Abstract
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.
