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Adsorption

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Measurement of competitive CO2 and N2 adsorption on Zeolite 13X for post-combustion CO2 capture

  • Nicholas Stiles Wilkins
  • Arvind Rajendran
Article

Abstract

Single component CO2 and N2 equilibrium loadings were measured on Zeochem Zeolite 13X from 0 to 150 °C and 0–5 bar using volumetry and gravimetry. CO2 equilibrium data was fit to a dual-site Langmuir (DSL) isotherm. The equilibrium data for N2 was fit using four isotherm schemes: two single site Langmuir isotherms, the DSL with the equal energy sites and the DSL with unequal energy site pairings. A series of single and multicomponent CO2 and N2 dynamic column breakthrough (DCB) experiments were measured on Zeolite 13X at 22 °C and 0.98 bar. The adsorption breakthrough experiments were able to provide accurate data for CO2 competitive adsorption, while failing to provide reliable N2 data. It was shown that desorption experiments from a bed fully saturated with the desired composition provides a better estimate of the competitive N2 loading. A detailed mathematical model that used inputs from the batch equilibrium experiments was able to predict the composition and thermal breakthrough curves well while underpredicting the single component N2 loading. The DSL isotherm with unequal energy sites was shown to predict the competitive loading and breakthrough curves well. The impact of the chosen adsorption isotherm model on process performance was evaluated by simulating a 4-step vacuum swing adsorption process to concentrate CO2 from dry post-combustion flue gas. The results show that the purity, recovery, energy and productivity are affected by the choice of the competitive adsorption isotherm.

Keywords

Dynamic column breakthrough Desorption Post-combustion carbon capture Carbon dioxide Nitrogen Zeolite 13X 

Abbreviations

CCS

Carbon capture and storage

DCB

Dynamic column breakthrough

DSL

Dual-site Langmuir isotherm

DOE

Department of energy

EES

Equal energy site DSL model

IAST

Ideal adsorbed solution theory

LDF

Linear driving force

MFC

Mass flow controller

MFM

Mass flow meter

MS

Mass spectrometer

MSB

Magnetic suspension balance

ODE

Ordinary differential equation

PN

Perfect negative pairing

PP

Perfect positive pairing

PSA

Pressure-swing adsorption

PT

Pressure transducer

\(\Delta\) PT

Differential pressure transducer

SSL

Single-site Langmuir model

TC

Thermocouple

UES

Unequal energy site DSL model

VSA

Vacuum-swing adsorption

Roman symbols

A

Adsorbent surface area (m2)

b

Adsorption equilibrium constant for site 1 (m\(^{3}\) mol−1)

c

Fluid phase concentration (mol m−3)

\(C_\text {p}\)

Heat capacity (J mol−1 K−1)

d

Adsorption equilibrium constant for site 2 (m\(^{3}\) mol−1)

D

Diffusivity (m\(^2\) s−1)

E

Energy consumption (\(\text {kWh}_\text {e}\) tonne of CO2 captured−1)

h

Heat transfer coefficient (W m−2 K−1)

\(\Delta H\)

Heat of adsorption (J mol−1)

k

Mass transfer coefficient (s−1)

K

Thermal conductivity (W m−1 K−1)

L

Length (m)

m

Adsorbent mass (kg)

n

Number of species (–)

p

Partial pressure (bar)

P

Total pressure (bar)

Pu

Purity (mol%)

Pr

Productivity (mol CO2 m−3  s−1)

q

Solid phase loading (mol kg−1)

\(q^*\)

Equilibrium solid phase loading (mol kg−1)

Q

Outlet volumetric flow rate (m\(^3\) s−1)

r

Radius (m)

R

Universal gas constant (Pa m\(^{3}\) mol−1 K−1)

Re

Recovery (%)

t

Time (s)

\({\bar{t}}\)

dimensionless time (–)

T

Temperature (K)

\(\Delta U\)

Internal energy (J mol−1)

v

Interstitial velocity (m s−1)

V

Volume (m\(^{3}\))

x

Solid phase fraction (–)

y

Mole fraction (–)

z

Axial direction (m)

Greek symbols

\(\alpha\)

Competitive selectivity (–)

\(\gamma\)

\(C_\text {p}/C_\text {v}\) (–)

\(\epsilon\)

Bed voidage (–)

\(\eta\)

Vacuum pump efficiency (–)

\(\mu\)

Viscosity (Pa s−1)

\(\pi\)

Spreading pressure (Pa)

\(\rho\)

Adsorbent density (kg m−3)

\(\tau\)

Tortuosity (–)

Subscripts and superscripts

a

Adsorbed phase

acc

Solid and fluid phase accumulation

ads

Adsorbent or adsorption

amb

Ambient

ADS

Adsorption step

ave

Average

b

Bed or column

BLO

Blowdown step

comp

Component

d

Extra-column

des

Desorption

EVAC

Evacuation step

g

Fluid phase

H

High

i

Index of species

I

Intermediate

iso

Isosteric

in

Inlet or internal

L

Length or low

LPP

Light product pressurization

m

Molecular

o

At the spreading pressure

out

Outlet or external

p

Particle

scaled

Linear regression fit energy

s

Solid phase

sat

Ultimate saturation

tot

Total

w

Wall

z

Axial direction

0

Initial

Notes

Acknowledgements

Funding support from the Canada Foundation for Innovation Project Number 33801 and Canada First Excellence Fund through University of Alberta Future Energy Systems are acknowledged. We thank Zeochem for providing samples of the Zeolite 13X used in this study.

Supplementary material

10450_2018_4_MOESM1_ESM.pdf (1.2 mb)
Supplementary material 1 (pdf 1248 KB)

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Copyright information

© Springer Science+Business Media, LLC, part of Springer Nature 2019

Authors and Affiliations

  1. 1.Department of Chemical and Materials EngineeringUniversity of Alberta Donadeo Innovation Centre of EngineeringEdmontonCanada

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