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EU funded Project Innovation and Networks Executive Agency (INEA) Grant Agreement Number: 727734

h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

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Page 1: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

EU funded Project

Innovation and Networks Executive Agency(INEA)

Grant Agreement Number: 727734

Page 2: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Molecular Models Transport properties Explicit ionic species Polymer chain

conformation

SAFT Equation of State Water absorption “Reaction” equilibrium Speciation

Hard Chains Dispersion Association

Reference Fluid Molecular Interactions Ion-Ion

+ -

+ +

Empirical Models Diffusivity correlation Hydration/Permeabilit

y relationship Macroscopic behavior

Kim, T. J., Li, B., & Hägg, M. B., J. Pol. Sci. B: Pol. Phys., 42 (23), 4326-4336, 2004

Page 3: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Facilitated Transport for Gas Separation

Fixed CarrierMobile Carrier

Transport Mechanism

Dense

Solution Diffusion

i = 1…,nc

Sol-Diff Flux

FacilitatedSolution Diffusion

Chemical Reaction&

Facilitated Flux

Improved Performance

Page 4: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Highest Density of Amino Group on Chain

POLYBASE PROPERTIES Suitable for CO2 separation

Poly-(vinylamine)

Page 5: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

L. Deng and M. B. Hägg, J. Mem. Sci. 363, 295-301 (2010)

R. H. vs. Permeance+ CO2 absorption+ Reaction products+ Permeant mobility

Swelling Regimes

Page 6: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

0.1gH2OgPVAm

Water clusters as effective free volume Pore limiting diameter Pore size distribution Percolation degree

What is the effect of (poly) electrolytes?

0.5gH2OgPVAm

0.9gH2OgPVAm

Page 7: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Black: Neutral PVAmRed: 20% Protonated PVAmBlue: 50% Protonated PVAm

Page 8: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Simulated displacement as function of time

Diffusive dynamics dominated by H2O Pore limiting diameter Pore size distribution Percolation degree

Charged particles strongly couple to polymer motion

Page 9: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Black: Neutral PVAmRed: 20% Protonated PVAmBlue: 50% Protonated PVAm

Upper shaded area: maximum pore volumeLower shaded area: limiting pore diameter

a

Ac-

Slow-moving ionic species obstruct water channel formation

Page 10: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh
Page 11: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Black: Neutral PVAmRed: 20% Protonated PVAmBlue: 50% Protonated PVAmGreen: Bulk water

Similar activation energies, different volume effects

For highly hydrated systems, diffusion follows Arrhenius power law behavior. Tortuosity-controlled environment as function of protonation.

Page 12: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Numerous polymer + solvent theories, e.g. Mackie-Meares equation

D : diffusion coefficientD0 : bulk solvent diffusion coefficientΦ : effective free volume

H2O + gas solutes

J.S. Mackie, P. Meares, Proc. R. Soc. London A232, 1955

Page 13: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Black: Neutral PVAmRed: 20% Protonated PVAmBlue: 50% Protonated PVAm

For high T M-M model reasonable=Free volume effect

For low T, M-M model fails=Solvent-polymer coupling > kT

Page 14: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Ac-

Protonation-dependent Percolation threshold Charge groups acting

as gatekeepers H2O and gas transport

modulated by H2O channels

Free-volume effects dominate for high-T Decoupling of solvent-

polymer interactions H2O and gas diffusion

modulated by H2O

Effective Free Volume Ions strongly couple to

amine groups

Page 15: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Molecular Models Transport properties Explicit ionic species Polymer chain

conformation

SAFT Equation of State Water absorption “Reaction” equilibrium Speciation

Hard Chains Dispersion Association

Reference Fluid Molecular Interactions Ion-Ion

+ -

+ +

Empirical Models Diffusivity correlation Hydration/Permeabilit

y relationship Macroscopic behavior

Kim, T. J., Li, B., & Hägg, M. B., J. Pol. Sci. B: Pol. Phys., 42 (23), 4326-4336, 2004

Page 16: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

H2O + -[RNH2]- + CO2 HCO3- + -[RNH3

+]-

Reacting Water Swollen Polymer System

PVAm

Adsorbed Water Molecules Enhance the Reaction

Page 17: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Reacting Water Swollen Polymer System

PVAm

Adsorbed Water Molecules Swell the Polymer Matrix

Adsorbed Water Molecules Open New ‘Windows’

Page 18: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

-12

-11

-10

-9

-8

-7

-6

-5

-4

-3

-2

0.000 0.100 0.200 0.300 0.400 0.500

log

D [c

m2 /

s]

Water Content [g/g]

Water Diffusion in PVAm (35°C)H2O in PVAm Water Self DiffusionFirst Regime Second Regime

Two Regimes Identified:

- Water Sorption Around Amino Groups- Water Sorption in a Water Medium Environment

Page 19: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1

0.000 0.100 0.200 0.300 0.400 0.500

Poro

sity

Water Content [g/g]

Matrix Porosity

Two Regimes Identified:

- Water Sorption Around Amino Group- Water Sorption in a Water Medium Environment

S. Prager, J. Chem. Phys., 1960Choi P. et al., J. Electrochem Soc., 2005

Page 20: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

0

0.5

1

1.5

2

2.5

0.000 0.100 0.200 0.300 0.400 0.500

Tort

uosi

ty

Water Content [g/g]

Marix Tortuosity

Two Regimes Identified:

- Water Sorption Around Amino Group- Water Sorption in a Water Medium Environment

S. Prager, J. Chem. Phys., 1960Choi P. et al., J. Electrochem Soc., 2005

Page 21: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

PC-SAFT EoSPerturbed Chain Statistical Associating Fluid Theory Equation of State

(charged) Hard Chains Dispersive Interactions Associative Interactions

Reference Fluid Molecular Interactions

ares = aref + adisp+ ahb + aion

Ion interactions

+ -

+ +

Gross, Sadowski, Ind. Eng. Chem. Res., 2001Naeem, Sadowski, Fluid Phase Equilib, 2010

Huang, Radosz, Ind. Eng. Chem. Res., 1990

Page 22: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Water 2B: 2sites for H Bond (+/-)PVAm 2B: 2sites for H Bond (+/-)

PVAm / Water

Page 23: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

CO2 / Water

Water 2B: 2sites for H Bond (+/-)CO2 2B: 2sites for H Bond (+/-)

Page 24: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1

0.000001 0.00001 0.0001 0.001 0.01 0.1 1 10 100 1000 10000

RH

P CO2 kPa

0.01 g CO2 /g PVAm_308.15K 0.05 g CO2 / g PVAm_308.15K0.1 g CO2 / g PVAm_308.15K 0.15 g CO2 / g PVAm_308.15K0.2 g CO2 / g PVAm_308.15K 0.3 g CO2 / g PVAm_308.15K0.01 g CO2 /g PVAm_358.15K 0.05 g CO2 / g PVAm_358.15K0.1 g CO2 / g PVAm_358.15K 0.15 g CO2 / g PVAm_358.15K0.2 g CO2 / g PVAm_358.15K 0.3 g CO2 / g PVAm_358.15K

PVAm / CO2 / Water

Water 2B: 2sites for H Bond (+/-) CO2 2B: 2sites for H Bond (+/-)PVAm 2B: 2sites for H Bond (+/-)

T

Page 25: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

Understanding Diffusivity

The increase in water content open new windows in the internal structure

At higher water content the species flow towards the water channels

This causes the higher mobility / diffusivity values

Understanding Solubility

The PC-SAFT it is able to describe the water uptake in PVAm

The chemical reaction used can explain the water role in the ion formation

The pePC-SAFT can predict the total CO2

uptake as function of process parameters: Temperature Relative Humidity Partial

Pressure

Page 26: h ( µ v W } i / v v } À ] } v v E Á } l Æ µ ] À P v Ç ~/E€¦ · 0rohfxodu 0rghov 7udqvsruw surshuwlhv ([solflw lrqlf vshflhv 3ro\phu fkdlq frqirupdwlrq 6$)7 (txdwlrq ri 6wdwh

GUÓA DIDÆCTICA - Bautismo y Confirmación - Mayo 2018 · // X > } u v } o / v ] ] ] v ] ] v Ç v µ ] P v µ u } v u µ Ç v µ v µ ] P v µ v µ v o } µ } v }

GUÓA DIDÆCTICA - Bautismo y Confirmación - Mayo 2018 · // X > } u v } o / v ] ] ] v ] ] v Ç v µ ] P v µ u } v u µ Ç v µ v µ ] P v µ v µ v o } µ } v }

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