Abstract
<h2>Summary</h2> Sorbents with structures tailored at the molecular through device scales are needed to meet the demand for separations that can isolate trace analytes from complex mixtures. Here, direct-ink-writing three-dimensional (3D) printing is combined with a surface-segregation and vapor-induced phase separation (SVIPS) process to create hierarchically structured sorbents that satisfy this criterion. Composite inks containing polysulfone, polystyrene-<i>block</i>-poly(acrylic acid) (PS-PAA), and carbon nanotubes (CNTs) were formulated to allow these processes to proceed simultaneously. Enriching the inks with CNTs modulated their rheological characteristics such that microstructured sorbents with permeabilities of ∼10<sup>5</sup> L m<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup> could be printed. The SVIPS process generated an interconnected network of PAA-lined nanopores whose chemistry was tailored to produce sorbents that recovered Co<sup>2+</sup> selectively from mixtures of Co<sup>2+</sup> and Li<sup>+</sup> and efficiently treated sub-parts per million feed solutions under dynamic flow conditions. The versatile combination of 3D printing and SVIPS provides new strategies for manufacturing next-generation sorbents with structures controlled across multiple length scales.
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