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Article Abstract

Exclusive capture of carbon dioxide (CO) from hydrocarbons via adsorptive separation is an important technology in the petrochemical industry, especially for acetylene (CH) production. However, the physicochemical similarities between CO and CH hamper the development of CO-preferential sorbents, and CO is mainly discerned via C recognition with low efficiency. Here, we report that the ultramicroporous material Al(HCOO), ALF, can exclusively capture CO from hydrocarbon mixtures, including those containing CH and CH. ALF shows a remarkable CO capacity of 86.2 cm g and record-high CO/CH and CO/CH uptake ratios. The inverse CO/CH separation and exclusive CO capture performance from hydrocarbons are validated via adsorption isotherms and dynamic breakthrough experiments. Notably, the hydrogen-confined pore cavities with appropriate dimensional size provide an ideal pore chemistry to specifically match CO via a hydrogen bonding mechanism, with all hydrocarbons rejected. This molecular recognition mechanism is unveiled by in situ Fourier-transform infrared spectroscopy, X-ray diffraction studies, and molecular simulations.

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http://dx.doi.org/10.1021/jacs.3c01705DOI Listing

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Article Synopsis
  • The study focuses on a new material, Al(HCOO), ALF, that can selectively capture carbon dioxide (CO) from hydrocarbon mixtures, which is crucial in the petrochemical industry for acetylene production.
  • ALF exhibits a high CO capacity of 86.2 cm³/g and demonstrates impressive separation ratios of CO from both acetylene (CH) and ethylene (C2H4), making it an effective sorbent for this purpose.
  • The material's ability to preferentially capture CO is attributed to its unique pore structure, which facilitates hydrogen bonding specifically with CO, as confirmed by various scientific techniques including infrared spectroscopy and molecular simulations.
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