Structural evolution of atomically dispersed Pt catalysts dictates reactivity

• Published in: Nature materials Vol. 18; no. 7; pp. 746 - 751
• Main Authors: DeRita, Leo, Resasco, Joaquin, Dai, Sheng, Boubnov, Alexey, Thang, Ho Viet, Hoffman, Adam S., Ro, Insoo, Graham, George W., Bare, Simon R., Pacchioni, Gianfranco, Pan, Xiaoqing, Christopher, Phillip
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 01-07-2019; Nature Publishing Group; Springer Nature - Nature Publishing Group
• Subjects: 119/118; 639/638/77/887; 639/925/930/12; Anatase; Biomaterials; Catalysis; Catalysts; Chemical reactions; Chemistry and Materials Science; Condensed Matter Physics; Coordination; Dynamic response; Environmental conditions; First principles; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; MATERIALS SCIENCE; Nanoparticles; NANOSCIENCE AND NANOTECHNOLOGY; Nanotechnology; Optical and Electronic Materials; Organic chemistry; Oxidation; Platinum; Reactivity; Titanium dioxide
• ISSN: 1476-1122; 1476-4660
• DOI: 10.1038/s41563-019-0349-9

The use of oxide-supported isolated Pt-group metal atoms as catalytic active sites is of interest due to their unique reactivity and efficient metal utilization. However, relationships between the structure of these active sites, their dynamic response to environments and catalytic functionality have proved difficult to experimentally establish. Here, sinter-resistant catalysts where Pt was deposited uniformly as isolated atoms in well-defined locations on anatase TiO
2
nanoparticle supports were used to develop such relationships. Through a combination of in situ atomic-resolution microscopy- and spectroscopy-based characterization supported by first-principles calculations it was demonstrated that isolated Pt species can adopt a range of local coordination environments and oxidation states, which evolve in response to varied environmental conditions. The variation in local coordination showed a strong influence on the chemical reactivity and could be exploited to control the catalytic performance.
Oxide-supported isolated Pt-group metal atoms as catalytic active sites are of interest because of their unique reactivity. Isolated Pt species are now shown to adopt a range of local coordination environments and oxidation states in response to environmental conditions.