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Soft Matter · 2022 ·Vol. 18 ·期 11 ·2149-2156 · IF 4.046

Multi-level encryption of information in morphing hydrogels with patterned fluorescence

Li Xin Hou,Hongyao Ding,Xing Peng Hao,Chao Nan Zhu,Miao Du,Zi Liang Wu,Qiang Zheng

Fluorescent hydrogels have attracted tremendous attention recently in the field of information security due to the booming development of information technology. Along this line, it is highly desired to improve the security level of concealed information by the advancements of materials and encryption technologies. Here we report multi-level encryption of information in a bilayer hydrogel with shape-morphing ability and patterned fluorescence. This hydrogel is composed of a fluorescence layer containing chromophore units in the poly(acrylic acid) network and an active layer with UV-absorption agents in the poly(N-isopropylacrylamide-co-acrylic acid) network. The former layer exhibits tunable fluorescence tailored by UV light irradiation to induce unimer-to-dimer transformation of the chromophores, facilitating the write-in of information through photolithography. The latter layer is responsive to temperature, enabling morphing of the bilayer hydrogel. Therefore, the bilayer hydrogel encoded with patterned fluorescent patterns can deform into three-dimensional configurations at room temperature to conceal the information, which is readable only after successive procedures of shape recovery at an appropriate temperature and under UV light irradiation from the right direction. The combination of morphing materials and patterned fluorescence as a new avenue to improve the encryption level of information should merit the design of other smart materials with integrated functions for specific applications.

研究领域: 材料科学 · 信息安全
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Advanced Intelligent Systems · 2021 ·Vol. 3 ·期 7 ·2000270 · IF 0

Enhanced Locomotion of Shape Morphing Microrobots by Surface Coating

Suchun Ji,Xiying Li,Qianying Chen,Pengyu Lv,Huiling Duan

Mobile microrobots with shape morphing capability show great advantages for conducting tasks in complex environments. Combination of magnetically driven locomotion and stimuli-responsive shape morphing is an effective strategy to realize these microrobots. However, most existing microrobots fabricated by the combination strategy are of low locomotion efficiency due to the limited amount of magnetic material loaded. Herein, a novel scheme for coating the magnetic nanoparticles (NPs) on the surface of microrobot is proposed to increase the magnetic material loading amount. Theoretical analyses demonstrate that, below a critical size at microscale, surface coating NPs can load more magnetic material than embedding NPs into the volume due to the high surface area-to-volume ratio. Microrobots with both shape morphing and enhanced magnetically driven locomotion are fabricated by coating magnetic NPs on the surface of stimuli-responsive hydrogel microstructures. It is experimentally demonstrated that surface coating ensures that the microstructure has not only an efficient locomotion but also an excellent deformability. A four-claw microgripper is fabricated, which is smaller and has higher magnetically driven locomotion speed than the most existing shape morphing microrobots. This microgripper demonstrating carrying and delivery capabilities is of immediate interest to microobject manipulation and minimally invasive surgery.

研究领域: 生物医学工程 · 材料科学
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Materials Chemistry Frontiers · 2022 ·Vol. 6 ·期 15 ·2114-2121 · IF 8.683

Water-triggered synergistic fluorescence variation and shape deformation in a Zn-TCPP metal–organic framework-based gel

Xiangnan Wang,Zeyu Feng,Congyang Ye,Haofeng Zang,Yonghua Lu,Hongli Zhang,Gang Zou

Smart materials with programmable shape deformation and synergistic shape/fluorescence variation are highly desired in various practical applications, such as bio-inspired multifunctional robots and machines. However, it is still quite challenging to construct smart surfaces with dynamic fluorescence and morphology from MOFs, which potentially introduce superior performance. Herein, we proposed to utilize Zn-TCPP MOFs and polyurethane to construct a smart hybrid gel, which could exhibit synergistic dynamic fluorescence and reconfigurable patterns upon treating with pure water. Their reversible fluorescence variation as well as the swelling of the surface could be observed even directly by the naked eye. Based on the above results, we designed a dual-response rewriting pattern and flower-like artificial actuator with simultaneous fluorescence variation and shape deformation performance. This study would be of great fundamental value in the rational design of novel smart materials and surfaces.

CAS / MDL: 290-37-9
研究领域: 材料科学 · 化学工程
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Journal of Materials Chemistry C · 2021 ·Vol. 9 ·期 32 ·10295-10302 · IF 7.393

Bioinspired gradient hydrogel actuators with rewritable patterns and programmable shape deformation

Kangwei Mo,Jiehan Lin,Peng Wei,Jin Mei,Chunyu Chang

The botanical world inspires scientists to develop various smart actuators with diverse mechanical motions in response to external stimuli. However, it is challenging to obtain programmable and reversible hydrogel actuators. Herein, we presented a bioinspired nanocomposite hydrogel composed of poly(NIPAM-co-AA) and tunicate cellulose nanocrystals (TCNCs). A direct current electric field (DC-EF) was applied to induce controllable distribution of the TCNCs via electrophoresis for the formation of a gradient structure. To mimic the leaflet structure of Mimosa pudica, the patterns written using a lye pen on the hydrogel acted as the “pinnae” of leaves, while the residual regions worked as the “rachis” parts. With the increase of temperature, the “rachis” area of the nanocomposite hydrogel exhibited a large bending deformation because the gradient distribution of TCNCs induced asymmetric shrinkage, whereas the “pinnae” changed slightly because –COO−/–COO− electrostatic repulsion maintained the swelling state of the hydrogel network, like the leaflet folding of Mimosa pudica. Furthermore, these bioinspired hydrogel actuators with erasable and rewritable patterns exhibited programmable deformation, good stability, and good cycling performance. This work provided a facile yet efficient strategy for the fabrication of hydrogel actuators with rewritable patterns and programmable shape deformations.

研究领域: 材料科学 · 仿生学 · 智能材料
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Multi-stimuli responsive, shape deformation, and synergetic biomimetic actuator

Lian Chen,Yanlei Zhang,Kaihang Zhang,Fan Li,Gaigai Duan,Yue Sun,Xianshuo Wei,Xuxu Yang,Feng Wang,Chunmei Zhang,Shanshan Li,Xingyu Cao,Chunxin Ma,Shaohua Jiang

Hydrogel actuators with controllable deformation and excellent biocompatibility are widely used in soft robot, valve, drug delivery and lenses. However, the stimulation response performance of existing hydrogel actuators mostly focuses on a single active layer, which greatly affects its driving performance and service life. In this work, we integrate temperature-responsive hydrogel (Poly (N-isopropyl acrylamide), PNIPAM) and pH-responsive hydrogel (polyacrylic acid, PAAc) into one system to fabricate a dual active layer composite hydrogel actuator with high performance. Based on the PAAc hydrogels achieving contract or expand at different pH values, the obtained actuator exhibits admirable bidirectional bending characteristics. In addition, the anisotropic bamboo sheet endows the hydrogel actuator with programmable 3 D complex deformation. Benefitting from the synergy and different responsiveness between the two active layers, the hydrogel actuator not only has multiple response performance, but also greatly improves its deformation degree and response speed. More importantly, these promising properties of the actuator have broad application prospects in the development of pattern design and intelligent switch. This work proposes a promising strategy for the structural design of hydrogel actuators with excellent performance, and encourages more exploration of the application range of the actuator.

研究领域: 材料科学 · 生物医学工程
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Polymer Chemistry · 2020 ·Vol. 12 ·期 5 ·670-679 · IF 5.342

Salt-responsive polyampholyte-based hydrogel actuators with gradient porous structures

Zijian Shao,Shanshan Wu,Qian Zhang,Hui Xie,Tao Xiang,Shaobing Zhou

Stimuli-responsive materials with shape deformation properties play an important role in many fields such as artificial muscles, soft robots, and tissue engineering. Among them, stimuli-responsive hydrogels as actuators possessing shape deformation properties have been focused on. In this paper, a polyampholyte-based hydrogel with gradient pore construction is synthesized by a facile one-step random copolymerization, in which two sides of the reaction mold possess different hydrophilicity and hydrophobicity. The micro-Fourier transform infrared spectra prove the gradient distribution of chemical composition. Owing to the gradient pore construction and the ionic bonds, the polyampholyte-based hydrogel can rapidly change the shape when exposed to the environmental-friendly stimulus of water and recover to the original shape in salt solution, and the maximum bending angle reaches about 180°. Besides, this hydrogel actuator has a shorter recovery time compared with response time and the response/recovery time ratio is 2. By adjusting chemical and non-chemical factors including physical cross-link content, aspect ratio, salt solution concentration and soaking time, shape deformation degree and response/recovery time are controllable. Gradient pore construction and locomotion make this hydrogel actuator become a potential material for multiple applications.

研究领域: 材料科学 · 生物医学工程
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JOURNAL OF MATERIALS SCIENCE · 2021 ·Vol. 56 ·期 29 ·16324-16338 · IF 4.22

Anisotropic bilayer hydrogels with synergistic photochromism behaviors for light-controlled actuators

Gao Qiaofeng,Pan Pengju,Shan Guorong,Du Miao

Smart hydrogels have attracted widespread attention and have displayed comprehensive applications in many fields. The development of a novel type of bilayer hydrogel with synergistic function of anisotropic deformation and photochromic property is extremely challenging. Many previous researches have focused on multiple response hydrogels. However, it hardly achieves the synergy of deformation and color-changing through a method with the advantages of simplicity, stability, practicality, and precise control. Herein, a near-infrared light (NIR) photothermal thermoresponsive graphene oxide/poly( N -isopropylacrylamide- β -cyclodextrin) (PNIPAM- β -CD/GO) hydrogel layer and a reversible photochromic ammonium molybdate tetrahydrate/poly( N -isopropylacrylamide- co - β -cyclodextrin) (PNIPAM- β -CD/Mo 7 ) hydrogel layer were combined to obtain a bilayer hydrogel through the host–guest interactions between β -CD and the isopropyl group of NIPAM, exhibiting integrate anisotropic shape deformation and reversible photochromic behaviors. The designed actuators can undergo complex deformation owing to volume shrinkage caused by the photothermal effect under NIR of the PNIPAM- β -CD/GO layer, while the PNIPAM- β -CD/Mo 7 hydrogel layer shows the characteristics of quickly color changing within 5 s when irradiated by a UV light source. The multiple responsiveness of hydrogels on temperature, NIR irradiation, and UV irradiation displays valuable advantages in multifunctional smart materials, such as intelligent soft robots. Graphical abstract

研究领域: 材料科学 · 化学工程 · 生物医学工程
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Materials Chemistry Frontiers · 2021 ·Vol. 5 ·期 7 ·3192-3200 · IF 6.482

A facile approach for the preparation of liquid crystalline polyurethane for light-responsive actuator films with self-healing performance

Wenbo Shen,Bin Du,Jiaoshi Liu,Haitao Zhuo,Chuluo Yang,Shaojun Chen

In this study, liquid crystalline polyurethane was prepared by quaternization between ordinary polyurethane and mesogenic monomers. Meanwhile, a fast light-responsive actuator film with self-healing performance based on liquid crystalline polyurethane was successfully fabricated. In the film, the mesogenic units of the nematic compound were grafted on the polyurethane main chain, leading to liquid crystal phase of the polymer. The photoresponsive units of the liquid crystalline azobenzene were utilized as photosensitive components, and polyurethane was employed as the polymer matrix to endow the material with good film-forming and mechanical properties. The as-obtained actuator film not only showed a quick response and large shape deformation upon UV-irradiation but also exhibited temperature-induced self-healing performance. Moreover, the as-prepared light-responsive actuator film exhibited excellent properties coupled with easy fabrication, low cost, and good film-forming and relevant mechanical properties, showing promise for future practical applications in photo-driven and optomechanical devices.

研究领域: 材料科学 · 高分子化学
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MATERIALS & DESIGN · 2018 · IF 4.525

Supramolecular hydrogel hybrids having high mechanical property, photoluminescence and light-induced shape deformation capability: Design, preparation and characterization

Hangning Wang,Le Chen,Liang Fang,Lingyu Li,Jiaojiao Fang,Chunhua Lu,Zhongzi Xu

Integration of property, function, and intelligence in one single material obviously can further exploit applications of hydrogels, which remains a challenge. Physical mixing or chemical grating of functional components into hydrogels cannot easily achieve this goal. Here, we designed a new approach to prepare supramolecular hydrogel hybrids that presented high mechanical property, good photoluminescent function, and evident light-induced shape-deformation intelligence. Hydrogen bonding was constructed between nitrates in rare earth organic complex of Sm(TTA)Phen(NO 3 ) 3 (STPN) (TTA and Phen stand for α-thenoyltrifluoroacetone and 1,10-phenanthroline) and carboxyl groups in smart hydrogel networks. A facile solution mixing step without any harsh conditions allowed the successful preparation of hydrogel hybrids, which was suggested by the results of FTIR, 1 H NMR and UV–vis spectrophotometer. The compressive strength of hydrogel hybrids was increased greatly from 50 to 556 kPa after mixing STPN, while evident photoluminescence was demonstrated as well. More importantly, the presence of STPN enabled such supramolecular hydrogel hybrids to increase their temperatures and to contract shapes under the irradiation of near-infrared light at 1064 nm. This work provides a simple method to create supramolecular hydrogel hybrids that can be potentially used in the fields of soft actuators, drug delivery carriers, and so on.

研究领域: 材料科学 · 化学工程 · 生物医学工程
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Mechanically Strong, Tough, and Shape Deformable Poly(acrylamide-co-vinylimidazole) Hydrogels Based on Cu2+ Complexation

Chen Jiao,Jianan Zhang,Tianqi Liu,Xin Peng,Huiliang Wang

Shape deformable hydrogels have drawn great attention due to their wide applications as soft actuators. Here we report a novel kind of mechanically strong, tough, and shape deformable poly(acrylamide-co-vinylimidazole) [poly(AAm-co-VI)] hydrogel prepared by photoinitiated copolymerization and the followed immersing in a Cu2+ aqueous solution. Strong Cu2+ complexation with imidazole groups dramatically enhances the mechanical properties of the hydrogels, whose tensile strength, elastic modulus, toughness, and fracture energy reach up to 7.7 ± 0.76 MPa, 15.4 ± 1.2 MPa, 23.2 ± 2.5 MJ m–3, and 22.1 ± 2.3 kJ m–2, respectively. More impressively, shape deformation (bending) can be easily achieved by coating Cu2+ solution on one side of hydrogel strips. Furthermore, precise control of the shape deformation from 1D to 2D and 2D to 3D can be achieved by adjusting Cu2+ concentration, coating time, region, and one or two side(s) of hydrogel samples. The Cu2+ complexation provides a simple way to simultaneously improve the mechanical properties of hydrogels and enable them with shape deformability. The mechanically strong, tough, and shape deformable hydrogels might be a promising candidate for soft actuators.

研究领域: 材料科学 · 生物医学工程
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MATERIALS & DESIGN · 2018 · IF 4.525

Preparation and assembly of five photoresponsive polymers to achieve complex light-induced shape deformations

Tianyu Fang,Liangliang Cao,Shunping Chen,Jiaojiao Fang,Jia Zhou,Liang Fang,Chunhua Lu,Zhongzi Xu

Five photoresponsive polymers towards ultraviolet (UV), visible, and near-infrared (NIR) light were prepared and assembled to achieve complicated light-induced shape deformation. The UV light responsive polymer was contributed by a synthesized linear polyurethane elastomer (azo-PU) containing azobenzene groups in the main chains, which presented both shape-memory effect and UV light-induced shape deformation behavior . The other four polymers that were sensitive to visible or NIR light consisted of crosslinked poly(ethylene-co-vinyl acetate) (EVA) composites mixing with gold nanoparticles (AuNPs), Nd(TTA) 3 Phen, Yb(TTA) 3 Phen, and Sm(TTA) 3 Phen as photothermal fillers, respectively. The results showed that the shape recoveries of these EVA composites were triggered merely by visible and/or NIR light with suitable wavelengths. Moreover, the assembly of the prepared five light-induced polymers in three different manners improved the spatiotemporal control of complicated shape deformations upon different light illumination sequences. Benefiting from the creation and assembly of five photoresponsive polymers with high wavelength selectivities, complex shapes of polymer specimens can be achieved in a remote and non-contact manner via simply tuning irradiation sequences. The reported materials here and their assembly manners provide a strategy to expand the applications of photoresponsive polymers.

研究领域: 材料科学 · 高分子化学 · 光化学
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CHEMISTRY OF MATERIALS · 2023 · IF 8.6

Anisotropic Hydrogels Constructed via a Novel Bilayer-Co-Gradient Structure Strategy toward Programmable Shape Deformation

Shan Ye,Wenjing Ma,Guodong Fu

The bilayer hydrogel actuators have attracted extensive attention for their unique stimulus-responsive properties. Most of the current research studies only focused on changing the constituent materials of two layers in the fixed bilayer structure to enhance the responsive deformability of bilayer hydrogels without involving the exploration on a structural level, which limited its further development. In this study, we proposed a novel bilayer-co-gradient structure constructed via a simple and low-cost structural programming strategy, which was self-assembled by introducing an embedded gradient structure into a single bilayer structure with the assistance of gradient-dissolved oxygen in nature. This multistructure endowed the hydrogel with a faster bending response than a single bilayer structure due to the synergistic asymmetry of the simple bilayer structure and the embedded gradient structure. It was found that the prepared hydrogels exhibited significantly anisotropic electrical conductivity and swelling properties. Moreover, the stimulus-responsive shape deformation exhibited superior temperature- and pH-based deformation programmability. Additionally, this hydrogel could serve as a hydrogel gripper to perform grasping behavior, which demonstrated that our study opens up a new route for designing and fabricating smart actuators.

研究领域: 材料科学 · 智能材料 · 生物医学工程
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