Hydrothermal Synthesis of Sub-20 nm Amine-Functionalized MIL-101(Cr) Nanoparticles with High Surface Area and Enhanced CO2 Uptake
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acs.iecr.0c00535.pdf
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Published version
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3.1 MB
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Author(s) • • •
Han, Gang
Qian, Qihui
Mizrahi Rodriguez, Katherine
Smith, Zachary
Date Issued
March 2020
Journal
Industrial and Engineering Chemistry Research
Publisher
American Chemical Society (ACS)
Citation
Han, Gang et al. "Hydrothermal Synthesis of Sub-20 nm Amine-Functionalized MIL-101(Cr) Nanoparticles with High Surface Area and Enhanced CO2 Uptake." Industrial and Engineering Chemistry Research 59, 16 (March 2020): 7888–7900. © 2020 American Chemical Society
Version
Final published version
Abstract
An assortment of hydrothermal reactions of chromic(III) nitrate and 2-aminoterephthalic acid was systematically studied to yield high-quality amine-functionalized MIL-101(Cr) nanoparticles (MIL-101(Cr)-NH₂). A comprehensive understanding of the role that synthesis conditions and basic modulators have on the formation of MIL-101(Cr)-NH₂ in aqueous media was extracted and reported herein. With the aid of a NaOH modulator at optimized concentration, sub-20 nm MIL-101(Cr)-NH₂ nanoparticles were prepared with good yield, minimized particle agglomeration, and a high Brunauer-Emmett-Teller (BET) surface area of 2800 ± 200 m²/g. To the best of our knowledge, these are the smallest particle sizes and the highest surface areas reported for directly synthesized MIL-101(Cr)-NH₂. Owing to their superior surface area and Lewis basic amine functionality, the MIL-101(Cr)-NH₂ nanoparticles exhibit a high CO₂ adsorption of up to 3.4 mmol/g at 288 K and 1 bar and a superior CO₂/N₂ selectivity of 26.5 at 308 K and 0.1 bar. A high isosteric heat of-54.6 kJ/mol for CO₂ adsorption implies the strong interaction between CO₂ and the amine-functionalized framework. The successful synthesis of sub-20 nm amine-functionalized MIL-101(Cr) nanoparticles offers a great opportunity to engineer advanced MIL-101(Cr)-based functional adsorbents and membranes for CO₂ capture and separation.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
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Creative Commons Attribution 4.0 International license
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DOI of Published Version
https://doi.org/10.1021/acs.iecr.0c00535