CO<sub>2</sub> Deactivation of Supported Amines: Does the Nature of Amine Matter?

Sayari, Abdelhamid; Belmabkhout, Youssef; Da’na, Enshirah

doi:10.1021/la204667v

Cited by 178 publications

(206 citation statements)

References 47 publications

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“…Only a few works have considered the recyclability and degradation in terms of the stability of CO 2 adsorbents. 6,[13][14][15][16] (vi) Tolerance to impurities: The degree of tolerance and the affinity of the adsorbent to impurities such as moisture and acid gases may significantly affect their use. When materials are affected by such impurities, additional purification steps are required.…”

Section: Discussionmentioning

confidence: 99%

Low concentration CO2 capture using physical adsorbents: Are metal–organic frameworks becoming the new benchmark materials?

Belmabkhout¹,

Guillerm²,

Eddaoudi³

2016

Chemical Engineering Journal

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277

168

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KeywordsCO 2 capture, traces CO 2 removal, air capture, physical adsorbents, MOFs AbstractThe capture and separation of traces and concentrated CO 2 from important commodities such as CH 4 , H 2 , O 2 and N 2, is becoming important in many areas related to energy security and environmental sustainability. While trace CO 2 concentration removal applications have been modestly studied for decades, the spike in interest in the capture of concentrated CO 2 was motivated by the need for new energy vectors to replace highly concentrated carbon fuels and the necessity to reduce emissions from fossil fuel-fired power plants. CO 2 capture from various gas streams, at different concentrations, using physical adsorbents, such as activated carbon, zeolites, and metal-organic frameworks (MOFs), is attractive. However, the adsorbents must be designed with consideration of many parameters including CO 2 affinity, kinetics, energetics, stability, capture mechanism, in addition to cost. Here, we perform a systematic analysis regarding the key technical parameters that are required for the best CO 2 capture performance using physical adsorbents. We also experimentally demonstrate a suitable 2 material model of Metal Organic Framework as advanced adsorbents with unprecedented properties for CO 2 capture in a wide range of CO 2 concentration. These recently developed class of MOF adsorbents represent a breakthrough finding in the removal of traces CO 2 using physical adsorption.This platform shows colossal tuning potential for more efficient separation agents.

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Section: Discussionmentioning

confidence: 99%

Low concentration CO2 capture using physical adsorbents: Are metal–organic frameworks becoming the new benchmark materials?

Belmabkhout¹,

Guillerm²,

Eddaoudi³

2016

Chemical Engineering Journal

Self Cite

277

168

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“…This capacity loss is suggested to be mainly due to the deactivation of secondary amine groups as a result of non-desorbed SO 2 , which was strongly bonded to the fiber adsorbents. The other possible reason for this capacity loss could be due to the presence of some propylamine impurities in MAPS silane [41,42]. Correspondingly, the deactivation of primary amine impurities upon exposure to SO 2 would lead to the loss of capacity as well.…”

Section: Cyclic Stability Of Secondary Amine Adsorbent Ca-s-mapsmentioning

confidence: 99%

Stability of amine-based hollow fiber CO2 adsorbents in the presence of NO and SO2

Fan

Rezaei

Labreche

et al. 2015

Fuel

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h i g h l i g h t s SO 2 -deactivated primary amine fibers reversibly adsorb additional SO 2 . Secondary amine fibers exhibit better SO 2 tolerance than primary amine fibers. Tertiary amine grafted fibers have good SO 2 reversibility under dry or humid conditions. NO does not affect the CO 2 capacity of the fibers over 120 adsorption-desorption cycles. a b s t r a c tComparative studies of the cyclic stability of primary, secondary, and tertiary amine-grafted silica/polymer composite fiber adsorbents upon exposure to simulated flue gas are reported. A simulated dry flue gas mixture with 200 ppm NO does not cause degradation of the amine grafted fiber adsorbents and all fibers retain their CO 2 capacity in the presence of NO. In contrast, upon exposure to dry flue gas in the presence of 200 ppm SO 2 at 35°C, the primary amine containing adsorbent, CA-S-APS, shows a CO 2 capacity reduction of 55% over 120 cyclic adsorption-desorption runs. As the initial SO 2 induced degradation occurs in this adsorbent, the amine sites first irreversibly adsorb SO 2 and then begin to gradually adsorb SO 2 reversibly, as evidenced from a quantitative comparison of the amount of adsorbed SO 2 to the amount of desorbed SO 2 . The secondary amine containing adsorbent, CA-S-MAPS, exhibits an improved stability and approximately 25% CO 2 capacity loss is observed during cycling in the presence of SO 2 . Therefore, the secondary amine based CA-S-MAPS adsorbent demonstrates some degree of tolerance to SO 2 in comparison to the CA-S-APS sample. Under humid conditions, SO 2 imposes significant detrimental impacts on the two adsorbents, as a result of increased SO 2 adsorption capacities in the presence of moisture. Although the CO 2 uptake is nearly zero in the tertiary amine adsorbent, CA-S-DMAPS, the SO 2 capacity of this adsorbent reaches 0.43 mmol/g under humid conditions and this material has the highest SO 2 /N ratio of the fiber adsorbents studied. More importantly, this CA-S-DMAPS sample demonstrates reversible SO 2 adsorption, as indicated from the SO 2 cyclic adsorption experiments. The tertiary amine based fiber adsorbents have good potential for flue gas desulfurization, with advantageous characteristics of high SO 2 /N ratio, excellent reversibility, low CO 2 adsorption and relatively low regeneration temperature.

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“…[5] However,t his system is far from being optimal due to problems of corrosion, amine degradation and high energy consumption for regeneratingt he solutions. [6][7][8] Anchoring of polyamines onto solid supports hasb een proposed as an alternative to using aqueous solutions. In contrast to small amine scrubbers, solid-supported polymerica mines offer significant advantages for CO 2 capture, including the potential elimination of corrosion, alower energy cost for sorbent regeneration, and sufficiently low volatilities for avoiding excessive loss of activity.…”

Section: Introductionmentioning

confidence: 99%

Effect of Chain Topology of Polyethylenimine on Physisorption and Chemisorption of Carbon Dioxide

et al. 2015

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Polyethylenimine (PEI) is a promising candidate for CO2 capture. In this work, the physisorption and chemisorption of CO2 on various low-molecular-weight PEIs are investigated to identify the effect of chain architecture on sorption. The reliability of theoretical calculations are partially supported by our experimental measurements. Physisorption is calculated independently by the reference interaction-site model integral equation theory; chemisorption is distinguished from the total sorption given by the quantum density functional theory. It is shown that, as the chain length increases, both chemisorption and physisorption drop off nonlinearly, but the decay amplitude of chemisorption is more apparent. Conversely, as the amine group approaches the central triamine unit of each oligomer, the sorption capacity decreases, affecting the sorption equilibrium in a complex way. This arises from the cooperative contribution of an increased steric effect and renormalized electronic distribution.

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CO₂ Deactivation of Supported Amines: Does the Nature of Amine Matter?

Cited by 178 publications

References 47 publications

Low concentration CO2 capture using physical adsorbents: Are metal–organic frameworks becoming the new benchmark materials?

Low concentration CO2 capture using physical adsorbents: Are metal–organic frameworks becoming the new benchmark materials?

Stability of amine-based hollow fiber CO2 adsorbents in the presence of NO and SO2

Effect of Chain Topology of Polyethylenimine on Physisorption and Chemisorption of Carbon Dioxide

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CO2 Deactivation of Supported Amines: Does the Nature of Amine Matter?

Cited by 178 publications

References 47 publications

Low concentration CO2 capture using physical adsorbents: Are metal–organic frameworks becoming the new benchmark materials?

Low concentration CO2 capture using physical adsorbents: Are metal–organic frameworks becoming the new benchmark materials?

Stability of amine-based hollow fiber CO2 adsorbents in the presence of NO and SO2

Effect of Chain Topology of Polyethylenimine on Physisorption and Chemisorption of Carbon Dioxide

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CO₂ Deactivation of Supported Amines: Does the Nature of Amine Matter?