Laser‐Induced Porosity Engineering of Metal‐Organic Frameworks for Enhanced CO ₂ /CH ₄ Adsorption Properties

Effective adsorption separation of CO₂/CH₄ requires porous materials with high porosity and tunability, such as metal-organic frameworks (MOFs). However, structural defects and high production costs often limit their practical application. Here, we propose a laser-induced post-synthetic modification technique, termed Laser-Induced Porosity Engineering (LIPE), to enhance CO₂/CH₄ separation performance through defect-driven pore refinement in MOFs. Using low-energy, massless near-infrared laser irradiation, structural rearrangement of defective HKUST-1 was induced through vibrational excitation followed by rapid cooling, leading to an unprecedented transformation of mesopores into micropores. This transformation resulted in a 94% increase in surface area and a 75% improvement in CO₂ uptake. Moreover, simultaneously generated polar surface functionalities synergistically enhanced CO₂ selectivity. Kinetic studies under temperature swing conditions revealed enhanced desorption rates and stable cyclic performance. LIPE was further applied to defective MOF-801 synthesized from low-cost precursors, demonstrating its potential as a scalable and economically viable strategy for upgrading porous materials with compromised structural quality.