单原子层分离膜：进展与展望

doi:10.11949/0438-1157.20241432

化工学报 ›› 2025, Vol. 76 ›› Issue (5): 1943-1959.DOI: 10.11949/0438-1157.20241432

• 综述与专论 • 上一篇

单原子层分离膜：进展与展望

王金月¹^,²(), 谢恩泽¹^,²(), 马翰泽¹^,², 袁晟¹^,², 何光伟¹^,²^,³(), 姜忠义¹^,²^,³()

^1.天津大学化工学院绿色化学化工教育部重点实验室，天津 300072
^2.物质绿色创造与制造海河实验室，天津 300051
^3.天津大学-新加坡国立大学福州联合学院，天津大学福州国际校区，福建福州 350207

收稿日期:2024-12-10 修回日期:2025-01-24 出版日期:2025-05-25 发布日期:2025-06-13
通讯作者: 何光伟,姜忠义
作者简介:王金月（1999—），女，硕士研究生，wjy0829@tju.edu.cn
谢恩泽（2001—），男，硕士研究生，xez_120@tju.edu.cn
基金资助:
国家自然科学基金联合重点基金项目(U22A20412);国家自然科学基金面上项目(22278301)

Monoatomic layer separation membrane: progress and prospect

Jinyue WANG¹^,²(), Enze XIE¹^,²(), Hanze MA¹^,², Sheng YUAN¹^,², Guangwei HE¹^,²^,³(), Zhongyi JIANG¹^,²^,³()

^1.Key Laboratory for Green Technology, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
^2.Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300051, China
^3.Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou 350207, Fujian, China

Received:2024-12-10 Revised:2025-01-24 Online:2025-05-25 Published:2025-06-13
Contact: Guangwei HE, Zhongyi JIANG

摘要/Abstract

摘要：

原子级制造是在原子精度对材料结构进行精准控制，是制备高端材料的变革性新技术。在原子级别对膜材料厚度和孔结构进行精密调控，开发单原子层纳米孔膜，可显著降低传质阻力，实现分子极限渗透与分离，将为膜分离领域的发展与难分离物系的突破带来新机遇。本综述介绍了多种单层纳孔膜材料（single layer nanoporous membranes， SLNM），总结其纳米孔构筑方法及单层膜制备方法，探讨其在气体分离、液体分离、离子分离等领域的应用现状。最后，针对单层纳孔膜面临的机遇与挑战进行了剖析与总结，并对其未来发展方向进行了展望。

关键词: 分离, 单层纳孔膜, 纳米材料, 单层石墨烯, 制备方法

Abstract:

Precisely controlling the thickness and pore structure of membrane materials at the atomic level and developing single atomic layer nanoporous membranes can significantly reduce mass transfer resistance and achieve molecular limit permeation and separation, which will bring new opportunities for the development of membrane separation and breakthroughs in difficult-to-separate systems. A variety of single layer nanoporous membranes (SLNM) materials are introduced, and their nanoporous construction methods and nondestructive transfer methods of single layer membranes are summarized, and their application status in gas separation, liquid separation, ion separation and other fields are discussed. Finally, the opportunities and challenges faced by single layer nanoporous separation membranes are analyzed and summarized, and its development direction is prospected.

Key words: separation, single layer nanoporous membrane, nanomaterials, single layer graphene, preparation methods

中图分类号:

TQ 028.8

王金月, 谢恩泽, 马翰泽, 袁晟, 何光伟, 姜忠义. 单原子层分离膜：进展与展望[J]. 化工学报, 2025, 76(5): 1943-1959.

Jinyue WANG, Enze XIE, Hanze MA, Sheng YUAN, Guangwei HE, Zhongyi JIANG. Monoatomic layer separation membrane: progress and prospect[J]. CIESC Journal, 2025, 76(5): 1943-1959.

图/表 15

图1 典型SLNM材料结构示意图及典型SLNM高分辨电镜图像

Fig.1 Schematic diagram of crystal structure

图2 多种石墨炔异构体的化学结构[28]

Fig.2 Chemical structures of various graphdiyne isomers

图3 典型的2D COF结构示意图及其合成路径

Fig.3 Typical 2D COF structure schematic diagram and its synthesis path

图4 典型的2D MOF结构示意图及其合成路径[51]

Fig.4 Typical 2D MOF structure schematic diagram and its synthesis pathway

表1 单层膜纳米孔构筑策略对比

Table 1 Comparison of nanopore construction strategies for SLNM

构筑策略	自上而下	自下而上
原理和方法	通过外部能量或化学试剂在二维材料中移除原子或引入空位形成纳米孔。 • 物理轰击 • 化学蚀刻 • 高能等离子体	基于界面反应或分子组装，通过气/固、液/液或液/固界面化学反应自组装形成二维材料，直接构筑具有孔洞结构的单层膜。 • 气/固界面 • 液/液界面 • 液/固界面
孔径控制能力	精确性高：通过控制轰击能量、蚀刻剂浓度、等离子体能量等实现孔径尺寸和密度的高精度调控；如“级联压缩”可显著改善孔径分布并增加孔密度。	受工艺限制：孔径尺寸及均匀性取决于界面反应条件、前体性质及合成动力学的调控，需要优化工艺参数以提升孔径控制水平。
技术优势	• 孔径分布精准 • 适配多种单层材料 • 易与其他策略耦合	• 适合大面积制备 • 功能化设计灵活
工艺复杂性	中高：工艺条件苛刻，制备成本较高，但能满足高性能膜材料的需求。	低：工艺条件相对温和，设备要求低，适合实验室研究和大规模工业制备。
适用材料范围	适用于多种二维材料，尤其是对孔径分布和密度要求严格的膜分离应用。	可应用于有机和无机材料，适用于多种薄膜分离应用场景。
典型膜分离应用场景	• 气体分离：如H₂/CO₂、H₂/CH₄的高选择性分离，适用于严苛工业环境。 • 液体分离：海水淡化、渗透蒸发等高性能分离场景。	• 气体分离：可用于一般气体分离场景。 • 液体分离：适用于纳滤、超滤及有机溶剂分离，具有大面积制备潜力。

图5 自上而下的合成方法示意图

Fig.5 Schematic diagram of top-down synthesis method

图6 自下而上的合成方法示意图

Fig.6 Schematic diagram of bottom-up synthesis method

图7 采用不同支撑层转移的石墨烯薄膜的AFM图

Fig.7 AFM images of graphene films transferred by different support layers

图8 PIM/多孔SLG膜的制备流程的示意图[82]

Fig.8 Schematic diagram of preparation process of PIM/ porous SLG membrane[82]

图9 NPC的制备与形貌特征[85]

Fig.9 Preparation and morphological characteristics of NPC[85]

图10 采用CVD制备的单层多晶石墨烯合成大面积多孔SLG膜的过程示意图[90]

Fig.10 Overview of the process of synthesizing large-area nanoporous single layer graphene membranes from single-layer polycrystalline graphene prepared by CVD[90]

表2 部分二维/多孔材料的H2/CH4分离性能

Table 2 H2/CH4 separation performance of some 2D/porous materials

材料	膜制备方法	H₂渗透通量		H₂/CH₄选择性	文献
材料	膜制备方法	GPU^①	Barrer^②	H₂/CH₄选择性	文献
PIM-EA-TB	相转化法	—	7760	11.1	[94]
GO/AAO	逐层自组装法	589	—	66.7	[95]
ZIF-62/AAO	熔融淬火法	—	4156	50	[96]
COF-LZU1–ACOF-1	溶剂热法	—	543.6	105	[36]
碳分子筛	浸渍炭化法	324	—	435	[97]
SLG	CVD	>4000	—	>2000	[98]
SLG	O₂ plasma、O₃刻蚀	3400	—	25.1	[61]
SLG	O₃、O₂刻蚀	7200	—	37.5	[62]

图11 多孔SLG膜用于气体分离的膜制备示意图与分离性能

Fig.11 Preparation schematic diagram and separation performance of porous SLG membrane for gas separation

图12 多孔SLG膜用于液体分离的膜制备示意图与分离性能

Fig.12 Preparation schematic diagram and separation performance of porous SLG membrane for liquid separation

图13 多孔SLG膜用于离子分离的膜制备示意图与分离性能

Fig.13 Preparation schematic diagram and separation performance of porous SLG membrane for ion separation

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单原子层分离膜：进展与展望

Monoatomic layer separation membrane: progress and prospect

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