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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Reversible Emission Color, Brightness, and Shape Changes of AIEgen-containing Bulk Polymers

Kaojin Wang,Han Si,Xianchao Du,Pengbo Han,Gaohuai Mei,Yanhua Cheng,Anjun Qin,Ben Zhong Tang

Bulk polymers generally exhibit faster response, higher shape-deformation speed, and stronger mechanical properties than the hydrogels. However, it still remains a formidable challenge to enable bulk polymers to exhibit reversible changes in shape and fluorescence simultaneously. Herein, for the first time, the temperature-responsive reversible changes in fluorescence color, brightness, and shape of semi-crystalline poly( ε -caprolactone) (PCL) network doped with a D-A based aggregation-induced emission luminogen (AIEgen) is realized. The fabricated flower-like and dragonfly-shaped actuators show reversible blooming-closing and wing fanning behaviors, respectively, as well as reversible fluorescence-changing effects. Notably, the response and shape-deformation speed as well as mechanical properties of the system is much better than the reported hydrogels. Moreover, a smart switch is developed to demonstrate the potential applications. The stick fabricated by the sample can lift and release an object 1000 times larger than its weight, serving as a color-changing artificial muscle. This material design strategy may shine light on the design and preparation of other reversible shape-deformation polymers in combination with stimuli-responsive luminescence-changing AIEgens, such as mechanochromic, thermochromic, and photochromic luminogens.

CAS / MDL: 10294-33-4 301-10-0
研究领域: 材料科学 · 聚合物化学 · 智能材料 · 纳米技术
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ADVANCED MATERIALS · 2025 · IF 26.8

Michell's-Instability-Mediated Fast Reconfiguration of Hydrogel-Based Ring Actuators

Qing Li Zhu,Zhijie Li,Hanlei Cheng,Weixuan Liu,Zhi Jian Wang,Olena Khoruzhenko,Josef Breu,Wei Hong,Qiang Zheng,Zi Liang Wu

Michell's instability, a classic type of mechanical instability, has received tremendous interest from different disciplines. It occurs when the pre-torsion in an elastic ring surpasses a critical value; the elastic ring spontaneously undergoes a transition from a flat or warped shape to a figure-of-eight configuration. However, such instability has rarely been exploited in designing soft actuators. Here, by employing a stimulus-triggered Michell's instability, hydrogel-based ring actuators capable of fast shape morphing are developed. Upon heating or light irradiation, the hydrogel ring transforms rapidly from the saddle-shape into the figure-of-eight configuration. Rigorous experiments and simulations reveal the underlying mechanism and attribute it to the stimuli-induced variations in bending and torsional stiffnesses of the gel string with anisotropic structure and response, which reduces the critical twist for Michell's instability of the ring actuator. Moreover, effects of light intensity, environmental temperature, ring size, and pre-torsion on reconfiguration are also investigated. The fast action of the ring actuators in aqueous conditions has been demonstrated through various tasks, such as screwing a bottle cap, kicking a ball, and triggering synergetic deformations. The design principle of soft actuators by harnessing Michell's instability should merit the development of other soft machines with fast action and large-amplitude reconfiguration.

CAS / MDL: 2210-25-5
研究领域: 软体机器人 · 材料科学 · 机械工程 · 智能材料 · 生物医学工程
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Tough Interfacial Adhesion of Bilayer Hydrogels with Integrated Shape Memory and Elastic Properties for Controlled Shape Deformation

Qilin Wang,Zhao Liu,Chen Tang,Huan Sun,Lin Zhu,Zhuangzhuang Liu,Ke Li,Jia Yang,Gang Qin,Gengzhi Sun,Qiang Chen

The weak adhesion between two hydrogel layers may lead to the delamination of bilayer hydrogels or low force transfer efficiency during deformation. Here, tough interfacial adhesive bilayer hydrogels with rapid shape deformation and recovery were prepared by simple attachment-heating of two gel layers. The bilayer hydrogels, composed of a shape memory gel (S-gel) and an elastic gel (E-gel), exhibited extremely tough interfacial adhesion between two layers (Γ ∼ 2200 J/m2). The shape deformation and shape recovery of the bilayer hydrogels, tuned by “heating–stretching” mode and “stretching–heating–stretching” mode, were rapid (<5 s) and no delamination between two gel layers was detected during shape deformation. Based on the fast shape deformation and recovery, the bilayer hydrogels could mimic the flower and hand, and a gel gripper could be fabricated to catch the object in the hot water. This work provides a simple method to prepare tough adhesive bilayer hydrogels with controlled shape deformation.

CAS / MDL: 29964-84-9 151-21-3
研究领域: 材料科学 · 聚合物化学 · 软体机器人
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Gels · 2022 ·Vol. 8 ·期 6 ·331 · IF 4.432

Anti-Freezing, Non-Drying, Localized Stiffening, and Shape-Morphing Organohydrogels

Jiayan Shen,Shutong Du,Ziyao Xu,Tiansheng Gan,Stephan Handschuh-Wang,Xueli Zhang

Artificial shape-morphing hydrogels are emerging toward various applications, spanning from electronic skins to healthcare. However, the low freezing and drying tolerance of hydrogels hinder their practical applications in challenging environments, such as subzero temperatures and arid conditions. Herein, we report on a shape-morphing system of tough organohydrogels enabled by the spatially encoded rigid structures and its applications in conformal packaging of “island–bridge” stretchable electronics. To validate this method, programmable shape morphing of Fe (III) ion-stiffened Ca-alginate/polyacrylamide (PAAm) tough organohydrogels down to −50 °C, with long-term preservation of their 3D shapes at arid or even vacuum conditions, was successfully demonstrated, respectively. To further illustrate the potency of this approach, the as-made organohydrogels were employed as a material for the conformal packaging of non-stretchable rigid electronic components and highly stretchable liquid metal (galinstan) conductors, forming a so-called “island–bridge” stretchable circuit. The conformal packaging well addresses the mechanical mismatch between components with different elastic moduli. As such, the as-made stretchable shape-morphing device exhibits a remarkably high mechanical durability that can withstand strains as high as 1000% and possesses long-term stability required for applications under challenging conditions.Keywords:organohydrogels;anti-freezing;shape-morphing;tough hydrogels;flexible electronics

研究领域: 材料科学 · 柔性电子 · 生物医学工程 · 聚合物科学
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Programmable Deformations of Biomimetic Composite Hydrogels Embedded with Printed Fibers

Si Yu Zheng,Chen Yu Li,Miao Du,Jun Yin,Jin Qian,Zi Liang Wu,Qiang Zheng

Shape deformations are prevalent in nature, which are closely related to the heterogeneous structures with a feature of fibrous elements embedded in a matrix. The microfibers with specific orientations act as either passive geometrical constraints in an active matrix or active elements in a passive matrix, which generate programmed internal stresses and drive shape morphing under external stimuli. Morphing materials can be designed in a biomimetic way, yet it is challenging to fabricate composite hydrogels with well-distributed fibers by a facile strategy. Here, we demonstrate the fabrication of microfiber-embedded hydrogels facilitated by the extrusion-based printing technology. Programmed deformations are achieved in these hydrogels with microfibers distributed in the upper and/or bottom layers of the gel matrix. Under external stimuli, the microfibers and the gel matrix have different responses that produce internal stresses and result in programmable deformations of the composite gel. Multiple shape transformations are realized in the hydrogel by embedding multiple types of responsive microfibers in the passive or active matrix, which is fabricated with the assistance of multinozzle printing. A soft hook is designed to show the capacity of the composite hydrogel to hold and move an object in a saline solution. This facile and versatile strategy provides an alternative way to prepare biomimetic hydrogels with potential applications in biomedical devices, flexible electronics, and soft robots.

研究领域: 材料科学 · 生物医学工程 · 机器人技术 · 纳米技术
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Polymer Chemistry · 2021 ·Vol. 13 ·期 6 ·829-837 · IF 5.582

Recyclable silicone elastic light-triggered actuator with a reconfigurable Janus structure and self-healable performance

Xiaowei Xu,Xinyue Hao,Jing Hu,Weisheng Gao,Nanying Ning,Bing Yu,Liqun Zhang,Ming Tian

Silicone rubber is a type of elastomer that possesses excellent biocompatibility and a good resistance to high and low temperatures and can be used as the matrix of smart materials in the biomedical field. As one of the attractive functions of smart materials, their regional shape transformation behavior under multiple stimuli is very useful. In order to produce silicone elastomers with these characteristics, a special structure such as a Janus structure is usually required. Herein, a novel strategy to prepare a silicone elastic light-triggered actuator with a Janus structure has been developed, which was fabricated via heterogeneous crosslinking induced by a gradient intensity of UV light due to carbon nanotube (CNT) accretion. By tailoring the geometric shapes, the region and time of the UV irradiation and the location of the stimulus, the Janus membranes can be programmed with multiple types of deformations and exhibit a shape transformation triggered by organic solvent or laser irradiation. Additionally, the membrane can be readily switched between Janus and homogeneous structures due to the reversible dimerization of anthracene, resulting in the reconfiguration of the membrane. Meanwhile, the composite membrane exhibits an excellent self-healing ability at 60 °C, or even room temperature, and can be recycled repeatedly via the hot-pressing or solution casting methods because of the introduction of reversible imine bonds into the crosslinked networks. This strategy provides significant guidance for the design of self-healable and reconfigurable soft biocompatible actuators, and so forth.

研究领域: 材料科学 · 生物医学工程 · 纳米技术 · 智能材料
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DYES AND PIGMENTS · 2022 · IF 5.122

Multi-responsive chromatic hydrogel exhibiting reversible shape deformations

Xiaozhen Xiao,Guiqiang Yang,Anbei Chen,Zhiyu Zheng,Chao Zhang,Yang Zhang,Liqiong Liao

In this work, deformable and chromatic hydrogel triggered by multi-stimuli was fabricated. This hydrogel was composed of N-isopropylacrylamide (NIPAAm), acryl-6-aminocaproic acid (A6ACA), and spiropyran (SP) derivatives, which possessed ferric ion (Fe 3+ ) and temperature-triggered shape deformations properties as well as chromatic behavior. Under ultraviolet light irradiation, the SP isomer in the hydrogel transformed to the merocyanine (MC) isomer, and the hydrogel showed the characteristic UV–Vis absorption peak of MC at 540 nm. The hydrogel revealed the selective chromatic response to Fe 3+ with the disappearance of the absorption peak of MC. Using ionoprinting technology, the hydrogel deformed programmatically in the presence of Fe 3+ . Moreover, owing to the anisotropic structure of the chromatic hydrogel, it realized reversible bending deformation triggered by temperature. The behaviors of hydrogels in response to dual stimuli (Fe 3+ and temperature) were further investigated, and the hydrogel showed programmable, spatiotemporal, and complex deformation behaviors , accompanying by the color change. This hydrogel will have great application potential in soft robotics, soft actuators, and environmental sensors.

研究领域: 材料科学 · 化学 · 软体机器人 · 环境科学
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Journal of the American Chemical Society · 2024 · IF 14.4

Construction of the Glycolysis Metabolic Pathway Inside an Artificial Cell for the Synthesis of Amino Acid and Its Reversible Deformation

Boyu Yang,Chao Li,Yongshuo Ren,Weichen Wang,Xiangxiang Zhang,Xiaojun Han

The bottom-up construction of artificial cells is beneficial for understanding cell working mechanisms. The glycolysis metabolism mimicry inside artificial cells is challenging. Herein, the glycolytic pathway (Entner–Doudoroff pathway in archaea) is reconstituted inside artificial cells. The glycolytic pathway comprising glucose dehydrogenase (GDH), gluconate dehydratase (GAD), and 2-keto-3-deoxygluconate aldolase (KDGA) converts glucose molecules to pyruvate molecules. Inside artificial cells, pyruvate molecules are further converted into alanine with the help of alanine dehydrogenase (AlaDH) to build a metabolic pathway for synthesizing amino acid. On the other hand, the pyruvate molecules from glycolysis stimulate the living mitochondria to produce ATP inside artificial cells, which further trigger actin monomers to polymerize to form actin filaments. With the addition of methylcellulose inside the artificial cell, the actin filaments form adjacent to the inner lipid bilayer, deforming the artificial cell from a spherical shape to a spindle shape. The spindle-shaped artificial cell reverses to a spherical shape by depolymerizing the actin filament upon laser irradiation. The glycolytic pathway and its further extension to produce amino acids (or ATP) inside artificial cells pave the path to build functional artificial cells with more complicated metabolic pathways.

研究领域: 合成生物学 · 代谢工程 · 细胞生物学 · 生物物理学 · 生物化学
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