As one dynamic aspect of catalysis, spillover is known as species diffusion between an active metal and its support1–3, especially in reactions involving hydrogen and oxygen4–8.
; however, it remains unclear whether the bulk catalyst participates in the reactions through non-surface spillover. Here we track the oxygen spillover in Ru/TiOlattice at the subsurface was strained reversibly to provide channels for oxygen transport, as detected by the picometre-precision tracing of atomic displacement. The structural adaptability at the metal–support interface is critical for controlling oxygen spillover, which is switched on in Ru/rutile-TiO. As shown by the real-time atom-resolved evidence, this bulk oxygen spillover is generally viable in supported metal catalysts of an interfacial epitaxy nature and demonstrates the significance of rationally engineered metal–support interfaces for activating the oxygen in bulk catalyst to contribute to reactions.
Zecevic, J., Vanbutsele, G., de Jong, K. P. & Martens, J. A. Nanoscale intimacy in bifunctional catalysts for selective conversion of hydrocarbons. Sharma, V., Crozier, P. A., Sharma, R. & Adams, J. B. Direct observation of hydrogen spillover in Ni-loaded Pr-doped ceria. Im, J., Shin, H., Jang, H., Kim, H. & Choi, M. Maximizing the catalytic function of hydrogen spillover in platinum-encapsulated aluminosilicates with controlled nanostructures. Frey, H., Beck, A., Huang, X., van Bokhoven, J. A. & Willinger, M. G. Dynamic interplay between metal nanoparticles and oxide support under redox conditions. Ishikawa, R., Ueno, Y., Ikuhara, Y. & Shibata, N. Direct observation of atomistic reaction process between Pt nanoparticles and TiO Tauster, S. J., Fung, S. C. & Garten, R. L. Strong metal-support interactions. Group 8 noble metals supported on titanium dioxide. Green, I. X., Tang, W., Neurock, M. & Yates, J. T. Spectroscopic observation of dual catalytic sites during oxidation of CO on a Au/TiO Han, X., Li, L. & Wang, C. Synthesis of tin dioxide nanooctahedra with exposed high-index {332} facets and enhanced selective gas sensing properties. Kresse, G. & Furthmüller, J. Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set. Kühne, T. D. et al. CP2K: An electronic structure and molecular dynamics software package - Quickstep: Efficient and accurate electronic structure calculations. Henkelman, G., Uberuaga, B. P. & Jónsson, H. A climbing image nudged elastic band method for finding saddle points and minimum energy paths. Shu, D.-J., Ge, S.-T., Wang, M. & Ming, N.-B. Interplay between external strain and oxygen vacancies on a rutile TiO He, Y., Dulub, O., Cheng, H., Selloni, A. & Diebold, U. Evidence for the predominance of subsurface defects on reduced anatase TiO
We extend our sincere gratitude to A. Goldbach for providing expert insight during manuscript preparation. Y. Cui and Y. Li are thanked for their contributions to the APXPS experiments facilitated by Vacuum Interconnected Nanotech Workstation at Suzhou Institute of Nano-Tech and Nano-Bio-nics, Chinese Academy of Sciences . This work was supported by the Strategic Priority Research Programme of CAS , the NSFC Centre for Single-Atom-Catalysis , the CAS Project for Young Scientists in Basic Research , the National Natural Science Foundation of China , the Youth Innovation Promotion Association CAS , National Key R&D Programme of China , the Young Top-notch Talents of Liaoning Province , New Cornerstone Science Foundation through the XPLORER PRIZE and Guangdong Provincial Key Laboratory of Catalysis . The computational resources were supported by Centre for Computational Science and Engineering at Southern University of Science and Technology and the CHEM high-performance supercomputer cluster located in the Department of Chemistry, SUSTech.
W.L., Y.H. and T.Z. conceived this project and supervised the study. W.W. performed the material synthesis, microscopy, spectroscopy and other experiments. W.W., X.Y. and W.L. performed the data analysis. H.X. and Y.-G.W. conducted DFT calculations. S.L. and W.L. developed the method for atom displacement analysis. W.W., X.Y., W.L., Y.-G.W. and Y.H. wrote the manuscript, with the help of the other authors.
thanks Gianfranco Pacchioni, Marc Willinger and the other, anonymous, reviewer for their contribution to the peer review of this work., The status of Ru initial oxidation, and inset enlarges the oxidation region where spillover occurs first at the interior interface rather than exposed surface.
coverage states in function of pressure and temperature . The second row of panels shows for Ru/r-TiO, HRTEM images of Ru NPs from two locations during the reaction. In sharp contrary, the absence of interfacial synergy in Ru/a-TiO
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