Architecting Metal–Organic Frameworks at Molecular Level toward Direct Air Capture

Escalating carbon dioxide (CO 2 ) emissions have intensified the greenhouse effect, posing a significant long-term threat to environmental sustainability. Direct air capture (DAC) has emerged as a promising approach to achieving a net-zero carbon future, which offers several practical advantages, such as independence from specific CO 2 emission sources, economic feasibility, flexible deployment, and minimal risk of CO 2 leakage. The design and optimization of DAC sorbents are crucial for accelerating industrial adoption. Metal–organic frameworks (MOFs), with high structural order and tunable pore sizes, present an ideal solution for achieving strong guest–host interactions under trace CO 2 conditions. This perspective highlights recent advancements in using MOFs for DAC, examines the molecular-level effects of water vapor on trace CO 2 capture, reviews data-driven computational screening methods to develop a molecularly programmable MOF platform for identifying optimal DAC sorbents, and discusses scale-up and cost of MOFs for DAC.