Design of Unique Amorphous FeO_x Mesoporous Nanosheets for Structural-Electronic Synergy toward Highly Selective and...

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 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 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.