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In Situ Implanting of Single Tungsten Sites into Defective UiO‐66(Zr) by Solvent‐Free Route for Efficient Oxidative Desulfurization at Room Temperature
Author(s) -
Ye Gan,
Wang Hanlu,
Chen Wenxing,
Chu Hongqi,
Wei Jinshan,
Wang Dagang,
Wang Jin,
Li Yadong
Publication year - 2021
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202107018
Subject(s) - flue gas desulfurization , catalysis , tungsten , solvent , sulfur , chemistry , in situ , homogeneous , chemical engineering , atom (system on chip) , materials science , inorganic chemistry , combinatorial chemistry , organic chemistry , physics , thermodynamics , computer science , embedded system , engineering
Design of single‐site catalysts with catalytic sites at atomic‐scale and high atom utilization, provides new opportunities to gain superior catalytic performance for targeted reactions. In this contribution, we report a one‐pot green approach for in situ implanting of single tungsten sites (up to 12.7 wt.%) onto the nodes of defective UiO‐66(Zr) structure via forming Zr‐O‐W bonds under solvent‐free condition. The catalysts displayed extraordinary activity for the oxidative removal of sulfur compounds (1000 ppm S) at room temperature within 30 min. The turnover frequency (TOF) value can reach 44.0 h −1 at 30 °C, which is 109.0, 12.3 and 1.2 times higher than that of pristine UiO‐66(Zr), WO 3 , and WCl 6 (homogeneous catalyst). Theoretical and experimental studies show that the anchored W sites can react with oxidant readily and generate W VI ‐peroxo intermediates that determine the reaction activity. Our work not only manifests the application of SSCs in the field of desulfurization of fuel oil but also opens a new solvent‐free avenue for fabricating MOFs based SSCs.