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New bifunctional catalysts for ammon...

Lu, Zhiyao.

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New bifunctional catalysts for ammonia-borane dehydrogenation, nitrile reduction, formic acid dehydrogenation, lactic acid synthesis, and carbon dioxide reduction.

Record Type:	Electronic resources : Monograph/item
Title/Author:	New bifunctional catalysts for ammonia-borane dehydrogenation, nitrile reduction, formic acid dehydrogenation, lactic acid synthesis, and carbon dioxide reduction./
Author:	Lu, Zhiyao.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2016,
Description:	394 p.
Notes:	Source: Dissertation Abstracts International, Volume: 78-04(E), Section: B.
Contained By:	Dissertation Abstracts International78-04B(E).
Subject:	Organic chemistry. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=10160146
ISBN:	9781369150643

New bifunctional catalysts for ammonia-borane dehydrogenation, nitrile reduction, formic acid dehydrogenation, lactic acid synthesis, and carbon dioxide reduction.
Lu, Zhiyao.

New bifunctional catalysts for ammonia-borane dehydrogenation, nitrile reduction, formic acid dehydrogenation, lactic acid synthesis, and carbon dioxide reduction. - Ann Arbor : ProQuest Dissertations & Theses, 2016 - 394 p.

Source: Dissertation Abstracts International, Volume: 78-04(E), Section: B.

Thesis (Ph.D.)--University of Southern California, 2016.

This thesis focuses on new catalytic chemistry of hydride manipulation for processes such as hydrogenation and dehydrogenation. The research projects mostly involve design and synthesis of novel catalysts as well as mechanistic analysis of catalytic processes. Such mechanistic understandings lead to improvement in catalysis in terms of efficiency, selectivity, and catalyst longevity. These are introduced in Chapter one.

ISBN: 9781369150643Subjects--Topical Terms:

523952
Organic chemistry.

New bifunctional catalysts for ammonia-borane dehydrogenation, nitrile reduction, formic acid dehydrogenation, lactic acid synthesis, and carbon dioxide reduction.
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020 $a 9781369150643
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100 1 $a Lu, Zhiyao. $3 3281108
245 1 0 $a New bifunctional catalysts for ammonia-borane dehydrogenation, nitrile reduction, formic acid dehydrogenation, lactic acid synthesis, and carbon dioxide reduction.
260 1 $a Ann Arbor : $b ProQuest Dissertations & Theses, $c 2016
300 $a 394 p.
500 $a Source: Dissertation Abstracts International, Volume: 78-04(E), Section: B.
500 $a Adviser: Travis J. Williams.
502 $a Thesis (Ph.D.)--University of Southern California, 2016.
520 $a This thesis focuses on new catalytic chemistry of hydride manipulation for processes such as hydrogenation and dehydrogenation. The research projects mostly involve design and synthesis of novel catalysts as well as mechanistic analysis of catalytic processes. Such mechanistic understandings lead to improvement in catalysis in terms of efficiency, selectivity, and catalyst longevity. These are introduced in Chapter one.
520 $a Chapter two proposes and provides evidence for a mechanistic model for three-stage dehydrogenation of ammonia--borane (AB) catalyzed by Shvo's cyclopentadienone-ligated ruthenium complex. In particular, we characterized the mechanism of catalyst deactivation: a borazine-mediated hydroboration of the active catalyst to afford less reactive ruthenium species. We are inspired by these findings to discover catalysts that do not suffer from the same deactivation chemistry So doing, we either use a "semi-site protection strategy" or introduce a borate ligand into the catalyst.
520 $a Chapter three shows complex {[(kappa3-(N,N,O )-py2B(Me)OH)Ru(NCMe)3]}+ TfO -- is not a ligand-metal bifunctional catalyst and in case of alcohol oxidation, the mechanism most likely involves reactivity only at the ruthenium center. Further we present a novel ruthenium bis(pyrazolyl)borate scaffold that enables cooperative reactivity in which boron and ruthenium centers work in concert to effect selective nitrile reduction. The pre-catalyst compound {[kappa3-(1-pz)2HB(N=CHCH3)]Ru(cymene)} + TfO-- (pz = pyrazolyl) was synthesized using readily-available materials through a straightforward route, thus making it an appealing catalyst for a number of reactions.
520 $a In chapter four, a prolific homogeneous iridium catalyst is introduced for selective dehydrogenation of neat formic acid under mild conditions. Mechanistic study on this catalysis reveals that the promising reactivity is enabled by in situ formation of a novel dimeric iridium species {[(P-N)Ir(CH2Cl 2)(H)]2(mu-H)(mu2-OCHO)2} + TfO--.
520 $a Chapter five describes the synthesis and reactivity of a very robust iridium catalyst for glycerol to lactate conversion. The high reactivity and selectivity of this catalyst enable a sequence for the conversion of biodiesel waste stream to lactide monomers for the preparation of poly(lactic acid). Furthermore, experimental data collected with this system provide a general understanding of its reactive mechanism.
520 $a Chapter six recounts the design and synthesis of structurally novel di(carbene)-supported nickel species, which are efficient catalysts for the room-temperature reduction of CO2 to methanol in the presence of sodium borohydride. The catalysts feature unprecedented stability, particularly for a base metal catalyst, enabling > 1,100,000 turnovers of CO2. Moreover, while other systems involve more expensive or air-sensitive borane reagents, sodium borohydride is inexpensive and easily handled. Further, effecting reduction in the presence of water enables direct access to methanol without a subsequent hydrolysis step. Preliminary mechanistic data collected for the catalysis are most consistent with a mononuclear nickel active species that mediates rate-determining reduction of a boron formate.
590 $a School code: 0208.
650 4 $a Organic chemistry. $3 523952
650 4 $a Inorganic chemistry. $3 3173556
690 $a 0490
690 $a 0488
710 2 $a University of Southern California. $b Chemistry. $3 1022232
773 0 $t Dissertation Abstracts International $g 78-04B(E).
790 $a 0208
791 $a Ph.D.
792 $a 2016
793 $a English
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=10160146