Modulating the strong metal-support interactions by regulating the chemical microenvironment of Pt confined in MOFs for low temperature hydrogenation of DCPD

Strong metal-support interaction (SMSI) plays an important role in heterogeneous catalysis, but the influence of the chemical microenvironment of metal on it is often neglected. In this study, a mesoporous Ce-MOFs with pyridine N sites and open metal sites (OMS) were constructed, and highly dispersed Pt nanoclusters (NCs) and Pt-Nx interface were subsequently introduced and constructed via SMSI effect for hydrogenation of dicyclopentadiene (DCPD). The spectroscopic results and density functional theory (DFT) computations demonstrate that pyridine N and OMS can regulate the SMSI effect between Ce-PyDC and Pt through Pt-Nx interface and electronic interaction between Pt and OMS, which increase electron cloud density of Pt nanoclusters, promote DCPD adsorption, H2 activation. The optimal Pt NCs@Ce-PyDC-3 can efficiently convert DCPD to tetrahydrodicyclopentadiene (THDCPD) at 50 °C, giving a 100 % DCPD conversion and 99 % THDCPD selectivity. This work provides an in-depth understanding of the correlation between the metal nanoparticle microenvironment and SISM effect.