新型无机二维材料在气体分离膜领域的研究进展

doi:10.15541/jim20190548

无机材料学报 ›› 2020, Vol. 35 ›› Issue (9): 959-971.DOI: 10.15541/jim20190548 CSTR: 32189.14.10.15541/jim20190548

所属专题：封面文章； MXene材料专辑(2020~2021)；【虚拟专辑】层状MAX，MXene及其他二维材料

• 综述 • 下一篇

新型无机二维材料在气体分离膜领域的研究进展

杨浏鑫^1,²(),罗文华²,汪长安¹,徐晨²()

1.清华大学材料科学与工程学院, 北京 100084
2.中国工程物理研究院材料研究所, 江油 621700

收稿日期:2019-10-28 修回日期:2019-12-04 出版日期:2020-09-20 网络出版日期:2020-04-05
作者简介:杨浏鑫(1995-), 女, 博士研究生. E-mail: yanglx13@foxmail
YANG Liuxin(1995-), female, PhD candidate. E-mail: yanglx13@foxmail
基金资助:
中国工程物理研究院院长基金(YZJJLX2017009);中国工程物理研究院材料研究所特聘基金(TP20160208);中国工程物理研究院材料研究所统筹授权项目(TCSQ2016213)

Novel Inorganic Two-dimensional Materials for Gas Separation Membranes

YANG Liuxin^1,²(),LUO Wenhua²,WANG Changan¹,XU Chen²()

1. School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China
2. Institute of Materials, China Academy of Engineering Physics, Jiangyou 621700, China

Received:2019-10-28 Revised:2019-12-04 Published:2020-09-20 Online:2020-04-05
Supported by:
The Dean Foundation of China Academy of Engineering Physics(YZJJLX2017009);Foundation of Institute of Materials, China Academy of Engineering Physics(TP20160208);Project of Institute of Materials, China Academy of Engineering Physics(TCSQ2016213)

摘要/Abstract

摘要：

气体膜分离技术是过滤与分离工业的重要技术之一, 相比于传统分离技术更加高效、节能、环保。新型无机二维材料在分离膜领域的应用, 有望同时实现高选择性和高渗透率, 突破商业聚合物膜渗透率和选择性相互制约的瓶颈, 极大地促进高性能分离膜的发展。本文简述了膜的气体分离机制, 综述了石墨烯基、过渡金属硫族化物(TMDs)和二维过渡金属碳化物/氮化物(MXene)等新型无机二维材料近年来在气体分离膜领域的研究进展, 包括其设计、制造和应用, 探讨了不同材料分离膜的特点、面临的挑战和发展前景。此外, 本文对其他新兴二维材料——层状双氢氧化物(LDHs)、六方氮化硼(h-BN)、云母纳米片等的分离膜研究也进行了概述。最后, 对新型无机二维材料在气体分离膜领域的研究方向及面临的挑战作出了评价。

关键词: 膜, 气体分离, 无机材料, 二维材料, 综述

Abstract:

Membrane-based gas separation is one of the critical technologies in filtration and separation industry, since it is more efficient, energy-saving and environmentally friendly compared with traditional separation technologies. Novel inorganic two-dimensional materials (2DMs) for gas separation are expected to achieve both high selectivity and high permeability, breaking through the trade-off between selectivity and permeability of commercial polymer membranes. This review begins with a brief explanation of gas separation mechanisms for membranes. Afterwards, special attention will be given to the recent advances in novel inorganic 2DMs including graphene and their derivatives, TMDs and MXene, about their design, fabrication and application in gas separation. The gas separation characteristics of different materials, their challenges and directions for future research are summarized. Moreover, the application of other novel inorganic 2DMs, such as LDH, h-BN and mica nanosheets in gas separation technology is also discussed. Finally, the perspectives and challenges for future research of novel inorganic 2DMs in gas separation field are outlined.

Key words: membrane, gas separation, inorganic material, two-dimensional material, review

中图分类号:

TQ174

杨浏鑫,罗文华,汪长安,徐晨. 新型无机二维材料在气体分离膜领域的研究进展[J]. 无机材料学报, 2020, 35(9): 959-971.

YANG Liuxin,LUO Wenhua,WANG Changan,XU Chen. Novel Inorganic Two-dimensional Materials for Gas Separation Membranes[J]. Journal of Inorganic Materials, 2020, 35(9): 959-971.

图/表 13

图1 膜的传输机制示意图, 孔直径定义为Dp = Dc -Dvdw/$\sqrt{2}$, 其中Dc是碳原子中心之间的直径, Dvdw是碳原子的范德华直径[1,10,11,14-17]

Fig. 1 Schematic representation of transport mechanisms in membranes, where Dc is the location of carbon centers, and the pore diameter is defined as Dp = Dc - Dvdw/$\sqrt{2}$, where Dvdw is the van der Waals diameter of a carbon atom[1,10,11,14-17]

图2 石墨烯上形成纳米孔的示意图(a~b)和多孔石墨烯的孔电子密度等值面(c~d)[28]

Fig. 2 Schematic of pores in graphene sheet (a-b) and pore electron density isosurfaces of porous graphene (c-d)[28] (a) Creation of a nitrogen-functionalized pore within a graphene sheet; (b) An all-hydrogen passivated pore in graphene; (c) Pore electron density isosurface of the nitrogen-functionalized porous graphene; (d) The all-hydrogen passivated porous grapheme Color code: C-black; N-green; H-cyan (isovalue is at 0.2 e/nm)

图3 气体分子通过孔的示意图[29]

Fig. 3 Snapshots of passing-through events of gas molecules[29] (a, d) CO2; (b, e) N2; (c, f) CH4. (a-c) Top view; (d-f) Side view

图4 纳米多孔碳膜辅助转移法制备大面积石墨烯膜示意图(a)和石墨烯点阵中本征缺陷的高分辨TEM照片(b)[33]

Fig. 4 Schematic of fabrication of a large-area graphene membrane by the nanoporous carbon film-assisted transfer method (a) and high-resolution TEM images of the intrinsic defects in graphene lattice (b)[33]

图5 1 μm厚GO膜的照片(a), 分离膜的截面SEM照片(b), 分子在GO膜层间的渗透路径示意照片(c)和自支撑的亚微米厚GO膜和对照组PET膜的He渗透性能对比(d)[40] (1 mbar=100 Pa)

Fig. 5 Photo of a 1-μm-thick GO film (a), electron micrograph of the film’s cross section (b), schematic view for possible permeation through the laminates (c), and examples of He-leak measurements for a freestanding submicrometer-thick GO membrane and a reference PET film (d)[40] (1 mbar=100 Pa)

图6 不同的GO膜制备方法示意图(a), GO膜可能的气体传输途径示意图(b), GO膜表面的AFM图与表面深度分布(c, d)[19]

Fig. 6 Schematic illustration of two different GO coating methods (Method one and Method two) (a), schematic illustration of possible gas transport through graphene membrane (b), AFM images of GO membrane surfaces with insert images showing depth profiles of GO membrane surfaces: (c) method one [root mean square roughness (Rq) = 0.8 nm, average roughness (Ra) = 0.614 nm] and (d) method two (Rq = 0.608 nm, Ra = 0.467 nm)[19]

图7 PEBA基膜中组装的GO纳米片示意图(a), 含有0.1wt%GO的膜(b)和TEM照片(黄色虚线指示GO片层) (c), 以及GO-1膜横截面的TEM照片(d)[17]

Fig. 7 Schematic representation of the assembly of GO nanosheets in polymeric environment (a), digital photographs of the membrane with 0.1wt% GO (b), overview (the yellow dashed lines are eye-guiding lines indicating the GO laminates in these regions) (c) and expanded TEM image of the cross section of GO-1 membrane (d)[17]

图8 GO纳米片和聚合物链组成的二维通道的受力分析示意图(a), 本征力诱导的无序结构(左)和协同外力驱动的高度有序层状结构(右)示意图(b)[54]

Fig. 8 Force analysis for one 2D channel unit consisting of GO nanosheets and polymer chain (a), schematic illustration of intrinsic force induced disordered structure (left) and highly ordered laminar structures (right) driven by introduced synergistic external forces (b)[54]

图9 气体通过GO-SILM膜溶解-扩散传输路径示意图(a), 限制在GO纳米通道中的[BMIM][BF4]离子液体分子结构(b), GO膜(c)和GO-SILM膜(d)的截面SEM照片[55]

Fig. 9 Schematic illustration of the gas solution-diffusion transport pathway through a GO-SILM (a), molecular structures of [BMIM][BF4] IL confined in the GO nanochannels (b), the cross section of the GO membrane (c) and GO-SILM (d), respectively[55]

表1 石墨烯基膜的气体分离性能比较

Table 1 Graphene-based membranes for gas separation

Materials^a	Preparation method	Feed condition	Selectivity	Permeate rate/ permeance/permeability	Ref.
Porous graphene monolayer	Simulation All-H passivation	H₂/CH₄	10²³	10^-20 mol?s^-1?Pa^-1	[28]
Porous graphene bilayer	Ultraviolet-induced oxidative etching	H₂/CH₄	104	4.5×10^-23 mol?s^-1?Pa^-1	[30]
Porous graphene bilayer	Focused ion beam perforation	H₂/CO₂	4.6	5.0×10³ mol?m^-2?s^-1?Pa^-1	[32]
Porous graphene	Ozone functionalization-based pore-etching	H₂/CH₄	25	4.1×10^-7 mol?m^-2?s^-1?Pa^-1	[33]
GO/PES	Spin coating	H₂/CO₂	30	4.02×10^-17 mol?m?m^-2?s^-1?Pa^-1	[19]
GO/PES	Dip and spin coating	H₂/CO₂	20	5.69×10^-17 mol?m?m^-2?s^-1?Pa^-1	[19]
GO/AAO	Vacuum filtration	H₂/CO₂	3400	10^-7 mol?m^-2?s^-1?Pa^-1	[20]
GO/AAO	Vacuum filtration	H₂/CO₂	22.5	1.14×10^-7 mol?m^-2?s^-1?Pa^-1	[41]
TU-GOF	Hydrothermal Self-assembly synthesis	H₂/CO₂	225	10^-7 mol?m^-2?s^-1?Pa^-1	[42]
GO/AAO	Spin coating	H₂/CO₂	240	3.4×10^-7 mol?m^-2?s^-1?Pa^-1	[44]
PEBA-GO	Drop casting	CO₂/N₂	91	3.35×10^-14 mol?m?m^-2?s^-1?Pa^-1	[17]
SPEEK/S-GO	Drop casting	CO₂/CH₄	72.2	4.44×10^-13 mol?m?m^-2?s^-1?Pa^-1	[53]
EFDA-GO	Vaccum-spin	H₂/CO₂	29-33	2.8-4.0×10^-13 mol?m?m^-2?s^-1?Pa^-1	[54]
GO-[BMIM][BF₄]	Vacuum filtration	CO₂/ H₂	24	2.29×10^-8 mol?m^-2?s^-1?Pa^-1	[55]
		CO₂/ CH₄	234
		CO₂/N₂	382

图10 MoS2膜160 ℃热处理前后的气体渗透路径示意图(a)[63], 膜截面的SEM照片(b~e)[64]和MoS2-SILM制备过程示意图(f)[69]

Fig.10 Schematic of gas permeation pathway across MoS2 membranes before and after heating at 160 ℃(a)[63], cross section SEM images of the membrane (b-e)[64], and synthesis process for MoS2-SILM (f)[69](b) GO membrane; (c) MoS2 membrane; (d) GO-MoS2 (50/50) hybrid membrane; (e) GO-MoS2 (75/25) hybrid membrane

图11 AAO衬底上MXene的SEM照片(a) (插图为MXene胶体水溶液的科根达尔效应), MXene膜的截面SEM照片(b) (插图为弯折的膜), MXene片层的AFM图(c), 相邻MXene纳米片示意图(d)[77], 以及MXene膜分别选择性渗透H2和CO2的示意图(e)[78]

Fig. 11 SEM image of the delaminated MXene nanosheets on porous anodic aluminum oxide (AAO) (a) with insert showing the Tyndall scattering effect in MXene colloidal solution in water, cross-sectional SEM image of the MXene membrane (b) with insert showing a tweezer bent membrane, AFM image of the Mxene nanosheet on cleaved mica (c), illustration of the spacing between the neighboring MXene nanosheets in the membrane (d)[77], structures and gas transport of H2-selective and CO2-selective Mxene nanofilms (e)[78]

表2 其他新型无机2D材料气体膜分离性能比较

Table 2 Other novel inorganic 2DMs for membrane gas separation

Materials^a	Preparation method	Feed Condition	Selectivity	Permeate rate/permeance/ permeability	Ref.
MoS₂/AAO	Vacuum filtration	H₂/CO₂	3.4	9.19×10^-6 mol?m^-2?s^-1?Pa^-1	[62]
MoS₂	Vacuum filtration	H₂/CO₂	8.29	3.94×10^-13 mol?m?m^-2?s^-1?Pa^-1	[63]
GO/MoS₂	Vacuum filtration	H₂/CO₂	26.7	8.04×10^-7 mol m^-2 s^-1 Pa^-1	[64]
MoS₂-Pebax	Spin coating	CO₂/N₂	93	2.14×10^-14 mol?m?m^-2?s^-1?Pa^-1	[68]
MoS₂-[BMIM][BF₄]	Vacuum filtration and drop	CO₂/N₂	131.42	1.60×10^-8 mol?m^-2?s^-1?Pa^-1	[69]
WS₂-[BMIM][BF₄]	Vacuum filtration and spin-coating	CO₂/N₂	153.21	1.58×10^-8 mol?m^-2?s^-1?Pa^-1	[70]
Ti₂C₃T_x	Vacuum filtration	H₂/CO₂	160	7.37×10^-13 mol?m?m^-2?s^-1?Pa^-1	[77]
Ti₂C₃T_x/borate-PEI	Vacuum filtration and spin-coating	CO₂/CH₄	15.3	1.17×10^-7 mol?m^-2?s^-1?Pa^-1	[78]
MgAl-CO₃ LDH	Electrophoretic deposition	CO₂/N₂	1.53	2.34×10^-7 mol?m^-2?s^-1?Pa^-1	[83]
MgAl-CO₃ LDH	Vacuum-suction	CO₂/N₂	34.4	5.5×10^-10 mol?m^-2?s^-1?Pa^-1	[83]
NiAl-CO₃ LDH	In situ growth	H₂/CH₄	80	4.5×10^-8 mol?m^-2?s^-1?Pa^-1	[84]
h-BN-XTR	Drop casting	H₂/CH₄	24.1	7.03×10^-14 mol?m?m^-2?s^-1?Pa^-1	[85]
mica-[BMIM][BF₄]	Vacuum filtration and drop-casting	CO₂/N₂	87	2.68×10^-8 mol?m^-2?s^-1?Pa^-1	[89]

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新型无机二维材料在气体分离膜领域的研究进展

Novel Inorganic Two-dimensional Materials for Gas Separation Membranes

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