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Noble Metal Heterogeneous Catalysts ...

Mannel, David S.

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Noble Metal Heterogeneous Catalysts for Aerobic Alcohol Oxidation: Discovery and Mechanism.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Noble Metal Heterogeneous Catalysts for Aerobic Alcohol Oxidation: Discovery and Mechanism./
Author:	Mannel, David S.
Description:	265 p.
Notes:	Source: Dissertation Abstracts International, Volume: 76-07(E), Section: B.
Contained By:	Dissertation Abstracts International76-07B(E).
Subject:	Chemical engineering. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3685067
ISBN:	9781321606515

Noble Metal Heterogeneous Catalysts for Aerobic Alcohol Oxidation: Discovery and Mechanism.
Mannel, David S.

Noble Metal Heterogeneous Catalysts for Aerobic Alcohol Oxidation: Discovery and Mechanism. - 265 p.

Source: Dissertation Abstracts International, Volume: 76-07(E), Section: B.

Thesis (Ph.D.)--The University of Wisconsin - Madison, 2015.

This item must not be sold to any third party vendors.

Transformation of hydrocarbon feedstocks to complex molecules found in the fine chemical, agro chemical, and pharmaceutical industries require selective oxidations to impart the desired functionality. Oxidation of alcohols is commonly done employing harsh and potentially hazardous oxidants with stoichiometric amounts of byproducts being produced. The use of O2 as the terminal oxidant provides a safe and environmentally benign alternative with selectivity control being realized through the use of a catalyst.

ISBN: 9781321606515Subjects--Topical Terms:

560457
Chemical engineering.

Noble Metal Heterogeneous Catalysts for Aerobic Alcohol Oxidation: Discovery and Mechanism.
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100 1 $a Mannel, David S. $3 3178433
245 1 0 $a Noble Metal Heterogeneous Catalysts for Aerobic Alcohol Oxidation: Discovery and Mechanism.
300 $a 265 p.
500 $a Source: Dissertation Abstracts International, Volume: 76-07(E), Section: B.
500 $a Advisers: Thatcher W. Root; Shannon S. Stahl.
502 $a Thesis (Ph.D.)--The University of Wisconsin - Madison, 2015.
506 $a This item must not be sold to any third party vendors.
520 $a Transformation of hydrocarbon feedstocks to complex molecules found in the fine chemical, agro chemical, and pharmaceutical industries require selective oxidations to impart the desired functionality. Oxidation of alcohols is commonly done employing harsh and potentially hazardous oxidants with stoichiometric amounts of byproducts being produced. The use of O2 as the terminal oxidant provides a safe and environmentally benign alternative with selectivity control being realized through the use of a catalyst.
520 $a The use of a Ru(OH)x/Al2O3 catalyst for the oxidation of alcohols to aldehydes or ketones was studied for applicability and scalability in a continuous process. The catalyst was found to undergo rapid deactivation in the first 50-100 turnovers. High yields of diverse aldehydes and ketones were realized in the continuous process over the deactivated Ru(OH) x/Al2O3 catalyst.
520 $a The discovery of a new heterogeneous catalyst was accomplished through rapid admixture screening and optimization using design of experiment techniques. The optimized catalyst compositions of PdBi0.47Te0.09/C (PBT-1) and PdBi0.35Te0.23/C (PBT-2) were found to be very active and selective for the aerobic oxidation of 1-octanol to methyl octanoate. These optimized catalysts show high yields of many diverse methyl esters from the oxidation of alcohols, and their stability was demonstrated in a continuous process achieving nearly 60,000 turnovers with no apparent loss in activity. The role of the Bi and Te promoters and mechanism of the PBT-2 catalyst was explored through kinetic studies and characterization of the catalyst. Through the use of kinetics and other mechanistic probes we discovered that the reaction shows saturation dependence in [substrate] and [K2CO3] and is first order in pO2, supporting a Langmuir-Hinshelwood mechanism with the reaction occurring between alkoxide and O2 adsorbed to the catalyst. The promoters are proposed to protect the Pd catalyst from over oxidation to inactive PdOx species as well as prevent side reactions (Bi) and electronically modify the Pd (Te).
520 $a Oxidation of alcohols to aldehydes or nitriles was demonstrated in a continuous process using a CuI/TEMPO catalyst. The oxidation to the nitrile was accomplished through the addition of anhydrous ammonia, and excellent yields were observed from the oxidation of diverse primary benzylic alcohols.
590 $a School code: 0262.
650 4 $a Chemical engineering. $3 560457
650 4 $a Organic chemistry. $3 523952
690 $a 0542
690 $a 0490
710 2 $a The University of Wisconsin - Madison. $b Chemical Engineering. $3 2094015
773 0 $t Dissertation Abstracts International $g 76-07B(E).
790 $a 0262
791 $a Ph.D.
792 $a 2015
793 $a English
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3685067