Controllable construction of ionic frameworks for multi-site synergetic enhancement of CO<sub>2</sub> capture

doi:10.1007/s11705-023-2370-4

Front. Chem. Sci. Eng.

2024, Vol. 18

Issue (1) : 4 https://doi.org/10.1007/s11705-023-2370-4

RESEARCH ARTICLE

Controllable construction of ionic frameworks for multi-site synergetic enhancement of CO₂ capture

Yuke Zhang¹, Hongxue Xu², Haonan Wu², Lijuan Shi²(

), Jiancheng Wang¹(

), Qun Yi^2,³(

)

¹. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China
². School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430205, China
³. Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan 030024, China

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Abstract

CO₂ capture is one of the key technologies for dealing with the global warming and implementing low-carbon development strategy. The emergence of ionic metal-organic frameworks (I-MOFs) has diversified the field of porous materials, which have been extensively applied for gas adsorption and separation. In this work, amino-functionalized imidazolium ionic liquid as organic monodentate ligand was used for one step synthesis microporous Cu based I-MOFs. Precise tuning of the adsorption properties was obtained by incorporating aromatic anions, such as phenoxy, benzene carboxyl, and benzene sulfonic acid group into the I-MOFs via a facile ion exchange method. The new I-MOFs showed high thermal stability and high capacity of 5.4 mmol·g^–1 under atmospheric conditions for selective adsorption of CO₂. The active sites of microporous Cu-MOF are the ion basic center and unsaturated metal, and electrostatic attraction and hydroxyl bonding between CO₂ and modified functional sulfonic groups are responsible for the adsorption. This work provides a feasible strategy for the design of I-MOF for functional gas capture.

Keywords carbon dioxide capture micropores ionic liquids multi-site synergism ionic metal-organic frameworks

Corresponding Author(s): Lijuan Shi,Jiancheng Wang,Qun Yi

About author:

Peng Lei and Charity Ngina Mwangi contributed equally to this work.

Just Accepted Date: 15 September 2023 Issue Date: 09 November 2023

Cite this article:

Yuke Zhang,Hongxue Xu,Haonan Wu, et al. Controllable construction of ionic frameworks for multi-site synergetic enhancement of CO₂ capture[J]. Front. Chem. Sci. Eng., 2024, 18(1): 4.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-023-2370-4
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I1/4

Fig.1 (a) Schematic diagram of the synthesis of Cu-AFIL-M; (b) experimental and calculated XRD pattern for Cu-BTC and Cu-AFIL-M; (c) FTIR spectra for AFIL, BTC and Cu-AFIL-M (450–4000 cm^–1); (d) comparative N₂ adsorption-desorption curve and (e) pore size distribution of Cu-AFIL-M and Cu-BTC.

Fig.2 (a) XPS survey spectra of Cu-AFIL-M; high-resolution spectra of Cu 2p (b) and N 1s (c); (d) weight loss curve and thermal analysis curve of Cu-AFIL-M; (e) SEM images of Cu-AFIL-M and the EDS analysis corresponding to different surface elements.

Fig.3 (a) FTIR spectra of Cu-AFIL-M-x samples in the range of 450–4000 cm^–1;(b) enlarged view of the FTIR spectra in (a) in the range of 1000–1250 cm^–1; (c) crystal structures of Cu-AFIL-M-x with different counterions; (d) CO₂ adsorption capacity of Cu-AFIL-M-x samples in the range of 10–90 kPa, 25 °C.

Fig.4 (a) Comparison of the adsorption isotherms and the adsorption rate of Cu-BTC, Cu-AFIL-M and Cu-AFIL-M-SB for CO₂ at 25 °C; (b) reusability test of Cu-AFIL-M and Cu-AFIL-M-SB samples; (c) crystal structure and (d) FTIR spectra of fresh and used Cu-AFIL-M-SB.

Tab.1 Comparison of the CO₂ adsorption performance at 25 °C, 100 kPa

Tab.2 The content of active sites in Cu-AFIL-M-SB and Cu-AFIL-M samples obtained from CO₂-TPD

Fig.5 TPD curves for CO₂ corresponding to the Cu-AFIL-M and Cu-AFIL-M-SB samples.

Fig.6 IAST selectivity for (a) CO₂/N₂ and (b) CO₂/CH₄ at 298 K.

Fig.7 (a) Interaction energy of Cu-BTC and Cu-AFIL-M-SB with CO₂; (b) isothermal curve of Cu-AFIL-M and Cu-AFIL-M-SB; (c) views of binding sites (A: Cl⁻, B: O⁻, C: COO⁻, D: SO₃⁻) for CO₂ adsorption on different Cu-MOFs (c-1: Cu-AFIL-M, c-2: Cu-AFIL-M-Phe, c-3: Cu-AFIL-M-CB, c-4: Cu-AFIL-M-SB) with various anions (distance units: Å).

Fig.8 Fitting of experimental (solid line) and isothermal models (dot line): (a) Langmuir model; (b) Freundlich model; (c) Temkin model for the adsorption of CO₂ on Cu-AFIL-M-x; (d) pseudo-second-order kinetics plots for the adsorption of CO₂ on Cu-AFIL-M-x at 25 °C and 98 kPa.

Tab.3 Relevant parameters of Langmuir, Freundlich and Temkin isothermal adsorption models on Cu-AFIL-M-x

Tab.4 Kinetic fitting parameters obtained for the adsorption of CO₂ on Cu-AFIL-M-x

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