3D‐Printed Bioinspired Meta‐Structural Perovskite Catalysts for Dry Reforming of CH 4 and CO 2

Abstract Conventional packed‐bed catalysts suffer from single‐scale porosity, insufficient mechanical strength, and suboptimal mass transfer efficiency. Inspired by the fractal structure of the lung bronchi, a design and 3D printing method for gradient meta‐structural catalysts is proposed by integrating synthesized LaFe 0.5 Ni 0.5 O 3 (LFN) perovskite with pseudo‐boehmite, achieving ultralow pressure drop and high catalytic efficiency. Computational fluid dynamics and reaction simulations guide the design of uniform and gradient‐structured catalysts with hierarchical woodpile channels (0.5–3 mm). Compared with homogeneous catalysts, the gradient design theoretically exhibits 1.5‐fold and 1.1‐fold increases in flow velocity and hydrogen production, respectively. Meta‐structural catalysts are fabricated with gradient multi‐peak pore distribution (9.32 nm, 103.75 nm) by regionally modulating unit cell sizes and LFN content (11–35%) combined with the dehydroxylation of pseudo‐boehmite. 3D‐printed perovskite catalysts demonstrate a 78.7‐fold increase in specific surface area (102.26 m 2 g −1 ) and compressive strength of 8.48 MPa. In dry reforming of methane (DRM) tests, it achieves 82.13% CH 4 conversion, and 9.69 mmol g −1 syngas yield, outperforming conventional powder‐packed beds by 10% efficiency. This study achieves mass transfer and catalytic performance coupling by tuning gradient hierarchical pores and tailoring flow dynamics, offering a paradigm for robust, high‐efficiency catalyst design across diverse applications.