Xu Maotong, Qu Zheng-Wang, Grimme Stefan, Stephan Douglas W
Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, Ontario M5S 3H6, Canada.
Mulliken Center for Theoretical Chemistry, Institut für Physikalische und Theoretische Chemie, Rheinische Friedrich-Wilhelms-Universität Bonn, Beringstrasse 4, 53115 Bonn, Germany.
J Am Chem Soc. 2021 Jan 20;143(2):634-638. doi: 10.1021/jacs.0c11482. Epub 2021 Jan 5.
Lithium dicyclohexylamide (CyNLi) reacts with syn-gas or CO to generate transient intermediates with carbene character, which are capable of reacting further with CO or H, effecting sequential C-C and C-H bond formations from CO or H, thus providing a transition-metal-free avenue to the fundamental reactions of the Fischer-Tropsch process. Further experimental and computational data indicate that reactions with CO and H are thermodynamically accessible, with a kinetic bias toward CO homologation.
二环己基锂酰胺（CyNLi）与合成气或一氧化碳反应生成具有卡宾特性的瞬态中间体，这些中间体能够与一氧化碳或氢气进一步反应，实现由一氧化碳或氢气进行连续的碳-碳键和碳-氢键形成，从而为费托合成过程的基本反应提供了一条无过渡金属的途径。进一步的实验和计算数据表明，与一氧化碳和氢气的反应在热力学上是可行的，动力学上倾向于一氧化碳同系化。
