Self-adaptive Ni nanoparticles in perovskite LaNi<sub>1-x</sub>Al<sub>x</sub>O<sub>3</sub>/CaO for durable CO<sub>2</sub> capture and in-situ conversion.

Shao, Bin; Jia, Zhonghao; Dai, Sheng; Hu, Jun · Nat Commun · 2026

basic_science · Level V

Where this comes from

Abstract

Integrated CO<sub>2</sub> 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 CO<sub>2</sub>/CH<sub>4</sub> redox switching. Al-doping induces the Jahn-Teller distortion in LaNiO<sub>3</sub> perovskite, making the lattice contracted to enrich Ni<sup>2+</sup> and oxygen vacancies; thereby tailoring the smooth exsolution-dissolution of Ni nano-catalyst and creating fast O<sup>2-</sup> migration channels for facilitating CO<sub>2</sub> adsorption. The optimized perovskite LaNi<sub>0.8</sub>Al<sub>0.2</sub>O<sub>3</sub>/CaO exhibits exceptional durability over 50 cycles, achieving a high CO<sub>2</sub> capture capacity of 10.2 mmol g<sub>DFM</sub><sup>-1</sup> and both high conversions of 91.5% for CO<sub>2</sub> and 93.5% for CH<sub>4</sub>. 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.