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Solving the Structure of Reaction Intermediates by Time-Resolved Synchrotron X-ray Absorption Spectroscopy

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.3040271· OSTI ID:980468

We present a robust data analysis method of time-resolved x-ray absorption spectroscopy experiments suitable for chemical speciation and structure determination of reaction intermediates. Chemical speciation is done by principal component analysis (PCA) of the time-resolved x-ray absorption near-edge structure data. Structural analysis of intermediate phases is done by theoretical modeling of their extended x-ray absorption fine-structure data isolated by PCA. The method is demonstrated using reduction and reoxidation of Cu-doped ceria catalysts where we detected reaction intermediates and measured fine details of the reaction kinetics. This approach can be directly adapted to many time-resolved x-ray spectroscopy experiments where new rapid throughput data collection and analysis methods are needed.

Research Organization:
Brookhaven National Laboratory (BNL) National Synchrotron Light Source
Sponsoring Organization:
Doe - Office Of Science
DOE Contract Number:
AC02-98CH10886
OSTI ID:
980468
Report Number(s):
BNL--93386-2010-JA
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Vol. 129; ISSN JCPSA6; ISSN 0021-9606
Country of Publication:
United States
Language:
English