5 years ago

Revealing the Role of Interfacial Properties on Catalytic Behaviors by in Situ Surface-Enhanced Raman Spectroscopy

Revealing the Role of Interfacial Properties on Catalytic Behaviors by in Situ Surface-Enhanced Raman Spectroscopy
Hua Zhang, De-Yin Wu, Han-Lei Sun, Zhong-Qun Tian, Zhi-Lin Yang, Jie Wei, Jian-Feng Li, Bing-Hui Chen, Chen Wang, Xia-Guang Zhang, Shu Chen, Ya-Hao Wang
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 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.

Publisher URL: http://dx.doi.org/10.1021/jacs.7b04011

DOI: 10.1021/jacs.7b04011

You might also like
Discover & Discuss Important Research

Keeping up-to-date with research can feel impossible, with papers being published faster than you'll ever be able to read them. That's where Researcher comes in: we're simplifying discovery and making important discussions happen. With over 19,000 sources, including peer-reviewed journals, preprints, blogs, universities, podcasts and Live events across 10 research areas, you'll never miss what's important to you. It's like social media, but better. Oh, and we should mention - it's free.

  • Download from Google Play
  • Download from App Store
  • Download from AppInChina

Researcher displays publicly available abstracts and doesn’t host any full article content. If the content is open access, we will direct clicks from the abstracts to the publisher website and display the PDF copy on our platform. Clicks to view the full text will be directed to the publisher website, where only users with subscriptions or access through their institution are able to view the full article.