Carbon Dioxide Capture by Functionalized Solid Amine Sorbents with

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Carbon Dioxide Capture by Functionalized Solid Amine Sorbents with Simulated Flue Gas Conditions Yamin Liu, Qing Ye, Mei Shen, Jingjin Shi, Jie Chen, Hua Pan, Yao Shi *

Institute of Industrial Ecology and Environment, Department of Chemical and Biological Engineering,

Zhejiang University (Yuquan Campus)

Hangzhou 310027, P. R. China

* Corresponding author. e-mail: [email protected] (Y. Shi).

Phone: +86-571-88273591; Fax: +86-571-88273693

Supporting Information Contents: The explanation of Equation 1 Supplemental Tables S1-S4 Supplemental Figure S1-S3 Supplemental Reference

S1

The explanation of Equation 1 Adsorption capacity of CO2 on adsorbents (1 g) )at a certain time is calculated using Equation 1. Where qa is the adsorption capacity of CO2, mmol g-1; M is the weight of adsorbent, g; Q and Qou are the inlet and outlet gas flow rate, cm3 min-1; C0 and C are influent and effluent CO2 concentrations, vol.%; t denotes as time, min; T0 is 273 K and T is the gas temperature, K; Vm is 22.4 cm3 mmol-1. qa =

 T 1  t 1 ×  (Q × C 0 − Qou × C )dt  × 0 × M  0  T Vm



1

And Qou can be calculated using Equation 2.

Qou × (1 − C ) = Q × (1 − C0 )

2

So we can obtain the Equation 3 from Equation 1 and 2. qa =

C − C  T0 1  t 1 × Q× 0 × dt  × M  0 1− C  T Vm



3

Table S1 Isosteric Heats of 10% CO2 Adsorption on KIT-6-TEPA qa (mmol g-1)

-Qst (kJ mol-1)a

r2

293-333K 1.6

51.5

0.978

1.8

49.8

0.994

2.0

42.9

0.996

2.2

39.2

0.994

2.4

38.8

0.995

average

43.8

a: The “-” in front of Qst means that the adsorption process is exothermic. S2

Table S2. Energy requirement of the process adsorption adsorbent (g)

2

adsorbent density (g cm-3)

0.51

adsorption time(min)

20

amount of adsorbed CO2(g)

0.2816 desorption

desorption time(min)

11

amount of desorbed CO2(g)

0.2675

specific heat of adsorbent(J g-1 K)

0.96

energy for heating adsorbent (KJ)

0.0955

adsorption column (KJ)

0.011

desorption heat (KJ)

0.2716

total energy requirement(MJ kg-1CO2)

1.41

Table S3 Energies consumption for CO2 capture from literature and our work sorbent

process

purity

recovery

energy

(%)

(%)

(MJ kg-1CO2)

90

1.2~2.4

(S1)

MEA-MDEA advanced amine 90

Ref.

technologies UOP13X

VSA

95

67

1.1

(S2)

Zeolite 13X

PSA

90

85

1.7

(S3)

Zeolite 5A

TSA

94

83

4.4

(S4)

KIT-6-TEPA

VTSA

98

95

1.41

This work

S3

Table S4. Comparisons of gas conditions between liquid amine absorption and KIT-6-TEPA adsorption Temperature

RH

SO2

NOx

(K)

(%)

(ppm)

(ppm)

Liquid amine

≤313

≤100

≤10

≤400

(S1)

KIT-6-TEPA adsorption

313~353

≤100

≤100

≤400

This work

Figure S1. Schematic drawing for CO2 adsorption experimental system

S4

Ref.

Figure S2. Regression lines of lnP versus 1/T under various qa

Figure S3. Conceived schematic of multipollutant control including CO2 adsorption unit in a power plant

S5

Supplemental Reference (S1)

Aroonwilas, A.; Veawab, A. Integration of CO2 Capture Unit Using Blended MEA-AMP Solution Into Coal-Fired Power Plants. Greenhouse Gas Control Technologies. 9. 2009, 1, 4315-4321.

(S2) Zhang, J.; Webley, P. A. Cycle Development and Design for CO2 Capture from Flue Gas by Vacuum Swing Adsorption. Environ. Sci. Technol. 2008, 42,563-569. (S3) Agarwal, A.; Biegler, L. T.; Zitney, S. E. A Superstructure-Based Optimal Synthesis of PSA Cycles for Post-Combustion CO2 Capture. Aiche J. 2010, 56, 1813-1828. (S4) Merel, J.; Clausse, M.; Meunier, F. Experimental Investigation on CO2 Post-Combustion Capture by Indirect Thermal Swing Adsorption Using 13x and 5a Zeolites. Ind. Eng. Chem. Res. 2008, 47 ,209-215. (S5) Rao, A. B.; Rubin, E. S. A Technical, Economic, and Environmental Assessment of Amine-based CO2 Capture Technology for Power Plant Greenhouse Gas Control. Environ. Sci. Technol. 2002, 36,4467-4475.

S6