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Visualizing electronic interactions between iron and carbon by X-ray chemical imaging and spectroscopy
Authors:Xiaoqi Chen  Jianping Xiao  Jian Wang  Dehui Deng  Yongfeng Hu  Jigang Zhou  Liang Yu  Thomas Heine  Xiulian Pan  Xinhe Bao
Institution:a State Key Laboratory of Catalysis , iChEM , Dalian Institute of Chemical Physics , Chinese Academy of Sciences , Zhongshan Road 457 , Dalian , 116023 , China . Email: ; Email: ; Fax: +86-411-84379128 ; Tel: +86-411-84686637 ;b Canadian Light Source Inc. , University of Saskatchewan , 44 Innovation Boulevard , Saskatoon , SK S7N 2V3 , Canada ;c Department of Physics and Earth Science , Jacobs University Bremen , Campus Ring 1 , 28759 Bremen , Germany
Abstract:The electronic interaction of a catalyst and its support is of vital importance to its catalytic performance. However, it is still a great challenge to directly probe the interaction due to the lack of well-defined models and efficient technical means. In this study, we report that pod-like carbon nanotubes with encapsulated iron particles (Pod-Fe) and scanning transmission X-ray microscopy (STXM) can be used as an ideal model and technique to study the electronic interaction between carbon shells and iron particles. The chemical imaging and spectroscopy of Pod-Fe by STXM show that the local electronic structures at C K-edge near edge (π*) of carbon shells can be significantly modified by the encapsulated iron particles, which promotes the adsorption of oxygen-containing species, and thereby further modifies the electronic structure (π* and σ*) of the carbon shells. Moreover, computed X-ray absorption near edge structure spectra (XANES) confirmed the electronic modifications of carbon shells by the encapsulated iron particles. The present study provides a direct evidence of electronic interactions with simultaneously collected images and spectra, which can promote the understanding towards the nature of active sites and supports.
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