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Title: Dual reactor for in situ/operando fluorescent mode XAS studies of sample containing low-concentration 3d or 5d metal elements

Abstract

Transition metal elements are the most important elements of heterogeneous catalysts used for chemical and energy transformations. Many of these catalysts are active at a temperature higher than 400 °C. For a catalyst containing a 3d or 5d metal element with a low concentration, typically their released fluorescence upon the K-edge or L-edge adsorption of X-rays is collected for the analysis of chemical and coordination environments of these elements. However, it is challenging to perform in situ/operando X-ray absorption spectroscopy (XAS) studies of elements of low-energy absorption edges at a low concentration in a catalyst during catalysis at a temperature higher than about 450 °C. Here a unique reaction system consisting two reactors, called a dual reactor system, was designed for performing in situ or operando XAS studies of these elements of low-energy absorption edges in a catalyst at a low concentration during catalysis at a temperature higher than 450 °C in a fluorescent mode. This dual-reactor system contains a quartz reactor for preforming high-temperature catalysis up to 950 °C and a Kapton reactor remaining at a temperature up to 450 °C for collecting data in the same gas of catalysis. With this dual reactor, chemical and coordination environments ofmore » low-concentration metal elements with low-energy absorption edges such as the K-edge of 3d metals including Ti, V, Cr, Mn, Fe, Co, Ni, and Cu and L edge of 5d metals including W, Re, Os, Ir, Pt, and Au can be examined through first performing catalysis at a temperature higher than 450 °C in the quartz reactor and then immediately flipping the catalyst in the same gas flow to the Kapton reactor remained up to 450 °C to collect data. The capability of this dual reactor was demonstrated by tracking the Mn K-edge of the MnOx/Na2WO4 catalyst during activation in the temperature range of 300-900 °C and catalysis at 850 °C.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1]
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  1. Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemical and Petroleum Engineering. Dept. of Chemistry
Publication Date:
Research Org.:
Univ. of Kansas, Lawrence, KS (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1526016
Grant/Contract Number:  
SC0014561; OIA-1539105
Resource Type:
Accepted Manuscript
Journal Name:
Review of Scientific Instruments
Additional Journal Information:
Journal Volume: 89; Journal Issue: 5; Journal ID: ISSN 0034-6748
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
47 OTHER INSTRUMENTATION

Citation Formats

Nguyen, Luan, Tang, Yu, Li, Yuting, Zhang, Xiaoyan, Wang, Ding, and Tao, Franklin Feng. Dual reactor for in situ/operando fluorescent mode XAS studies of sample containing low-concentration 3d or 5d metal elements. United States: N. p., 2018. Web. doi:10.1063/1.5022738.
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Nguyen, Luan, Tang, Yu, Li, Yuting, Zhang, Xiaoyan, Wang, Ding, & Tao, Franklin Feng. Dual reactor for in situ/operando fluorescent mode XAS studies of sample containing low-concentration 3d or 5d metal elements. United States. https://doi.org/10.1063/1.5022738
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Nguyen, Luan, Tang, Yu, Li, Yuting, Zhang, Xiaoyan, Wang, Ding, and Tao, Franklin Feng. Fri . "Dual reactor for in situ/operando fluorescent mode XAS studies of sample containing low-concentration 3d or 5d metal elements". United States. https://doi.org/10.1063/1.5022738. https://www.osti.gov/servlets/purl/1526016.
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@article{osti_1526016,
title = {Dual reactor for in situ/operando fluorescent mode XAS studies of sample containing low-concentration 3d or 5d metal elements},
author = {Nguyen, Luan and Tang, Yu and Li, Yuting and Zhang, Xiaoyan and Wang, Ding and Tao, Franklin Feng},
abstractNote = {Transition metal elements are the most important elements of heterogeneous catalysts used for chemical and energy transformations. Many of these catalysts are active at a temperature higher than 400 °C. For a catalyst containing a 3d or 5d metal element with a low concentration, typically their released fluorescence upon the K-edge or L-edge adsorption of X-rays is collected for the analysis of chemical and coordination environments of these elements. However, it is challenging to perform in situ/operando X-ray absorption spectroscopy (XAS) studies of elements of low-energy absorption edges at a low concentration in a catalyst during catalysis at a temperature higher than about 450 °C. Here a unique reaction system consisting two reactors, called a dual reactor system, was designed for performing in situ or operando XAS studies of these elements of low-energy absorption edges in a catalyst at a low concentration during catalysis at a temperature higher than 450 °C in a fluorescent mode. This dual-reactor system contains a quartz reactor for preforming high-temperature catalysis up to 950 °C and a Kapton reactor remaining at a temperature up to 450 °C for collecting data in the same gas of catalysis. With this dual reactor, chemical and coordination environments of low-concentration metal elements with low-energy absorption edges such as the K-edge of 3d metals including Ti, V, Cr, Mn, Fe, Co, Ni, and Cu and L edge of 5d metals including W, Re, Os, Ir, Pt, and Au can be examined through first performing catalysis at a temperature higher than 450 °C in the quartz reactor and then immediately flipping the catalyst in the same gas flow to the Kapton reactor remained up to 450 °C to collect data. The capability of this dual reactor was demonstrated by tracking the Mn K-edge of the MnOx/Na2WO4 catalyst during activation in the temperature range of 300-900 °C and catalysis at 850 °C.},
doi = {10.1063/1.5022738},
journal = {Review of Scientific Instruments},
number = 5,
volume = 89,
place = {United States},
year = {Fri May 25 00:00:00 EDT 2018},
month = {Fri May 25 00:00:00 EDT 2018}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1063/1.5022738
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Cited by: 8 works
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Figures / Tables:

FIG. 1 FIG. 1: Quantified absorption of the X-ray with energy 1 keV-100 keV by three common tube materials including Kapton, quartz, and h-BN. (a) Mass attenuation coefficient as a function of X-ray energy for Kapton, quartz, and h-BN. (b) Transmission of Kapton with a thickness of 0.076 mm, quartz with amore » thickness of 0.2 mm, and h-BN with a thickness of 1 mm for X-rays with an energy of 1 keV-100 keV. (c) Absorbance (%) of Kapton with a thickness of 0.076 mm, quartz with a thickness of 0.2 mm, and h-BN with a thickness of 1 mm for X-rays with an energy of 1 keV-100 keV. (d) List of low-energy K-edges of 3d metal elements and L3-edges of some 5d metal elements.« less
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