National Center of Applied Microfluidic Chemistry, Department of Chemical Engineering, POSTECH (Pohang University of Science and Technology), Pohang 37673, Korea.
Division of Natural Product Chemistry, CSIR-Indian Institute of Chemical Technology, Hyderabad 500007 India.
Nat Commun. 2017 Mar 6;8:14676. doi: 10.1038/ncomms14676.
Simultaneous capture of carbon dioxide (CO) and its utilization with subsequent work-up would significantly enhance the competitiveness of CO-based sustainable chemistry over petroleum-based chemistry. Here we report an interfacial catalytic reaction platform for an integrated autonomous process of simultaneously capturing/fixing CO in gas-liquid laminar flow with subsequently providing a work-up step. The continuous-flow microreactor has built-in silicon nanowires (SiNWs) with immobilized ionic liquid catalysts on tips of cone-shaped nanowire bundles. Because of the superamphiphobic SiNWs, a stable gas-liquid interface maintains between liquid flow of organoamines in upper part and gas flow of CO in bottom part of channel. The intimate and direct contact of the binary reagents leads to enhanced mass transfer and facilitating reactions. The autonomous integrated platform produces and isolates 2-oxazolidinones and quinazolines-2,4(1H,3H)-diones with 81-97% yields under mild conditions. The platform would enable direct CO utilization to produce high-valued specialty chemicals from flue gases without pre-separation and work-up steps.
同时捕获二氧化碳(CO)并加以利用,随后进行后处理,这将显著提高基于 CO 的可持续化学相对于基于石油的化学的竞争力。在这里,我们报告了一个用于界面催化反应的平台,用于在气-液层流中同时进行 CO 的捕获/固定的集成自主过程,并随后提供一个后处理步骤。连续流微反应器具有内置的硅纳米线(SiNWs),其尖端固定有离子液体催化剂,位于锥形纳米线束上。由于 SiNWs 的超疏水性,在通道的上部的有机胺的液体流动和底部的 CO 的气体流动之间保持稳定的气-液界面。二元试剂的紧密和直接接触促进了传质并有利于反应。该自主集成平台在温和条件下以 81-97%的产率生产并分离 2-恶唑烷酮和喹唑啉-2,4(1H,3H)-二酮。该平台将能够直接利用 CO 从烟道气中生产高附加值的特种化学品,而无需进行预分离和后处理步骤。