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A Strong Positive Allosteric Effect in the Molecular Recognition of Dicarboxylic Acids by a Cerium(IV) Bis[tetrakis(4-pyridyl)porphyrinate] Double Decker.铈（IV）双[四（4-吡啶基）卟啉]双层对二元羧酸分子识别中的强正变构效应
Angew Chem Int Ed Engl. 1998 Aug 17;37(15):2096-2099. doi: 10.1002/(SICI)1521-3773(19980817)37:15<2096::AID-ANIE2096>3.0.CO;2-B.
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A new intermolecular interaction: unconventional hydrogen bonds with element-hydride bonds as proton acceptor.一种新的分子间相互作用：以元素 - 氢化物键作为质子受体的非常规氢键。
Acc Chem Res. 1996 Jul;29(7):348-54. doi: 10.1021/ar950150s.
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Reduction of imines by hydroxycyclopentadienyl ruthenium hydride: intramolecular trapping evidence for hydride and proton transfer outside the coordination sphere of the metal.羟基环戊二烯基氢化钌对亚胺的还原：金属配位球外氢化物和质子转移的分子内捕获证据。
J Am Chem Soc. 2005 Oct 12;127(40):14062-71. doi: 10.1021/ja053956o.
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Using mechanistic and computational studies to explain ligand effects in the palladium-catalyzed aerobic oxidation of alcohols.利用机理和计算研究来解释钯催化醇类有氧氧化反应中的配体效应。
J Am Chem Soc. 2005 Jun 15;127(23):8499-507. doi: 10.1021/ja050949r.
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Oxidative formation of thiolesters in a model system of the pyruvate dehydrogenase complex.丙酮酸脱氢酶复合体模型系统中硫酯的氧化形成
J Org Chem. 2005 Apr 15;70(8):3140-7. doi: 10.1021/jo047737h.
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Cooperative catalysis of a cationic ruthenium complex, amine base, and na salt: catalytic activation of acetonitrile as a nucleophile.阳离子钌配合物、胺碱和钠盐的协同催化：乙腈作为亲核试剂的催化活化
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Reversibly addressing an allosteric catalyst in situ: catalytic molecular tweezers.原位可逆调控变构催化剂：催化分子镊子
Angew Chem Int Ed Engl. 2004 Oct 18;43(41):5503-7. doi: 10.1002/anie.200460932.
8
Mechanistic characterization of aerobic alcohol oxidation catalyzed by Pd(OAc)(2)/pyridine including identification of the catalyst resting state and the origin of nonlinear [catalyst] dependence.由Pd(OAc)₂/吡啶催化的需氧醇氧化反应的机理表征，包括催化剂静止态的确定以及非线性[催化剂]依赖性的起源。
J Am Chem Soc. 2004 Sep 15;126(36):11268-78. doi: 10.1021/ja049962m.
9
Cooperative dual catalysis: application to the highly enantioselective conjugate cyanation of unsaturated imides.协同双催化：在不饱和酰亚胺的高对映选择性共轭氰化反应中的应用
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10
Cooperative multi-catalyst systems for one-pot organic transformations.用于一锅法有机转化的协同多催化剂体系。
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用于醇氧化反应的高度协同的四金属钌-μ-氧-μ-羟基催化剂。

Highly Cooperative Tetrametallic Ruthenium-mu-Oxo-mu-Hydroxo Catalyst for the Alcohol Oxidation Reaction.

作者信息

Yi Chae S, Zeczycki Tonya N, Guzei Ilia A

机构信息

Department of Chemistry, Marquette University, Milwaukee, Wisconsin 53201-1881, and Molecular Structure Laboratory, Department of Chemistry, University of Wisconsin-Madison, Madison, Wisconsin 53706-1396.

出版信息

Organometallics. 2006;25(4):1047-1051. doi: 10.1021/om0510674.

DOI:10.1021/om0510674
PMID:18726005
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC2519863/
Abstract

The tetrametallic ruthenium-oxo-hydroxo-hydride complex {(PCy(3))(CO)RuH(mu(4)-O)(mu(3)-OH)(mu(2)-OH)} (1) was synthesized in two steps from the monomeric complex (PCy(3))(CO)RuHCl (2). The tetrameric complex 1 was found to be a highly effective catalyst for the transfer dehydrogenation of alcohols. Complex 1 showed a different catalytic activity pattern towards primary and secondary benzyl alcohols, as indicated by the Hammett correlation for the oxidation reaction of p-X-C(6)H(4)CH(2)OH (rho = -0.45) and p-X-C(6)H(4)CH(OH)CH(3) (rho = +0.22) (X = OMe, CH(3), H, Cl, CF(3)). Both a sigmoidal curve from the plot of initial rate vs [PhCH(OH)CH(3)] (K(0.5) = 0.34 M; Hill coefficient, n = 4.2+/-0.1) and the phosphine inhibition kinetics revealed the highly cooperative nature of the complex for the oxidation of secondary alcohols.

摘要

四金属钌-氧-氢氧根-氢配合物{(PCy(3))(CO)RuH(μ(4)-O)(μ(3)-OH)(μ(2)-OH)} (1)由单体配合物(PCy(3))(CO)RuHCl (2)分两步合成。发现四聚体配合物1是醇转移脱氢的高效催化剂。如对p-X-C(6)H(4)CH(2)OH (ρ = -0.45)和p-X-C(6)H(4)CH(OH)CH(3) (ρ = +0.22) (X = OMe、CH(3)、H、Cl、CF(3))氧化反应的哈米特相关性所示，配合物1对伯苄醇和仲苄醇表现出不同的催化活性模式。初始速率对[PhCH(OH)CH(3)]作图得到的S形曲线(K(0.5) = 0.34 M；希尔系数，n = 4.2±0.1)以及膦抑制动力学均表明该配合物对仲醇氧化具有高度协同性。