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Green oxidation technologies for env...

Popescu, Delia-Laura.

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Green oxidation technologies for environmental applications: Degradation of persistent pollutants by iron-TAML-activated hydrogen peroxide and kinetic and mechanistic studies.

紀錄類型:	書目-語言資料,印刷品 : Monograph/item
正題名/作者:	Green oxidation technologies for environmental applications: Degradation of persistent pollutants by iron-TAML-activated hydrogen peroxide and kinetic and mechanistic studies./
作者:	Popescu, Delia-Laura.
面頁冊數:	195 p.
附註:	Adviser: Terrence J. Collins.
Contained By:	Dissertation Abstracts International68-09B.
標題:	Chemistry, Inorganic. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3281239
ISBN:	9780549226420

Green oxidation technologies for environmental applications: Degradation of persistent pollutants by iron-TAML-activated hydrogen peroxide and kinetic and mechanistic studies.
Popescu, Delia-Laura.

Green oxidation technologies for environmental applications: Degradation of persistent pollutants by iron-TAML-activated hydrogen peroxide and kinetic and mechanistic studies. - 195 p.

Adviser: Terrence J. Collins.

Thesis (Ph.D.)--Carnegie Mellon University, 2007.

Chapter I. Part A includes the motivation, objectives, achievements, and the outline of this dissertation. Part B provides a brief background on FeIII-TAML activators of hydrogen peroxide.

ISBN: 9780549226420Subjects--Topical Terms:

517253
Chemistry, Inorganic.

Green oxidation technologies for environmental applications: Degradation of persistent pollutants by iron-TAML-activated hydrogen peroxide and kinetic and mechanistic studies.
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100 1 $a Popescu, Delia-Laura. $3 1263778
245 1 0 $a Green oxidation technologies for environmental applications: Degradation of persistent pollutants by iron-TAML-activated hydrogen peroxide and kinetic and mechanistic studies.
300 $a 195 p.
500 $a Adviser: Terrence J. Collins.
500 $a Source: Dissertation Abstracts International, Volume: 68-09, Section: B, page: 5949.
502 $a Thesis (Ph.D.)--Carnegie Mellon University, 2007.
520 $a Chapter I. Part A includes the motivation, objectives, achievements, and the outline of this dissertation. Part B provides a brief background on FeIII-TAML activators of hydrogen peroxide.
520 $a Chapter II. The degradation of triclosan using the Fe III-TAML/H2O2 oxidizing system was investigated.
520 $a Chapter III. The development and application of an environmentally friendly approach to degrade fluoxetine at treatment plant relevant time scales and concentrations is presented. FeIII-TAML activated H 2O2 was used to break down fluoxetine. Final products of these reactions include small acids, such as maleic acid, methyl-maleic, formic acid, and oxalic acid. The degradation of alpha,alpha,alpha-trifluoro- p-cresol, the principal degradation product of fluoxetine detected under the employed conditions, was monitored.
520 $a Chapter IV. Oxidation of Orange II ([4-[(2-hydroxynaphtyl)azo]benzenesulfonic acid], sodium salt) by hydrogen peroxide catalyzed by iron(III) complexed to Tetra Amido Macrocyclic Ligands (FeIII-TAML activators) in aqueous solutions at pH 9-11 leads to CO2, CO, phthalic acid and smaller aliphatic carboxylic acids as major degradation products. The products are non-toxic according to the Daphnia magna test. Several organic intermediates have been identified. The catalytic oxidation can also be performed by organic oxidants such as benzoyl peroxide, tert-butyl and cumyl hydroperoxides. Kinetic studies of the catalyzed oxidation indicated that FeIII-TAML activators react first with ROOR' to form an oxidized catalyst (kI), which then oxidizes Orange II (kII). The rate constant k I equals (74+/-3)x103, (1.4+/-0.1) x10 3, 24+/-2, and 11+/-1 M-1 s-1 for benzoyl peroxide, H2O2, t-BuOOH, and cumyl hydroperoxide at pH 9 and 25°C, respectively. An average value of kII equals (3.1+/-0.9)x104 M-1 s-1 under the same conditions.
520 $a Chapter V. Stopped-flow kinetic studies of the oxidation of FeIII-TAML activators, a series of oxidation catalysts derived from TetraAmido Macrocycle Ligands, by H2O2 and tert-butyl hydroperoxide provide significant information for consolidating the mechanistic picture of the first step in the FeIII-TAML-catalyzed oxidations. The data collected for this usually rate-limiting step using a series of substituted FeIII-TAMLs at pH 6.0--13.8 and 15--45°C showed a first order dependency in both the catalyst and the oxidizing agent. Bell-shaped pH-profiles for the effective second-order rate constants, k I, have maxima in the pH range 10.5-12.5 depending on the nature of the FeIII-TAML activator and the hydroperoxide used. In the current favored mechanism, the "acidic" part is governed by the mono-deprotonation of the axial diaqua form of FeIII-TAMLs, [Fe(TAML)(H2 O2]-. Therefore, the attachment of electron-withdrawing groups at the "head" and the "tail" of the macrocyclic ligand broadens and moves the pH profile of the catalytic activity to the neutral region. An increase in the electrophilicity of FeIII-TAMLs does not enhance the rate constant kI, in which Fe(III) is oxidized to high-valent iron species during this step, suggesting a "binding"-oxidation model.
520 $a Chapter VI. Recent detailed mechanistic studies of Fe III-TAML activators of H2O2 and organic peroxides have outlined a clear-cut strategy for designing improved catalysts. The criteria applied to evaluate the performance of FeIII-TAML catalysts are: (i) hydrolytic stability, (ii) operational stability, (iii) speed of H2O2 and organic peroxide activation, and (iv) pH range of the highest activity. [Fe{1-NO2C6H3-3,4-(NCOCMe 2NCO)2CF2}(OH2)]-, ( 1a), has been synthesized and systematic kinetic studies as described in this chapter have demonstrated that it is the best performing Fe III-TAML activators produced so far.
520 $a Chapter VII. This study describes the first incorporation of transition metal ions into a PNA duplex. Substitution of a natural base pair by an artificial metal-coordinating base pair in a PNA duplex leads to duplex destabilization similar to that observed for a mismatch. Incorporation of metal ions into these modified PNAs leads to an increase in thermal stability of the duplexes. (Abstract shortened by UMI.)
590 $a School code: 0041.
650 4 $a Chemistry, Inorganic. $3 517253
650 4 $a Environmental Sciences. $3 676987
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710 2 $a Carnegie Mellon University. $3 1018096
773 0 $t Dissertation Abstracts International $g 68-09B.
790 $a 0041
790 1 0 $a Collins, Terrence J., $e advisor
791 $a Ph.D.
792 $a 2007
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