College of Chemistry and Chemical Engineering, Jiangxi Inorganic Membrane Materials Engineering Research Centre, Jiangxi Normal University, Nanchang, 330022, P.R. China.
Department of Chemistry, University of California, Riverside, CA, 92521, USA.
Angew Chem Int Ed Engl. 2017 Jun 6;56(24):6843-6847. doi: 10.1002/anie.201701919. Epub 2017 Apr 26.
A novel method for the highly efficient and reversible capture of CO in carbanion-functionalized ionic liquids (ILs) by a C-site interaction is reported. Because of its supernucleophilicity, the carbanion in ILs could absorb CO efficiently. As a result, a relatively high absorption capacity for CO (up to 0.046 mol mol ) was achieved under ambient conditions, compared with CO solubility in a commonly used IL [Bmim][Tf N] (2×10 mol mol ). The results of quantum mechanical calculations and spectroscopic investigation confirmed that the chemical interaction between the C-site in the carbanion and CO resulted in the superior CO absorption capacities. Furthermore, the subsequent conversion of captured CO into valuable chemicals with good reactivity was also realized through the alkoxycarbonylation reaction under mild conditions. Highly efficient CO absorption by carbanion-functionalized ILs provides a new way of separating and converting CO.
报道了一种新型方法,通过 C 位相互作用,可在阴离子功能化离子液体(ILs)中高效、可逆地捕获 CO。由于其超亲核性,ILs 中的碳负离子可以有效地吸收 CO。因此,与 CO 在常用 IL [Bmim][Tf N](2×10 mol/mol)中的溶解度相比,在环境条件下实现了相对较高的 CO 吸收容量(高达 0.046 mol/mol)。量子力学计算和光谱研究结果证实,碳负离子中 C 位与 CO 之间的化学相互作用导致了优异的 CO 吸收能力。此外,通过温和条件下的烷氧基羰基化反应,还实现了将捕获的 CO 转化为具有良好反应性的有价值化学品。阴离子功能化 ILs 对 CO 的高效吸收为分离和转化 CO 提供了一种新途径。