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Berchtold, Kathryn A.

Publications and source records attributed to Berchtold, Kathryn A..

Polybenzimidazole-derived carbon molecular sieve hollow fiber membranes with tailored oxygen selective transport

Polymer membrane carbonization is a promising strategy to obtain carbon molecular sieve (CMS) membrane materials with tailorable cavity size distributions for high gas selectivities beyond that attained from traditional polymer membrane materials. Despite their already demonstrated exceptional separation performance characteristics for several gas separation applications (e.g. CO 2 /CH 4 and H 2 /CO 2 ), further development of CMS membranes having high O 2 /N 2 perm-selectivity for energy-efficient high-purity O 2 production has proven challenging. Herein, we explore CMS hollow fiber membranes (HFMs) derived from highly rigid and tightly-packed polybenzimidazole (PBI) materials. Nearly defect-free PBI-derived CMS HFMs were fabricated and evaluated for O 2 /N 2 separation performance for the first time. The micro-structural and O 2 selective gas separation characteristics of PBI-CMS HFMs pyrolyzed at different pyrolysis conditions were intensively studied. With rigorous carbonization protocol optimization, we obtained highly O 2 permselective PBI-CMS HFMs having O 2 /N 2 selectivities approaching 14, enabling high purity O 2 production. The PBI-CMS HFM O 2 /N 2 separation performance dependence on operating conditions (e.g. temperature and feed pressure) are reported.

36 MATERIALS SCIENCE↗

Macrovoid-free high performance polybenzimidazole hollow fiber membranes for elevated temperature H 2 /CO 2 separations

Thermally robust membranes are required for H 2 production and carbon capture from hydrocarbon fuel derived synthesis (syn) gas. Polybenzimidaole (PBI) materials have exceptional thermal, chemical and mechanical characteristics and high H 2 perm-selectivity for efficient syngas separations at process relevant conditions. The large gas volumes processed mandate the use of a high-throughput, small footprint hollow fiber membrane (HFM) platform. Here in this work, an industrially attractive spinning protocol is developed to fabricate PBI HFMs with unprecedented H 2 /CO 2 separation performance. A unique dope composition incorporating an acetonitrile diluent is discovered enabling asymmetric macro-void free PBI HFM fabrication using a water coagulant. The influences of dope viscosity, coagulant chemistry, and air gap on HFM morphology are evaluated. Elevated temperature (up to 350 °C) H 2 permeances of 400 GPU with H 2 /CO 2 selectivities > 20 are achieved. This unprecedented separation performance is a ground breaking achievement at temperatures traditionally considered out-of-reach for polymeric membranes.

08 HYDROGEN↗

Influence of non-solvent chemistry on polybenzimidazole hollow fiber membrane preparation

Polybenzimidazole membrane materials have attractive H 2 /CO 2 separation characteristics and high thermo-chemical stability for elevated temperature synthesis (syn) gas separations. The development of PBI membranes with a thin defect-free selective layer and porous support morphology is vital to achieving industrially attractive separation performance. This work is focused on developing a fundamental understanding of the liquid-liquid demixing-based phase inversion process for asymmetric PBI hollow fiber membrane (HFM) formation. The development of industrially attractive HFMs is a challenging process due to the complex interplay between phase equilibria, phase inversion kinetics, and interfacial mass transfer that exist during the liquid-liquid demixing process. Numerous parameters including the dope, bore, and outer coagulant chemistries and compositions significantly influence the HFM morphologies produced. Here, a systematic study is conducted to investigate the phase inversion process parameters including the roles of the non-solvent solubility and diffusivity parameters with respect to the solvent and PBI on the phase inversion process. Furthermore, the influence of dope, bore and coagulant chemistries and compositions on PBI HFM morphology are investigated. As a result, the fabricated PBI HFMs are evaluated for their ideal H 2 and CO 2 permeance and H 2 /CO 2 selectivity at 250 °C to benchmark their separation performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Polybenzimidazole based random copolymers containing hexafluoroisopropylidene functional groups for gas separations at elevated temperatures

Polybenzimidazoles (PBIs) are attractive membrane materials for H 2 /CO 2 separation at hydrocarbon fuel derived synthesis gas operating conditions due to their exceptional physicochemical stability and promising permselectivity character. PBI molecular structure modification is a viable approach to disrupt chain packing altering the free-volume architecture which results in improved gas transport characteristics. This work is focused on the synthesis and characterization of novel PBI random copolymers for application as elevated temperature H 2 /CO 2 membranes. The co-polymerization route is expected to result in tailorable permeability and selectivity by combining the high H 2 permeability aspect of the highly disrupted loosely packed hexafluoroisopropylidene diphenyl group containing PBI segments (6F-PBI) with the highly selective tightly packed phenylene group containing PBI segments (m-PBI). 6F/m-PBI copolymers with varying 6F-PBI and m-PBI ratios having high inherent viscosity were synthesized. The structure and ratio of the 6F- and m-PBI fractions were confirmed using FTIR and NMR spectroscopic techniques. The measured gas transport properties of copolymer thin films cast in controlled environment were measured as a function of the operating conditions. Lastly, the H 2 permeability increased while H 2 /CO 2 selectivity decreased as the 6F-PBI copolymer fraction was increased.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Energy-Efficient Purification of Bio-Fuels and Bio-Chemicals Using a Novel Advanced Polymeric Membrane System: CRADA Final Report

The team collaborated to develop, demonstrate and move toward the commercialization of a pervaporation membrane system, which reduces the energy required for product isolation from dilute fermentation broths. Avoiding the energy consumption associated with the latent heat of vaporization for water was the key benefit. Essentially, this work isolated high boilers from dilute feeds without evaporating water. These activities lead to the development, fabrication, and demonstration of proprietary, advanced polymer membrane cartridges that dramatically reduce the cost of bio-chemical and bio-fuel manufacture.

09 BIOMASS FUELS↗

Robust, high temperature-ceramic membranes for gas separation

A method of making ceramic membranes, and the ceramic membranes so formed, comprising combining a ceramic precursor with an organic or inorganic comonomer, forming the combination as a thin film on a substrate, photopolymerizing the thin film, and pyrolyzing the photopolymerized thin film.

36 MATERIALS SCIENCE↗

Fact Sheet: Polymer-Based Carbon Dioxide Capture Membrane Systems

To develop and demonstrate polymer-based membrane structures, deployment platforms, and sealing technologies that achieve the critical combination of high selectivity, high permeability, chemical stability, and mechanical stability all at elevated temperatures (>150°C) and packaged in a scalable, economically viable, high area density system amenable to incorporation into an integrated gasification combined cycle (IGCC) plant for pre-combustion carbon dioxide (CO2) capture.

Energy Conservation, Consumption, & Utilization(32↗

High Temperature Polymer-Based Membrane Systems for Pre-Combustion Carbon Dioxide Capture

This report describes the activities conducted by Los Alamos National Laboratory and our project partners in support of DOE’s program to develop carbon capture technologies for power systems. This work was aimed at continued development and demonstration of a membrane based pre-combustion hydrogen purification/carbon capture technology and separation schemes developed by LANL.

Carbon Capture↗