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
Institute for Decarbonization Materials, University of California, Berkeley, CA 94720, USA.
Department of Chemistry, University of California, Berkeley, CA 94720, USA.
Science. 2024 Nov 15;386(6723):814-819. doi: 10.1126/science.adk5697. Epub 2024 Nov 14.
Carbon capture can mitigate point-source carbon dioxide (CO) emissions, but hurdles remain that impede the widespread adoption of amine-based technologies. Capturing CO 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 CO absorption kinetics and instability to cycling. Here, we report a porous metal-organic framework featuring terminal zinc hydride sites that reversibly bind CO 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 CO concentrations and high temperatures relevant to postcombustion capture.
碳捕获可以减少点源二氧化碳（CO）排放，但仍然存在阻碍胺基技术广泛应用的障碍。在更接近许多工业废气流温度（>200°C）的条件下捕获CO是人们所关注的，尽管在这些温度下运行的金属氧化物吸收剂通常表现出缓慢的CO吸收动力学和循环稳定性问题。在此，我们报道了一种具有末端氢化锌位点的多孔金属有机框架，其在200°C以上的温度下可逆地结合CO，这对于本征多孔材料来说是前所未有的条件。气体吸附、结构、光谱和计算分析阐明了这种转变的快速、可逆性质。延长的循环和突破分析表明，该材料能够在与燃烧后捕获相关的低CO浓度和高温下进行深度碳捕获。
