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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-8 · IF 16.6

3D printing of dynamic covalent polymer network with on-demand geometric and mechanical reprogrammability

Fang Zizheng,Shi Yunpeng,Mu Hongfeng,Lu Runzhi,Wu Jingjun,Xie Tao

Delicate geometries and suitable mechanical properties are essential for device applications of polymer materials. 3D printing offers unprecedented versatility, but the geometries and mechanical properties are typically fixed after printing. Here, we report a 3D photo-printable dynamic covalent network that can undergo two independently controllable bond exchange reactions, allowing reprogramming the geometry and mechanical properties after printing. Specifically, the network is designed to contain hindered urea bonds and pendant hydroxyl groups. The homolytic exchange between hindered urea bonds allows reconfiguring the printed shape without affecting the network topology and mechanical properties. Under different conditions, the hindered urea bonds are transformed into urethane bonds via exchange reactions with hydroxyl groups, which permits tailoring of the mechanical properties. The freedom to reprogram the shape and properties in an on-demand fashion offers the opportunity to produce multiple 3D printed products from one single printing step.

研究领域: 材料科学 · 化学工程 · 高分子科学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Lightweight and geometrically complex ceramics derived from 4D printed shape memory precursor with reconfigurability and programmability for sensing and actuation applications

Siyao Chen,Jinping Li,Haofan Shi,Xuliang Chen,Guo Liu,Songhe Meng,Jian Lu

There is growing interest in additive manufacturing (AM) of ceramics due to the feasibility of achieving geometrically complex shapes for various engineering applications. Polymer-derived ceramics (PDCs), pyrolyzed from polymeric ceramic precursors, act as a competitive material for ceramic AM with advantages such as easy processability, flexible designability, and relatively low sintering temperature. However, the functionality of preceramic polymers is far from being fully exploited, thus restricting the development and applications of 3D printed ceramics. Herein, a novel multifunctional preceramic polymer composite with reconfigurability and shape memory effect is synthesized. By tuning the material compositions, the precursor inks suitable for 4D printing are pyrolyzed into lightweight self-shaping ceramics, allowing complex geometries to be fabricated. The preceramic polymers undergo a stepwise partial-to-full crosslinking process to form interpenetrating polymer networks , resulting in reconfigurability where the as-printed parts can be transformed into shapes with higher complexity. Unlike traditional precursors with static shapes, the precursor here possesses shape memory capability ( T g  ∼ 95 °C). During the sintering process, the 3D printed precursor could successively undergo programmable active shape transformation with a high recovery ratio (∼100 %) and pyrolysis conversion into lightweight ceramics (1.05 g/cm 3 ). By exploring the semiconducting behavior of resulting ceramics, temperature sensors leveraging the advantages of reshaping are designed to detect the surface over a wide range (25–750 °C) with good conformability. The development of 4D printed reconfigurable and programmable precursors for the construction of complex ceramics enriches both the complexity and self-shaping capability of ceramics, allowing them to be applied as smart thermistors and deployable structures.

CAS / MDL: 1675-54-3 19438-60-9
研究领域: 材料科学 · 智能材料 · 增材制造
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Additive Manufacturing · 2024 · IF 10.3

Integrated 3D printing of reconfigurable soft machines with magnetically actuated crease-assisted pixelated structures

Youchao Zhang,Xiaoyang Zhu,Huangyu Chen,Ruichen Wang,Siqi Qiu,Houchao Zhang,Hongke Li,Zhenghao Li,Rui Wang,Fan Zhang,Guangming Zhang,Yuan-Fang Zhang,Dong Wang,Hongbo Lan

Reconfigurable magnetic soft machines have a wide range of applications in soft robotics, aerospace, medical devices and flexible electronics. However, the high-precision reconfiguration of magnetically actuated soft machines is hindered by the absence of rational structural design and integrated manufacturing techniques. Here, we report an innovative design and manufacturing approach to realize magnetically actuated high-precision reconfigurability. We present a crease-assisted pixelated design using a mixture of magnetic particles and phase-change medium as the pixel points, with an elastomer as the crease to connect the pixel points, simulating origami. The design of elastomer creases improves pixel stiffness without loss of reconfigurable accuracy, thereby significantly improves the magnetic particle concentration in the pixel. An effective multi-material 3D printing technique is used to achieve the integrated printing of the designed structure. The resulting magnetically actuated soft machines exhibit remarkable capabilities, achieving small curvature bending and precise reconfiguration with weaker actuating magnetic fields (100mT). The superior performance of this design has been confirmed through demonstrations of crawling and rolling machines, magnetically controlled switches, and logic circuits. The work enhances the reconfiguration accuracy of magnetically actuated soft machines, increasing their potential for soft robotics and flexible electronics applications.

研究领域: 软体机器人学 · 柔性电子 · 材料科学
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CELLULOSE · 2021 ·Vol. 28 ·期 5 ·2879-2888 · IF 5.044

Construction of a new green vitrimer material: introducing dynamic covalent bond into carboxymethyl cellulose

Li Chang,Ju Benzhi,Zhang Shufen

The synthesis of the first cellulose-based vitrimer is described. Dynamic ester bonds were responsible for the dynamic properties of carboxymethyl cellulose (CMC)-based vitrimer. The addition of suitable catalyst and glycerol in the vitrimer formulations was crucial for the reprocessability of these materials. Thermogravimetric and dynamic mechanical analyses tensile strength tests were performed to investigate the effect of the catalyst and glycerol on the thermal stability and mechanical properties of the materials. A minimum amount of 5 mol% of 1,5,7-triazabicyclo[4.4.0]dec-5-ene with respect to the carboxyl group content was required to maintain reprocessability by hot press. The CMC vitrimer exhibited good reprocessability and shape memory ability. Our work demonstrates that cellulose, the most abundant bio-resource on the planet, can be a promising raw material for bio-based vitrimer due to its excellent renewability and low cost. Graphic abstract

研究领域: 材料科学 · 化学工程
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA · 2023 ·Vol. 120 ·期 28 ·e2302907120 · IF 11.1

Open millifluidics based on powder-encased channels

Xiaoguang Li,Xianglong Pang,Haohao Jiang,Mei Duan,Heng Liu,Zhujun Yang,Yuhang Xi,Thomas P. Russell

Millifluidics, the manipulation of liquid flow in millimeter-sized channels, has been a revolutionary concept in chemical processing and engineering. The solid channels that contain the liquids, though, are not flexible in their design and modification, and prevent contact with the external environment. All-liquid constructs, on the other hand, while flexible and open, are imbedded in a liquid environment. Here, we provide a route to circumvent these limitations by encasing the liquids in a hydrophobic powder in air that jams on the surface, containing and isolating flowing fluids, offering flexibility and adaptability in design, as manifest in the ability to reconfigure, graft, and segment the constructs. Along with the open nature of these powder-contained channels that allow arbitrary connections/disconnections and substance addition/extraction, numerous applications can be opened in the biological, chemical, and material arenas.

CAS / MDL: 9002-84-0
研究领域: 化学工程 · 生物学 · 材料科学
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SmartMat · 2024 · IF 15.3

Reconfigurable and orthogonal stiffness-structure patterning of dynamically crosslinked amphigels

Chen Yang,Weizhong Zheng,Chujun Ni,Ye Li,Di Chen,Tao Xie,Qian Zhao

Patterning diversified properties and surface structure of polymer materials are of great importance toward their potential in biology, optics, and electronics. However, achieving both the patternability of stiffness and microstructure in a reconfigurable manner remains challenging. Here, we prepare amphigels crosslinked by dynamic disulfide bonds, which can be reversibly swollen by immiscible water or liquid paraffin. In the paraffingel form, the materials exhibited a high modulus of 130 MPa due to densified hydrogen bonds. Whereas swollen by water, the modulus fell over two orders of magnitude owing to the destruction of the hydrogen bonds. Via regionalized swelling of the solvents, well-controlled and rewritable soft/stiff mechanical patterns can be created. On the other hand, the dynamic exchange of the disulfide crosslinking enables mechanophoto patterning to fabricate sophisticated macrogeometries and microstructures. The reconfigurable stiffness-structure patterning can be manipulated orthogonally, which will create more application opportunities beyond conventional hydrogels and organogels.

研究领域: 材料科学 · 生物工程 · 化学工程
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Advanced Science · 2024 · IF 14.3

Reconfigurability-Encoded Hierarchical Rectifiers for Versatile 3D Liquid Manipulation

Jiaqi Miao,Alan C. H. Tsang

Manipulating small-volume liquids is crucial in natural processes and industrial applications. However, most liquid manipulation technologies involve complex energy inputs or non-adjustable wetting gradient surfaces. Here, a simple and adjustable 3D liquid manipulation paradigm is reported to control liquid behaviors by coupling liquid–air–solid interfacial energy with programmable magnetic fields. This paradigm centers around a hierarchical rectifier with magnetized microratchets, using Laplace pressure asymmetry to enable multimodal directional steering of various surface tension liquids (23–72 mN m −1 ). The scale-dependent effect in microratchet design shows its superiority in handling small-volume liquids across three orders of magnitude (10 0 –10 3 µL). Under programmed magnetic fields, the rectifier can reconfigure its morphology to harness interfacial energy to exhibit richer liquid behaviors without dynamic real-time control. Reconfigured rectifiers show improved rectification performance in the inertia-dominant fluid regime, i.e., a remarkable 2000-fold increase in the critical Weber number for pure ethanol. Moreover, the rectifier's switchable reconfigurations offer flexible control over liquid transport directions and spatiotemporally controllable 3D liquid manipulation reminiscent of inchworm motions. This scalable liquid manipulation paradigm promotes versatile engineering and biochemistry applications, e.g., portable liquid purity testing (screening resolution <1 mN m −1 ), logical open-channel microfluidics, and automated chemical reaction platforms.

研究领域: 材料科学 · 生物工程 · 化学工程
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Bio-Mimetic Actuators of a Photothermal-Responsive Vitrimer Liquid Crystal Elastomer with Robust, Self-Healing, Shape Memory, and Reconfigurable Properties

Die Tang,Lun Zhang,Xiaoyu Zhang,Liqiang Xu,Ke Li,Aimin Zhang

Soft actuators with apparent uniqueness in exhibiting complex shape morphing are highly desirable for artificial intelligence applications. However, for the majority of soft actuators, in general, it is challenging to achieve versatility, durability, and configurability simultaneously. Enormous works are devoted to meet the multifunctional smart actuators, to little effect. Herein, self-healing and bio-mimetic smart actuators are proposed based on azobenzene chromophores and dynamic disulfide bonds. Benefiting from the dynamic and drivable vitrimer liquid crystal elastomer (V-LCE) materials, a series of actuators with single or compound dynamic three-dimensional structures were fabricated, which were capable of double-stimuli response and complex “bionic” motions, such as the blooming of a flower, grasping and loosening an object, and so forth. Moreover, these flexible actuators showed fascinating properties, such as high robustness, excellent elasticity–plasticity shape-memory properties (Rf and Rr are close to 100%), easily reconfigurable property, and self-healing. This smart V-LCE provides a guideline to design and fabricate soft versatility actuators, which has prospects for developing smart bionic and artificial intelligence devices.

CAS / MDL: 62-23-7 90-72-2
研究领域: 材料科学 · 智能材料 · 仿生学
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Harnessing the Day–Night Rhythm of Humidity and Sunlight into Mechanical Work Using Recyclable and Reprogrammable Soft Actuators

Qiaomei Chen,Xiaojie Qian,Yanshuang Xu,Yang Yang,Yen Wei,Yan Ji

Toward a sustainable society, soft actuators driven by environmentally friendly energy from nature are of great social and economic significance. Meanwhile, recyclability, repeated reconfiguration for other use, and complex three-dimensional (3D) geometries are also essential for mitigating the energy crisis and practical application demands. Here, we integrate all of the above features in one actuator using vitrimers with exchangeable disulfide links. By reconfiguration, welding, patterning, and kirigami techniques, complex 3D actuators can be easily fabricated, which can be repeatedly reconfigured for other applications to save cost in new material preparation. These actuators operate synergistically with the day–night rhythm of humidity and sunlight without the need of extra energy input.

CAS / MDL: 111-20-6
研究领域: 材料科学 · 可持续能源 · 智能材料
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Nature Communications · 2022 ·Vol. 13 ·期 1 ·1-14 · IF 17.694

Exploiting ferrofluidic wetting for miniature soft machines

Sun Mengmeng,Hao Bo,Yang Shihao,Wang Xin,Majidi Carmel,Zhang Li

Miniature magnetic soft machines could significantly impact minimally invasive robotics and biomedical applications. However, most soft machines are limited to solid magnetic materials, whereas further progress also relies on fluidic constructs obtained by reconfiguring liquid magnetic materials, such as ferrofluid. Here we show how harnessing the wettability of ferrofluids allows for controlled reconfigurability and the ability to create versatile soft machines. The ferrofluid droplet exhibits multimodal motions, and a single droplet can be controlled to split into multiple sub-droplets and then re-fuse back on demand. The soft droplet machine can negotiate changing terrains in unstructured environments. In addition, the ferrofluid droplets can be configured as a liquid capsule, enabling cargo delivery; a wireless omnidirectional liquid cilia matrix capable of pumping biofluids; and a wireless liquid skin, allowing multiple types of miniature soft machine construction. This work improves small magnetic soft machines’ achievable complexity and boosts their future biomedical applications capabilities.

研究领域: 机器人学 · 材料科学 · 生物医学工程
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Advanced Materials Technologies · 2023 ·Vol. 8 ·期 14 ·2300029 · IF 6.8

Reconfigurable and Reprocessable Thermadapt Stress-Free Two-Way Shape Memory Polymers Based on a Dual Crosslinking Network with Outstanding Mechanical Properties

Sijia Ren,Jiachun Feng

The reconfigurable and reprocessable thermadapt two-way shape memory polymers (2W-SMPs) are highly desirable for many advanced biomimetic applications, but the preparation of these polymers with economical raw materials and convenient approaches still remains a challenge. In this work, thermadapt 2W-SMPs based on a dual crosslinking network are synthesized by linking polyethylene glycol with hydroxylated modified SBS via dynamic covalent bonds. Benefiting from the synergistic effect of combining a dynamic covalent network and a physical cross-linking network, the thermadapt 2W-SMPs exhibit a good balance of mechanical properties and favorable two-way shape memory effect (2W-SME) with the reversible actuation strain of 11.9%. The 2W-SMPs can be reprocessed and transformed into complex 3D shapes after multiple folding processes due to the dynamic covalent exchange as well as the reversible physical crosslinking, and the obtained new samples still exhibit good 2W-SMEs. Furthermore, the transition temperature of 2W-SMPs is designed to be close to human body temperature, and it is manufactured into a biomimetic mimosa actuator that can undergo shape changes through finger contact and cooling. This work provides a new idea for the development of thermadapt 2W-SMPs, and the obtained materials show great potential applications in intelligent actuators.

研究领域: 材料科学 · 生物仿生学
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POLYMER · 2020 · IF 4.231

Epoxy-vitrimer composites based on exchangeable aromatic disulfide bonds: Reprocessibility, adhesive, multi-shape memory effect

Fance Ji,Xiangdong Liu,Dekun Sheng,Yuming Yang

Vitrimers are a class of polymers integrating the advantage of thermosets and thermoplastics . The dynamic crosslinking networks endow vitrimers with interesting rheological behavior and functional applications, such as self-healing, thermally plasticity and shape memory properties. Here, based on the dynamic aromatic disulfide bonds, a series of vitrimer composites with reconfigurability and tunable mechanical properties were successfully prepared. Using the time-temperature superposition, we prove that the relaxation of vitrimer composites should be divided into two distinct parts, including the topological rearrangement of epoxy network and the relaxation of thermoplastic components. Meanwhile, the physical entanglement of thermoplastics and the reconfigurability of chemical cross-links enable vitrimer composites to have excellent adhesive property . Based on the reconfigurability of vitrimer composites, the multi-shape memory effect was readily realized through blending the vitrimer composites of different glass transition by a simple hot-pressing method. It is anticipated that this novel strategy will pave way for the fabrication of thermosetting polymers with both reconfigurability and functional applications.

CAS / MDL: 109-99-9
研究领域: 材料科学 · 高分子化学
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