Structured Layered Double Hydroxide-Based Catalysts for Process Intensification: Transport, Stability, and Scale-Up in Monoliths, Foams, Films, and Washcoats

There is increasing interest in structured layered double hydroxide (LDH)-based catalysts because they combine tunable acid–base/redox chemistry with reactor architectures that can reduce diffusion lengths, improve heat management, and lower pressure-drop penalties. This review evaluates LDH, LDH-derived oxide (LDO/MMO), reduced metal/LDO, reconstructed hydroxide-rich, and mixed dynamic states integrated into honeycomb monoliths, open-cell foams, meshes/felts, thin films, washcoats, coated plates, microchannels, capillaries, and additively manufactured lattices. To move beyond descriptive comparison, the literature is assessed using unified evaluation dimensions: operative active state, support architecture, coating/integration route, active-phase loading, coating thickness and uniformity, reactor-volume-normalized productivity or STY, ΔP/L, axial/radial thermal gradients, time-on-stream, coating loss, regeneration recovery, and pilot-readiness. Representative benchmarks illustrate both the promise and reporting gaps of the field: NiFe-LDH-derived monoliths for CO₂ methanation have reached ~70% CO₂ conversion at 300 °C with >90% CH₄ selectivity and only 0.7% post-test mass loss; NiFe-LDH/iron-foam monoliths retained 85% ozone conversion after 168 h; high-entropy LDH-derived oxides showed T50/T90 values of 246/254 °C for toluene oxidation; and Au/LDH capillary films achieved 31.9% glycerol carbonate yield and 3.78 g h⁻¹ g⁻¹ productivity. The strongest current cases are pollution abatement and CO₂ methanation, whereas biomass upgrading, fine-chemical flow, high-entropy coatings, and photo/electrocatalytic films require deeper module-level validation. Overall, structured LDH catalysts should be treated as coupled chemistry–coating–reactor systems whose performance must be judged simultaneously by activity, accessible catalyst inventory, transport efficiency, pressure drop, thermal profile, durability, regeneration, and manufacturability.