Chloroplast‐Mimicking Interfaces on In Situ Derived La‐Ni Based Perovskite for Solar‐Driven CO 2 Reduction to CH 4

Artificial photosynthesis technology holds great promise for sustainable energy conversion and value‐added chemical synthesis, yet integrating efficient light absorption with high product selectivity remains a major challenge. This study constructs an Ni‐La 2 O 3 /La 2 NiO 4 catalyst through in situ perovskite derivation that mechanistically and functionally mimics the chloroplast for artificial photosynthesis by coupling photo and photothermal catalysis with the integration of broad‐spectrum light harvesting, directional charge transfer, as well as CO 2 adsorption and hydrogenation. Three functional interfaces are formed: La 2 O 3 ‐La 2 NiO 4 (Z‐scheme), Ni‐La 2 NiO 4 (Schottky junction), and La 2 O 3 (adsorption)‐Ni(activation). The two heterojunctions facilitate electron transfer to metallic Ni nanoparticles, which activates H + to form an NADPH‐like surface Ni‐H species by enabling the collection of photo and photothermal generated electrons. Meanwhile, the Lewis‐basic La 2 O 3 captures CO 2 and promotes its activation at the La 2 O 3 ‐Ni interface. In CO 2 ‐to‐CH 4 conversion, Ni‐La 2 O 3 /La 2 NiO 4 demonstrates an exceptional CH 4 production rate of 9.96 µmol h −1 g −1 and a selectivity of 92.5% under natural conditions (i.e., AM 1.5 irradiation, ambient temperature, and atmospheric pressure) without external assistance, which outperforms pure La 2 NiO 4 by 10.2 and 4.6 times, respectively. This work advances a new strategy for efficient solar‐to‐fuel conversion.