Butanol Separation from Humid CO2-Containing Multicomponent Vapor Mixtures by Zeolitic Imidazolate Frameworks

Bhattacharyya, Souryadeep; Jayachandrababu, Krishna C.; Chiang, Yadong; Sholl, David S.; Nair, Sankar

doi:10.1021/acssuschemeng.7b02604

Title: Butanol Separation from Humid CO₂-Containing Multicomponent Vapor Mixtures by Zeolitic Imidazolate Frameworks

Journal Article · Tue Aug 29 00:00:00 EDT 2017 · ACS Sustainable Chemistry & Engineering

DOI:https://doi.org/10.1021/acssuschemeng.7b02604· OSTI ID:1469890

Bhattacharyya, Souryadeep ^[1]; Jayachandrababu, Krishna C. ^[1]; Chiang, Yadong ^[1];

^[1];

^[1]

Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering

Butanol is a promising renewable fuel and feedstock. A major challenge in fermentative butanol production is to find a cost-effective butanol separation process from dilute aqueous solutions, usually an acetone-butanol-ethanol (ABE) mixture. Nanoporous zeolitic imidazolate frameworks (ZIFs) have shown potential for alcohol separation from dilute solutions. However, little is known about butanol separation from multicomponent mixtures using ZIFs, including the effects of the humid acid gas (CO₂) used to sparge the fermenter and generate the vapor product stream. We present a study of butanol separation by ZIF-8, ZIF-90, ZIF-71 and hybrid ZIF-8–90 and ZIF-8–71 adsorbents with binary butanol/water and multicomponent ABE feeds. To obtain reliable structure–property relations for ZIF adsorbents in realistic conditions, we combine multicomponent vapor breakthrough with structural, textural, and stability characterization techniques in humid CO₂ environments. In the absence of CO₂, more hydrophobic materials such as ZIF-8, ZIF-8₅₅-71₄₅, ZIF-8₇₀-90₃₀, and ZIF-71 are found to be excellent candidates with butanol/water selectivities >10 and butanol capacities >3.5 mmol/g. However, in the presence of humid CO₂, all the materials except ZIF-71 are found to degrade. The mechanistic aspects of this degradation are studied by FTIR spectroscopy and explained based upon acid gas attack of Zn–N coordinate bonds. ZIF-71 emerges as an excellent candidate owing to its acid gas stability, good butanol adsorption capacity, and selectivity. Vapor breakthrough with a model ABE solution demonstrates the high butanol selectivity of ZIF-71 relative to acetone, ethanol, and water and the recovery of a 65 mol % butanol product by desorption at 453 K. Finally, this study highlights the importance of determining structure–property relationships of MOF/ZIF materials in realistic multicomponent conditions, and the importance of acid gas stability in their applications.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012577

OSTI ID:: 1469890

Journal Information:: ACS Sustainable Chemistry & Engineering, Vol. 5, Issue 10; Related Information: UNCAGE-ME partners with Georgia Institute of Technology (lead); Lehigh University; Oak Ridge National Laboratory; University of Alabama; University of Florida; University of Wisconsin; Washington University in St. Louis; ISSN 2168-0485

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 35 works

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09 BIOMASS FUELS
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
catalysis (heterogeneous)
defects
membrane
carbon capture
materials and chemistry by design
synthesis (novel materials)
synthesis (self-assembly)
synthesis (scalable processing)
biobutanol
adsorption
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Title: Butanol Separation from Humid CO2-Containing Multicomponent Vapor Mixtures by Zeolitic Imidazolate Frameworks

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Title: Butanol Separation from Humid CO₂-Containing Multicomponent Vapor Mixtures by Zeolitic Imidazolate Frameworks