Journal ArticleDOI
Environmentally Friendly One-Pot Synthesis of α-Alkylated Nitriles Using Hydrotalcite-Supported Metal Species as Multifunctional Solid Catalysts
Ken Motokura,Noriaki Fujita,Kohsuke Mori,Tomoo Mizugaki,Kohki Ebitani,Koichiro Jitsukawa,Kiyotomi Kaneda +6 more
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TLDR
These hydrotalcite-supported metal catalysts can effectively promote alpha-alkylation reactions of various nitriles with primary alcohols or carbonyl compounds through tandem reactions consisting of metal-catalyzed oxidation and reduction, and an aldol reaction promoted by the base sites of the HT.Abstract:
A ruthenium-grafted hydrotalcite (Ru/HT) and hydrotalcite-supported palladium nanoparticles (Pd(nano)/HT) are easily prepared by treating basic layered double hydroxide, hydrotalcite (HT, Mg(6)Al(2)(OH)(16)CO(3)) with aqueous RuCl(3)n H(2)O and K(2)[PdCl(4)] solutions, respectively, using surface impregnation methods. Analysis by means of X-ray diffraction, and energy-dispersive X-ray, electron paramagnetic resonance, and X-ray absorption fine structure spectroscopies proves that a monomeric Ru(IV) species is grafted onto the surface of the HT. Meanwhile, after reduction of a surface-isolated Pd(II) species, highly dispersed Pd nanoclusters with a mean diameter of about 70 A is observed on the Pd(nano)/HT surface by transmission electron microscopy analysis. These hydrotalcite-supported metal catalysts can effectively promote alpha-alkylation reactions of various nitriles with primary alcohols or carbonyl compounds through tandem reactions consisting of metal-catalyzed oxidation and reduction, and an aldol reaction promoted by the base sites of the HT. In these catalytic alpha-alkylations, homogeneous bases are unnecessary and the only by-product is water. Additionally, these catalyst systems are applicable to one-pot syntheses of glutaronitrile derivatives.read more
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Catalytic applications of layered double hydroxides: recent advances and perspectives
TL;DR: This Review article is mainly focused on the most recent developments in smart design strategies for LDH materials and the potential catalytic applications of the resulting materials.
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Heterogeneous Catalysts for the One-Pot Synthesis of Chemicals and Fine Chemicals
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Alcohols as electrophiles in C--C bond-forming reactions: the hydrogen autotransfer process.
TL;DR: The hydrogen autotransfer process allows the alkylation of different nucleophilic agents using environmentally benign alcohols as electrophiles, mild conditions, and soft bases, with water produced as the only waste material.
Journal ArticleDOI
Exploring, tuning, and exploiting the basicity of hydrotalcites for applications in heterogeneous catalysis.
TL;DR: The aim is to provide the tools for understanding how series of parameters involved in the preparation of hydrotalcite-based catalytic materials can be employed to control and adapt the basic properties of the catalyst towards the basicity demanded by each target chemical reaction.
Journal ArticleDOI
Boosting oxygen evolution of single-atomic ruthenium through electronic coupling with cobalt-iron layered double hydroxides
Pengsong Li,Maoyu Wang,Xinxuan Duan,Lirong Zheng,Xiaopeng Cheng,Yuefei Zhang,Yun Kuang,Yaping Li,Qing Ma,Zhenxing Feng,Wen Liu,Xiaoming Sun +11 more
TL;DR: It is disclosed that the isolated single atom ruthenium was kept under the oxidation states of 4+ even at high overpotential due to synergetic electron coupling, which endow exceptional electrocatalytic activity and stability simultaneously.
References
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TL;DR: Transition metal-catalyzed methods that are both selective and economical for formation of cyclic structures, of great interest for biological purposes, represent an important starting point for this long-term goal.
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Atom Economy—A Challenge for Organic Synthesis: Homogeneous Catalysis Leads the Way
TL;DR: The ability of transition metal complexes to preorganize π-electron systems serves as the basis both of simple additions usually accompanied by subsequent hydrogen shifts and of cycloadditions as mentioned in this paper.
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On Inventing Reactions for Atom Economy
TL;DR: Using mechanistic reasoning, over 20 new processes of varying complexity have been designed and implemented that involved C-C bond-forming reactions and the prospect for such developments is probed in the context of ruthenium-catalyzed reactions.