Abstract
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.
Original language | English |
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Pages (from-to) | 6526-6532 |
Number of pages | 7 |
Journal | Angewandte Chemie - International Edition |
Volume | 60 |
Issue number | 12 |
DOIs | |
State | Published - Mar 15 2021 |
Funding
We acknowledge the National Natural Science Fund of China (22025203), the Municipal Natural Science Fund of Tianjin (18JCJQJC47400), the Royal Society and the University of Manchester for funding. S.W. and S.Y. thank the Royal Society for a Newton Advanced Fellowship. We thank STFC/ISIS Facility for the access to Beamline WISH. Inelastic neutron scattering experiments were conducted at the VISION beamline at ORNL's Spallation Neutron Source, which is supported by the Scientific User Facilities Division, Office of Basic Energy Sciences (BES), U.S. Department of Energy (DOE), under Contract No. DE-AC0500OR22725 with UT Battelle, LLC. JL thanks China Scholarship Council for funding.
Keywords
- acetylene
- gas separation
- neutron diffraction
- neutron scattering
- zeolites