Additive manufacturing of geopolymers with hierarchical porosity for highly efficient removal of Cs

Geopolymers (GPs) have emerged as promising adsorbents for wastewater treatment due to their superior adsorption stability, tunable porosity, high adsorption capacity, and low-energy production. Despite their great promise, developing GPs with well-controlled hierarchical structures and high porosity remains challenging, and the mechanism underlying the ion adsorption process remains elusive. Here we report a cost-effective and universal approach to fabricate Na or K GPs with sophisticated architectures, high porosity, and arbitrary cation species exchange by means of additive manufacturing and a surfactant. The introduction of sodium lauryl sulfate (SLS) enhanced the porosity of the GP adsorbents, yielding NaGP-lattice-10%SLS adsorbent with a high total porosity of 80.8 vol%. Combining static and dynamic adsorption tests, the effects of morphology, surfactant content, and cation species on Cs⁺ adsorption performance were systemically investigated. With an initial Cs⁺ concentration of 900 mg/L, the printed NaGP exhibited a maximum Cs⁺ adsorption capacity of 80.1 mg/g, outperforming other adsorbents reported so far. The quasi-second-order fit of the NaGP adsorbent showed overall higher R² values than the quasi-first-order fit, indicating that the adsorption process was dominated by ion exchange. Combined with first-principles calculations, we verified that the content of water in the GP sod cages also affected the ion-exchange process between Na⁺ and Cs⁺.