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Small · 2021 ·Vol. 18 ·期 2 ·2104440 · IF 13.281

Precisely Defining Local Gradients of Stimuli-Responsive Hydrogels for Complex 2D-to-4D Shape Evolutions

Jincai Yin,Wenxin Fan,Zihan Xu,Jinghua Duan,Yanzhi Xia,Zhihong Nie,Kunyan Sui

The intellectualization and complication of existing self-shaping materials are limited by the inseparable monotonic relationship between their deformation rate and deformation degree (i.e., a higher deformation rate is accompanied by a high deformation degree). This causes that they can only deform from 2D to 3D states. Here, a simple yet versatile strategy to decouple the monotonic correlation between the deformation rate and deformation degree of self-shaping hydrogels is presented for achieving complex deformations from 2D to temporary 3D to 3D (2D-to-4D). It is demonstrated that when the gradient hydrogels prepared by photopolymerization possess dense polymer networks, the local regions with a high deformation rate can exhibit a low deformation degree. The resulting hydrogels can thus deform in a novel 2D-to-4D mode under external stimuli. During the deformation, they first transform into the temporary shapes induced by the local deformation rate difference, and then transform into the final shapes determined by the local deformation degree difference. Through controlling the ultraviolet irradiation direction and time to precisely program the local gradients of self-shaping hydrogels, they can be designed to produce various unprecedented yet controllable 2D-to-4D shape evolutions on demand, such as transformable origami, sequential gesture actions in finger-guessing games, mobile octopuses, time switch, etc.

研究领域: 生物材料学 · 高分子化学 · 软体机器人 · 组织工程 · 智能材料 · 仿生学
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ACS Omega · 2022 · IF 4.132

Controlled Transformation of Liquid Metal Microspheres in Aqueous Solution Triggered by Growth of GaOOH

Xiaofei Li,Xin Ding,Yuhang Du,Chao Xiao,Kang Zheng,Xianglan Liu,Xingyou Tian,Xian Zhang

Liquid metals (LMs) are playing an increasingly important role in the fields of flexible devices, electronics, and thermal management due to their low melting point and excellent thermal and electrical conductivity, and the transformation of LMs in deionized water has recently received much attention. In this paper, we investigate the transformation process of EGaIn microspheres in deionized water and propose a two-step process of microspherical transformation, whereby the microspheres are first deformed into a spindle shape and then into lamellar nanorods. It is also shown that the growth of GaOOH crystals drives the transformation. Based on this result, EGaIn microspheres with controllable transformation could be prepared, such as spindle or lamellar rod shapes, extending the application area of LMs.

研究领域: 材料科学 · 纳米技术 · 化学工程
✓ 已验证 DOI PubMed 高影响因子
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BIOMACROMOLECULES · 2015 · IF 5.75

Shape Transformation of Light-Responsive Pyrene-Containing Micelles and Their Influence on Cytoviability

Haisheng Wang,Wenbo Zhang,Changyou Gao

The amphiphilic pyrene-containing random copolymers with light-responsive pyrene ester bonds were synthesized by copolymerizing 1-pyrenemethyl acrylate (PA) and N,N-dimethylacrylamide (DMA). The P(DMA-co-PA) copolymers formed spherical micelles in water, which were transformed into nanorods as a result of cleavage of the pyrene ester bonds under UV irradiation. In vitro culture with A549 cells and Raw cells showed that compared to the nonphotodegradable ones, the photodegradable P(DMA-co-PA) micelles caused significantly higher cytotoxicity under the same UV irradiation. The intracellular reactive oxygen species (ROS) level had a positive correlation with the cytotoxicity regardless of the cell types. The nonphotodegradable pyrene-containing micelles produced a lower level of ROS under UV irradiation. However, the photodecomposable P(DMA-co-PA) micelles produced a significant higher level of ROS under the same trigger of UV irradiation, which caused the shape transformation of micelles to nanorods and higher cytotoxicity simultaneously.

CAS / MDL: 78-67-1
研究领域: 高分子化学 · 生物医学工程 · 细胞生物学
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CHEMBIOCHEM · 2024 · IF 2.6

Oligoadenine Strand Functionalized Polyacrylamide Hydrogel Film Exhibiting pH-Triggered High-Degree Inverse Shape Deformations

Mengyuan Yin,Xiaohong Hu,Yu Chen,Hanxue Liang,Yuxin Shen,Weiwei Guo

Smart shape-memory DNA hydrogels, which can respond to various types of external stimuli and undergo macroscopic shape deformations, have shown great potential in various applications. By constructing free-standing films, the deformation and response properties of these hydrogels can be further enhanced, and visualized deformation can be achieved. However, DNA hydrogels that can exhibit rapid and high-degree shape deformations, such as the inverse shape deformations, are still lacking. Herein, free-standing oligoadenine strand-functionalized polyacrylamide hydrogel films were developed that can exhibit rapid and high-degree of inverse shape deformation upon cyclic pH changes. The oligoadenine strands exhibit a pH-stimulated reversible conformational transition between a flexible single-stranded state and parallel duplex A-motif structures, resulting in their role change in the film from negatively charged side chains to “head-to-head” crosslinking structures, driving a high degree of inverse shape deformation with a relative bending angle change of 223.7%, which is more than 5 times that of a film driven by pH-responsive i-motif structures, facilitating the development of bilayer hydrogel film actuators with potential in flexible sensors and robots.

研究领域: 生物材料学 · 高分子化学 · 智能材料
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MOLECULES · 2025 ·Vol. 30 ·期 10 ·2106 · IF 4.6

Study on Photodeformation of Solvent Resistance in Hydrogen-Bonded Cross-Linked Main-Chain Azobenzene Films

Zhaoyang Zhang,Shengkui Ma,Jianfeng Gao

Hydrogen-bonded cross-linked main chain azobenzene (azo) photoactive polymers have broad application prospects in flexible actuators, optical actuators, and other fields. Most of the research on this kind of photoresponsive material is mainly focused on air, and exploration in solvents remains underexplored. In this paper, azobenzene polyamide ester semicrystalline polymer (PEA-6T) with hydrogen-bond cross-linking was synthesized by Michael addition polymerization. The uniaxially oriented polymer film with high orientation (48.85%) and fast response (5 s under UV light and 55 s under visible light) was obtained by a simple solution casting/mechanical stretching method. Compared with PEA-2T and PEA-4T, PEA-6T exhibits enhanced mechanical properties (elastic modulus increased by 17.4%; yield strength increased by 34.1%; breaking strength increased by 75.4%; elongation at break increased by 33.8%; toughness increased by 101.3%; photoinduced stress increased by 43.5%) and reduced light response time (decreased by 58.3% in ultraviolet light and 50% in visible light) due to the elongation of the compliant chain length. The thin PEA-6T film exhibited light-induced deformation not only in air but also in polar solvents such as water, methanol, ethanol, butanol, and saline solutions (e.g., normal saline, 0.9 wt% NaCl, and simulated seawater, 3.5 wt% NaCl). In addition, polarizing optical microscope (POM) observations showed that the brightness and texture direction of the films remained stable (ΔBrightness< 5%), the light response time was consistent (6 s under UV light, 65 s under visible light), the light-induced stress retention rate was 95%, and the films exhibited good solvent resistance. This study bridges the research gap in azobenzene photoresponsive materials in solvent environments, and the material shows potential for applications in marine equipment coatings or biomedical actuators.

CAS / MDL: 1191-08-8 1191-43-1
研究领域: 材料科学 · 光化学 · 生物医学工程
✓ 已验证 产品关联 DOI PubMed 高影响因子
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SENSORS AND ACTUATORS B-CHEMICAL · 2025 · IF 7.7

An acoustically actuated hydrogel shape-morphing micromachine

Yaxuan Xiao,Xiong Zhao,Li Ma,Yichen Wang,Guoxin Mao,Jinhua Zhang,Bin Fang,Nanjing Hao

Bioinspired by the transformations of animals and plants such as pangolins and mimosas, many biomimetic shape-morphing systems have been developed. However, due to scale effect, microscale interactions become the dominant force, which may make the traditional shape-morphing systems ineffective. Acoustic actuation is expected to overcome this challenge. Here, we have developed an acoustically actuated hydrogel shape-morphing micromachine (AHSMM). It has a variable stiffness design, with the lower stiffness part serving as a flexible hinge to achieve transformation. Under the excitation of acoustic field, the flexible hinge produces strong oscillation and quickly provides the force and torque required for the transformation of AHSMM (generally less than 500 ms). In addition, we have developed a preprogrammed design for the transformation of micromachine to predict its transformation morphology. Furthermore, through the AHSMM, we have separately designed morphing transformations between Chinese characters (e.g., “夫” (fu) to “央” (yang)) and English letters (e.g., “k” to “x”). Finally, we developed a shape-morphing microrobot (width: 174.33 μm) utilizing this flexible hinge, which can pass through a narrow channel through its own shape-morphing, providing great potential in targeted drug delivery (the shape-morphing time is less than 100 ms, the forward speed can reach about 800 μm/s). Our work not only provides innovative ideas for shape-morphing design at the microscale, but also expands the coupling applications of acoustics, soft matter, and microrobots.

CAS / MDL: 126-96-5 7473-98-5
研究领域: 生物医学工程 · 微型机器人技术 · 柔性机器人 · 声学 · 仿生学 · 水凝胶技术
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ACS Applied Polymer Materials · 2019 · IF 0

Multiresponsive Reversible Deformation of Patterned Polyacrylamide Hydrogel Constructed by a Computer-Assisted Dispenser

Xiao-Qin Zhang,Di Wu,Jun-Bo Hou,Jun-Feng Feng,Duo Ke,Sheng Zhang,Bang-Jing Li

Materials that can undergo shape deformation have potential applications in biomedical field, yet it has always been a challenge to pattern hydrogels and accurately program target three-dimensional (3D) shapes through a simple method. Here, we develop a facile method that permits fabrication of inhomogeneous hydrogels, which can reversibly deform from planar sheet to 3D shape in response to multistimuli, such as pH values, SLDC (solutions with lower dielectric constant), and SBF (simulated body fluid). By printing NaOH solution ink on classic PAAm hydrogel sheet, the amide side groups of PAAm hydrolyzed to acrylate. The swelling mismatch of the printed and unprinted areas generates internal stress to activate hydrogel deformation. Adjusting concentration of NaOH solution or number of times of printing, it is convenient to introduce in-plane and through-thickness gradient distribution to hydrogel sheet. The inkjet printing process is easily controlled by computer, enabling the direct printing of batched and complicated patterns. Three-dimensional structures, such as helix, tube, and surface of constant Gaussian curvature can be achieved simply.

研究领域: 材料科学 · 生物医学工程
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ADVANCED MATERIALS · 2021 ·Vol. 34 ·期 5 ·2107855 · IF 30.849

Solvent-Assisted 4D Programming and Reprogramming of Liquid Crystalline Organogels

Binjie Jin,Jiaqi Liu,Yunpeng Shi,Guancong Chen,Qian Zhao,Shu Yang

Encoding molecular ordering during liquid crystalline network (LCN) formation endows preprogrammed but fixed shape morphing in response to external stimuli. The incorporation of dynamic covalent bonds enables shape reprogramming but also permanently alters the network structures. Here, an entropic approach that can program complex shapes via directed solvent evaporation from an isotropic LCN organogel is discoursed. Different shapes can be erased and reprogrammed from the same LCN on demand depending on the modes of deformation of the organogel during solvent evaporation. The ability to decouple network synthesis and molecular alignment relaxes the requirements to LCN chemistry and alignment methods, allowing for the realization of a variety of origami/kirigami structures and 4D shape morphing of LCNs printed from the digital light processing technique with unattainable spatial and temporal controls.

研究领域: 高分子科学 · 软物质物理 · 智能材料 · 功能材料 · 4D打印技术
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Small Methods · 2018 ·Vol. 2 ·期 6 ·1800017 · IF 0

Engineering Microstructure with Evaporation-Induced Self-Assembly of Microdroplets

Pingan Zhu,Tiantian Kong,Chunmei Zhou,Leyan Lei,Liqiu Wang

Natural systems have exceptional capabilities of constructing structures across multiple length scales for remarkable performances from limited choices of building blocks. However, simultaneous control over structures at both the macroscopic and microscopic length scales is restricted by the high requirements in the type and property of building blocks. Here, directed self-assembly of microdroplets in an evaporating liquid is harnessed to fabricate large-scale ordered films with precisely controlled microstructures. Evaporation-induced variations in liquid confinement allow microdroplets to reassemble for large-scale ordered patterns. Deformation of microdroplets into different shapes accurately defines multiple topographical structures at the microdroplet level. The fabrication process is facile and scalable, and works with various materials for manufacturing functional films with tunable properties. These results suggest a facile yet effective strategy for engineering microstructures by combining directed self-assembly with manipulation of the property of building components for both structural fidelity and diversity.

研究领域: 材料科学 · 纳米科技 · 软物质物理 · 表面科学 · 功能薄膜
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Soft Matter · 2025 · IF 2.8

Lipid bilayer-mediated spatiotemporal correlation between near-wall confined motion of micro-carriers

Wei Liu,Jinwei Zhong,Pui Wo Felix Yeung,Xiahui Xiao,Yuwei Zhu,To Ngai

We employed intensity fluctuations of evanescent light scattering to probe spatiotemporal correlations in the near-wall confined motion of microspheres on supported lipid bilayers (SLBs). Normalized cross-correlation analysis revealed long-range, time-resolved correlations in particle–wall separation distances, demonstrating that interfacial stress propagation can transmit mechanical signals across membrane interfaces. The motion exhibited broadly corralled diffusion, with both the corral size and diffusion constant confined to the nanoscale. This confinement could be further classified into fast and slow modes, with most diffusion constants residing in the slow regime, indicating that SLBs predominantly retard and localize microsphere dynamics at the interface. Furthermore, a transition in the interbilayer interaction profile—from bimodal to single-peak behavior—introduced a characteristic length scale and a kT-scale energy barrier, underscoring the cooperative interplay between interfacial stress propagation and membrane shape remodeling.

CAS / MDL: 4235-95-4
研究领域: 生物物理学 · 纳米生物技术 · 细胞膜生物学 · 分子影像学 · 软物质物理
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Small · 2025 ·Vol. 21 ·期 39 ·e06930 · IF 12.1

Fire-Ant-Inspired Magnetic Swarms with Stable Flotation for Programmable Shape Morphing and Cooperative Multitasking

Yuhang Hu,Xiaofeng Chen,Qiuhuang Chen,Zhigang Wang,Ziming Song,Shun Liu,Chunjie Yan,Chi Zhang,Heng Deng

Inspired by the remarkable buoyancy and collective adaptability of fire ant rafts, this study presents magnetic composite micro-floaters (MCMs) capable of stable flotation at air-water interfaces—a key advancement for magnetic microrobotic swarms in fluid environments. The system overcomes the intrinsic sinking tendency of high-density NdFeB microparticles through bioinspired surface engineering. MCMS are fabricated via a solvent-exchange phase inversion process, encapsulating NdFeB cores with hydrophobic polycaprolactone (PCL) and engineered surface roughness. This design emulates the hydrophobic cuticle and air-trapping strategies of fire ants, conferring exceptional resistance to vertical magnetic fields (up to 0.5 T) without submersion. Unlike conventional approaches, this eliminates reliance on restrictive parallel-field configurations. When subjected to programmable magnetic fields, MCM swarms exhibit dynamic self-assembly, reconfiguration into complex structures, and stable navigation through wave-disturbed environments while preserving swarm cohesion. Their multifunctional performance includes cargo transport at 70 times their weight, guided oil spill remediation via controlled aggregation, and precise manipulation of droplets (200 times their volume) for merging, stirring, and maze navigation—all achieved at the air–water interface. By synergizing fire ant-inspired flotation stability with magnetic reconfigurability, this work establishes a versatile platform for surface-based microrobotics, unlocking new opportunities in environmental remediation, microfluidics, and programmable matter.

✓ 已验证 DOI PubMed 高影响因子
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

High-Strength and Fast-Response Liquid Crystal Elastomer Fiber and Fabric Actuators

Yuhang Wang,Shengbo Zhou,Jianyong Feng

LCE (liquid crystal elastomer) fibers can achieve large and reversible deformation under stimulation, which has attracted widespread attention in the field of materials. Current LCE fiber production methods include 3D/4D printing that uses layer-by-layer deposition principles. While wet spinning overcomes these limitations by achieving in situ active alignment of mesogens during curing, enabling reliable kilometer-scale continuous fiber fabrication. By varying the polymerization times of LCE oligomers in spinning solutions, we achieved different polymerization degrees, resulting in distinct viscosities. We use wet spinning to prepare LCE fibers with spinning solutions of different viscosities (200, 220, 240, 260, 280, 300, and 320 mPa·s). The strength of LCE fibers prepared at a viscosity of 280 mPa·s reaches up to 170 MPa, and the tensile property reaches 520%, which is higher than those in previous representative works. Temperature response tests showed 35% reversible shrinkage within 2 s at 80 °C. In addition, by blending LCE fibers with traditional cotton yarn fabrics, we prepared smart fabrics that retain the comfort of traditional fabrics and are temperature-responsive. Under active contraction of the LCE fibers, the fabric can show a 32% reversible shrinkage. The LCE continuous fibers prepared by this method can be widely used in the textile industry, providing new insights into the field of smart textiles.

CAS / MDL: 174063-87-7
研究领域: 材料科学 · 高分子科学 · 智能材料 · 纺织工程 · 驱动器技术
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