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Understanding on the surfactants engineered morphology evolution of block copolymer particles and their precise mesoporous silica replicas

Surfactant-directed block copolymer (BCP) particles have gained intensive attention owing to their attractive morphol-ogies and ordered domains. However, their controllable fabri-cation suffers several limitations including complex design and syn-thesis of multiple surfactant systems, limited choices of block copol-ymers, and time-consuming post-processes, etc. Herein, a surfactant size-dependent phase separation route is proposed to precisely ma-nipulate the architectures of the anionic block copolymer particles in the binary co-assembly system of BCP and surfactants. It is veri-fied that facile control on the ordered phase separation structures and morphologies of BCP particles can be achieved via simply vary-ing the alkyl lengths of the surfactants. Especially, the cationic sur-factants are demonstrated to integrate into the anionic polyacrylic acid (PAA) domain of BCP particles of polystyrene block polyacrylic acid (PS-b-PAA) to influence the volume fraction of PAA blocks, so that varied architectures of BCP particles are constructed. Based on these understandings, spherical or ellipsoidal BCP particles are ob-tained as expected, as well as their precisely inorganic mesoporous silica replicas through the block copolymer nanoparticle replicating route. Interestingly, the ellipsoidal mesoporous silica exhibits higher cellular internalization capability due to its lower energy expendi-ture during the internalization process. These findings may provide valuable insights into the confinement assembly of anionic block co-polymers and the creation of special nanocarriers for high-efficiency biomacromolecule delivery in the biomedical community.   

  1. 1. Lab of Low-Dimensional Materials Chemistry, Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, China
    2. Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, School of Chemistry and Chemical Engineering, Shihezi University, Shihezi 832003, China
    3. State Key Laboratory of High Performance Ceramics and Superfine Micro-structure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China
  • Received:2021-09-30 Revised:2021-12-02 Accepted:2021-12-03 Published:2021-12-03
  • Contact: LI Yongsheng ysli@ecust.edu.cn SHI Jianlin jlshi@mail.sic.ac.cn
  • Supported by:
    National Natural Science Foundation of China (Nos.51621002, 51972112, 22005096), Basic Research Pro-gram of Shanghai Municipal Government (Grant Nos. 21JC1406000, 19JC1411700), Shanghai Sailing program (20YF1410100), the Leading Talents in Shanghai in 2018 and the 111 project (B14018).

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Abstract: Surfactant-directed block copolymer (BCP) particles have gained intensive attention owing to their attractive morphol-ogies and ordered domains. However, their controllable fabri-cation suffers several limitations including complex design and syn-thesis of multiple surfactant systems, limited choices of block copol-ymers, and time-consuming post-processes, etc. Herein, a surfactant size-dependent phase separation route is proposed to precisely ma-nipulate the architectures of the anionic block copolymer particles in the binary co-assembly system of BCP and surfactants. It is veri-fied that facile control on the ordered phase separation structures and morphologies of BCP particles can be achieved via simply vary-ing the alkyl lengths of the surfactants. Especially, the cationic sur-factants are demonstrated to integrate into the anionic polyacrylic acid (PAA) domain of BCP particles of polystyrene block polyacrylic acid (PS-b-PAA) to influence the volume fraction of PAA blocks, so that varied architectures of BCP particles are constructed. Based on these understandings, spherical or ellipsoidal BCP particles are ob-tained as expected, as well as their precisely inorganic mesoporous silica replicas through the block copolymer nanoparticle replicating route. Interestingly, the ellipsoidal mesoporous silica exhibits higher cellular internalization capability due to its lower energy expendi-ture during the internalization process. These findings may provide valuable insights into the confinement assembly of anionic block co-polymers and the creation of special nanocarriers for high-efficiency biomacromolecule delivery in the biomedical community.

Key words: binary co-assembly, block copolymer, surfactant, mor-phology evolution, mesoporous materials