Nitrogen-Doped Ultrahigh Microporous Carbons Derived from Two Nitrogen-Containing Post-Cross-Linked Polymers for Efficient CO2 Capture
2020
The
nitrogen (N)-doped porous carbons have always been one of the
important categories of the adsorbents for CO2 capture.
Herein, we prepared N-doped porous carbons from two kinds of N-containing
post-cross-linked polymers (HPDV and HPDN) by KOH activation carbonization.
By changing the carbonization temperature and KOH dosage, the porosity
and chemical structure of two porous carbons were effectively tuned,
and strictly N-doped microporous carbons with ultrahigh microporosity
were acquired (80.00–90.00%). They exhibited high CO2 uptake (3.93–6.56 mmol/g at 273 K and 1 bar), acceptable
CO2/N2 selectivity (IAST: 21.5–39.7),
moderate isosteric heat of adsorption (20.3–41.8 kJ/mol), and
good reusability. Moreover, the adsorption energy results from DFT
calculation indicated that diversified N-functional groups had improved
CO2 uptake through Lewis acid–base interactions
and hydrogen-bonding interactions, and the study further clarified
that the large micropore volume, especially the ultramicropore volume
(Vultra, d < 0.8 nm),
played a key role for CO2 capture. These porous carbons
developed therein become promising CO2 adsorbents.
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