Design of Unique Amorphous FeO _<i>x</i> Mesoporous Nanosheets for Structural–Electronic Synergy toward Highly Selective and Efficient CO ₂ Photoconversion into Multicarbon Fuels

The photocatalytic conversion of CO 2 into high-energy-density hydrocarbons presents significant challenges, requiring not only high photon utilization efficiency but also superior catalytic activity. Herein, we present a rationally designed photocatalyst that leverages the structural flexibility and tunable electronic properties of amorphous FeO x to effectively address these requirements. The catalyst, based on several synergistic factors, exhibits an apparent quantum efficiency of 1.60% at 520 nm, with ethane selectivities of ∼70% (yield-based) and ∼94% (electron-based). Specifically, the amorphous framework combined with mesoporosity provides abundant disordered sites, strongly enhancing molecule adsorption and activation; the thin walls of the mesopores shorten charge diffusion paths to the surface; and the laser-induced oxygen vacancies increase Fe 2+ /Fe 3+ ratio and establish a tandem catalytic pathway, where Fe 2+ can promote C–C coupling effectively by stabilizing *OCCO intermediates. This study offers a design principle for steering CO 2 conversion toward value-added multicarbon fuels through cross-scale structural synergy.