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

• 成果类型: Article
• 署名作者: Rohde, Rachel C.; Carsch, Kurtis M.; Dods, Matthew N.; Jiang, Henry Z. H.; Mcisaac, Alexandra R.; Klein, Ryan A.; Kwon, Hyunchul; Karstens, Sarah L.; Wang, Yang; Huang, Adrian J.; Taylor, Jordan W.; Yabuuchi, Yuto; Tkachenko, Nikolay V.; Meihaus, Katie R.; Furukawa, Hiroyasu; Yahne, Danielle R.; Engler, Kaitlyn E.; Bustillo, Karen C.; Minor, Andrew M.; Reimer, Jeffrey A.; Head-Gordon, Martin; Brown, Craig M.; Long, Jeffrey R.
• 署名单位: University of California System; University of California Berkeley; University of California System; University of California Berkeley; University of California System; University of California Berkeley; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; National Institute of Standards & Technology (NIST) - USA; United States Department of Energy (DOE); National Renewable Energy Laboratory - USA; United States Department of Energy (DOE); Oak Ridge National Laboratory; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; University of California System; University of California Berkeley; University of Delaware
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-13415
• DOI: 10.1126/science.adk5697
• 发表日期: 2024-11-15
• 页码: 814-819
• 关键词: metal-organic frameworks; co2 capture; quantitative-analysis; basis-sets; COORDINATION; adsorption; complex; nmr; activation; relaxation

摘要

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 degrees 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 degrees 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.