Enhanced separation of tetrafluoropropanol from water via carbon nanotubes membranes: insights from molecular dynamics simulations

doi:10.1007/s11783-023-1740-y

Front. Environ. Sci. Eng.

2023, Vol. 17

Issue (11) : 140 https://doi.org/10.1007/s11783-023-1740-y

RESEARCH ARTICLE

Enhanced separation of tetrafluoropropanol from water via carbon nanotubes membranes: insights from molecular dynamics simulations

Qing Li¹, Xiaomeng Wang¹, Ying Liu¹, Zhun Ma¹(

), Qun Wang¹, Dongmei Xu¹(

), Jun Gao¹, Ruirui Wu², Hui Sun³, Xueli Gao⁴(

)

¹. College of Chemical and Biological Engineering, Shandong University of Science and Technology, Qingdao 266590, China
². SEPCOIII Electric Power Construction Co. Ltd., Qingdao 266100, China
³. State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan 750021, China
⁴. Key Laboratory of Marine Chemistry Theory and Technology (Ministry of Education), Ocean University of China, Qingdao 266100, China

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Abstract

● MD simulations unveil the transport mechanism for TFP-water mixture through CNTs.

● The (7,7) CNTs provided a dramatic mass fraction (97.51%) of TFP.

● Fluorine modified CNTs favor water preferential transport compare to pristine CNTs.

● CNTs modified at entrance and interior prompt permselectivity for water molecules.

Fluorinated alcohols exhibit promising prospects in chemical industry because of their special structure and many exciting properties, in which tetrafluoropropanol (TFP) is extensive applied in synthesis of pesticides, dyestuffs, variety of solvents and detergents. However, the presence of TFP in water garners increasing attention globally because of their intrinsic potential to threat ecosystems and human health. Carbon nanotubes (CNTs) membranes are burgeoning candidates for TFP-water separation owing to well-endowed extraordinary structural and transport properties. However, a grand challenge lies in the rational design of CNTs for improving separation performance. Herein, molecular dynamics (MD) simulations were performed to investigate the effects of various parameters on the separation of TFP-water mixtures including feed temperature, CNTs pore diameters, and fluorine functionalization position. It was found that TFP was pre-selected in CNTs ranging from 9.48 to 18.98 Å due to preferential adsorption and diffusion mechanism. Excellent separation factor of 16 was achieved by (7,7) CNTs and the mass fraction of TFP was purified from 75% to 97.51%. Fluorine modified CNTs separated TFP and water by preferentially permeating water due to hydrogen bonding interaction. Simulation results showed that CNTs modified at both the entrance and interior had better separation performance than CNT modified only at one of these positions. The 100wt% water content in permeate was achieved by (11,11) CNTs modified with fluorine at the entrance and interior. These findings provide valuable insights for designing potential candidates for fluorinated alcohol-water azeotropic mixtures membrane separation, and promise extensive application aspects for the reclamation of fluorinated alcohol.

Keywords Fluorinated alcohol Carbon nanotube Molecular simulation Fluorine modified

Corresponding Author(s): Zhun Ma,Dongmei Xu,Xueli Gao

Issue Date: 15 November 2023

Cite this article:

Qing Li,Xiaomeng Wang,Ying Liu, et al. Enhanced separation of tetrafluoropropanol from water via carbon nanotubes membranes: insights from molecular dynamics simulations[J]. Front. Environ. Sci. Eng., 2023, 17(11): 140.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-023-1740-y
https://academic.hep.com.cn/fese/EN/Y2023/V17/I11/140

Fig.1 Schematic of simulation box consists of a feed solution contains TFP and water molecules, a CNTs pervaporation membrane and a vacuum section representing the filtered layer.

Fig.2 TFP and water fluxes and separation factor of TFP(α) as a function of temperature.

Fig.3 TFP and water fluxes in CNTs membrane and mass fraction of TFP.

Fig.4 The distribution of TFP and water molecules in the CNTs membrane: (5,5) CNTs (a), (6,6) CNTs (b).

Fig.5 TFP/water structures inside (7,7), (11,11) and (14,14) CNTs (red: TFP molecules; blue: water molecules) (a); Density distribution profiles of TFP molecules in the CNTs, and y = 0 corresponds to the middle position of CNTs (b).

Fig.6 Deformation charge density distributions for guest molecules adsorbed on the CNTs pores: TFP (a) and water (b) (gray: electron loss; blue: electron gain).

Fig.7 TFP and water fluxes in entrance fluorine modification CNTs membrane and mass fraction of water.

Fig.8 TFP/water structures inside modified (10,10) CNTs (red: TFP molecules; blue: water molecules; pink: F groups) (a); Density distribution profiles of TFP molecules in the CNTs, and y = 0 corresponds to the middle position of CNTs (b).

Fig.9 TFP/water structures inside modified (11,11) CNTs (red: TFP molecules; blue: water molecules, pink: F groups doped in entrance and interior) (a); Density distribution profiles of TFP/water molecules in the CNTs, and y = 0 corresponds to the middle position of CNTs (b).

Fig.10 PMF profiles for TFP (a) and water molecule (b) in fluorine modified CNTs, where the CNTs lies from z = −14 to z = 14 Å, the center of CNTs is z = 0 Å. C10-em represents entrance and interior modified CNTs, C10-m represents interior modified CNTs, and C10-e represents entrance modified CNTs.

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