NDLI: Designing green oxidation catalysts for purifying environmental waters

Content Provider	PubMed Central
Author	Ellis, W. Chadwick Tran, Camly T. Roy, Riddhi Rusten, Marte Fischer, Andreas Ryabov, Alexander D. Blumberg, Bruce Collins, Terrence J.
Abstract	We describe the synthesis, characterization, aqueous behavior, and catalytic activity of a new generation of FeIII-TAML (TetraAmido Macrocycle Ligand) activators of peroxides (2), variants of (2d), which have been designed to be especially suitable for purifying water of recalcitrant oxidizable pollutants. Activation of H2O2 by 2 (k I) as a function of pH was analyzed via kinetic studies of Orange II bleaching. This was compared with the known behavior of the first generation of FeIII-TAMLs (1). Novel reactivity features impact the potential for oxidant activation for water purification by 2d and its aromatic ring substituted dinitro (2e) and tetrachloro (2f) derivatives. Thus, the maximum activity for 2e occurs at pH 9, the closest yet to the EPA guidelines for drinking water (6.5–8.5) allowing 2e to rapidly activate H2O2 at pH 7.7. In water, 2e has two axial water ligands with pK as of 8.4 and 10.0 (25 °C). The former is the lowest for all FeIII-TAMLs developed to date and is key to 2e’s exceptional catalytic activity in neutral and slightly basic solutions. Below pH 7 2d was found to be quite sensitive to demetalation in phosphate buffers. This was overcome by iterative design to give 2e (hydrolysis rate 2d > 100×2e). Mechanistic studies highlight 2e’s increased stability by establishing that to demetalate 2e at a comparable rate to which H2PO4 − demetalates 2d, H3PO4 is required. A critical criterion for green catalysts for water purification is the avoidance of endocrine disruptors, which can impair aquatic life. FeIII-TAMLs do not alter transcription mediated by mammalian thyroid, androgen or estrogen hormone receptors, suggesting that 2 do not bind to the receptors and reducing concerns that the catalysts might have endocrine disrupting activity.
Related Links	http://dx.doi.org/10.1021/ja102524v
Ending Page	9781
Page Count	8
Starting Page	9774
File Format	PDF
ISSN	00027863
e-ISSN	15205126
Journal	Journal of the American Chemical Society
Issue Number	28
Volume Number	132
Language	English
Publisher Date	2010-07-21
Access Restriction	Open
Subject Keyword	Colloid and Surface Chemistry Biochemistry Chemistry(all) Catalysis Research in Higher Education
Content Type	Text
Resource Type	Article
Subject	Chemistry Colloid and Surface Chemistry Biochemistry Catalysis

Sl.	Authority	Responsibilities	Communication Details
1	Ministry of Education (GoI), Department of Higher Education	Sanctioning Authority	https://www.education.gov.in/ict-initiatives
2	Indian Institute of Technology Kharagpur	Host Institute of the Project: The host institute of the project is responsible for providing infrastructure support and hosting the project	https://www.iitkgp.ac.in
3	National Digital Library of India Office, Indian Institute of Technology Kharagpur	The administrative and infrastructural headquarters of the project	Dr. B. Sutradhar bsutra@ndl.gov.in
4	Project PI / Joint PI	Principal Investigator and Joint Principal Investigators of the project	Dr. B. Sutradhar bsutra@ndl.gov.in Prof. Saswat Chakrabarti will be added soon
5	Website/Portal (Helpdesk)	Queries regarding NDLI and its services	support@ndl.gov.in
6	Contents and Copyright Issues	Queries related to content curation and copyright issues	content@ndl.gov.in
7	National Digital Library of India Club (NDLI Club)	Queries related to NDLI Club formation, support, user awareness program, seminar/symposium, collaboration, social media, promotion, and outreach	clubsupport@ndl.gov.in
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9	IDR Setup or Support	Queries related to establishment and support of Institutional Digital Repository (IDR) and IDR workshops	idr@ndl.gov.in

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