Sammis Glenn M, Danjo Hiroshi, Jacobsen Eric N
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, USA.
J Am Chem Soc. 2004 Aug 18;126(32):9928-9. doi: 10.1021/ja046653n.
Cooperative heterobimetallic catalysis was used as a design principle to achieve a highly reactive system for the enantioselective conjugate addition of cyanide to alpha,beta-unsaturated imides. A dual-catalyst pathway involving chiral (salen)Al complex 1b and chiral (pybox)Er complex 4b provides measurable improvements in rates and enantioselectivities relative to single-catalyst systems. Mechanistic studies point to a cooperative bimetallic mechanism involving activation of the imide by the Al complex and activation of cyanide by the Er complex.
协同异双金属催化被用作一种设计原则,以实现用于氰化物对α,β-不饱和酰亚胺的对映选择性共轭加成的高活性体系。涉及手性(salen)铝配合物1b和手性(pybox)铒配合物4b的双催化剂途径相对于单催化剂体系在反应速率和对映选择性方面有显著提高。机理研究表明存在一种协同双金属机理,其中铝配合物活化酰亚胺,铒配合物活化氰化物。