Supramolecular Assembly of One-Dimensional Coordination Polymers for Efficient Separation of Xenon and Krypton

Journal Article · Thu Aug 24 00:00:00 EDT 2023 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.3c04037· OSTI ID:2305735

Li, Liangying ^[1]; Chen, Lihang ^[2]; Guo, Lidong ^[3]; Zheng, Fang ^[2]; Zhang, Zhiguo ^[2]; Yang, Qiwei ^[2]; Yang, Yiwen ^[2]; Su, Baogen ^[3]; Ren, Qilong ^[2]; Li, Jing ^[4]; Bao, Zongbi ^[2]

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1. Zhejiang University, Hangzhou (China); Rutgers University, Piscataway, NJ (United States); Hangzhou Hangyang Co., Ltd. (China); Rutgers University
2. Zhejiang University, Hangzhou (China); Institute of Zhejiang University-Quzhou (China)
3. Zhejiang University, Hangzhou (China)
4. Rutgers University, Piscataway, NJ (United States)

Efficient separation and purification of xenon (Xe) from krypton (Kr) represent an industrially crucial but challenging process. While the adsorption-based separation of these atomic gases represents an energy-efficient process, achieving highly selective adsorbents remains a difficult task. Here, we demonstrate a supramolecular assembly of coordination polymers, termed as M(II)-dhbq (M = Mg, Mn, Co, and Zn; dhbq = 2,5-dihydroxy-1,4-benzoquinone), with high-density open metal sites (5.3 nm^–3) and optimal pore size (5.5 Å), which are able to selectively capture Xe among other chemically inert gases including Kr, Ar, N₂, and O₂. Among M(II)-dhbq materials, Mn-dhbq exhibits the highest Xe uptake capacity of 3.1 mmol/g and a Xe/Kr selectivity of 11.2 at 298 K and 1.0 bar, outperforming many state-of-the-art adsorbents reported so far. Remarkably, the adsorption selectivity of Mn-dhbq for Xe/O₂, Xe/N₂, and Xe/Ar at ambient conditions reaches as high as 70.0, 139.3, and 64.0, respectively. Direct breakthrough experiments further confirm that all M(II)-dhbq materials can efficiently discriminate Xe atoms from other inert gases. Furthermore, it is revealed from the density functional theory calculations that the strong affinity between Xe and the coordination polymer is mainly attributed to the polarization by open metal sites.

• Research Organization: Wake Forest University, Winston-Salem, NC (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES)
• Grant/Contract Number: SC0019902
• OSTI ID: 2305735
• Journal Information: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 35 Vol. 15; ISSN 1944-8244
• Publisher: American Chemical Society (ACS)
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
adsorption
adsorptive separation
atmospheric chemistry
coordination polymer
krypton
materials
mixtures
open metal sites
selectivity
xenon