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Synergized catalysis of La and Ce on Fe2O3 Al2O3 for intensive CO2 utilization via chemical-looping based CO2/CH4 reforming.

Record Type:	Language materials, manuscript : Monograph/item
Title/Author:	Synergized catalysis of La and Ce on Fe2O3 Al2O3 for intensive CO2 utilization via chemical-looping based CO2/CH4 reforming./
Author:	Tang, Mingchen.
Description:	1 online resource (85 pages)
Notes:	Source: Dissertation Abstracts International, Volume: 78-12(E), Section: B.
Contained By:	Dissertation Abstracts International78-12B(E).
Subject:	Chemical engineering. -
Online resource:	click for full text (PQDT)
ISBN:	9780355096170

Synergized catalysis of La and Ce on Fe2O3 Al2O3 for intensive CO2 utilization via chemical-looping based CO2/CH4 reforming.
Tang, Mingchen.

Synergized catalysis of La and Ce on Fe2O3 Al2O3 for intensive CO2 utilization via chemical-looping based CO2/CH4 reforming. - 1 online resource (85 pages)

Source: Dissertation Abstracts International, Volume: 78-12(E), Section: B.

Thesis (Ph.D.)

Includes bibliographical references

This dissertation comprehensively compiles the latest major milestones for chemical-looping reforming of CH4 (CLR) terminology, which breaks down the conventional CH4 reforming reactions into two separate half-steps, namely CH4 oxidation and regeneration of oxygen carrier (OC) using oxidizing agents (i.e., steam, CO2, O2). Chemical-looping based CO2/CH4 reforming (CLDR) paves a novel route for syngas production, which essentially allows effective CO2 utilization. However, the adoption of CO2 with much weaker oxidization ability, in place of commonly used steam and O2 for OC replenishment, sets more stringent screening criteria for OC material. In the present contribution, LaxCe1-xFeO3 Al2O3 (x = 0, 0.33, 0.67, and 1) OCs were synthesized to investigate the synergistic promoting effect of La and Ce on the performance of Fe2O3 Al2O3 for cyclic CLDR operation. The physical and chemical properties of the prepared OCs were characterized by using N2-physisorption, H2-chemisorption, H2-TPR, CH4-TPO, CO2-TPO, XRD, XPS, and DRIFT. The experimental results revealed the evolution CeFeO3 and LaFeO3 is beneficial for the lattice oxygen mobility, contributing to the significantly enhanced OC selectivity toward partial oxidation of CH4 (POM) and OC reactivity toward CO2 splitting (CS). It was also found the CeO2-decoration gives rise to the surface dispersion of active Fe species but higher CeO2 loading may have adverse effect due to the agglomeration. Moreover, the coexistence of CeO2 and LaFeO3 induces the evolution of Ce3+ and Fe2+, at the interface of which additional oxygen vacancies build up to further improve the OC mobility. In addition, it was highlighted CH4-pyrolysis derived carbon deposition has negligible deteriorative influence on the CLDR cyclability of LaxCe1-xFeO3 Al2O3, and the efficient removal of deposited carbon by CO2 contributes to the additional CO formation which allows a steady syngas production with H2/CO ratio close to unity. In these regards, our findings demonstrate the potential of utilizing LaxCe1-xFeO3 Al2O3 as a promising OC candidate for CLDR process.

Electronic reproduction.
Ann Arbor, Mich. :
ProQuest,
2018

Mode of access: World Wide Web

ISBN: 9780355096170Subjects--Topical Terms:

555952
Chemical engineering.
Index Terms--Genre/Form:

554714
Electronic books.

Synergized catalysis of La and Ce on Fe2O3 Al2O3 for intensive CO2 utilization via chemical-looping based CO2/CH4 reforming.
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245 1 0 $a Synergized catalysis of La and Ce on Fe2O3 Al2O3 for intensive CO2 utilization via chemical-looping based CO2/CH4 reforming.
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300 $a 1 online resource (85 pages)
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500 $a Source: Dissertation Abstracts International, Volume: 78-12(E), Section: B.
500 $a Advisers: Maohong Fan; Dean M. Roddick.
502 $a Thesis (Ph.D.) $c University of Wyoming $d 2017.
504 $a Includes bibliographical references
520 $a This dissertation comprehensively compiles the latest major milestones for chemical-looping reforming of CH4 (CLR) terminology, which breaks down the conventional CH4 reforming reactions into two separate half-steps, namely CH4 oxidation and regeneration of oxygen carrier (OC) using oxidizing agents (i.e., steam, CO2, O2). Chemical-looping based CO2/CH4 reforming (CLDR) paves a novel route for syngas production, which essentially allows effective CO2 utilization. However, the adoption of CO2 with much weaker oxidization ability, in place of commonly used steam and O2 for OC replenishment, sets more stringent screening criteria for OC material. In the present contribution, LaxCe1-xFeO3 Al2O3 (x = 0, 0.33, 0.67, and 1) OCs were synthesized to investigate the synergistic promoting effect of La and Ce on the performance of Fe2O3 Al2O3 for cyclic CLDR operation. The physical and chemical properties of the prepared OCs were characterized by using N2-physisorption, H2-chemisorption, H2-TPR, CH4-TPO, CO2-TPO, XRD, XPS, and DRIFT. The experimental results revealed the evolution CeFeO3 and LaFeO3 is beneficial for the lattice oxygen mobility, contributing to the significantly enhanced OC selectivity toward partial oxidation of CH4 (POM) and OC reactivity toward CO2 splitting (CS). It was also found the CeO2-decoration gives rise to the surface dispersion of active Fe species but higher CeO2 loading may have adverse effect due to the agglomeration. Moreover, the coexistence of CeO2 and LaFeO3 induces the evolution of Ce3+ and Fe2+, at the interface of which additional oxygen vacancies build up to further improve the OC mobility. In addition, it was highlighted CH4-pyrolysis derived carbon deposition has negligible deteriorative influence on the CLDR cyclability of LaxCe1-xFeO3 Al2O3, and the efficient removal of deposited carbon by CO2 contributes to the additional CO formation which allows a steady syngas production with H2/CO ratio close to unity. In these regards, our findings demonstrate the potential of utilizing LaxCe1-xFeO3 Al2O3 as a promising OC candidate for CLDR process.
533 $a Electronic reproduction. $b Ann Arbor, Mich. : $c ProQuest, $d 2018
538 $a Mode of access: World Wide Web
650 4 $a Chemical engineering. $3 555952
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