连续流聚合诱导自组装

doi:10.6023/A26030073

化学学报 ›› 2026, Vol. 84 ›› Issue (7): 1153-1164.DOI: 10.6023/A26030073 上一篇下一篇

综述

连续流聚合诱导自组装

李牧舟^a, 徐婷婷^a, 胡欣^b^,^*(), 孙冰^c^,^*(), 朱宁^a^,^*()

^a 南京工业大学生物与制药工程学院材料化学工程全国重点实验室材料化学工程全国重点实验室南京 211800
^b 南京工业大学材料科学与工程学院南京 211800
^c 中石化安全工程研究院有限公司化学品安全全国重点实验室化学品安全全国重点实验室青岛 266000

投稿日期:2026-03-12 发布日期:2026-06-12

作者简介:

胡欣, 西安交通大学材料科学与工程专业博士, 南京工业大学材料科学与工程学院教授. 主要从事功能高分子材料开发及微化工制备研究, 加入南工至今以第一或通讯作者(含共同作者)在Adv. Sci.、ACS Appl. Mater. Interfaces、ACS Macro Lett.、Chem. Eng. J.、Carbohydr. Polym.等期刊发表论文40余篇, 主持国家自然科学基金面上项目和青年项目各1项、企业委托开发项目3项, 获中国化工学会基础研究成果奖一等奖, 入选江苏省科技副总.

孙冰, 美国加州理工学院博士, 中石化安全工程研究院化工过程安全研究所所长、研究员, 主要从事化工过程安全技术开发、新型本质安全化工艺与装备开发工作. 在Angew. Chem. Int. Ed.等期刊发表SCI论文70余篇, 获国内外授权发明专利80余件, 研究成果曾获化工学会基础研究一等奖、石化联合会科技进步一等奖等科技奖励, 担任国家重点研发计划首席科学家, 获得侯德榜化工科学技术创新奖等荣誉.

朱宁, 浙江大学高分子化学与物理专业博士, 南京工业大学生物与制药工程学院教授. 主要研究化工新材料绿色制造, 加入南工以来作为第一或通讯作者(含共同)在Nat. Mater.、Angew. Chem. Int. Ed.、Adv. Funct. Mater.、Adv. Sci.、AIChE J.等期刊发表论文60余篇, 获授权中国发明专利70余件、美国专利5件, 主持科技部项目课题1项/子课题1项、国家自然科学基金面上项目3项/青年项目1项、企业委托开发项目6项, 获省部级科研奖励6项.

基金资助:
国家自然科学基金(22478188); 国家自然科学基金(22278223); 国家自然科学基金(22278205); 化学品安全全国重点实验室开放课题(SKLCS-2025008)

Continuous-Flow Polymerization-Induced Self-Assembly

Muzhou Li^a, Tingting Xu^a, Xin Hu^b^,^*(), Bing Sun^c^,^*(), Ning Zhu^a^,^*()

^a College of Biotechnology and Pharmaceutical Engineering, State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, Jiangsu 211800, China
^b College of Materials Science and Engineering, Nanjing Tech University, Nanjing, Jiangsu 211800, China
^c SINOPEC Research Institute of Safety Engineering Co., Ltd., State Key Laboratory of Chemical Safety, Qingdao, Shandong 266000, China

Received:2026-03-12 Published:2026-06-12
Contact: * E-mail: xinhu@njtech.edu.cn; sunb.qday@sinopec.com; ningzhu@njtech.edu.cn
Supported by:
National Natural Science Foundation of China(22478188); National Natural Science Foundation of China(22278223); National Natural Science Foundation of China(22278205); R&D Program of State Key Laboratory of Chemical Safety(SKLCS-2025008)

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摘要/Abstract

聚合诱导自组装(PISA)作为高效制备高固含量、形貌多样聚合物纳米颗粒的新策略, 在高分子合成化学等领域引起了广泛的研究兴趣. 相较于传统釜式间歇反应, 基于微反应器的流动化学与聚合诱导自组装相结合, 展示出更快的反应速度、独特的高级形貌、更好的与新技术耦合赋能等诸多优势. 本综述聚焦连续流聚合诱导自组装, 分别介绍了连续流热引发PISA、连续流光诱导PISA、耦合新技术PISA的研究进展, 对相关领域存在的机遇与挑战进行了探讨和展望, 希望对流动化学和聚合诱导自组装的发展提供借鉴.

关键词: 连续流, 聚合诱导自组装, 嵌段共聚物, 纳米颗粒, 可控聚合

As an efficient strategy for preparing polymer nano-objects with high solid contents and diverse morphologies, polymerization-induced self-assembly (PISA) has attracted growing research interest in the fields such as polymer chemistry. Compared with the traditional batch reactions, the combination of microreactor-based flow chemistry with PISA offers unique advantages, including but not limited to accelerated reaction rates, access to higher-order morphologies, and easy to integrations of new technologies. This review focuses on continuous-flow PISA, covering continuous-flow thermal-initiated PISA, continuous-flow photo-induced PISA, and continuous-flow PISA integrated with emerging technologies. Opportunities and challenges in the related topics are proposed and discussed with the aim to promote the development of flow chemistry and polymerization-induced self-assembly.

Key words: continuous-flow, polymerization-induced self-assembly, block copolymer, nano-object, controlled polymerization

引用此文

李牧舟, 徐婷婷, 胡欣, 孙冰, 朱宁. 连续流聚合诱导自组装[J]. 化学学报, 2026, 84(7): 1153-1164.

Muzhou Li, Tingting Xu, Xin Hu, Bing Sun, Ning Zhu. Continuous-Flow Polymerization-Induced Self-Assembly[J]. Acta Chimica Sinica, 2026, 84(7): 1153-1164.

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图/表 10

图1. (a)聚合诱导自组装(V和lc分别表示成核嵌段的体积和长度, α0表示嵌段连接点处的有效界面面积). (b)基于微反应器的流动化学

Figure 1. (a) Polymerization-induced self-assembly (V and lc denote the volume and the length of the core-forming block and α0 is the effective interfacial area of the block junction). (b) Microreactor-based flow chemistry

图2. RAFT聚合反应机理

Figure 2. Mechanism of RAFT polymerization

图3. 在微反应器中进行连续流热引发RAFT-PISA

Figure 3. Thermal-initiated RAFT-PISA in a continuous-flow microreactor

图4. PDMAm大分子链转移剂及PDMAm-b-PDAAm嵌段共聚物的连续流合成

Figure 4. Continuous-flow synthesis of PDMAm macro-CTA and PDMAm-b-PDAAm diblock copolymer

图5. (a)以PDMAm113为大分子链转移剂, 在目标聚合度分别为50、100和200的条件下, DAAm进行连续流RAFT水相分散聚合的转化率-时间曲线. (b) PDMAm113-b-PDAAmy聚合物纳米颗粒的DLS谱图, 其中y=50至200. (c)在微反应器中合成的一系列PDMAm46-b-PDAAmy聚合物纳米颗粒的GPC谱图, 其中y=50至200. (d)在微反应器中合成的PDMAm46-b-PDAAmy聚合物纳米颗粒的TEM图像, 其中y=50、75、100、200、300、400[85]

Figure 5. (a) Conversion vs. time curves for the continuous-flow RAFT aqueous dispersion polymerization of diacetoneacrylamide (DAAm) using a PDMAm113 macro-CTA targeting DPs of 50, 100, and 200. (b) DLS traces for PDMAm113-b-PDAAmy polymer nano-objects. (c) GPC traces for a series of PDMAm46-b-PDAAmy diblock copolymer nanoparticles (y=50~200) synthesized in a microreactor. (d) TEM images of PDMAm46-b-PDAAmy nanoparticles (y=50, 75, 100, 200, 300, 400) synthesized in a microreactor[85]. Copyright 2020, Royal Society of Chemistry, under the terms of the CC BY 3.0

图6. 三种光引发RAFT聚合的机理

Figure 6. Mechanisms of photo-induced RAFT polymerizations

图7. (a)基于连续流工艺, 通过可见光介导的引发-转移-终止聚合合成PEG-b-PHPMA纳米颗粒示意图. (b)针对不同目标聚合度, 连续流水相RAFT-PISA所制备样品的TEM图像. (c)用于合成PEG-b-PHPMA纳米颗粒并可实现颗粒形貌监测的反应装置[100]

Figure 7. (a) General scheme for synthesis of PEG-b-PHPMA nanoparticles via visible-light-mediated iniferter polymerization in a continuous process. (b) TEM images for aqueous RAFT dispersion PISA in flow for targeted degrees of polymerization. (c) Reactor setup for the synthesis of PEG-b-PHPMA nanoparticles enabling monitoring of particle morphology[100]. Copyright 2018, American Chemical Society

图8. (a)在水相中, 分别在紫光和蓝光照射下, 以mPEG-CEPA为macro-CTA, Eosin Y/AscA为催化体系, SPTP为I型光引发剂, 合成mPEG-b-PHPMA的带光引发剂的RAFT聚合反应机理. (b)用于双波长photo-PISA的微反应器实物照片, 以及该微反应器的所有尺寸参数示意图. (c)在微反应器中, 通过双波长/单波长光照的HPMA水相photo-PISA的聚合动力学. (d)在微反应器中进行的HPMA (15% (w))双波长水相photo-PISA的相关数据曲线. (e)在微反应器中进行的HPMA (15% (w))双波长水相photo-PISA过程中, 数均分子量Mn和分散度Đ随单体转化率的变化关系. (f)在微反应器中通过双波长水相photo-PISA形成的嵌段共聚物的GPC谱图(HPMA浓度为15% (w)). (g, h)分别在微反应器和釜式反应器中, 通过HPMA的双波长水相photo-PISA制备的mPEG-b-PHPMA嵌段共聚物纳米颗粒的TEM图像[109]

Figure 8. (a) RAFT polymerization with photoinitiator for synthesis of mPEG-b-PHPMA under purple and blue light irradiation in water with mPEG-CEPA as macro-CTA, Eosin Y/AscA as catalytic system, and SPTP as type I photoinitiator. (b) Digital image of the flow reactor used for dual-wavelength photo-PISA and schematic illustration of the flow reactor including all dimensions. (c) Polymerization kinetics of aqueous photo-PISA of HPMA performed in a continuous-flow reactor through dual-/single-wavelength light irradiation. (d) Plots of dual-wavelength aqueous photo-PISA of HPMA (15% (w)) performed in a continuous-flow reactor. (e) Evolution of Mn and Đ with monomer conversion for aqueous dual-wavelength photo-PISA of HPMA (15% (w)) performed in a continuous-flow reactor. (f) GPC traces of diblock copolymers formed by dual-wavelength aqueous photo-PISA of HPMA (15% (w)) in a continuous-flow reactor. (g, h) Representative TEM images of mPEG-b-PHPMA diblock copolymer nano-objects prepared by dual-wavelength aqueous photo-PISA of HPMA in the flow reactor and batch reactor[109]. Copyright 2020, American Chemical Society

图9. (a)反应器平台示意图, 包括75 ℃管式反应器、20 ℃的淬灭盘管、位于真空样品室内的SAXS流通池以及样品收集装置. (b)当保持PDAAm成核嵌段的DP恒定在约400, 而将PDMAm macro-CTA的DP从47增加至143时, 颗粒尺寸变化的示意图. (c)同一反应体系获得的原位SAXS谱图, 其中实验SAXS数据用空心圆表示, 模型拟合曲线用实线表示. (d)通过RAFT分散聚合合成的一系列PDMAmx-b-PDAAm400共聚物(x=47, 62, 80, 98和143), 其颗粒直径DParticle随停留时间的变化关系. (e)反应1500 s后所得样品的流体动力学直径(Dh, 由DLS测定)与核直径(Dcore, 由SAXS测定)随PDMAm聚合度的变化关系. 图中误差棒根据所测得的流体动力学直径的多分散指数确定[115]

Figure 9. (a) A schematic of the reactor platform comprising a heated tubular coil reactor, a quench coil at 20 ℃, a SAXS compatible flow cell in an evacuated sample chamber and sample collection. (b) Schematic representation of the change in particle dimensions when the DP of the PDMAm macro-CTA is increased from 47 to 143 while maintaining a constant PDAAm core DP of approximately 400. (c) In situ SAXS patterns obtained for the same reactions where experimental SAXS data are shown as hollow circles whilst the fitted model is indicated by the solid line. (d) Diameter of the particle (DParticle) as a function of residence time for a series of PDMAmx-b-PDAAm400 copolymers synthesized by RAFT dispersion polymerization was x=47, 62, 80, 98, and 143. (e) Hydrodynamic diameter (Dh; determined by DLS) and core diameter (Dcore; determined by SAXS) as a function of PDMAm degree of polymerization for samples obtained after 1500 s. Error bars shown are determined by PDI of the hydrodynamic diameter[115]. Copyright 2023, American Chemical Society

图10. (a)用于PDMAm-b-PDAAm嵌段共聚物纳米颗粒合成及线内表征的反应器平台示意图. (b)在稳态样品收集期间, 通过在线SRDLS测定的7种PDMAm150-b-PDAAmn嵌段共聚物的粒径汇总(插图显示了粒径分布); (c)目标疏水嵌段长度与从筛选数据(黑色方块)获得的粒径(黑色实线)之间的关系[116]

Figure 10. (a) Schematic of the reactor platform for synthesis and inline characterization of PDMAm-b-PDAAm block copolymer nanoparticles. (b) Particle size summary with particle size distributions (inset) for seven PDMAm150-b-PDAAmn block copolymers measured during steady-state sample collection by inline SRDLS. (c) Relationship between targeted hydrophobic block length and resulting particle size (black solid line) obtained from screening data (black squares)[116]. Copyright 2025, American Chemical Society, under the terms of the CC BY 4.0

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连续流聚合诱导自组装

Continuous-Flow Polymerization-Induced Self-Assembly

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