Revealing Correlation of Valence State with Nanoporous Structure in Cobalt Catalyst Nanoparticles by In Situ Environmental TEM

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• 作者：Huolin L. Xin ; Elzbieta A. Pach ; Rosa E. Diaz ; Eric A. Stach ; Miquel Salmeron ; Haimei Zheng
• 刊名：ACS Nano
• 出版年：2012
• 出版时间：May 22, 2012
• 年：2012
• 卷：6
• 期：5
• 页码：4241-4247
• 全文大小：543K
• 年卷期：v.6,no.5(May 22, 2012)
• ISSN：1936-086X

文摘

Simultaneously probing the electronic structure and morphology of materials at the nanometer or atomic scale while a chemical reaction proceeds is significant for understanding the underlying reaction mechanisms and optimizing a materials design. This is especially important in the study of nanoparticle catalysts, yet such experiments have rarely been achieved. Utilizing an environmental transmission electron microscope equipped with a differentially pumped gas cell, we are able to conduct nanoscopic imaging and electron energy loss spectroscopy in situ for cobalt catalysts under reaction conditions. Studies reveal quantitative correlation of the cobalt valence states with the particles鈥?nanoporous structures. The in situ experiments were performed on nanoporous cobalt particles coated with silica, while a 15 mTorr hydrogen environment was maintained at various temperatures (300鈥?00 掳C). When the nanoporous particles were reduced, the valence state changed from cobalt oxide to metallic cobalt and concurrent structural coarsening was observed. In situ mapping of the valence state and the corresponding nanoporous structures allows quantitative analysis necessary for understanding and improving the mass activity and lifetime of cobalt-based catalysts, for example, for Fischer鈥揟ropsch synthesis that converts carbon monoxide and hydrogen into fuels, and uncovering the catalyst optimization mechanisms.

Keywords:

environmental TEM; in situ TEM; cobalt catalysts; porosity control; Fischer鈭扵ropsch synthesis