The
emerging polyethylenimine (PEI)-functionalized solid adsorbents
have witnessed significant development in the implementation of CO2 capture and separation because of their decent adsorption
capacity, recyclability, and scalability. As an indispensable substrate,
the importance of selecting porous solid supports in PEI functionalization
for CO2 adsorption was commonly overlooked in many previous
investigations, which instead emphasized screening amine types or
developing complex porous materials. To this end, we scrutinized the
critical role of different commercial porous supports (silica, alumina,
activated carbon, and polymeric resins) in PEI impregnation in this
study, taking into account multiple perspectives. Hereinto, the present
results identified that abundant larger pore structures and surface
functional groups were conducive to loading a considerable amount
of PEI molecules. Various supports after PEI functionalization had
great differences in adsorption capacities, amine efficiencies, and
the corresponding optimal temperatures. In addition, more attention
was paid to the role of porous supports in long-term stability during
the consecutive adsorption–regeneration cycles, while N2 and CO2 purging as regeneration strategies, respectively.
Especially, CO2-induced degradation due to urea species
formation was specifically recognized in a SiO2-based adsorbent,
which would induce serious concerns in CO2 cyclic capture.
On the other side, we also confirmed that adopting conventional porous
supports, for example, HP20, could achieve superior adsorption performance
(above 4 mmol CO2/g) and cyclic stability (around 1% loss
after 30 cycles) rather than the ones synthesized through complex
approaches, which ensured the availability and scalability of PEI-functionalized
CO2 adsorbents.