Quantification of rhenium oxide dispersion on zeolite: Effect of zeolite acidity and mesoporosity

Yiqing Wu; Scott Holdren; Yuan Zhang; Su Cheun Oh; Dat T. Tran; Laleh Emdadi; Zheng Lu; Mei Wang; Taylor J. Woehl; Michael Zachariah; Yu Lei; Dongxia Liu

doi:10.1016/j.jcat.2019.02.024

Quantification of rhenium oxide dispersion on zeolite: Effect of zeolite acidity and mesoporosity

Yiqing Wu
, Scott Holdren
, Yuan Zhang
, Su Cheun Oh
, Dat T. Tran
, Laleh Emdadi
, Zheng Lu
, Mei Wang
, Taylor J. Woehl
, Michael Zachariah
, Yu Lei
, Dongxia Liu

Surface Chemistry & Catalysis Group

Research output: Contribution to journal › Article › peer-review

24 Scopus citations

Abstract

The anchoring nature and spatial distribution of rhenium oxide (ReO_x) supported on zeolites (ReO_x/zeolite) were determined as a function of the support acidity and mesoporosity. The ReO_x/zeolite samples were characterized collectively using Argon isotherm, XRD, Raman, XAS, DRIFTS, and organic chemical titrations. The results show that the ReO_x species formed the isolated distorted tetrahedral ReO₄⁻ structure. On the zeolite support, ReO_x species anchored predominantly on Brønsted acid sites (Si-OH⁺-Al) enclosed in micropores (internal acid sites), by replacing the protons in Si-OH⁺-Al sites at a H⁺/Re ratio of ∼1.1 in zeolites with high acidity. The decrease in zeolite acidity led to the anchoring of ReO_x species onto both Si-OH⁺-Al and silanol group (Si-OH). The increase in zeolite mesoporosity migrated the ReO_x species onto both internal acid sites and those on the external surface and mesopores (external acid sites), as well as Si-OH groups. The implication of distribution of ReO_x in zeolite was explored by direct non-oxidative methane conversion reaction.

Original language	English
Pages (from-to)	128-141
Number of pages	14
Journal	Journal of Catalysis
Volume	372
DOIs	https://doi.org/10.1016/j.jcat.2019.02.024
State	Published - Apr 2019

Funding

The authors gratefully acknowledge financial support from the National Science Foundation (NSF-CBET 1264599 and 1351384 ). We acknowledge the support of Maryland NanoCenter and its NispLab . The NispLab is supported in part by the NSF as a MRSEC Shared Experimental Facility. Yiqing Wu thanks for the Hulka Energy Research Fellowship from University of Maryland Energy Research Center (UMERC) to support this research. Scott Holdren also thanks the GAANN Fellowship program for financial support. Zheng Lu and Yu Lei thank the support from the American Chemical Society Petroleum Research Fund ( ACS-PRF , 56197DNI5 ). MRCAT operations are supported by the Department of Energy and the MRCAT member institutions . This research used resources of the Advanced Photon Source, a U.S. Department of Energy ( DOE ) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract DEAC02-06CH11357 .

Keywords

2D lamellar zeolite
Brønsted acid site
DRIFTS
Raman spectra
Rhenium oxide
Silanol group
Spatial distribution

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10.1016/j.jcat.2019.02.024

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@article{9ccc9a75d9434977ab813d05daad83e0,

title = "Quantification of rhenium oxide dispersion on zeolite: Effect of zeolite acidity and mesoporosity",

abstract = "The anchoring nature and spatial distribution of rhenium oxide (ReOx) supported on zeolites (ReOx/zeolite) were determined as a function of the support acidity and mesoporosity. The ReOx/zeolite samples were characterized collectively using Argon isotherm, XRD, Raman, XAS, DRIFTS, and organic chemical titrations. The results show that the ReOx species formed the isolated distorted tetrahedral ReO4− structure. On the zeolite support, ReOx species anchored predominantly on Br{\o}nsted acid sites (Si-OH+-Al) enclosed in micropores (internal acid sites), by replacing the protons in Si-OH+-Al sites at a H+/Re ratio of ∼1.1 in zeolites with high acidity. The decrease in zeolite acidity led to the anchoring of ReOx species onto both Si-OH+-Al and silanol group (Si-OH). The increase in zeolite mesoporosity migrated the ReOx species onto both internal acid sites and those on the external surface and mesopores (external acid sites), as well as Si-OH groups. The implication of distribution of ReOx in zeolite was explored by direct non-oxidative methane conversion reaction.",

keywords = "2D lamellar zeolite, Br{\o}nsted acid site, DRIFTS, Raman spectra, Rhenium oxide, Silanol group, Spatial distribution",

author = "Yiqing Wu and Scott Holdren and Yuan Zhang and Oh, \{Su Cheun\} and Tran, \{Dat T.\} and Laleh Emdadi and Zheng Lu and Mei Wang and Woehl, \{Taylor J.\} and Michael Zachariah and Yu Lei and Dongxia Liu",

note = "Publisher Copyright: {\textcopyright} 2019 Elsevier Inc.",

year = "2019",

month = apr,

doi = "10.1016/j.jcat.2019.02.024",

language = "English",

volume = "372",

pages = "128--141",

journal = "Journal of Catalysis",

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T1 - Quantification of rhenium oxide dispersion on zeolite

T2 - Effect of zeolite acidity and mesoporosity

AU - Wu, Yiqing

AU - Holdren, Scott

AU - Zhang, Yuan

AU - Oh, Su Cheun

AU - Tran, Dat T.

AU - Emdadi, Laleh

AU - Lu, Zheng

AU - Wang, Mei

AU - Woehl, Taylor J.

AU - Zachariah, Michael

AU - Lei, Yu

AU - Liu, Dongxia

PY - 2019/4

Y1 - 2019/4

N2 - The anchoring nature and spatial distribution of rhenium oxide (ReOx) supported on zeolites (ReOx/zeolite) were determined as a function of the support acidity and mesoporosity. The ReOx/zeolite samples were characterized collectively using Argon isotherm, XRD, Raman, XAS, DRIFTS, and organic chemical titrations. The results show that the ReOx species formed the isolated distorted tetrahedral ReO4− structure. On the zeolite support, ReOx species anchored predominantly on Brønsted acid sites (Si-OH+-Al) enclosed in micropores (internal acid sites), by replacing the protons in Si-OH+-Al sites at a H+/Re ratio of ∼1.1 in zeolites with high acidity. The decrease in zeolite acidity led to the anchoring of ReOx species onto both Si-OH+-Al and silanol group (Si-OH). The increase in zeolite mesoporosity migrated the ReOx species onto both internal acid sites and those on the external surface and mesopores (external acid sites), as well as Si-OH groups. The implication of distribution of ReOx in zeolite was explored by direct non-oxidative methane conversion reaction.

AB - The anchoring nature and spatial distribution of rhenium oxide (ReOx) supported on zeolites (ReOx/zeolite) were determined as a function of the support acidity and mesoporosity. The ReOx/zeolite samples were characterized collectively using Argon isotherm, XRD, Raman, XAS, DRIFTS, and organic chemical titrations. The results show that the ReOx species formed the isolated distorted tetrahedral ReO4− structure. On the zeolite support, ReOx species anchored predominantly on Brønsted acid sites (Si-OH+-Al) enclosed in micropores (internal acid sites), by replacing the protons in Si-OH+-Al sites at a H+/Re ratio of ∼1.1 in zeolites with high acidity. The decrease in zeolite acidity led to the anchoring of ReOx species onto both Si-OH+-Al and silanol group (Si-OH). The increase in zeolite mesoporosity migrated the ReOx species onto both internal acid sites and those on the external surface and mesopores (external acid sites), as well as Si-OH groups. The implication of distribution of ReOx in zeolite was explored by direct non-oxidative methane conversion reaction.

KW - 2D lamellar zeolite

KW - Brønsted acid site

KW - DRIFTS

KW - Raman spectra

KW - Rhenium oxide

KW - Silanol group

KW - Spatial distribution

UR - https://www.scopus.com/pages/publications/85062676394

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DO - 10.1016/j.jcat.2019.02.024

M3 - Article

AN - SCOPUS:85062676394

SN - 0021-9517

VL - 372

SP - 128

EP - 141

JO - Journal of Catalysis

JF - Journal of Catalysis

ER -

Quantification of rhenium oxide dispersion on zeolite: Effect of zeolite acidity and mesoporosity

Abstract

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