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Title: Dynamical observation and detailed description of catalysts under strong metal–support interaction

Understanding the structures of catalysts under realistic conditions with atomic precision is crucial to design better materials for challenging transformations. Under reducing conditions, certain reducible supports migrate onto supported metallic particles and create strong metal–support states that drastically change the reactivity of the systems. The details of this process are still unclear and preclude its thorough exploitation. Here, we report an atomic description of a palladium/titania (Pd/TiO 2) system by combining state-of-the-art in situ transmission electron microscopy and density functional theory (DFT) calculations with structurally defined materials, in which we visualize the formation of the overlayers at the atomic scale under atmospheric pressure and high temperature. We show that an amorphous reduced titania layer is formed at low temperatures, and that crystallization of the layer into either mono- or bilayer structures is dictated by the reaction environment and predicted by theory. Moreover, it occurs in combination with a dramatic reshaping of the metallic surface facets.
Authors:
 [1] ;  [2] ;  [3] ;  [1] ;  [1] ;  [1] ;  [3] ;  [4] ;  [5]
  1. Univ. of California, Irvine, CA (United States); Univ. of Michigan, Ann Arbor, MI (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
  3. Stanford Univ., Stanford, CA (United States)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. Univ. of California, Irvine, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-76SF00515
Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 16; Journal Issue: 7; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; in situ microcopy; Pd nanoparticles; SMSI; TiO2
OSTI Identifier:
1349404

Zhang, Shuyi, Plessow, Philipp N., Willis, Joshua J., Dai, Sheng, Xu, Mingjie, Graham, George W., Cargnello, Matteo, Abild-Pedersen, Frank, and Pan, Xiaoqing. Dynamical observation and detailed description of catalysts under strong metal–support interaction. United States: N. p., Web. doi:10.1021/acs.nanolett.6b01769.
Zhang, Shuyi, Plessow, Philipp N., Willis, Joshua J., Dai, Sheng, Xu, Mingjie, Graham, George W., Cargnello, Matteo, Abild-Pedersen, Frank, & Pan, Xiaoqing. Dynamical observation and detailed description of catalysts under strong metal–support interaction. United States. doi:10.1021/acs.nanolett.6b01769.
Zhang, Shuyi, Plessow, Philipp N., Willis, Joshua J., Dai, Sheng, Xu, Mingjie, Graham, George W., Cargnello, Matteo, Abild-Pedersen, Frank, and Pan, Xiaoqing. 2016. "Dynamical observation and detailed description of catalysts under strong metal–support interaction". United States. doi:10.1021/acs.nanolett.6b01769. https://www.osti.gov/servlets/purl/1349404.
@article{osti_1349404,
title = {Dynamical observation and detailed description of catalysts under strong metal–support interaction},
author = {Zhang, Shuyi and Plessow, Philipp N. and Willis, Joshua J. and Dai, Sheng and Xu, Mingjie and Graham, George W. and Cargnello, Matteo and Abild-Pedersen, Frank and Pan, Xiaoqing},
abstractNote = {Understanding the structures of catalysts under realistic conditions with atomic precision is crucial to design better materials for challenging transformations. Under reducing conditions, certain reducible supports migrate onto supported metallic particles and create strong metal–support states that drastically change the reactivity of the systems. The details of this process are still unclear and preclude its thorough exploitation. Here, we report an atomic description of a palladium/titania (Pd/TiO2) system by combining state-of-the-art in situ transmission electron microscopy and density functional theory (DFT) calculations with structurally defined materials, in which we visualize the formation of the overlayers at the atomic scale under atmospheric pressure and high temperature. We show that an amorphous reduced titania layer is formed at low temperatures, and that crystallization of the layer into either mono- or bilayer structures is dictated by the reaction environment and predicted by theory. Moreover, it occurs in combination with a dramatic reshaping of the metallic surface facets.},
doi = {10.1021/acs.nanolett.6b01769},
journal = {Nano Letters},
number = 7,
volume = 16,
place = {United States},
year = {2016},
month = {6}
}