Efficient and Reversible Capture of CO₂ in CO₂-Binding Organic Liquids Formed by 1,1,3,3-Tetramethylguanidine and Glycerol Derivatives

Abstract

A class of CO 2 -binding organic liquids (CO 2 -BOLs) composed of 1,1,3,3-Tetramethylguanidine (TMG) and Glycerol (Gly) and Gly's amino derivatives were developed for highly efficient and reversible CO 2 capture. These CO 2 -BOLs exhibited high gravimetric CO 2 solubility up to 0.196 g CO 2 •g −1 at 313.2 K and 1.0 atm, superior to most functionalized ILs and other absorbents. The influential factors of CO 2 absorption, such as components of CO 2 -BOLs, absorption temperature, and CO 2 partial pressure together with water contents were investigated, and the recyclability of CO 2 -BOLs was verified to be excellent. The absorption mechanism of CO 2 -BOLs was explored with the help of spectral analysis, quantum chemical calculation, and thermodynamic analysis. All the results revealed that chemisorption took place once these CO 2 -BOLs were exposed to CO 2 , and alkyl guanidine carbonates were produced. Besides, it is illustrated that introducing the amino group to Gly could reduce the nucleophilic reactivity of CO 2 -BOLs, along with the absorption enthalpy simultaneously.

Demystifying Solvent Effects on Diels–Alder Reactions in Pure and Mixed Solvents: A Combined Electronic DFT and QM/MM Study

“…The genmer program is a subprogram of Molclus, which is capable of performing molecular and conformational searches for clusters consisting of any element and number of atoms. Molclus has successfully searched for the initial structure of the triphenylamine unit and the organic structure of captured CO 2 . − The initial structures are then optimized with Guassian 16 at the B3LYP/6-31G* level of theory. Finally, these optimized structures are clustered and sorted using the isostat component to obtain the structures with the lowest energy.…”

Rapid Absorption and Desorption of CO2 by Deep Eutectic Solvents via Reversible CO2-Triggered Proton Transfer Process

“…In general, DESs are prepared by simply mixing of two or more components, including both hydrogen bond acceptors (HBAs) and hydrogen bond donors (HBDs), to form a solution with a melting point lower than that of any of its components by means of hydrogen bonding interactions. Organic amines and azoles are widely used to synthesize ILs to capture CO 2 , which can also be used as HBDs and HBAs. − Three types of the most studied DESs for CO 2 capture are as follows: amino-based functionalized DESs, − azole-based functionalized DESs, − and super base functionalized DESs. − Due to the low cost and highly efficient capture of CO 2 by amines, amino-based functionalized DESs have been widely investigated. Zhang et al selected monoethanolamine (MEA) as a HBD and synthesized several 1-butyl-3-methylimidazolium chloride (BmimCl):MEA DESs.…”

“…For example, the mole absorption capacity of [TETA]­Cl/EG DES increased from 0.75 mol CO 2 /mol [TETA]Cl to 1.456 mol CO 2 /mol [TETA]Cl as the molar ratio of EG to [TETA]Cl increased from 1:1 to 3:1. Additionally, EG has also been reported to be involved in the chemical capture of CO 2 in super base functionalized DESs, in which EG acted as a chemical interaction site and formed carbonate with CO 2 after being deprotonated by the super base. , So, in this work, EG was selected as the HBD to form DES with aromatic amines.…”