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Title: Trailblazing Kr/Xe Separation: The Birth of the First Kr-Selective Material

Journal Article · · ACS Applied Materials and Interfaces
 [1];  [2];  [2];  [3];  [4];  [3];  [5];  [3]; ORCiD logo [6];  [7];  [7]; ORCiD logo [7]; ORCiD logo [3]; ORCiD logo [8]
  1. Illinois Institute of Technology, Chicago, IL (United States); SE-MAT Smartly Engineered Materials LLC, Pittsburgh, PA (United States); Illinois Institute of Technology
  2. Illinois Institute of Technology, Chicago, IL (United States)
  3. Massachusetts Institute of Technology (MIT), Cambridge, MA (United States)
  4. Massachusetts Institute of Technology (MIT), Cambridge, MA (United States); Nuclear Materials Authority, Cairo (Egypt)
  5. Argonne National Laboratory (ANL), Argonne, IL (United States)
  6. University of South Florida, Tampa, FL (United States)
  7. North Carolina State University, Raleigh, NC (United States)
  8. Illinois Institute of Technology, Chicago, IL (United States); SE-MAT Smartly Engineered Materials LLC, Pittsburgh, PA (United States)
+ Show Author Affiliations

Efficient separation of Kr from Kr/Xe mixtures is pivotal in nuclear waste management and dark matter research. Thus far, scientists have encountered a formidable challenge: the absence of a material with the ability to selectively adsorb Kr over Xe at room temperature. This study presents a groundbreaking transformation of the renowned metal–organic framework (MOF) CuBTC, previously acknowledged for its Xe adsorption affinity, into an unparalleled Kr-selective adsorbent. This achievement stems from an innovative densification approach involving systematic compression of the MOF, where the crystal size, interparticle interaction, defects, and evacuation conditions are synergistically modulated. The resultant densified CuBTC phase exhibits exceptional mechanical resilience, radiation tolerance, and notably an unprecedented selectivity for Kr over Xe at room temperature. Simulation and experimental kinetic diffusion studies confirm reduced gas diffusion in the densified MOF, attributed to its small pore window and minimal interparticle voids. The lighter Kr element demonstrates facile surface passage and higher diffusivity within the material, while the heavier Xe encounters increased difficulty entering the material and lower diffusivity. This Kr-selective MOF not only represents a significant breakthrough in Kr separation but also demonstrates remarkable processability and scalability to kilogram levels. Furthermore, the findings presented herein underscore the transformative potential of engineered MOFs in addressing complex challenges, heralding a new era of Kr separation technologies.

Research Organization:
Illinois Institute of Technology, Chicago, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation Graduate Research Fellowship Program; North Carolina State and ACCESS
Grant/Contract Number:
SC0024594; AC02-06CH11357
OSTI ID:
2367178
Alternate ID(s):
OSTI ID: 2370513
Journal Information:
ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 22 Vol. 16; ISSN 1944-8244
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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36 MATERIALS SCIENCE
metal−organic frameworks
Kr/Xe separation
Kr-selective materials
HKUST-1
flexibility
defect engineering
adsorption
diffusion
materials
metal organic frameworks
nanoparticles