Catecholase activity of a structurally characterized dinuclear iron(III) complex [FeIII2(L)2] [H3L=N,N′-bis(3-methoxysalicylaldimine)-1,3-diaminopropan-2-ol]

Mitra, Merry; Maji, Ashis Kumar; Ghosh, Barindra Kumar; Raghavaiah, Pallepogu; Ribas, Joan; Ghosh, Rajarshi

doi:10.1016/j.poly.2013.08.064

Cited by 39 publications

(11 citation statements)

References 47 publications

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“…To investigate the efficiency of the catalytic activity we draw a comparison between our complex 1 and some recently reported iron complexes which show efficient catecholase activity (Table ) . This comparison also indicates that complex 1 acts as a better and effective catalyst towards catecholase activity than the reported ones …”

Section: Resultsmentioning

confidence: 92%

Catalytic promiscuity of an iron(II)–phenanthroline complex

De¹,

Garai²,

Yadav

et al. 2016

Applied Organom Chemis

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A mononuclear iron(II) complex, [Fe(phen) 3 ]Cl 2 (1) (phen =1,10-phenanthroline), has been synthesized in crystalline phase and characterized using various spectroscopic techniques including single crystal X-ray diffraction. Crystal structure analysis revealed that 1 crystallizes in a monoclinic system with C2/m space group. Complex 1 acts as a functional model for a biomimetic catalyst promoting the aerobic oxidation of 3,5-di-tert-butylcatechol (3,5-DTBC) through radical pathways with a significant turnover number (k cat =3.55 × 10 3 h À1 ) and exhibits catechol dioxygenase activity towards the same 3,5-DTBC substrate at room temperature in oxygen-saturated ethanol medium. The existence of an isobestic point at 610 nm from spectrophotometric data indicates the presence of Fe 3+ À3,5-DTBC adduct favouring an enzyme-substrate binding phenomenon. Upon stoichiometric addition of 3,5-DTBC pretreated with two equivalents of triethylamine to the iron complex, two catecholate-to-iron(III) ligand-to-metal charge transfer bands (575 and 721 nm) are observed and the in situ generated catecholate intermediate reacts with dioxygen (k obs =9.89 × 10 À4 min À1 ) in ethanol medium to afford exclusively intradiol cleavage products along with a small amount of benzoquinone, and a small amount of extradiol cleavage products, which provide substantial evidence for a substrate activation mechanism.

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Section: Resultsmentioning

confidence: 92%

Catalytic promiscuity of an iron(II)–phenanthroline complex

De¹,

Garai²,

Yadav

et al. 2016

Applied Organom Chemis

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show abstract

“…It appears that although there are many excellent Ni II catalysts for CO activity but in case of Ni II the importance of the ligand is very much appreciated since Ni II acetate by itself has a very low turnover number even at 10 −4 M concentration (Table 1). Fe II -acetate also has a low k cat even at 10 −4 M concentration and it appears from the literature that there has not been much attempts to use Fe II based complexes as mimics of CO [25,[55][56][57]. Fe II/III seems to be a better choice for catechol dioxygenase (which leads to intradiol or extradiol cleavage) based on the literature data [116][117][118][119][120][121][122][123].…”

Section: Catecholase Activity Studiesmentioning

confidence: 99%

“…The metals were chosen from the list of 3d-metals used so far to design mimics of CO or PHS using different ligand systems viz. copper [24,, iron [25,[55][56][57], cobalt [58][59][60][61][62][63][64][65], manganese [66][67][68][69][70][71][72][73][74][75][76][77][78][79], nickel [26,68,[80][81][82][83] and zinc [33,84]. PHS mimics cannot be found as much as CO but yet are well studied with 3d-metals viz.…”

Section: Introductionmentioning

confidence: 99%

Investigation of 3d-transition metal acetates in the oxidation of substituted dioxolene and phenols

Dey

Mukherjee

2015

Journal of Molecular Catalysis A: Chemical

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“…The original UPM6 and UPM7 methods were also tested for comparison [70]. As aforementioned, our test set specifically consisted of (i) dinuclear 14 dimanganese (from FEBKOM to BARFOQ) and 11 diiron (from YOCKAC to RITHAD) complexes corresponding to the Cambridge Structural Database reference codes as depicted in Figure 1 [18,19,20,21,22,23,24,25,26,27,28,29,30,31,32,33,34,35,36,37,38], and (ii) an ethylene epoxidation reaction catalyzed by 3 [Cl–Mn V = O(salen)] and a toluene fluorination reaction catalyzed by 3 [F–Mn V =O(salen)] [2,10,71].…”

Section: Computational Detailsmentioning

confidence: 99%

“…In addition to catalytic activities, magnetic properties of polynuclear complexes have also been studied with the aim of developing promising candidates for quantum computing and high-density magnetic storage devices [16,17]. To understand fundamentally the mechanism of magnetic coupling, studies on dinuclear complexes with fluoride and chloride bridges have been carried out as well as those with oxo and hydroxo bridges [18,19,20,21,22,23,24,25,26,27,28,29,30,31,32,33,34,35,36,37,38].…”

Section: Introductionmentioning

confidence: 99%

Quantitative Assessment of rPM6 for Fluorine- and Chlorine-Containing Metal Complexes: Comparison with Experimental, First-Principles, and Other Semiempirical Results

2018

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We report a reparameterization of PM6 parameters for fluorine and chlorine using our training set containing transition metal complexes. Spin unrestricted calculations with the resulting rPM6 (UrPM6) were examined quantitatively using two test sets: (i) the description of magnetic interactions in 25 dinuclear metal complexes and (ii) the prediction of barrier heights and reaction energies for epoxidation and fluorination reactions catalyzed by high-valent manganese-oxo species. The conventional UPM6 and UPM7 methods were also evaluated for comparison on the basis of either experimental or computational (the UB3LYP/SVP level) outcomes. The merits of UrPM6 are highlighted by both the test sets. As regards magnetic exchange coupling constants, the UrPM6 method had the smallest mean absolute errors from the experimental data (19 cm−1), followed by UPM7 (119 cm−1) and UPM6 (373 cm−1). For the epoxidation and fluorination reactions, all of the transition state searches were successful using UrPM6, while the success rates obtained by UPM6 and UPM7 were only 50%. The UrPM6-optimized stationary points also agreed well with the reference UB3LYP-optimized geometries. The accuracy for estimating reaction energies was also greatly remedied.

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Catecholase activity of a structurally characterized dinuclear iron(III) complex [FeIII2(L)2] [H3L=N,N′-bis(3-methoxysalicylaldimine)-1,3-diaminopropan-2-ol]

Cited by 39 publications

References 47 publications

Catalytic promiscuity of an iron(II)–phenanthroline complex

Catalytic promiscuity of an iron(II)–phenanthroline complex

Investigation of 3d-transition metal acetates in the oxidation of substituted dioxolene and phenols

Quantitative Assessment of rPM6 for Fluorine- and Chlorine-Containing Metal Complexes: Comparison with Experimental, First-Principles, and Other Semiempirical Results

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