期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 299, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120659
关键词
Bimetallic MOFs; Defect sites; Solvent-free; Oxidation desulfurization; Room temperature
资金
- National Natural Science Foundation of China [22022508]
- Science and Technology Key Project of Guangdong Province of China [2020B010188002]
- China Postdoctoral Science Foundation [2020M672806]
- Natural Science Foundation of Guangdong Basic and Applied Basic Research Fund [2021A1515010278]
- Guangdong Provincial Characteristic Innovation Projects of Universities [2018KTSCX149]
This work demonstrates a green approach for rapid preparation of defective bimetallic MOFs with enhanced catalytic activity, showcasing the fabrication of UiO-66(Hf-Zr) with plentiful defect sites under solvent-free condition. The bimetallic UiO-66(0.13Hf-Zr) exhibits superior desulfurization activity for fuel oil, with a turnover frequency significantly higher than pristine UiO-66(Zr).
Desulfurization of fuel oil is an indispensable step to obtain clean energy source. Design of bimetallic metalorganic frameworks (MOFs) with plentiful defects and highly dispersion active species, opens a new door to boost the catalytic activity for targeted reactions. In this work, we demonstrate a rapid green approach for fabricating bimetallic UiO-66(Hf-Zr) with highly dispersion of Hf/Zr-OH defect sites under solvent-free condition. UiO-66(0.13Hf-Zr) exhibited superior activity for oxidating sulfur compounds (1000 ppm S) of fuel oil at room temperature within 15 min. The turnover frequency (TOF) number reach 129.5 h-1 at 30 degrees C, which is 32.2 times higher than pristine UiO-66(Zr). Theoretical results reveal that the exposed Hf-OH sites readily react with H2O2 to produce Hf-OOH intermediates which manipulate the reaction performance. Our work not only proposes a green solvent-free avenue for rapid preparation of defective bimetallic MOFs but also extends the application of bimetallic MOFs in the field of desulfurization.
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