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Townsend, Jacob

Publications and source records attributed to Townsend, Jacob.

Evaluating the impact of functional groups on membrane‐mediated CO 2 / N 2 gas separations using a common polymer backbone

Abstract Polymeric membranes have shown tremendous promise for the separation of CO 2 from flue gas streams. However, few systematic studies have been conducted to better understand the impact that chemical functionalities have on membrane‐based gas separation performance. To address this gap, we herein describe the synthesis and gas separation performance of a series of vinyl‐addition polynorbornenes bearing various CO 2 ‐philic functional groups. To facilitate direct comparison between functional groups, each material was designed to maintain a common polymer backbone. Though the incorporation of CO 2 ‐philic moieties within a dense polymeric membrane is frequently hypothesized to enhance CO 2 solubility, and thereby increase CO 2 /N 2 selectivity, our results demonstrate that the incorporation of CO 2 ‐philic groups onto a common polymer backbone do not necessarily result in increased gas separation performance. Experimental and computational results demonstrate that the incorporation of amidoxime groups onto a polynorbornene backbone increase CO 2 /N 2 selectivity, whereas commonly employed ethereal side chains only increased permeability.

Higgins, Morgan A.↗

Elastic Single-Ion Conducting Polymer Electrolytes: Toward a Versatile Approach for Intrinsically Stretchable Functional Polymers

Fabrication of stretchable functional polymeric materials usually relies on the physical adhesion between functional components and elastic polymers, while the interfacial resistance is a potential problem. Herein, a versatile approach on the molecular-level intrinsically stretchable polymer materials with defined functionality is reported. The single-ion conducting polymer electrolytes (SICPEs) were employed to demonstrate the proposed concept along with its potential application in stretchable batteries/electronics with improved energy efficiency and prolonged cell lifetime. The obtained membranes exhibit 88–252% elongation before breaking, and the mechanical properties are well adjustable. The galvanostatic test of the assembled cells using the obtained SICPE membrane exhibited a good cycling performance with a capacity retention of 81.5% after 100 cycles. The applicability of a proposed molecular-level design for intrinsically stretchable polymer materials is further demonstrated in other types of stretchable functional materials, including poly(vinylcarbazole)-based semiconducting polymers and poly(ethylene glycol)-based gas separation membranes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Addition-type alkoxysilyl-substituted polynorbornenes for post-combustion carbon dioxide separations

The separation of CO 2 from N 2 using polymeric membranes has proven a particularly challenging task. One promising class of polymers for this application is alkoxysilyl-substituted vinyl-added polynorbornenes (VAPNBs), which are high T g materials that often exhibit notable CO 2 /N 2 separation performance. This performance is believed to arise from their anomalous behavior in which they display high levels of solubility selectivity, a trait more commonly encountered in rubbery polymers than high T g glassy materials. While this trait has been documented in literature, no systematic investigations have been reported that probe the relationship between alkoxysilyl-substituted VAPNB structure and their resultant gas separation behavior. Here, we describe the synthesis and evaluation of three sets of alkoxysilyl-substituted VAPNBs that are designed to probe distinct facets of their structure-transport relationship. This includes investigations into the effect that alkoxysilyl branching, chain length, and carbon linker length have on CO 2 /N 2 permeability, solubility, and diffusivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Elimination of CO 2 /N 2 Langmuir Sorption and Promotion of “N 2 -Phobicity” within High- T g Glassy Membranes

In this work, we demonstrate that the CO 2 /N 2 gas separation performance of alkoxysilyl-substituted vinyl-added polynorbornenes (VAPNBs) may be significantly enhanced via incorporation of the monomer 5-tris(2-methoxyethoxy)-silyl-2-norbornene. As the molar ratio of this monomer is increased, substantial increases in CO 2 /N 2 selectivity are realized with minimal decrease in CO 2 permeability. This trend ignores the traditional permeability/selectivity “tradeoff” relationship and yields an optimal membrane whose performance reaches the 2008 upper bound for CO 2 /N 2 separations. Though the inclusion of 5-tris(2-methoxyethoxy)-silyl-2-norbornene units was initially hypothesized to maximize CO 2 solubility, detailed gas sorption studies reveal that these highly glassy materials essentially lack any Langmuir sorption component and indicate that their improved CO 2 /N 2 selectivity is due to decreased N 2 solubility within the matrix. Computational modeling suggests that the source of this apparent “N 2 -phobicity” is likely explained through comparative analyses of polymer–polymer and polymer–gas interactions. Lastly, mixed-gas permeation tests are performed to provide a more realistic look at real-world gas separation performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗