Herein we address the efficiency of the CO2 sorption
of ionic liquids (IL) with hydrogen bond donors (e.g., glycols) added
as viscosity modifiers and the impact of encapsulating them to limit
sorbent evaporation under conditions for the direct air capture of
CO2. Ethylene glycol, propylene glycol, 1,3-propanediol,
and diethylene glycol were added to three different ILs: 1-ethyl-3-methylimidazolium
2-cyanopyrrolide ([EMIM][2-CNpyr]), 1-ethyl-3-methylimidazolium tetrafluoroborate
([EMIM][BF4]), and 1-butyl-3-methylimidazolium tetrafluoroborate
([BMIM][BF4]). Incorporation of the glycols decreased viscosity
by an average of 51% compared to bulk IL. After encapsulation of the
liquid mixtures using a soft template approach, thermogravimetric
analysis revealed average reductions in volatility of 36 and 40% compared
to the unencapsulated liquid mixtures, based on 1 h isothermal experiments
at 25 and 55 °C, respectively. The encapsulated mixtures of [EMIM][2-CNpyr]/1,3-propanediol
and [EMIM][2-CNpyr]/diethylene glycol exhibited the lowest volatility
(0.0019 and 0.0002 mmol/h at 25 °C, respectively) and were further
evaluated as CO2 absorption/desorption materials. Based
on the capacity determined from breakthrough measurements, [EMIM][2-CNpyr]/1,3-propanediol
had a lower transport limited absorption rate for CO2 sorption
compared to [EMIM][2-CNpyr]/diethylene glycol with 0.08 and 0.03 mol
CO2/kg sorbent, respectively; however, [EMIM][2-CNpyr]/diethylene
glycol capsules exhibited higher absorptions capacity at ∼500
ppm of CO2 (0.66 compared to 0.47 mol of CO2/kg sorbent for [EMIM][2-CNpyr]/1,3-propanediol). These results show
that glycols can be used to not only reduce IL viscosity while increasing
physisorption sites for CO2 sorption, but also that encapsulation
can be utilized to mitigate evaporation of volatile viscosity modifiers.