Advances in Metal-Organic Frameworks for High-Performance Direct Air Capture of CO2.

The escalating climate crisis demands gigaton-scale carbon dioxide removal, positioning Direct Air Capture (DAC) as a critical technological frontier. However, its widespread deployment is constrained by a fundamental trilemma involving cost, energy consumption, and sorbent longevity. Overcoming this challenge necessitates transformative material innovation. This review comprehensively examines recent breakthroughs in the molecular engineering of metal-organic frameworks (MOFs), emphasizing their application for the precise recognition of CO2 in DAC. We analyze material-level design strategies aimed at enhancing key performance indicators, i.e., CO2 capacity, selectivity, sorption kinetics, and cyclic stability. A comparative assessment is presented to elucidate inherent performance trade-offs, delineating a clear cost-performance landscape to guide rational material selection. Finally, we outline emerging frontiers and future research trajectories, including intelligent adaptive sorbents, integrated capture-conversion systems, and AI-accelerated discovery. This review aims to serve not only as a snapshot of the current state of the art but also as a strategic roadmap for developing the economically viable, gigaton-scale systems imperative for climate mitigation.