Ni–Zn–Ga Alloy for Weak Sunlight‐Driven Methanol Production From CO 2 and H 2 O at Ambient Pressure

ABSTRACT The sunlight‐driven artificial photosynthesis that converts CO 2 and H 2 O into methanol is a promising approach for carbon‐neutral fuel synthesis, but conventional systems require elevated pressure while producing methane by‐products, hindering practical operation. Herein, we developed a Ni–Zn–Ga (NZG) ternary alloy‐assisted photothermal CO 2 hydrogenation system coupled with photovoltaic water splitting, which enables the natural sunlight‐driven conversion of CO 2 and H 2 O into methanol under ambient pressure. This system achieves a maximum methanol production rate of 709 μmol g −1 h −1 with 40% selectivity, and no detectable methane is formed, outperforming the state‐of‐the‐art traditional artificial photosynthesis technologies. Mechanistic studies demonstrate that structural modulation of the NZG catalyst facilitates the spatial separation of active sites for CO 2 adsorption and H 2 dissociation, thereby inhibiting CO and methane formation while enhancing methanol selectivity. This study provides fundamental insights into pathway tuning, deepens the understanding of catalytic control strategies for ambient‐pressure solar‐driven CO 2 hydrogenation into methanol, and paves the way for more efficient CO 2 conversion technologies.