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Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

CN 11-5981/TQ

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Front. Chem. Sci. Eng.    2021, Vol. 15 Issue (4) : 882-891    https://doi.org/10.1007/s11705-020-1990-1
RESEARCH ARTICLE
Nickel(II) ion-intercalated MXene membranes for enhanced H2/CO2 separation
Yiyi Fan1, Jinyong Li1, Saidi Wang1, Xiuxia Meng1(), Yun Jin1, Naitao Yang1, Bo Meng1, Jiaquan Li2, Shaomin Liu2,3()
1. School of Chemical Engineering, Shandong University of Technology, Zibo 255049, China
2. Department of Chemical Engineering, Curtin University, Perth, WA 6845, Australia
3. College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China
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Abstract

Hydrogen fuel has been embraced as a potential long-term solution to the growing demand for clean energy. A membrane-assisted separation is promising in producing high-purity H2. Molecular sieving membranes (MSMs) are endowed with high gas selectivity and permeability because their well-defined micropores can facilitate molecular exclusion, diffusion, and adsorption. In this work, MXene nanosheets intercalated with Ni2+ were assembled to form an MSM supported on Al2O3 hollow fiber via a vacuum-assisted filtration and drying process. The prepared membranes showed excellent H2/CO2 mixture separation performance at room temperature. Separation factor reached 615 with a hydrogen permeance of 8.35 × 10−8 mol·m−2·s−1·Pa−1. Compared with the original Ti3C2Tx/Al2O3 hollow fiber membranes, the permeation of hydrogen through the Ni2+-Ti3C2Tx/Al2O3 membrane was considerably increased, stemming from the strong interaction between the negatively charged MXene nanosheets and Ni2+. The interlayer spacing of MSMs was tuned by Ni2+. During 200-hour testing, the resultant membrane maintained an excellent gas separation without any substantial performance decline. Our results indicate that the Ni2+ tailored Ti3C2Tx/Al2O3 hollow fiber membranes can inspire promising industrial applications.
Keywords MXene      H2/CO2 separation      nickel ions      hollow fiber     
Corresponding Author(s): Xiuxia Meng,Shaomin Liu   
Just Accepted Date: 29 September 2020   Online First Date: 07 December 2020    Issue Date: 04 June 2021
 Cite this article:   
Yiyi Fan,Jinyong Li,Saidi Wang, et al. Nickel(II) ion-intercalated MXene membranes for enhanced H2/CO2 separation[J]. Front. Chem. Sci. Eng., 2021, 15(4): 882-891.
 URL:  
https://academic.hep.com.cn/fcse/EN/10.1007/s11705-020-1990-1
https://academic.hep.com.cn/fcse/EN/Y2021/V15/I4/882
Fig.1  Schematic diagram of hydrogen and CO2 mixture separation by Ni2+-Ti3C2Tx/Al2O3 hollow fiber membrane.
Fig.2  Preparation of Al2O3 supported Ni2+-Ti3C2Tx membranes.
Fig.3  Diagram of the home-made device for mixture gas permeability test of composite membranes.
Fig.4  (a) SEM images of synthesized Ti3C2Tx powder, (b) Ni2+-Ti3C2Tx nanosheets (inset showing the Tyndall scattering effect of Ni2+-Ti3C2Tx colloidal solution), and (c) TEM and (d) AFM images of Ni2+-Ti3C2Tx nanosheets.
Fig.5  (a) XRD patterns of Ti3AlC2, Ti3C2Tx, and Ni2+-Ti3C2Tx power with inset of the magnified XRD pattern at low Bragg angles; (b) FTIR spectra of MXene and nickel ion functionalized MXene.
Fig.6  SEM images of the outer surface (a) of the of Al2O3 hollow fiber support (before deposition of MXene) with the inset showing the cross-section, the high magnification of the Ni2+-Ti3C2Tx/Al2O3 membrane, (b) showing the thickness around 2.7 mm with the inset showing the lower magnification, (c) the surface of the Ni2+-Ti3C2Tx/Al2O3 membrane, and (d) the TEM image of the Ni2+-Ti3C2Tx/Al2O3 membrane.
Mixed gasa) Knudsen constant MXene/Al2O3 Ni2+-Ti3C2Tx/Al2O3
Separation factor Permeability/(10−8 mol·m−2·s−1·Pa−1) Separation factor Permeability/(10−8 mol·m−2·s−1·Pa−1)
H2/CO2 4.69 215.25 5.29 615 8.35
H2/N2 3.74 99.13 6.76 154.48 8.79
H2/CH4 2.82 94.35 7.11 147.27 9.52
Tab.1  Separation performance of MXene/Al2O3 and Ni2+-Ti3C2Tx/Al2O3 membrane
Fig.7  (a) Single-gas permeance through the supported Ni2+-Ti3C2Tx membrane at room temperature, (b) separation performance of the Ni2+-Ti3C2Tx/Al2O3 membrane as a function of temperature in the equimolar mixed-gas H2/CO2, (c) long-term separation of equimolar mixed-gas H2/CO2 through a Ni2+-Ti3C2Tx/Al2O3 membrane at RT, H2/CO2 separation performance, and (d) of the Ti3C2Tx/Al2O3 membrane compared with state-of-the-art gas separation membranes. The red line indicates the Robeson 2008 upper bound of polymeric membranes for H2/CO2 separation, and the dashed green line represents the 2017 upper bound of the best current membranes for H2/CO2 separation. More information of the data is given in Table S1 (cf. ESM).
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