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首页> 外文期刊>Chemistry: A European journal >Reactivity and Operational Stability of N-Tailed TAMLs through Kinetic Studies of the Catalyzed Oxidation of Orange II by H2O2: Synthesis and X-ray Structure of an N-Phenyl TAML
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Reactivity and Operational Stability of N-Tailed TAMLs through Kinetic Studies of the Catalyzed Oxidation of Orange II by H2O2: Synthesis and X-ray Structure of an N-Phenyl TAML

机译：N尾TAML的反应性和操作稳定性，通过动力学研究H2O2催化氧化橙II：N-苯基TAML的合成和X射线结构

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The catalytic activity of the N-tailed (biuret) TAML (tetraamido macrocyclic ligand) activators [Fe{4-XC6H3-1,2-(NCOCMe2NCO)(2)NR}Cl](2-) (3; N atoms in boldface are coordinated to the central iron atom; the same nomenclature is used in for compounds 1 and 2 below), [X, R=H, Me (a); NO2, Me (b); H, Ph (c)] in the oxidative bleaching of OrangeII dye by H2O2 in aqueous solution is mechanistically compared with the previously investigated activator [Fe{4-XC6H3-1,2-(NCOCMe2NCO)(2)CMe2}OH2](-) (1) and the more aggressive analogue [Fe(Me2C{CON(1,2-C6H3-4-X)NCO}(2))OH2](-) (2). Catalysis by 3 of the reaction between H2O2 and OrangeII (S) occurs according to the rate law found generally for TAML activators (v=k(I)k(II)[Fe-III][S][H2O2]/(k(I)[H2O2]+k(II)[S]) and the rate constants k(I) and k(II) at pH7 both decrease within the series 3b>3a>3c. The pH dependency of k(I) and k(II) was investigated for 3a. As with all TAML activators studied to-date, bell-shaped profiles were found for both rate constants. For k(I), the maximal activity was found at pH10.7 marking it as having similar reactivity to 1a. For k(II), the broad bell pH profile exhibits a maximum at pH about 10.5. The condition k(I)k(II) holds across the entire pH range studied. Activator 3b exhibits pronounced activity in neutral to slightly basic aqueous solutions making it worthy of consideration on a technical performance basis for water treatment. The rate constants k(i) for suicidal inactivation of the active forms of complexes 3a-c were calculated using the general formula ln([S-0]/[S])=(k(II)/k(i))[Fe-III]; here [Fe-III], [S-0], and [S] are the total catalyst concentration and substrate concentration at time zero and infinity, respectively. The synthesis and X-ray characterization of 3c are also described.
机译：N尾（缩二脲）TAML（四酰胺基大环配体）活化剂[Fe {4-XC6H3-1,2-（NCOCMe2NCO）（2）NR} Cl]（2-）的催化活性（3; N粗体字）与中心铁原子配位;以下化合物1和2使用相同的命名法），[X，R = H，Me（a）; NO2，我（b）;与以前研究的活化剂[Fe {4-XC6H3-1,2-（NCOCMe2NCO）（2）CMe2} OH2]（-）进行机械比较，比较了在水溶液中H2O2对OrangeII染料的氧化漂白中的H，Ph（c）] ）（1）和更具侵略性的类似物[Fe（Me2C {CON（1,2-C6H3-4-X）NCO}（2））OH2]（-）（2）。 H2O2与OrangeII（S）之间反应的3催化反应是根据通常针对TAML活化剂发现的速率定律发生的（v = k（I）k（II）[Fe-III] [S] [H2O2] /（k（ I）[H2O2] + k（II）[S]）以及pH7的速率常数k（I）和k（II）在3b> 3a> 3c系列中均减小。 （II）的3a值与迄今研究的所有TAML激活剂一样，都发现了两个速率常数的钟形曲线;对于k（I），在pH10.7处发现了最大活性，表明它具有相似的反应活性。对于k（II），宽钟形pH分布在pH约为10.5时表现出最大值;条件k（I） k（II）在整个研究的pH范围内均保持不变;活化剂3b在中性至弱碱性水溶液，值得在水处理的技术性能基础上加以考虑，使用通式ln（[S-0]计算复合物3a-c活性形式的自杀灭活的速率常数k（i） / [S]）=（k（II）/ k（i））[Fe-III];此处[Fe-III]，[S-0]和[S]分别是零时刻和无限远时刻的总催化剂浓度和底物浓度。还描述了3c的合成和X射线表征。

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