Defects engineering simultaneously enhances activity and recyclability of MOFs in selective hydrogenation of biomass

The catalytic performance of metal-organic frameworks can be tuned by introducing defects in their structure. Here, the authors introduce defects and impregnate ruthenium nanoparticles in cationic metal-organic frameworks, which enables enhanced recyclability and catalytic performance in D-glucose hydrogenation. The development of synthetic methodologies towards enhanced performance in biomass conversion is desirable due to the growing energy demand. Here we design two types of Ru impregnated MIL-100-Cr defect engineered metal-organic frameworks (Ru@DEMOFs) by incorporating defective ligands (DLs), aiming at highly efficient catalysts for biomass hydrogenation. Our results show that Ru@DEMOFs simultaneously exhibit boosted recyclability, selectivity and activity with the turnover frequency being about 10 times higher than the reported values of polymer supported Ru towards D-glucose hydrogenation. This work provides in-depth insights into (i) the evolution of various defects in the cationic framework upon DLs incorporation and Ru impregnation, (ii) the special effect of each type of defects on the electron density of Ru nanoparticles and activation of reactants, and (iii) the respective role of defects, confined Ru particles and metal single active sites in the catalytic performance of Ru@DEMOFs for D-glucose selective hydrogenation as well as their synergistic catalytic mechanism.

Automated summary

The study demonstrates the enhancement of catalytic performance and recyclability in D-glucose hydrogenation by introducing defects and impregnating ruthenium nanoparticles in cationic metal-organic frameworks. This is significant for the improvement in biomass conversion.