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Polymer membranes employed in gas separation play a pivotal role in advancing environmental sustainability, energy production, and gas purification technologies. Despite their significance, the current design and manufacturing of these membranes lack cradle-to-cradle approaches, contributing to plastic waste pollution. This study explores emerging solutions, including the use of biodegradable biopolymers such as polyhydroxybutyrate (PHB) and membrane recycling, with a focus on the specific impact of mechanical recycling on the performance of biodegradable gas separation membranes. This research represents the first systematic exploration of recycling biodegradable membranes for gas separation. Demonstrating that PHB membranes can be recycled and remanufactured without solvents using hot-melt extrusion and 3D printing, the research highlights PHB's promising performance in developing more sustainable CO 2 separations, despite an increase in gas permeability with successive recycling steps due to reduced polymer molecular weight. The study emphasizes the excellent thermal, chemical, and mechanical stability of PHB membranes, albeit with a marginal reduction in gas selectivity upon recycling. However, limitations in PHB's molecular weight affecting extrudability and processability restrict the recycling to three cycles. Anticipating that this study will serve as a foundational exploration, we foresee more sophisticated recycling studies for gas separation membranes, paving the way for a circular economy in future membrane technologies., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Gas separation polymer membranes play a pivotal role in various industrial processes including carbon capture and hydrogen production. However, the inherent trade-off between permeability and selectivity coupled with challenges in membrane manufacturing has hindered their widespread industrial deployment. To address the permselectivity challenges, researchers have explored increasingly complex polymers, composite systems, and other materials. In this study, we introduce a novel membrane manufacturing technique called "electro-casting" that not only enables efficient membrane fabrication but also enhances the trade-off of traditional polymer-based membranes. We fabricated cellulose acetate (CA) membranes embedded with 1-ethyl-3-methyl imidazolium via electro-casting and performed a comparative analysis of structural, morphological, and gas transport characteristics against membranes made via conventional casting techniques. We discovered that electro-casted membranes exhibited a unique crystalline structure, surface topology that induced a remarkable 200% improvement in CO 2 /N 2 selectivity and a 110% increase in CO 2 /CH 4 selectivity. The electric field generated during the manufacturing process played a crucial role in altering the supramolecular structure of the polymer, thereby increasing the separation properties of the membranes as well as their thermal and mechanical features. Electro-casting induced a polymer crystallization effect that disrupted the permeability-selectivity trade-off observed in conventional membranes, while producing highly stable membranes. Moreover, the simplicity of this manufacturing method and its significant impact on membrane properties have the potential to accelerate the deployment of gas separation membranes, facilitating the transition toward a NetZero chemical industry.

State-of-the-art gas separation membrane technologies combine the properties of polymers and other materials, such as metal-organic frameworks to yield mixed matrix membranes (MMM). Although, these membranes display an enhanced gas separation performance, when compared to pure polymer membranes; major challenges remain in their structure including, surface defects, uneven filler dispersion and incompatibility of constituting materials. Therefore, to avoid these structural issues posed by today's membrane manufacturing methodologies, we employed electrohydrodynamic emission and solution casting as a hybrid membrane manufacturing method, to produce ZIF-67/cellulose acetate asymmetric membranes with improved gas permeability and selectivity for CO 2 /N 2 , CO 2 /CH 4 , and O 2 /N 2 . Rigorous molecular simulations were used to reveal the key ZIF-67/cellulose acetate interfacial phenomena ( e.g. , higher density, chain rigidity, etc. ) that must be considered when engineering optimum composite membranes. In particular, we demonstrated that the asymmetric configuration effectively leverages these interfacial features to generate membranes superior to MMM. These insights coupled with the proposed manufacturing technique can accelerate the deployment of membranes in sustainable processes such as carbon capture, hydrogen production, and natural gas upgrading., Competing Interests: The authors declare no conflict of interest., (This journal is © The Royal Society of Chemistry.)