期刊介绍:
The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.