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@PHDTHESIS{Selmert:1047563,
author = {Selmert, Victor},
title = {{I}nvestigation of {P}olyacrylonitrile-based {C}arbon
{N}anofibers as {A}dsorbents for the {S}eparation of
{C}arbon {D}ioxide using {D}ynamic {G}as {A}dsorption},
school = {RWTH Aachen University},
type = {Dissertation},
publisher = {RWTH Aachen University},
reportid = {FZJ-2025-04389},
pages = {215},
year = {2025},
note = {Dissertation, RWTH Aachen University, 2025},
abstract = {Electrospun polyacrylonitrile-based carbon nanofibers
(CNFs) exhibit a molecular sieving effect. The pore size can
be controlled by the choice of the carbonization
temperature, making such nanofibers a promising material for
gas separation. In this work, these nanofibers are
investigated for the application in the field of gas
separation using dynamic gas adsorption and are tested
against common reference materials. These experiments allow
to analyze the adsorption behavior of a packed column of the
fibers in terms of selectivity, stability, as well as
adsorption and desorption kinetics under conditions similar
to the application in an adsorption swing process. First,
the procedure of the dynamic gas adsorption method is
optimized for small, laboratory-scale amounts of sample. It
is shown that an exact determination of the contribution of
the void volume is paramount for accurate results.
Furthermore, the measurement of desorption curves following
the breakthrough curves increases the accuracy in the case
of competitively adsorbing gases. In order to optimize the
volumetric packing density and the pressure drop along the
column, the pelletization of the fibers is also
investigated. It is shown that performing the pelletization
before carbonization of the fibers is advantageous, since
the low mechanical stability of the non-carbonized fibers
yields a greater compression of the fibrous material.
Accordingly, a higher bulk density and, thus, a higher
volumetric adsorption capacity is achieved. Subsequently,
the separation capabilities of the pelletized fibers are
evaluated on technically relevant separation problems such
as CO2 separation from N2-rich mixtures like flue gases or
CO2 and N2 separation from biogas-like or natural gas-like
mixtures. The CO2/N2 separation on the fibers shows an
exceptionally high selectivity, especially for a
carbon-based material, and exceeds the values for most
reference materials. The high selectivity of the CNFs is
attributed to the high adsorption potential of CO2
associated with the narrow ultramicropores as well as the
high heteroatom content present in CNFs carbonized at low
temperature. In contrast, the separation of CO2 and N2 from
CH4-richgas mixtures is kinetically driven and based on the
size difference of CH4 to N2 and CO2 and on the narrow pores
of the fibers. At higher carbonization temperature and thus,
a narrower pore system, CH4 is excluded from the pores,
leading to a strong kinetic limitation, while CO2 as well as
N2 are adsorbed sufficiently fast. While the separation
performance is attributed to the surface chemistry for the
CO2/N2 mixture, the separation performance for CO2 and N2
from CH4 is based on the molecularsieve effect. Water
adsorption experiments show that the CNFs adsorb water with
high affinity and to a high adsorption capacity, which has
significant influence on the CO2 adsorption. In cyclic
adsorption/desorption experiments with moistened CO2, there
is an accumulation of water on the CNFs, which reduces the
CO2 capacity significantly. Therefore, drying of the gas
mixture is necessary in order to apply the fibers for CO2
separation. However, the high water affinity also proves
that the CNFs could be applied in the field gas drying as
well. Overall, the electrospun polyacrylonitrile-based CNFs
achieve a selective separation in the tested applications
and offer the possibility to adjust selectivity as well as
kinetics via the carbonization temperature to the needs of a
given separation problem. Therefore, the material proves to
be promising for the separation of CO2 from dry gas mixtures
or for the drying of gases.},
keywords = {Hochschulschrift (Other) / carbon nanofibers ; gas
separation ; adsorption ; carbon capture ; carbon molecular
sieve ; breakthrough curve (Other)},
cin = {IET-1},
cid = {I:(DE-Juel1)IET-1-20110218},
pnm = {1232 - Power-based Fuels and Chemicals (POF4-123) / DFG
project G:(GEPRIS)390919832 - EXC 2186: Das Fuel Science
Center – Adaptive Umwandlungssysteme für erneuerbare
Energie- und Kohlenstoffquellen (390919832) / HITEC -
Helmholtz Interdisciplinary Doctoral Training in Energy and
Climate Research (HITEC) (HITEC-20170406)},
pid = {G:(DE-HGF)POF4-1232 / G:(GEPRIS)390919832 /
G:(DE-Juel1)HITEC-20170406},
typ = {PUB:(DE-HGF)11},
doi = {10.18154/RWTH-2025-05853},
url = {https://juser.fz-juelich.de/record/1047563},
}