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Studies of Heterogeneous Catalyst Se...
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O'Neill, Brandon J.
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Studies of Heterogeneous Catalyst Selectivity and Stability for Biorefining Applications.
紀錄類型:
書目-電子資源 : Monograph/item
正題名/作者:
Studies of Heterogeneous Catalyst Selectivity and Stability for Biorefining Applications./
作者:
O'Neill, Brandon J.
面頁冊數:
203 p.
附註:
Source: Dissertation Abstracts International, Volume: 76-03(E), Section: B.
Contained By:
Dissertation Abstracts International76-03B(E).
標題:
Chemical engineering. -
電子資源:
http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3645900
ISBN:
9781321353198
Studies of Heterogeneous Catalyst Selectivity and Stability for Biorefining Applications.
O'Neill, Brandon J.
Studies of Heterogeneous Catalyst Selectivity and Stability for Biorefining Applications.
- 203 p.
Source: Dissertation Abstracts International, Volume: 76-03(E), Section: B.
Thesis (Ph.D.)--The University of Wisconsin - Madison, 2014.
This item must not be sold to any third party vendors.
The conversion of raw resources into value-added end products has long underlain the importance of catalysts in economic and scientific development. In particular, the development of selective and stable heterogeneous catalysts is a challenge that continues to grow in importance as environmental, sociological, and economic concerns have motivated an interest in sustainability and the use of renewable raw materials. Within this context, biomass has been identified as the only realistic source of renewable carbon for the foreseeable future. The development of processes to utilize biomass feedstocks will require breakthroughs in fundamental understanding and practical solutions to the challenges related to selectivity and stability of the catalysts employed.
ISBN: 9781321353198Subjects--Topical Terms:
560457
Chemical engineering.
Studies of Heterogeneous Catalyst Selectivity and Stability for Biorefining Applications.
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The conversion of raw resources into value-added end products has long underlain the importance of catalysts in economic and scientific development. In particular, the development of selective and stable heterogeneous catalysts is a challenge that continues to grow in importance as environmental, sociological, and economic concerns have motivated an interest in sustainability and the use of renewable raw materials. Within this context, biomass has been identified as the only realistic source of renewable carbon for the foreseeable future. The development of processes to utilize biomass feedstocks will require breakthroughs in fundamental understanding and practical solutions to the challenges related to selectivity and stability of the catalysts employed.
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Selectivity is addressed on multiple fronts. First, the selectivity for C-O bond scission reactions of a bifunctional, bimetallic RhRe/C catalyst is investigated. Using multiple techniques, the origin of Bronsted acidity in the catalyst and the role of pretreatment on the activity, selectivity, and stability are explored. In addition, reaction kinetics experiments and kinetic modeling are utilized to understand the role of chemical functional group (i.e. carboxylic acid versus formate ester) in determining the decarbonylation versus decarboxylation selectivity over a Pd/C catalyst. Finally, kinetic studies over Pd/C and Cu/gamma-Al2O3 were performed so that that may be paired with density functional theory calculations and microkinetic modeling to elucidate the elementary reaction mechanism, identify the active site, and provide a basis for future rational catalyst design.
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Next, the issue of catalyst stability, important in the high-temperature, liquid-phase conditions of biomass processing, is examined, and a method for stabilizing the base-metal nanoparticles of a Cu/gamma-Al2O 3 catalyst using atomic layer deposition (ALD) is developed. This advancement may facilitate the development of biorefining by enabling the replacement of precious-metal catalysts (e.g. Pd, Pt, etc.) with less expensive, but previously unstable, base-metal catalysts. Using myriad techniques, the mechanisms of catalyst deactivation and stabilization of the nanoparticles by the ALD overcoat are elucidated. Finally, the use of ALD unlocks the potential for novel catalysts architectures, and the ability to physically and chemically tune the properties of the overcoat is examined with the goals of reducing catalyst deactivation and introducing bifunctional activity.
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