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Mesoporous carbon xerogel as a promising adsorbent for capture and storage of liquified natural gas vapors

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Abstract

Capture and storage of LNG vapors in the adsorbed state is envisioned as an effective way to improve the LNG terminal performance. A synthetic carbon xerogel was proposed as a promising adsorbent for methane vapors in the LNG terminal combined with an adsorbed natural gas (ANG) module. The textural properties of the adsorbent were investigated by X-ray diffraction, scanning electron microscopy, and low-temperature nitrogen adsorption. An approach based on the theories of volume filling of micropores, a monolayer capacity on the mesopore surface, and the capillary condensation in the mesopores was applied to the experimental data on methane adsorption to evaluate the adsorption capacity of the adsorbent over the sub- and supercritical P,T-ranges. It was found that the capillary condensation of methane in mesopores ensured an extraordinary adsorption capacity of the adsorbent, achieving 540 m3(NTP)·m−3 at the boiling point. The adsorption- and temperature-induced deformation of the adsorbent, and the thermal effects arising during adsorption were examined with a view of the performance of the LNG terminal combined with the adsorber for capturing and accumulating LNG vapors. The ANG tank loaded with the carbon xerogel ensured the maximum amount of gas supplied to the consumer at temperatures close to 140 K. A comparison of the adsorption performances of the carbon xerogel and a commercial activated carbon characterized by a wider pore size distribution made it possible to identify a difference in the optimal operational conditions of their application for the LNG–ANG technology.

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Data availability

The data that support the findings of this study are available from the corresponding author, I.E. Men’shchikov upon reasonable request.

Abbreviations

ALNG:

Adsorption-based capture of LNG vapors

ANG:

Adsorbed natural gas

ASC:

Activated carbon prepared from silicon carbide

BET:

Brunauer–Emmett–Teller

CX:

Carbon xerogel

CNG:

Compressed natural gas

CLTE:

Coefficient of linear thermal expansion

D-A:

Dubinin–Astakhov equation

D-R:

Dubinin–Radushkevich equation

EDX:

Energy dispersive X-ray

LNG:

Liquified natural gas

MOF:

Metal-organic framework

NG:

Natural gas

NLDFT:

Non-local density functional theory

NTP:

Normal temperature and pressure: 293 K and 101,325 Pa

PSD:

Pore size distribution

STP:

Standard temperature and pressure: 273.15 K and 100,000 Pa

XRD:

X-ray diffraction

A :

Differential molar work of adsorption [kJ·mol−1]

a :

Value of adsorption [mmol·g−1]

a 0 :

Limiting value of adsorption at a pressure equal to the saturated vapor pressure P0 [mmol·g−1]

a K :

Value of adsorption through capillary condensation in mesopores [mmol·g−1]

a meso :

Value of adsorption on the surface of the meso- and macropores through the formation of a monolayer [mmol·g−1]

a micro :

Value of adsorption in micropores through the micropore volume filling [mmol·g−1]

D 0 :

Effective diameter of micropores [nm]

d CX :

Density of the carbon xerogel rod evaluated from its dimensions and weight [kg·m−3]

D meso max :

Pore diameter corresponding to the maximum peak of the PSD functions for mesoporosity [nm]

D micro max :

Pore diameter corresponding to the maximum peak of the PSD functions for microporosity [nm]

E 0 :

Standard characteristic energy of adsorption [kJ·mol−1]

h g :

Molar enthalpy of the equilibrium gas phase [kJ·mol−1]

h 1 :

Differential molar enthalpy of the adsorption phase [kJ·mol−1]

k :

Correction for the methane adsorption in a monolayer on the surface of mesopores [mmol·(g·Pa)−1]

l 0 :

Initial length of the CX sample [mm]

m a :

Mass of regenerated adsorbent [g]

m am :

Mass of a quartz mockup [g]

m g :

Mass of methane adsorbed at specified pressure P and temperature T [g]

m gm :

Mass of methane adsorbed in the system when using the mockup [g]

n :

Dimensionless parameter related to the heterogeneity of the porous structure associated with the pore size distribution

P 0 :

The saturated vapor pressure [Pa]

P cr :

Critical pressure [Pa]

q st :

Differential molar isosteric heat of adsorption [kJ·mol−1]

R :

Universal gas constant [J/(mol·K]

S BET :

Specific BET surface area [m2·g−1]

S meso :

Specific surface area of mesopores [m2·g−1]

s 1 :

Differential molar entropy [kJ·(mol·K)−1]

s g :

Entropy of methane in the bulk phase [kJ·(mol·K)−1]

T b :

Boiling point [K]

T cr :

Critical temperature [K]

T D :

Discharge temperature [K]

T w :

Working temperature in the ALNG tank [K]

V A(P,T):

Total specific volumes of gas in the adsorbed state in a closed system of unit volume loaded with an adsorbent under specified pressure and temperature P and T [m3(NTP)·m−3]

V a :

Reduced volume of the adsorbent-adsorbate system [cm3·g−1]

V eff :

Specific methane volume that is discharged from the ALNG storage system to a consumer [m3(NTP)·m−3]

V G(P,T):

Total specific volume of free gas in a closed system of unit volume loaded with an adsorbent under specified pressure and temperature P and T [m3(NTP)·m−3]

V 0 :

Volume of the regenerated adsorbent with pores [cm3]

V Σ :

Total specific volumetric capacity of the ANG system [m3(NTP)·m−3]

ν g :

Specific gas phase volume [m3·kg−1]

W 0 :

Specific volume [cm3·g−1]

W meso :

Specific volume of mesopores [cm3·g−1]

W T :

Total pore volume [cm3·g−1]

w MOL :

Effective thickness of the adsorbed methane layer in mesopores [m]

Z :

Compressibility of the equilibrium gas phase at the specified temperature and pressure

α:

Coefficient of linear thermal expansion of adsorbent [K−1]

αII :

Coefficient of linear thermal expansion of a graphite crystal in a plane parallel and to a main crystallographic axis (or c-axis) [K−1]

α⊥ :

Coefficient of linear thermal expansion of a graphite crystal in a plane perpendicular to a main crystallographic axis [K−1]

Δl :

Absolute change in the CX adsorbent length [mm]

ε:

Porosity of the adsorbent layer or the fraction of the volume free of the adsorbent

η:

Relative linear deformation of carbon xerogel [%]

ηa :

Relative linear adsorption-stimulated deformation of carbon xerogel [%]

θ:

Scattering angle of X-rays relative to the incident beam

μ:

Molar mass [g·mol−1]

ρ:

Density of methane in a monolayer [g·m−3] 

ρa :

Skeletal density of the adsorbent calculated from helium pycnometry data [g·cm−3]

ρm :

Density of the quartz mockup [g·cm−3]

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Acknowledgements

We thank Dr. Gudrun Reichenauer from the Bavarian Center for Applied Energy Research (ZAE Bayern) for providing the sample of carbon xerogel. We also thank A.A. Shiryaev and V.V. Vysotskii for their help in the XRD and SEM experiments and constructive suggestions. The experiments were carried out with the use of equipment of the Center of Physical Methods of Investigations of the A.N. Frumkin Institute of Physical Chemistry and Electrochemistry of Russian Academy of Sciences.

Funding

The work was supported by the Russian Science Foundation (grant no. 22-73-00184).

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Authors and Affiliations

  1. M.M. Dubinin Laboratory of Sorption Processes, Frumkin Institute of Physical Chemistry and Electrochemistry, Russian Academy of Sciences, Leninskii Prospect, 31, Build. 4, 119071, Moscow, Russia

    Ilya E. Men’shchikov, Andrey V. Shkolin, Elena V. Khozina, Alexander E. Grinchenko & Anatoly A. Fomkin

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  1. Ilya E. Men’shchikov
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  2. Andrey V. Shkolin
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  3. Elena V. Khozina
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  4. Alexander E. Grinchenko
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  5. Anatoly A. Fomkin
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Contributions

Conceptualization: I.M., A.S., A.F.; methodology: A.S., I.M.; software: I.M., A.G.; validation: A.F., A.S.; formal analysis: A.G.; investigation: I.M., A.S., A.G.; resources: A.S.; data curation: A.S., E.K.; writing—original draft preparation: A.S., I.M., E.K.; writing—review and editing: E.K., A.F.; visualization: A.G., I.M., E.K.; supervision: I.M.; project administration: I.M., funding acquisition: I.M. All authors have read and agreed to the published version of the manuscript.

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Correspondence to Ilya E. Men’shchikov.

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The authors declare no conflict of interest. The funders had no role in the design of the study; in the collection, analyses, or interpretation of data; in the writing of the manuscript, or in the decision to publish the results.

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Men’shchikov, I.E., Shkolin, A.V., Khozina, E.V. et al. Mesoporous carbon xerogel as a promising adsorbent for capture and storage of liquified natural gas vapors. Adsorption 29, 255–273 (2023). https://doi.org/10.1007/s10450-023-00411-0

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