Fabricating Mechanically Robust Binder‐Free Structured Zeolites by 3D Printing Coupled with Zeolite Soldering: A Superior Configuration for CO(2) Capture

3D‐printing technology is a promising approach for rapidly and precisely manufacturing zeolite adsorbents with desirable configurations. However, the trade‐off among mechanical stability, adsorption capacity, and diffusion kinetics remains an elusive challenge for the practical application of 3D‐printed zeolites. Herein, a facile “3D printing and zeolite soldering” strategy is developed to construct mechanically robust binder‐free zeolite monoliths (ZM‐BF) with hierarchical structures, which can act as a superior configuration for CO(2) capture. Halloysite nanotubes are employed as printing ink additives, which serve as both reinforcing materials and precursor materials for integrating ZM‐BF by ultrastrong interfacial “zeolite‐bonds” subjected to hydrothermal treatment. ZM‐BF exhibits outstanding mechanical properties with robust compressive strength up to 5.24 MPa, higher than most of the reported structured zeolites with binders. The equilibrium CO(2) uptake of ZM‐BF reaches up to 5.58 mmol g(−1) (298 K, 1 bar), which is the highest among all reported 3D‐printed CO(2) adsorbents. Strikingly, the dynamic adsorption breakthrough tests demonstrate the superiority of ZM‐BF over commercial benchmark zeolites for flue gas purification and natural gas and biogas upgrading. This work introduces a facile strategy for designing and fabricating high‐performance hierarchically structured zeolite adsorbents and even catalysts for practical applications.