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Dual pH-Responsive Hydrogel Actuator for Lipophilic Drug Delivery

  • Zilong Han
    Zilong Han
    State Key Laboratory of Fluid Power & Mechatronic System, Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province, Center for X-Mechanics, and Department of Engineering Mechanics, Zhejiang University, Hangzhou 310027, China
    More by Zilong Han
  • Peng Wang
    Peng Wang
    State Key Laboratory of Fluid Power & Mechatronic System, Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province, Center for X-Mechanics, and Department of Engineering Mechanics, Zhejiang University, Hangzhou 310027, China
    More by Peng Wang
  • Guoyong Mao
    Guoyong Mao
    State Key Laboratory of Fluid Power & Mechatronic System, Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province, Center for X-Mechanics, and Department of Engineering Mechanics, Zhejiang University, Hangzhou 310027, China
    More by Guoyong Mao
  • Tenghao Yin
    Tenghao Yin
    State Key Laboratory of Fluid Power & Mechatronic System, Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province, Center for X-Mechanics, and Department of Engineering Mechanics, Zhejiang University, Hangzhou 310027, China
    More by Tenghao Yin
  • Danming Zhong
    Danming Zhong
    State Key Laboratory of Fluid Power & Mechatronic System, Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province, Center for X-Mechanics, and Department of Engineering Mechanics, Zhejiang University, Hangzhou 310027, China
  • Burebi Yiming
    Burebi Yiming
    State Key Laboratory of Fluid Power & Mechatronic System, Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province, Center for X-Mechanics, and Department of Engineering Mechanics, Zhejiang University, Hangzhou 310027, China
  • Xiaocheng Hu
    Xiaocheng Hu
    State Key Laboratory of Fluid Power & Mechatronic System, Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province, Center for X-Mechanics, and Department of Engineering Mechanics, Zhejiang University, Hangzhou 310027, China
    More by Xiaocheng Hu
  • Zheng Jia
    Zheng Jia
    State Key Laboratory of Fluid Power & Mechatronic System, Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province, Center for X-Mechanics, and Department of Engineering Mechanics, Zhejiang University, Hangzhou 310027, China
    More by Zheng Jia
  • Guodong Nian*
    Guodong Nian
    State Key Laboratory of Fluid Power & Mechatronic System, Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province, Center for X-Mechanics, and Department of Engineering Mechanics, Zhejiang University, Hangzhou 310027, China
    *E-mail: [email protected] (G.N.).
    More by Guodong Nian
  • Shaoxing Qu*
    Shaoxing Qu
    State Key Laboratory of Fluid Power & Mechatronic System, Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province, Center for X-Mechanics, and Department of Engineering Mechanics, Zhejiang University, Hangzhou 310027, China
    *E-mail: [email protected] (S.Q.).
    More by Shaoxing Qu
  • , and 
  • Wei Yang
    Wei Yang
    State Key Laboratory of Fluid Power & Mechatronic System, Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province, Center for X-Mechanics, and Department of Engineering Mechanics, Zhejiang University, Hangzhou 310027, China
    More by Wei Yang
Cite this: ACS Appl. Mater. Interfaces 2020, 12, 10, 12010–12017
Publication Date (Web):February 13, 2020
https://doi.org/10.1021/acsami.9b21713
Copyright © 2020 American Chemical Society

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    Abstract

    Abstract Image

    As one of the most promising drug delivery carriers, hydrogels have received considerable attention in recent years. Many previous efforts have focused on diffusion-controlled release, which allows hydrogels to load and release drugs in vitro and/or in vivo. However, it hardly applies to lipophilic drug delivery due to their poor compatibility with hydrogels. Herein, we propose a novel method for lipophilic drug release based on a dual pH-responsive hydrogel actuator. Specifically, the drug is encapsulated and can be released by a dual pH-controlled capsule switch. Inspired by the deformation mechanism of Drosera leaves, we fabricate the capsule switch with a double-layer structure that is made of two kinds of pH-responsive hydrogels. Two layers are covalently bonded together through silane coupling agents. They can bend collaboratively in a basic or acidic environment to achieve the “turn on” motion of the capsule switch. By incorporating an array of parallel elastomer stripes on one side of the hydrogel bilayer, various motions (e.g., bending, twisting, and rolling) of the hydrogel bilayer actuator were achieved. We conducted an in vitro lipophilic drug release test. The feasibility of this new drug release method is verified. We believe this dual pH-responsive actuator-controlled drug release method may shed light on the possibilities of various drug delivery systems.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.9b21713.

    • Tough bonding of the hydrogel layers; pH-dependent ionization of basic functional groups on hydrogels chains responsible for swelling (Figure S1); preparation of bilayer hydrogels (Figure S2); covalent bonds formed between two hydrogel networks (Figure S3); 90 degree peeling test (Figure S4); the force–displacement curve of the peeling test for the PAAm–PAAc hydrogel bilayer (Figure S5); mechanical properties of pure PAAm hydrogel and PAAc hydrogel (Figure S6); and experimental design of the actuators with VHB stripes glued on one side (Figure S7) (PDF)

    • 90-degree peeling test (Movie S1) (MP4)

    • Bidirectional bending can be achieved by adjusting the pH value of the solution (Movie S2) (MP4)

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