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This work demonstrates a straightforward method to convert real-world shoe waste midsoles into water remediation sorbents for the removal of cationic organic pollutants. 

This work demonstrates a series of functionalization methods to enhance the utility of thermoplastic-elastomer derived ordered mesoporous carbons, including chemical activation, heteroatom doping, and the introduction of nanoparticles. 

This work demonstrates a simple method to prepare hierarchically porous materials. The introduction of macropores in mesoporous matrix enables its improved sorbent performance against pollutants for water remediation. 

Abstract As the demand for clean water intensifies, developing effective methods for removing pollutants from contaminated sources becomes increasingly crucial. This work establishes a method for additive manufacturing of functional polymer sorbents with hollow porous features, designed to enhance interactions with organic micropollutants. Specifically, core–shell filaments are used as the starting materials, which contain polypropylene (PP) as the shell and poly(acrylonitrile‐co‐butadiene‐co‐styrene) as the core, to fabricate 3‐dimensional (3D) structures on‐demand via material extrusion. After 3D printing, the cores of the printed roads are removed through solvent extraction, creating hollow structures that increase accessible surface area for adsorption. Subsequently, a sulfonation‐induced crosslinking reaction installs sulfonic acid functionalities into the PP backbones, while enhancing their chemical stability. It is found that larger voids, and thinner polymer shells, enable improved structural retention during the sulfonation through limiting reaction‐induced stresses. The hollow sulfonated PP sorbents exhibit a strong affinity against cationic pollutants. Specifically, larger voids within these structures not only improve structural integrity but also result in accelerated adsorption kinetics by maximizing accessible surface area, thereby enhancing pollutant removal efficiency. This work provides a promising solution for advanced structured sorbent fabrication with hollow architectures, leading to more effective solutions for water contaminant removal in the future. 

The production of ordered mesoporous carbons (OMCs) can be achieved by direct pyrolysis of self-assembled polymers. Typically, these systems require a majority phase capable of producing carbon, and a minority phase to form pores through a thermal decomposition step. While polyacrylonitrile (PAN)-based block copolymers (BCPs) have been broadly reported as OMC precursors, these materials have a relatively narrow processing window for developing ordered nanostructures and often require sophisticated chemistry for BCP synthesis, followed by long crosslinking times at high temperatures. Alternatively, olefinic thermoplastic elastomers (TPEs) can be convered to large-pore OMCs after two steps of sulfonation-induced crosslinking and carbonization. Building on this platform, this work focuses on the precursor design concept for the efficient synthesis of OMCs through employing low-cost and widely available polystyrene-block-polybutadiene-block-polystyrene (SBS), which contains unsaturated bonds along the polymer backbone. As a result, the presence of alkene groups greatly enhances the kinetics of sulfonation-induced crosslinking reaction, which can be completed within only 20 min at 150 °C, nearly an order of magnitude faster than a recently reported TPE system containing a fully saturated polymer backbone. The crosslinking reaction enables the production of OMCs with pore sizes (∼9.5 nm) larger than most conventional soft-templating systems, while also doping sulfur heteroatoms into the carbon framework of the final products. This work demonstrates efficient synthesis of OMCs from TPE precursors which have a great potential for scaled production, and the resulting products may have broad applications such as for drug delivery and energy storage. 

Abstract Despite groundbreaking advances in the additive manufacturing of polymers, metals, and ceramics, scaled and accurate production of structured carbons remains largely underdeveloped. This work reports a simple method to produce complex carbon materials with very low dimensional shrinkage from printed to carbonized state (less than 4%), using commercially available polypropylene precursors and a fused filament fabrication-based process. The control of macrostructural retention is enabled by the inclusion of fiber fillers regardless of the crosslinking degree of the polypropylene matrix, providing a significant advantage to directly control the density, porosity, and mechanical properties of 3D printed carbons. Using the same printed plastic precursors, different mechanical responses of derived carbons can be obtained, notably from stiff to highly compressible. This report harnesses the power of additive manufacturing for producing carbons with accurately controlled structure and properties, while enabling great opportunities for various applications.