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Title: Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms8583· OSTI ID:1228968
 [1];  [2];  [3];  [4];  [5];  [5];  [1];  [6];  [2];  [1]
  1. Yeshiva Univ., New York, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Photon Sciences Division
  5. Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
  6. Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States); KTH Royal Inst. of Technology, Stockholm (Sweden)

Understanding how heterogeneous catalysts change size, shape and structure during chemical reactions is limited by the paucity of methods for studying catalytic ensembles in working state, that is, in operando conditions. Here by a correlated use of synchrotron X-ray absorption spectroscopy and scanning transmission electron microscopy in operando conditions, we quantitatively describe the complex structural dynamics of supported Pt catalysts exhibited during an exemplary catalytic reaction—ethylene hydrogenation. This work exploits a microfabricated catalytic reactor compatible with both probes. The results demonstrate dynamic transformations of the ensemble of Pt clusters that spans a broad size range throughout changing reaction conditions. Lastly, this method is generalizable to quantitative operando studies of complex systems using a wide variety of X-ray and electron-based experimental probes.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704; FG02-03ER15476; FG02-05ER15688
OSTI ID:
1228968
Report Number(s):
BNL-111043-2015-JA
Journal Information:
Nature Communications, Vol. 6; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 97 works
Citation information provided by
Web of Science

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Insight by In Situ Gas Electron Microscopy on the Thermal Behaviour and Surface Reactivity of Cobalt Nanoparticles journal July 2018
Surface‐supported cluster catalysis: Ensembles of metastable states run the show journal May 2019
In Situ Transmission Electron Microscopy book January 2019
Identification of carbon-encapsulated iron nanoparticles as active species in non-precious metal oxygen reduction catalysts journal August 2016
Electron ptychographic microscopy for three-dimensional imaging journal July 2017
Evolution and stabilization of subnanometric metal species in confined space by in situ TEM journal February 2018
Spatial and temporal exploration of heterogeneous catalysts with synchrotron radiation journal August 2018
Determination of bimetallic architectures in nanometer-scale catalysts by combining molecular dynamics simulations with x-ray absorption spectroscopy journal March 2017
Using in situ and operando methods to characterize phase changes in charged lithium nickel cobalt aluminum oxide cathode materials journal January 2020
Enabling liquid solvent structure analysis using hard x-ray absorption spectroscopy with a transferrable microfluidic reactor journal April 2018
The TES beamline (8-BM) at NSLS-II: tender-energy spatially resolved X-ray absorption spectroscopy and X-ray fluorescence imaging journal October 2019
On the role of the gas environment, electron-dose-rate, and sample on the image resolution in transmission electron microscopy journal May 2016