Abstract

Surface characterization and catalysis can significantly benefit from the application of generalized two-dimensional (2D) correlation analysis. This two-dimensional approach allows a better resolution of overlapping peaks, can reveal new features not readily observable in the raw spectra, gives clear evidence for spectral intensities that change as an effect of a perturbation applied to the system, and allows the establishment of time sequences for the changes occurring in different spectral features of interest for determining reaction intermediates and/or mechanisms. The interpretation of the synchronous and asynchronous plots was observed to lead to erroneous time sequences when spectral features change in a non-monotonic way, such as a biphasic or oscillatory behavior, under the influence of a perturbation. We propose a new approach to the 2D correlation analysis to avoid misinterpretation of the results calculated in the asynchronous plot. Progressive correlation analysis (ProCorA) calculates the synchronous plot from the first two spectra of the data matrix and one spectrum is added at every step of the analysis. The sequence of changes can be set up from the progressive evolution of peaks in both the synchronous and asynchronous plots.

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