One-Pot Preparation of Nitro-Functionalized Bimetallic UiO-66(Zr-Hf) with Hierarchical Porosity for Oxidative Desulfurization Performance.

Preparation of multifunctional metal-organic frameworks (MOFs) offers new opportunities to obtain ultrahigh synergistic catalytic performance for heterogeneous reactions; however, the application of a one-pot method for preparing multifunctional MOFs remains challenging. Herein, we develop a one-pot green route for synthesizing bimetallic nitro-functionalized UiO-66(Zr-Hf)-NO with hierarchical porosity under solvent-free conditions. The optimal UiO-66(Zr-Hf)-NO shows an ultrahigh enhancement of oxidative desulfurization (ODS) efficiency to oxidize sulfur compounds (1000 ppm sulfur) in a model fuel at 40 °C within 12 min due to the introduction of more active Hf sites in the nodes, the increased Lewis acidity of Zr/Hf-O nodes by the electron-withdrawing NO group, and the enhanced diffusion rates by the mesopores.

Insights into the sacrificial structure-activity relationship of a Ti-based metal-organic framework in an oxidative desulfurization reaction.

Insights into the relationship between the crystal structure and activity of metal-organic frameworks (MOFs) are meaningful to investigate the potential properties of pristine MOFs for targeted catalytic reactions. Herein, we develop a high-efficiency method for boosting the oxidative desulfurization (ODS) activity of Ti-MOF in the presence of H. The ODS activity of pristine Ti-MOF prepared a solvothermal approach is very poor at a low reaction temperature but can be enhanced in the presence of H.