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First-Principles-Based Kinetic Modeling of Bronsted and Lewis Acidic Zeolites for the Catalytic Conversion of Furans to Aromatics.

Record Type:	Language materials, manuscript : Monograph/item
Title/Author:	First-Principles-Based Kinetic Modeling of Bronsted and Lewis Acidic Zeolites for the Catalytic Conversion of Furans to Aromatics./
Author:	Patet, Ryan E.
Description:	1 online resource (252 pages)
Notes:	Source: Dissertation Abstracts International, Volume: 79-03(E), Section: B.
Contained By:	Dissertation Abstracts International79-03B(E).
Subject:	Chemical engineering. -
Online resource:	click for full text (PQDT)
ISBN:	9780355466058

First-Principles-Based Kinetic Modeling of Bronsted and Lewis Acidic Zeolites for the Catalytic Conversion of Furans to Aromatics.
Patet, Ryan E.

First-Principles-Based Kinetic Modeling of Bronsted and Lewis Acidic Zeolites for the Catalytic Conversion of Furans to Aromatics. - 1 online resource (252 pages)

Source: Dissertation Abstracts International, Volume: 79-03(E), Section: B.

Thesis (Ph.D.)

Includes bibliographical references

Polyethylene terephthalate (PET) plastics and fibers are produced through the reaction of terephthalic acid with monoethylene glycol. Current renewable PET products can only claim to be 30% renewable, as the terephthalic acid which makes up ca. 70% of its structure is still derived from petroleum sources. In order to achieve 100% bio-derived PET materials, a renewable route to terephthalic acid is needed. The discovery that biomass-derived furans and ethylene react to form aromatics over solid acid zeolites has provided a potential pathway for the renewable production of terephthalic acid.

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

Mode of access: World Wide Web

ISBN: 9780355466058Subjects--Topical Terms:

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

554714
Electronic books.

First-Principles-Based Kinetic Modeling of Bronsted and Lewis Acidic Zeolites for the Catalytic Conversion of Furans to Aromatics.
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245 1 0 $a First-Principles-Based Kinetic Modeling of Bronsted and Lewis Acidic Zeolites for the Catalytic Conversion of Furans to Aromatics.
264 0 $c 2017
300 $a 1 online resource (252 pages)
336 $a text $b txt $2 rdacontent
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500 $a Source: Dissertation Abstracts International, Volume: 79-03(E), Section: B.
500 $a Advisers: Dionisios G. Vlachos; Stavros Caratzoulas.
502 $a Thesis (Ph.D.) $c University of Delaware $d 2017.
504 $a Includes bibliographical references
520 $a Polyethylene terephthalate (PET) plastics and fibers are produced through the reaction of terephthalic acid with monoethylene glycol. Current renewable PET products can only claim to be 30% renewable, as the terephthalic acid which makes up ca. 70% of its structure is still derived from petroleum sources. In order to achieve 100% bio-derived PET materials, a renewable route to terephthalic acid is needed. The discovery that biomass-derived furans and ethylene react to form aromatics over solid acid zeolites has provided a potential pathway for the renewable production of terephthalic acid.
520 $a Computational studies of this system revealed a tandem reaction scheme, whereby furans and ethylene undergo a concerted Diels-Alder cycloaddition to form an oxanorbornene intermediate, which successively dehydrates to an aromatic. The role of Bronsted acidic zeolites has been shown, through first-principles density functional theory (DFT) calculations, to be on the dehydration reaction of the tandem scheme.
520 $a Direct comparisons between these DFT calculations and experimental observations have remained a challenge, due to the complicated nature of these systems, however. Experimentally, interesting behaviors were observed, whereby adding catalyst to the reactor caused an increase in aromatic production rate at low catalyst loadings, but had no effect on the rate at high catalyst loadings. Additionally, studies extended beyond well-understood Bronsted acidic zeolites to framework-substituted Lewis acid zeolites demonstrated this same behavior.
520 $a In this dissertation, DFT calculations are connected to experimental observations through the parameterization of microkinetic models of the reactor systems. A systematic approach is taken to create combined quantum mechanical, molecular mechanical model of zeolite active sites and the surrounding pore, which significantly improves the accuracy of adsorbate interactions with zeolites, without significantly increasing the computational costs. These improved zeolite models are used to parameterize microkinetic models of Bronsted acidic zeolites, providing fundamental explanations for the aforementioned experimental observations, but also to investigate the fundamental role of Bronsted acid strength in reactivity of these materials.
520 $a A study of Sn, Ti, and Zr, framework-substituted zeolites provides insights into the role of the active site of these materials for the aromatization of furans. The ability to isolate elementary reaction steps computationally is used to investigate the effects of Lewis and Bronsted acid sites in these materials on the Diels-Alder cycloaddition and dehydration reactions separately. Their overall contributions to furan aromatization are also examined. Finally, framework-substituted, Zn-containing zeolites are studied for their ability to catalyze the aromatization of oxygenated furans. Little is known about the active site in these materials, and so possible structures are explored for their intrinsic properties and their effect on reactivity.
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
655 7 $a Electronic books. $2 local $3 554714
690 $a 0542
710 2 $a ProQuest Information and Learning Co. $3 1178819
710 2 $a University of Delaware. $b Chemical Engineering. $3 1182261
773 0 $t Dissertation Abstracts International $g 79-03B(E).
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=10607385 $z click for full text (PQDT)