H2/D2 Separation Using UTSA-16@CAU-10-H@γ-AlOOH Composites as the Stationary Phase in Gas Chromatography via the Additive Effects of Kinetic Sieving and Chemical Affinity Quantum Sieving

被引:3
作者
Ping, Enming [1 ]
Chen, Xiaoxiao [1 ]
Zhou, Yunshan [1 ]
Zhang, Lijuan [1 ]
Kong, Lingyun [1 ]
Chen, Nan [1 ]
机构
[1] Beijing Univ Chem Technol, Coll Chem, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
关键词
METAL-ORGANIC FRAMEWORK; HYDROGEN ISOTOPE-SEPARATION; MOLECULAR-SIEVE; ADSORPTION; H-2; ALUMINA; D-2; MOFS;
D O I
10.1021/acs.inorgchem.2c03795
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
In this work, CAU-10-H@gamma-AlOOH is prepared, and then UTSA-16 is loaded on CAU-10-H@gamma-AlOOH to obtain UTSA-16@CAU-10-H@gamma-AlOOH. Using the as-prepared composites as stationary materials by cryogenic gas chromatography at 77 K, while CAU-10-H@gamma-AlOOH achieves the complete separation of ortho-H-2 (o-H-2) and D-2 with a resolution R of 1.66 and a separation time t of 9.52 min, UTSA-16@CAU-10-H@gamma-AlOOH achieves higher efficiency separation of hydrogen isotopes in a shorter separation time (4.56 min) with R = 1.7. Molecular simulation results show that CAU-10-H has both chemical affinity quantum sieving and kinetic sieving effects for H-2/D-2 at 77 K, and UTSA-16 can only exert the kinetic sieving effect. UTSA-16's load on CAU-10-H@gamma-AlOOH weakens the adsorption of hydrogen isotopes, and the presence of Co2+ in UTSA-16 promotes the conversion of para-H-2 to ortho-H-2. In gas chromatography, H-2 was preferentially desorbed from the system due to strong D-2 adsorption caused by the chemical affinity quantum sieving effect and faster H-2 diffusion caused by the kinetic sieving effect. These additive effects achieved efficient hydrogen isotope separation at 77 K.
引用
收藏
页码:1591 / 1601
页数:11
相关论文
共 53 条
[1]   Bimetallic Ni-Co-based metal-organic framework: An open metal site adsorbent for enhancing CO2 capture [J].
Abdoli, Yekta ;
Razavian, Marjan ;
Fatemi, Shohreh .
APPLIED ORGANOMETALLIC CHEMISTRY, 2019, 33 (08)
[2]   MOLECULAR-TRANSPORT IN SUBNANOMETER PORES - ZERO-POINT ENERGY, REDUCED DIMENSIONALITY AND QUANTUM SIEVING [J].
BEENAKKER, JJM ;
BORMAN, VD ;
KRYLOV, SY .
CHEMICAL PHYSICS LETTERS, 1995, 232 (04) :379-382
[3]   Isotope-selective pore opening in a flexible metal-organic framework [J].
Bondorf, Linda ;
Fiorio, Jhonatan Luiz ;
Bon, Volodymyr ;
Zhang, Linda ;
Maliuta, Mariia ;
Ehrling, Sebastian ;
Senkovska, Irena ;
Evans, Jack D. ;
Joswig, Jan-Ole ;
Kaskel, Stefan ;
Heine, Thomas ;
Hirscher, Michael .
SCIENCE ADVANCES, 2022, 8 (15)
[4]   Preparation of modified γ-alumina as stationary phase in gas-solid chromatography and its separation performance for hydrogen isotopes [J].
Cai, Jinjun ;
Xing, Yanlong ;
Yang, Menglong ;
Zhao, Xuebo .
ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY, 2013, 19 (05) :919-927
[5]   Quantum sieving: feasibility and challenges for the separation of hydrogen isotopes in nanoporous materials [J].
Cai, Jinjun ;
Xing, Yanlong ;
Zhao, Xuebo .
RSC ADVANCES, 2012, 2 (23) :8579-8586
[6]   Ultrahigh effective H2/D2 separation in an ultramicroporous metal-organic framework material through quantum sieving [J].
Cao, Dawei ;
Huang, Hongliang ;
Lan, Youshi ;
Chen, Xiaojun ;
Yang, Qingyuan ;
Liu, Dahuan ;
Gong, Yu ;
Xiao, Chengjian ;
Zhong, Chongli ;
Peng, Shuming .
JOURNAL OF MATERIALS CHEMISTRY A, 2018, 6 (41) :19954-19959
[7]   Surface interactions and quantum kinetic molecular sieving for H2 and D2 adsorption on a mixed metal-organic framework material [J].
Chen, Banglin ;
Zhao, Xuebo ;
Putkham, Apipong ;
Hong, Kunlun ;
Lobkovsky, Emil B. ;
Hurtado, Eric J. ;
Fletcher, Ashleigh J. ;
Thomas, K. Mark .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (20) :6411-6423
[8]  
Chen P, 2017, CHIN J CHROMATOGR, V35, P766, DOI 10.3724/SP.J.1123.2017.02028
[9]   New gas chromatographic packing ZIF-67@NH2-SiO2 for separation of hydrogen isotope H2/D2 [J].
Chen, Xiaoxiao ;
Liu, Mengyao ;
Zhang, Lijuan ;
Zhou, Yunshan ;
Ping, Enming ;
Ding, Chunyan .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2021, 46 (24) :13029-13037
[10]  
Chu X. Z., SEPARATION DYNAMICS