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Abstract Desulfurization is a significant approach to producing clean fuel. The design of novel host–guest catalysts with multiple active sites at atomic‐ and nano‐scales, opens a new door to gain an ultrahigh synergistic performance for targeted applications. Herein, an in situ solvent‐free approach is conducted for synchronously implanting Pd single sites (Pd SS ) and nanoparticles (Pd NP ) into a novel Zr‐based metal–organic framework (Zr‐MOF). The optimal catalyst exhibits ultrahigh oxidative desulfurization (ODS) performance that can oxidize 1 000 ppm sulfur with diluted oxidant at 40 °C within 5 min. The turnover frequency of the catalyst at 40 °C reaches 774.7 h −1 which is 47.4 times higher than host Zr‐MOF and surpasses the most reported ODS catalysts. A substantial synergistic effect between Pd SS and Pd NP is responsible for the upgradation of ODS performance. Experimental and theoretical results indicate that Pd SS in Zr‐MOF can readily absorb H 2 O 2 , and synergistically decompose H 2 O 2 with the assistance of Pd NP for accelerated generation of •OH radicals that dominates the ODS performance. This work provides a new solvent‐free way for in situ implanting synergistic catalytic sites into MOFs to upgrade their catalytic performance in targeted reactions.
Ye et al. (Wed,) studied this question.