NDLI: Spatial imaging of carbon reactivity centers in Pd/C catalytic systems

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Chemical Science Vol - 6 Issue - 5

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Spatial imaging of carbon reactivity centers in Pd/C catalytic systems

Content Provider	Royal Society of Chemistry (RSC)
Author	Kashin, A. S. Polynski, M. V. Glatzel, P. Ananikov, V. P. Pentsak, E. O. Kvashnina, K. O.
Copyright Year	2015
Abstract	Gaining insight into Pd/C catalytic systems aimed at locating reactive centers on carbon surfaces, revealing their properties and estimating the number of reactive centers presents a challenging problem. In the present study state-of-the-art experimental techniques involving ultra high resolution SEM/STEM microscopy (1 Å resolution), high brilliance X-ray absorption spectroscopy and theoretical calculations on truly nanoscale systems were utilized to reveal the role of carbon centers in the formation and nature of Pd/C catalytic materials. Generation of Pd clusters in solution from the easily available Pd2dba3 precursor and the unique reactivity of the Pd clusters opened an excellent opportunity to develop an efficient procedure for the imaging of a carbon surface. Defect sites and reactivity centers of a carbon surface were mapped in three-dimensional space with high resolution and excellent contrast using a user-friendly nanoscale imaging procedure. The proposed imaging approach takes advantage of the specific interactions of reactive carbon centers with Pd clusters, which allows spatial information about chemical reactivity across the Pd/C system to be obtained using a microscopy technique. Mapping the reactivity centers with Pd markers provided unique information about the reactivity of the graphene layers and showed that >2000 reactive centers can be located per 1 μm2 of the surface area of the carbon material. A computational study at a PBE-D3-GPW level differentiated the relative affinity of the Pd2 species to the reactive centers of graphene. These findings emphasized the spatial complexity of the carbon material at the nanoscale and indicated the importance of the surface defect nature, which exhibited substantial gradients and variations across the surface area. The findings show the crucial role of the structure of the carbon support, which governs the formation of Pd/C systems and their catalytic activity.
Starting Page	3302
Ending Page	3313
Page Count	12
File Format	HTM / HTML PDF
ISSN	20416520
Volume Number	6
Issue Number	6
Journal	Chemical Science
DOI	10.1039/c5sc00802f
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Subscribed
Subject Keyword	Spectroscopy Microscopy Graphene X-ray absorption spectroscopy Scanning transmission electron microscopy Carbon
Content Type	Text
Resource Type	Article
Subject	Chemistry

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