4.8 Article

Efficient Separation of Acetylene and Carbon Dioxide in a Decorated Zeolite

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 12, Pages 6526-6532

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202014680

Keywords

acetylene; gas separation; neutron diffraction; neutron scattering; zeolites

Funding

  1. National Natural Science Fund of China [22025203]
  2. Municipal Natural Science Fund of Tianjin [18JCJQJC47400]
  3. Royal Society
  4. University of Manchester
  5. Scientific User Facilities Division, Office of Basic Energy Sciences (BES), U.S. Department of Energy (DOE) [DE-AC0500OR22725]
  6. China Scholarship Council
  7. UT Battelle, LLC

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Efficient separation of acetylene and carbon dioxide was achieved under ambient conditions using faujasite zeolites decorated with atomically-dispersed copper(II) sites. The system displayed an unprecedented separation factor and effective dynamic uptake of acetylene, offering high purity acetylene recovery.
The almost identical molecular sizes and volatilities of acetylene and carbon dioxide make their separation extremely challenging in industry. Reported here is the efficient separation of acetylene and carbon dioxide (v/v=2/1, which is relevant to that in the industrial cracking stream) in faujasite zeolites decorated with atomically-dispersed copper(II) sites under ambient conditions. In situ neutron powder diffraction and inelastic neutron scattering confirm that the confined copper(II) site displays chemoselective yet reversible binding to acetylene, whereas adsorbed carbon dioxide molecules are stabilized by weak host-guest supramolecular interactions with the framework oxygen centers, thus resulting in the efficient separation of these two gases under flow conditions. A designed adsorption-purging-desorption system based upon Cu@FAU is established for the recovery of high purity acetylene (98-99 %) from the mixture of acetylene and carbon dioxide, offering an unprecedented separation factor of 22.2 with an effective dynamic uptake of acetylene of 1.51 mmol g(-1) at 298 K.

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