DataVXACS Applied Materials & InterfacesPaper
journal article·2023-01-25

Highly Effective H2/D2 Separation within the Stable Cu(I)Cu(II)-BTC: The Effect of Cu(I) Structure on Quantum Sieving

Xiaoyu Hu, Fengyun Ding, Renjin Xiong, Yongtao An, Xingwen Feng, Jiangfeng Song, Linsen Zhou, Peilong Li, Changlun Chen

ACS Applied Materials & Interfaces· Volume 15· Issue 3
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Abstract

Realizing ideal deuterium separation from isotopic mixtures remains a daunting challenge because of their almost identical sizes, shapes, and physicochemical properties. Using the quantum sieving effect in porous materials with suitable pore size and open metal sites (OMSs) enables efficient hydrogen isotope separation. Herein, synthetic HKUST-1-derived microporous mixed-valence Cu(I)Cu(II)-BTC (BTC = benzene-1,3,5-tricarboxylate), featuring a unique network of distinct Cu(I) and Cu(II) coordination sites, can remarkably boost the D 2 /H 2 isotope separation, which has a high selectivity ( S D 2 /H 2 ) of 37.9 at 30 K, in comparison with HKUST-1 and other porous materials. Density functional theory (DFT) calculations indicate that the introduction of Cu(I) macrocycles in the framework decreases the pore size and further leads to relatively enhanced interaction of H 2 /D 2 molecules on Cu(II) sites. The significantly enhanced selectivity of Cu(I)Cu(II)-BTC at 30 K can be mainly attributed to the synergistic effect of kinetic quantum sieving (KQS) and chemical affinity quantum sieving (CAQS). The results reveal that Cu(I) OMSs exhibit counterintuitive behaviors and play a crucial role in tuning quantum sieving without a complex structural design, which provides a deeper insight into quantum sieving mechanisms and a new strategy for the intelligent design of highly efficient isotope systems.
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Research context

OpenAlex topics: Metal-Organic Frameworks: Synthesis and Applications · Chemical Synthesis and Characterization · Radioactive element chemistry and processing

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute of Plasma Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, P. R. China

University of Science and Technology of China, Hefei 230026, P. R. China

Institute of Materials, China Academy of Engineering Physics, Mianyang 621907, P. R. China

Institute of Atomic and Molecular Physics, Sichuan University, Chengdu 610065, P. R. China

Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou 215123, P. R. China

Funding

Ministry of Science and Technology of the People's Republic of China · Hefei Institutes of Physical Science, Chinese Academy of Sciences · Department of Science and Technology of Sichuan Province · National Natural Science Foundation of China · Priority Academic Program Development of Jiangsu Higher Education Institutions · China Academy of Engineering Physics · Jiangsu Provincial Key Laboratory of Radiation Medicine and Protection · Foundation for Distinguished Talents from Institute of Materials, China Academy of Engineering Physics · Foundation of Science and Technology on Surface Physics and Chemistry Laboratory

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