[JACS] 我室李剑锋教授、吴德印教授和田中群教授发表论文:Revealing the role of interfacial properties on catalytic behaviors by in-situ surface-enhanced Raman spectroscopy

我室李剑锋教授、吴德印教授和田中群教授在 JACS 上发表论文:Revealing the role of interfacial properties on catalytic behaviors by in-situ surface-enhanced Raman spectroscopy

文章链接:http://pubs.acs.org/doi/abs/10.1021/jacs.7b04011

文章摘要:

Insightful understanding of how interfacial structures and properties affect catalytic processes is one of the most challenging issues in heterogeneous catalysis. Here, the essential roles of Pt-Au and Pt-oxide-Au interfaces on the activation of H2 and the hydrogenation of para-nitrothiophenol (pNTP) were studied at molecular level by in-situ surface-enhanced Raman spectroscopy (SERS) and shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS). Pt-Au and Pt-oxide-Au interfaces were fabricated through the synthesis of Pt-on-Au and Pt-on-SHINs nanocomposites. Direct spectroscopic evidence demonstrates that the atomic hydrogen species generated on the Pt nanocatalysts can spill over from Pt to Au via the Pt-Au and Pt-TiO2-Au interfaces, but would be blocked at the Pt-SiO2-Au interfaces, leading to the different reaction pathways and product selectivity on Pt-on-Au and Pt-on-SHINs nanocomposites. Such findings have also been verified by the density functional theory (DFT) calculation. In addition, it is found that nanocatalysts assembled on pinhole-free shell-isolated nanoparticles (Pt-on-pinhole-free-SHINs) can override the influence of the Au core on the reaction and can be applied as promising platforms for the in-situ study of heterogeneous catalysis. This work offers a concrete example of how SERS/SHINERS elucidate details about in-situ reaction and helps to dig out the fundamental role of interfaces in catalysis.