<p><span style="font-size: x-small;">Kinetics and mechanistic studies for the oxidation of N</span><span style="font-size: x-small;"><span style="font-size: xx-small;">-Benzylhydroxylamine by a Co</span><sup style="font-size: x-small;">III</sup><span style="font-size: xx-small;">-bound bridging superoxo complex in perchloric acid medium</span></span></p>
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Title Statement |
<p><span style="font-size: x-small;">Kinetics and mechanistic studies for the oxidation of N</span><span style="font-size: x-small;"><span style="font-size: xx-small;">-Benzylhydroxylamine by a Co</span><sup style="font-size: x-small;">III</sup><span style="font-size: xx-small;">-bound bridging superoxo complex in perchloric acid medium</span></span></p> |
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Added Entry - Uncontrolled Name |
GAIN, SEKHAR ; RKM VIDYAMANDIRA UGC |
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Uncontrolled Index Term |
Inorganic reaction mechanisms Keywords: N-benzylhydroxylamine, Superoxo, Kinetics, Mechanisms, Oxidation- Reduction. |
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Summary, etc. |
<p>In aqueous perchloric acid medium (pH = 0.522 – 1.3) , N–benzylhydroxylamine ( two electron reductant) reduces the one electron oxidant, superoxo ligand in [(dien)(en)Co<sup>III</sup>(O<sub>2</sub>)Co<sup>III</sup>(en)(dien)](ClO<sub>4</sub>)<sub>5</sub> (<strong>1</strong>) to the corresponding hydroperoxo complex, [(en)(dien)Co<sup>III</sup>(HO<sub>2</sub>)Co<sup>III</sup>(en)(dien)]<sup>5+</sup> (<strong>2</strong>) and itself gets oxidised to PhCH<sub>2</sub>NO following both proton coupled electron transfer (PCET) path and an electron – transfer (ET) reaction. The kinetics, stoichiometry and reaction mechanism clearly indicate that oxidation of PhCH<sub>2</sub>NHOH occurs through the formation of an intermediate, benzyl derivative of aminoxyl radical (PhCH<sub>2</sub>NHO<sup>•</sup>). In the presence of excess PhCH<sub>2</sub>NHOH over <strong>1</strong>, the reaction obeys first-order kinetics and rate of the reaction increases with [PhCH<sub>2</sub>NHOH]. The reaction rate, however, decreases with increase in [H<sup>+</sup>] and the plot of 1/<em>k<sub>o</sub></em> with [H<sup>+</sup>] is linear with a small but noteworthy intercept. It is also remarked that the reaction rate remarkably decreases with increasing proportion of D<sub>2</sub>O replacing H<sub>2</sub>O in the solvent. Therefore, an H-atom transfer (HAT) from PhCH<sub>2</sub>NHOH to the bridging superoxide in <strong>1</strong> seems reasonable at the rate determining step.</p><p><strong> </strong></p> |
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Publication, Distribution, Etc. |
Indian Journal of Chemistry -Section A (IJCA) 2021-09-22 10:50:13 |
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Electronic Location and Access |
application/pdf http://op.niscair.res.in/index.php/IJCA/article/view/46223 |
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Data Source Entry |
Indian Journal of Chemistry -Section A (IJCA); ##issue.vol## 60, ##issue.no## 7 (2021): INDIAN JOURNAL OF CHEMISTRY- SECTION A |
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Language Note |
en |
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Nonspecific Relationship Entry |
http://op.niscair.res.in/index.php/IJCA/article/download/46223/465548397 http://op.niscair.res.in/index.php/IJCA/article/download/46223/465548399 http://op.niscair.res.in/index.php/IJCA/article/download/46223/465548496 |
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