Self-adaptive Ni nanoparticles in perovskite LaNi_1-xAl_xO₃/CaO for durable CO₂ capture and in-situ conversion

Integrated CO₂ capture and conversion (iCCC) technology is promising for carbon neutrality, but the high-temperature deactivation of dual-functional materials (DFMs) limits its practicality. Herein, we develop adaptive metallic nano-catalysts via in-situ exsolution-dissolution in perovskite-based DFMs, enabling self-adjustment during cyclic CO₂/CH₄ redox switching. Al-doping induces the Jahn-Teller distortion in LaNiO₃ perovskite, making the lattice contracted to enrich Ni²⁺ and oxygen vacancies; thereby tailoring the smooth exsolution-dissolution of Ni nano-catalyst and creating fast O^2- migration channels for facilitating CO₂ adsorption. The optimized perovskite LaNi_0.8Al_0.2O₃/CaO exhibits exceptional durability over 50 cycles, achieving a high CO₂ capture capacity of 10.2 mmol g_DFM^-1 and both high conversions of 91.5% for CO₂ and 93.5% for CH₄. The mechanism study by the in-situ characterizations and surface energy calculations confirms that heteroatomic doping modulates the metal-support interactions, providing a solution for the long-sought deactivation problems of sintering and coking.