ACS Sustain Chem Eng
May 2025
Adsorbent materials with humidity-modulated CO sorption capacities are essential for direct air capture (DAC) based on moisture swing adsorption (MSA) processes. These materials have seldom been studied in the context of dynamic breakthrough experiments despite their efficacy in providing valuable equilibrium and kinetics information on the adsorbents and their resemblance to practical processes at large scales. Herein, we performed a series of breakthrough experiments to systematically investigate the DAC properties of the MSA adsorbent IRA-900-C.
View Article and Find Full Text PDFThe thermal distillation of crude oil mixtures is an energy-intensive process, accounting for nearly 1% of global energy consumption. Membrane-based separations are an appealing alternative or tandem process to distillation due to intrinsic energy efficiency advantages. We developed a family of spirocyclic polytriazoles from structurally diverse monomers for membrane applications.
View Article and Find Full Text PDFHydrocarbon separation relies on energy-intensive distillation. Membrane technology can offer an energy-efficient alternative but requires selective differentiation of crude oil molecules with rapid liquid transport. We synthesized multiblock oligomer amines, which comprised a central amine segment with two hydrophobic oligomer blocks, and used them to fabricate hydrophobic polyamide nanofilms by interfacial polymerization from self-assembled vesicles.
View Article and Find Full Text PDFZeolite nanosheets can be used for the fabrication of low-defect-density, thin, and oriented zeolite separation membranes. However, methods for manipulating their morphology are limited, hindering progress toward improved performance. We report the direct synthesis (i.
View Article and Find Full Text PDFThe fractionation of crude-oil mixtures through distillation is a large-scale, energy-intensive process. Membrane materials can avoid phase changes in such mixtures and thereby reduce the energy intensity of these thermal separations. With this application in mind, we created spirocyclic polymers with -aryl bonds that demonstrated noninterconnected microporosity in the absence of ladder linkages.
View Article and Find Full Text PDFZeolite MFI is a widely used catalyst and adsorbent that also holds promise as a thin-film membrane. The discovery of nanometre-thick two-dimensional (2D) MFI nanosheets has facilitated methods for thin-film zeolite fabrication that open new horizons for membrane science and engineering. However, the crystal structure of 2D-MFI nanosheets and their relationship to separation performance remain elusive.
View Article and Find Full Text PDFLiquid-phase separations of similarly sized organic molecules using membranes is a major challenge for energy-intensive industrial separation processes. We created free-standing carbon molecular sieve membranes that translate the advantages of reverse osmosis for aqueous separations to the separation of organic liquids. Polymer precursors were cross-linked with a one-pot technique that protected the porous morphology of the membranes from thermally induced structural rearrangement during carbonization.
View Article and Find Full Text PDFAn in situ FTIR thin film technique was used to study the sequential atomic layer deposition (ALD) reactions of SiCl4, tetraethyl orthosilicate (TEOS) precursors, and water on nonporous silica powder using supercritical CO2 (sc-CO2) as the solvent. The IR work on nonporous powders was used to identify the reaction sequence for using a sc-CO2-based ALD to tune the pore size of a mesoporous silica. The IR studies showed that only trace adsorption of SiCl4 occurred on the silica, and this was due to the desiccating power of sc-CO2 to remove the adsorbed water from the surface.
View Article and Find Full Text PDFWater and ethanol vapor adsorption phenomena are investigated systematically on a series of MFI-type zeolites: silicalite-1 samples synthesized via both alkaline (OH(-)) and fluoride (F(-)) routes, and ZSM-5 samples with different Si/Al ratios as well as different charge-balancing cations. Full isotherms (0.05-0.
View Article and Find Full Text PDFA room temperature method for synthesizing zeolitic imidizolate framework 71 (ZIF-71) is described. The methanol-based synthesis results in >95% yields (based on Zn) and produces crystals with 70% greater surface area than reported earlier. Ethanol uptake into the ZIF compares favorably with a recent modeling-based study.
View Article and Find Full Text PDFPermeability of a porous material with a fluid interface is shown to be related to the propagation of the slow longitudinal wave. The propagation threshold of the slow longitudinal wave occurs when the wave number is higher than the critical wave number, k(cr). Measuring k(cr) can provide the intrinsic permeability of a porous interface.
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