Applied Catalysis A: General, Vol.572, 34-43, 2019
Partial deligandation of M/Ce-BTC nanorods (M = Au, Cu, au-cu) with "Quasi-MOF" structures towards improving catalytic activity and stability
Integrated nanocatalysts comprised of metal-organic frameworks (MOFs) and noble metal nanoparticles (MNPs) have been widely used in a myriad of reactions, however, the interactions between guest MNPs and inorganic nodes in the framework are relatively weak due to the hindrance of organic moiety. Herein, Ce-bearing MOFs (viz., Ce-BTC nanorods) were used as support material to immobilize MNPs (e.g., Au, Cu, Au-Cu), and a variety of thermal treatments (e.g., inert gas, air, or dilute O-2 atmospheres) were conducted to partially or completely remove organic moiety in order to adjust the interactions between Ce nodes and the guest MNPs. It was found that M/CeBTC without deligandation treatments exhibited negligible activity in CO oxidation. Partial deligandation could greatly enhance the intimate interactions, however, the carbonization showed detrimental effect on the catalytic activity. Interestingly, a further treatment in a dilute O-2 atmosphere can selectively eliminate the carbon and retain a "quasi-MOF" state, and importantly the resultant catalysts exhibited excellent performance for CO oxidation without any activity loss over 250 h evaluation time. Our results will provide a new strategy for enhancing the interactions between the inorganic nodes in MOF and the guest MNPs for improving catalytic performance.