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CO2 adsorption capacity of modified LDHs at different temperatures

https://doi.org/10.1016/j.xcrp.2021.100484

“We have measured the CO2 adsorption isotherms at 25°C for all of the adsorbents prepared (Figure 3A). While the TRI-grafted bulk and stacked LDHs exhibited poor CO2 capacities under ultradilute conditions, obvious improvements were observed for TRI-grafted AMO-LDHs. Remarkably, TRI-Mg0.55Al-a achieved a CO2 uptake capacity of 1.049 mmol g−1 upon exposure to 0.4 mbar CO2, which is 16.7 times higher than that of TRI-Mg0.55Al-w (0.063 mmol g−1) and 30% higher than TRI-SBA-15 (0.808 mmol g−1). The fast coprecipitation process did not significantly improve the capacity of TRI-LDHs, which indicates that both reduction in LDH size and thickness and morphology exfoliation play an important role in establishing the desired amine-grafting sites. The monoamine-grafted AMO-LDHs were also tested. They exhibit a very promising capacity of 0.416 mmol g−1 for APS-Mg2Al-a and 0.778 mmol g−1 for APS-Mg0.55Al-a in 0.4 mbar.”

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Figure 3. CO2 adsorption capacity of modified LDHs

(A) Screening of CO2 adsorption isotherms of amine-grafted samples at 25°C.

(B) CO2 adsorption isotherms of TRI-Mg0.55Al-a at 25°C, 45°C, and 65°C.

(C) Isosteric heats of adsorption onto TRI-Mg0.55Al-a.

(D) CO2 adsorption capacities under 0.4 mbar and 25°C as a function of amine loadings.”

“Considering the low physisorption capacities of the LDHs under 0.4 mbar at 25°C (Figure S4) and the decreased surface areas after amine grafting, the enhanced CO2 capacity seen for TRI-LDHs is mainly attributed to chemisorption by the amine functional groups. The isosteric heat of adsorption of TRI-Mg0.55Al-a samples was calculated according to the Clausius-Clapeyron relation from isotherms measured at 25°C, 45°C, and 65°C (Figures 3B and 3C). The heat of adsorption was underestimated at low CO2 coverages, but quickly approached 79 kJ mol−1 and remained above 65 kJ mol−1 for loadings of up to 1.2 mmol g−1, which is typical for CO2 chemisorption on amines.36 At higher surface coverages, physisorption dominates the adsorption process, with the heat of adsorption ranging from 15 to 40 kJ mol−1.35

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