A Robust Mn Catalyst for H2O2 Disproportionation in Aqueous Solution

被引：22

作者：

Lee, Wei-Tsung ^{[1
]}

Xu, Song ^{[1
]}

Dickie, Diane A. ^{[2
]}

Smith, Jeremy M. ^{[1
]}

机构：

[1] New Mexico State Univ, Dept Chem & Biochem, Las Cruces, NM 88003 USA

[2] Univ New Mexico, Dept Chem & Chem Biol, Albuquerque, NM 87131 USA

来源：

EUROPEAN JOURNAL OF INORGANIC CHEMISTRY | 2013年 / 2013卷 / 22-23期

关键词：

Manganese; Reaction mechanisms; Peroxides; Homogeneous catalysis; Macrocycles; ELECTRON-PARAMAGNETIC-RESONANCE; HYDROGEN-PEROXIDE; MANGANESE(IV) COMPLEX; CATALASE ACTIVITY; METHYLENE-BLUE; MIMICS; ANTIOXIDANTS; EPOXIDATION; REACTIVITY; LIGANDS;

D O I：

10.1002/ejic.201300184

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

The pyridinophane complex [Mn(Py2N2)(H2O)(2)](2+) catalyses the disproportionation of H2O2 in aqueous solution over a wide pH range. Kinetic investigations reveal an induction period, which is proposed to involve the formation of a hydroperoxo intermediate, as well as evidence for catalyst self-inhibition. A catalytic cycle involving mononuclear intermediates has been proposed. Spectroscopic investigations under turnover conditions are consistent with this proposal and show that the resting state of the catalyst is a mononuclear Mn-II complex. The robustness of the catalyst is evidenced by its ability to achieve turnover numbers of 58000 in aqueous solution.

引用

页码：3867 / 3873

页数：7

共 50 条

[1] Oxidation of Alkenes with H2O2 by an in-Situ Prepared Mn(II)/Pyridine-2-carboxylic Acid Catalyst and the Role of Ketones in Activating H2O2
Dong, Jia Jia
Saisaha, Pattama
Meinds, Tim G.
Alsters, Paul L.
Ijpeij, Edwin G.
van Summeren, Ruben P.
Mao, Bin
Fananas-Mastral, Martin
de Boer, Johannes W.
Hage, Ronald
Feringa, Ben L.
Browne, Wesley R.
ACS CATALYSIS, 2012, 2 (06): : 1087 - 1096
[2] Reversible Deactivation of Manganese Catalysts in Alkene Oxidation and H2O2 Disproportionation
Kasper, Johann B.
Vicens, Laia
de Roo, C. Maurits
Hage, Ronald
Costas, Miquel
Browne, Wesley R.
ACS CATALYSIS, 2023, 13 (09) : 6403 - 6415
[3] VO(acac)2: An Efficient Catalyst for the Oxidation of Aldehydes to the Corresponding Acids in the Presence of Aqueous H2O2
Talukdar, Dhrubajyoti
Sharma, Kiran
Bharadwaj, Saitanya K.
Thakur, Ashim Jyoti
SYNLETT, 2013, 24 (08) : 963 - 966
[4] The reduction of I2 by H2O2 in aqueous solution
Ball, JM
Hnatiw, JB
CANADIAN JOURNAL OF CHEMISTRY-REVUE CANADIENNE DE CHIMIE, 2001, 79 (03): : 304 - 311
[5] Stereospecific C-H Oxidation with H2O2 Catalyzed by a Chemically Robust Site-Isolated Iron Catalyst
Gomez, Laura
Garcia-Bosch, Isaac
Company, Anna
Benet-Buchholz, Jordi
Polo, Alfonso
Sala, Xavier
Ribas, Xavi
Costas, Miquel
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2009, 48 (31) : 5720 - 5723
[6] Effect of nitrate on the degradation of bisphenol A by UV/H2O2 and ozone/H2O2 oxidation in aqueous solution
Park, C. G.
Choi, E. S.
Jeon, H. W.
Lee, J. H.
Sung, B. W.
Cho, Y. H.
Ko, K. B.
DESALINATION AND WATER TREATMENT, 2014, 52 (4-6) : 797 - 804
[7] Rate constant for the reaction of the H atom with H2O2 in aqueous solution
Ershov, BG
Gordeev, AV
Kelm, A
Janata, E
RADIATION PHYSICS AND CHEMISTRY, 2003, 67 (05) : 613 - 616
[8] A Peroxotungstate-Ionic Liquid Brush Assembly: an Efficient and Reusable Catalyst for Selectively Oxidizing Sulfides with Aqueous H2O2 Solution in Neat Water
Shi, Xianying
Ma, Wenjuan
Ou, Hui
Han, Xiaoyan
Lu, Congmin
Chen, Yan
Wei, Junfa
JOURNAL OF THE BRAZILIAN CHEMICAL SOCIETY, 2012, 23 (08) : 1536 - 1542
[9] Complete oxidation of low concentration ethanol in aqueous solution with H2O2 on nanosized Mn3O4/SBA-15 catalyst
Han, Yi-Fan
Chen, Fengxi
Zhong, Ziyi
Ramesh, Kanaparthi
Chen, Luwei
Jian, Dou
Ling, Wong Wan
CHEMICAL ENGINEERING JOURNAL, 2007, 134 (1-3) : 276 - 281
[10] C-H Hydroxylation Using a Heterocyclic Catalyst and Aqueous H2O2
Litvinas, Nichole D.
Brodsky, Benjamin H.
Du Bois, J.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2009, 48 (25) : 4513 - 4516

← 1 2 3 4 5 →