Solar-Driven Methane Coupling to Ethane over Layered Double Hydroxide-Based Heterojunction Photothermal Catalysts

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The conversion of earth-abundant CH 4 into high-value-added products (i.e., syngas and hydrocarbons) has received much attention but remains significantly challenging. Here, we report the preparation of a series of heterostructure catalysts by calcining ZnMgAl-layered double hydroxide (LDH) at 200–800 °C. The catalyst calcined at 600 °C (ZnMgAl-600) demonstrates significant activity for CH 4 coupling, achieving a high selectivity of 94.93% toward C 2 H 6 under full-spectrum irradiation. ZnMgAl-600 with a larger specific surface area and abundant oxygen vacancies enhances the charge-transfer efficiency and boosts the reaction activity of CH 4 coupling. In situ DRIFTS revealed that light irradiation alters the reaction pathway, promoting the formation of *CH 3, while suppressing the CO 2 production. This work presents a novel approach for utilizing LDH-derived catalysts in solar-driven CH 4 conversion to high-value-added chemicals.