High-temperature carbon dioxide capture in a porous material with terminal zinc hydride sites

Carbon capture can mitigate point-source carbon dioxide (CO₂) emissions, but hurdles remain that impede the widespread adoption of amine-based technologies. Capturing CO₂ at temperatures closer to those of many industrial exhaust streams (>200°C) is of interest, although metal oxide absorbents that operate at these temperatures typically exhibit sluggish CO₂ absorption kinetics and instability to cycling. Here, we report a porous metal-organic framework featuring terminal zinc hydride sites that reversibly bind CO₂ at temperatures above 200°C-conditions that are unprecedented for intrinsically porous materials. Gas adsorption, structural, spectroscopic, and computational analyses elucidate the rapid, reversible nature of this transformation. Extended cycling and breakthrough analyses reveal that the material is capable of deep carbon capture at low CO₂ concentrations and high temperatures relevant to postcombustion capture.