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

The photocatalytic conversion of CO2 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 FeOx 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 Fe2+/Fe3+ ratio and establish a tandem catalytic pathway, where Fe2+ can promote C–C coupling effectively by stabilizing *OCCO intermediates. This study offers a design principle for steering CO2 conversion toward value-added multicarbon fuels through cross-scale structural synergy.