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

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.
Authors:
; ;
Publication Date:
OSTI Identifier:
980468
Report Number(s):
BNL--93386-2010-JA
Journal ID: ISSN 0021-9606; JCPSA6; TRN: US1005504
DOE Contract Number:
DE-AC02-98CH10886
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 129
Research Org:
Brookhaven National Laboratory (BNL) National Synchrotron Light Source
Sponsoring Org:
Doe - Office Of Science
Country of Publication:
United States
Language:
English
Subject:
43 PARTICLE ACCELERATORS; ABSORPTION; ABSORPTION SPECTROSCOPY; CATALYSTS; DATA; DATA ANALYSIS; FINE STRUCTURE; POLAR-CAP ABSORPTION; REACTION INTERMEDIATES; REACTION KINETICS; REDUCTION; SIMULATION; SYNCHROTRONS; X-RAY SPECTROSCOPY national synchrotron light source