In this work, graphene-derived N-enriched
porous carbons were synthesized
by urea modification and KOH activation of thermally shocked graphene
oxide. The prepared sorbents were characterized by various techniques
and investigated as potential CO2 capture materials. The
as-prepared sorbents possess high CO2 adsorption capacity
of 2.40 mmol/g (25 °C) and 3.24 mmol/g (0 °C) at 1 bar,
which is higher than most graphene-based carbons reported previously.
The nitrogen incorporation and narrow microporosity are the two major
factors that determine CO2 uptake for these graphene-derived
carbonaceous adsorbents under ambient conditions. The adsorption kinetic
data of the optimized sample were well-described by the classical
Fick’s diffusion model with a high CO2 diffusion
rate. The fast CO2 adsorption kinetics can be attributed
to the short diffusion paths of this sample, which is composed of
thin layers of graphene sheets. Moreover, these graphene-derived sorbents
also demonstrate excellent stability and recyclability, high selectivity
of CO2 over N2, suitable heat of adsorption,
and excellent dynamic CO2 capture capacity. As a result,
these graphene-derived porous carbons deserve consideration for removal
of CO2 from exhausted flue gas.
The
synthesis of carbonaceous CO2 adsorbents doped with nitrogen
were carried out via a hydrothermal reaction of biomass d-glucose, followed by urea treatment and K2CO3 activation. These carbons display high uptake of CO2 at
1 bar and 25 and 0 °C, up to 3.92 and 6.23 mmol g–1, respectively. Additionally, the as-synthesized materials exhibit
superior reusability, high CO2/N2 selectivity,
fast CO2 adsorption kinetics, and excellent dynamic capture
capacity at the experimental conditions used. The synthetic effect
of the nitrogen content and narrow microporosity decide the capture
capacity for CO2 at 1 bar and 25 °C for these N-enriched
carbonaceous adsorbents. This study provides a viable method to prepare
high-performance CO2 carbonaceous sorbents without using
caustic KOH. In addition, this work gives further insights into the
CO2 adsorption mechanism for nitrogen-doped porous carbon
sorbents and, hence, inspires ways to synthesize novel carbonaceous
materials for removing CO2 from combustion exhaust gases.
In
this study, N-enriched porous carbons were prepared by a facile
synthesis method at low temperatures ranging from 400 to 500 °C.
Sodium amide was used as both activator and nitridation reagent, and
lotus stalk was used as the carbon precursor. The as-synthesized samples
demonstrate the maximum CO2 uptake of 3.88 and 5.62 mmol/g
at 25 and 0 °C, respectively, at atmospheric pressure. Moreover,
these lotus stalk-derived adsorbents exhibit a rapid CO2 adsorption rate, high CO2/N2 selectivity,
moderate CO2 isosteric heat of adsorption, stable cyclic
ability, and excellent dynamic CO2 capture capacity. Systematic
research shows that, besides the volume of narrow micropore and nitrogen
content, the pore size distribution is also a non-negligible factor
in determining CO2 adsorption capacity under ambient condition
for these adsorbents. The good CO2 adsorption performance
together with single-step and low-temperature preparation indicates
that these sorbents are very promising for CO2 capture
from flue gas.
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