Integration of CO2 capture, activation, and conversion with a ternary acetylglucosyl 2-methyl-imidazolium modified Pd catalyst. Issue 8 (21st March 2023)

• Record Type: Journal Article
• Authors: Zhou, Zhong-Gao; He, Peng; Li, Jing; Zhang, Jia; Xu, Guo-Hai; Zhang, Shi-Yong; Deng, Xiao-Xiao; Du, Zi-Yi; Luo, Guo-Tian; Zhen, Hong-Yu; Chen, Yi-Wang; He, Chun-Ting
• Is Part Of: Organic chemistry frontiers. Volume 10:Issue 8(2023)
• Page Start: 2045
• Page End: 2053
• Publication Date: 2023-03-21
• Subjects: Chemistry, Organic -- Periodicals; 547.005
• DOI: 10.1039/d3qo00067b
• Languages: English
• ISSNs: 2052-4110

Abstract

Abstract : High-efficiency ternary acetylglucosyl 2-methyl-imidazolium modified Pd catalyst for integration of CO2 capture, activation, and conversion in carboxycyclization of propargyl amines and dilute CO2 with a record TOF of 1440 h −1 has been developed. Abstract : The efficient catalytic conversion of thermodynamically and kinetically stable carbon dioxide (CO2 ) into value-added chemicals is challenging. Herein, we developed a high-efficiency ternary Pd catalyst (AcGlu-MeIm-PdCl4 ) modified with acetylglucosyl 2-methyl-imidazolium for the integration of CO2 capture, activation, and catalytic conversion simultaneously. The Lewis acid–Lewis base interactions between CO2 and AcGlu groups increased the solubility of CO2, while the N-heterocyclic olefin (NHO) derived from 2-methyl-imidazolium cations can capture and activate CO2 by forming NHO-CO2 adducts, as well as stabilizing the metal Pd. 2-Oxazolidinones can be prepared even using dilute CO2 (CO2 /N2, vol/vol = 15 : 85) and propargyl amines over this ternary Pd catalyst, achieving a record turnover frequency of 1440 h −1 . The CO2 capture, activation, and conversion mechanism of this catalytic system was unveiled by quasi-in situ NMR, 13 C-isotope-labeling NMR and FT-IR. These findings highlight the potential of exploring multifunctional catalysts for efficient catalytic CO2 conversion.