CANDYBOTS: A New Generation of 3D-Printed Sugar-Based Transient Small-Scale Robots

Sugars are ubiquitous in food, and are among the main sources of energy for almost all forms of life. Sugars can also form structural building blocks such as cellulose in plants. Because of their inherent degradability and biocompatibility characteristics, sugars are compelling materials for transient devices. Here, an additive manufacturing approach for the production of magnetic sugar-based composites is introduced. First, it is shown that sugar-based 3D architectures can be 3D printed by selective laser sintering. This method enables not only the caramelization chemistry but also the mechanical properties of the sugar architectures to be adjusted by varying the laser energy. It is also demonstrated that mixtures of sugar and magnetic particles can be processed as 3D composites. As a proof of concept, a sugar-based millimeter-scale helical swimmer, which is capable of corkscrew motion in a solution with a viscosity comparable to those of biological fluids, is fabricated. The millirobot quickly dissolves in water, while being manipulated through magnetic fields. The present fabrication method can pave the way to a new generation of transient sugar-based small-scale robots for minimally invasive procedures. Due to their rapid dissolution, sugars can be used as an intermediate step for transporting swarms of particles to specific target locations.     

Two in One: Light as a Tool for 3D Printing and Erasing at the Microscale

The ability to selectively remove sections from 3D‐printed structures with high resolution remains a current challenge in 3D laser lithography. A novel photoresist is introduced to enable the additive fabrication of 3D microstructures at one wavelength and subsequent spatially controlled cleavage of the printed resist at another wavelength. The photoresist is composed of a difunctional acrylate cross‐linker containing a photolabile o‐nitrobenzyl ether moiety. 3D microstructures are written by photoinduced radical polymerization of acrylates using Ivocerin as photoinitiator upon exposure to 900 nm laser light. Subsequent scanning using a laser at 700 nm wavelength allows for the selective removal of the resist by photocleaving the o‐nitrobenzyl group. Both steps rely on two‐photon absorption. The fabricated and erased features are imaged using scanning electron microscopy (SEM) and laser scanning microscopy (LSM). In addition, a single wire bond is successfully eliminated from an array, proving the possibility of complete or partial removal of structures on demand.     

Characterization of rapid PDMS casting technique utilizing molding forms fabricated by 3D rapid prototyping technology (RPT)

In this work we characterize a novel possibility for PDMS (PolyDiMethylSiloxane) casting/ micromolding methods with the utilization of molding forms fabricated by a commercially available novel acrylic photopolymer based 3D printing method. The quality and absolute spatial accuracy of 1) different 3D printing modes (‘matt’ vs. ‘glossy’); 2) the molded PDMS structures and 3) the subsequently produced complementary structures made of epoxy resin were investigated. The outcome of these two form transfer technologies were evaluated by the cross sectional analysis of open microfluidic channels (trenches) with various design. Our results reveal the spatial accuracy in terms of real vs. CAD (Computer Aided Design) values for the 3D printed acrylic structures and the limits of their form transfer to PDMS, then to epoxy structures. Additionally the significant differences between the various spatial directions (X, Y, Z) have been characterized, and the conclusion was drawn that the ‘glossy’ printing mode is not appropriate for 3D printing of microfluidic molds.     

Bioinspired Soft Microrobots with Precise Magneto-Collective Control for Microvascular Thrombolysis

New-era soft microrobots for biomedical applications need to mimic the essential structures and collective functions of creatures from nature. Biocompatible interfaces, intelligent functionalities, and precise locomotion control in a collective manner are the key parameters to design soft microrobots for the complex bio-environment. In this work, a biomimetic magnetic microrobot (BMM) inspired by magnetotactic bacteria (MTB) with speedy motion response and accurate positioning is developed for targeted thrombolysis. Similar to the magnetosome structure in MTB, the BMM is composed of aligned iron oxide nanoparticle (MNP) chains embedded in a non-swelling microgel shell. Linear chains in BMMs are achieved due to the interparticle dipolar interactions of MNPs under a static magnetic field. Simulation results show that, the degree and speed of assembly is proportional to the field strength. The BMM achieves the maximum speed of 161.7 µm s⁻¹ and accurate positioning control under a rotating magnetic field with less than 4% deviation. Importantly, the locomotion analyses of BMMs demonstrate the frequency-dependent synchronization under 8 Hz and asynchronization at higher frequencies due to the increased drag torque. The BMMs can deliver and release thrombolytic drugs via magneto-collective control, which is promising for ultra-minimal invasive thrombolysis.     

Polymer magnetic microactuators fabricated with hot embossing and layer-by-layer nano self-assembly

Polymer-based magnetic microactuators have been fabricated with hot embossing technique and layer-by-layer (LbL) nano self-assembly. Silicon molds are fabricated with conventional UV lithography and wet etching techniques. Hot embossing is used to transfer the patterns from silicon molds to polymethylmethacrylate (PMMA) sheets. The overall processing time for the pattern transfer is less than 20 min. Low-cost devices with massive and rapid replication can be fabricated. Six layers of magnetic iron oxide (Fe2O3) nanoparticles are LbL self-assembled on the PMMA surface as the magnetically sensitive material. Positive photoresist PR1813 is used as the sacrificial layer to protect the gold electrode on the back side of the membrane. LbL nano self-assembly technique provides a simple method to obtain the magnetic film with low cost, short processing time, simple fabrication steps at room temperature. The volume of the magnetic material can be precisely controlled by the number of nano-assembled iron oxide layers. The mechanical, electrical, and magnetic properties of the microactuator are characterized by a laser interferometer. The natural frequency of the actuator is approximately 151 Hz; and the maximum deflection amplitude is about 34 nm. At all frequencies, the increase of the magnetic field increases the deflection amplitude which is in agreement with the theoretical equation.     

Toward Efficient Wound Management: Bioinspired Microfluidic and Microneedle Patch (Small 3/2023)

Microneedle (MN) patches hold demonstrated prospects in intelligent wound management. Herein, inspired by the highly folded structure of insect wings, a three-dimensional (3D) origami MN patch with superfine miniature needle structures, microfluidic channels, and multiple functions was reported to detect biomarkers, release drugs controllably and monitor motions to facilitate wound healing. By simply replicating the pre-stretched silicone rubber (Ecoflex) molds patterned by a laser engraving machine, the superfine structure MN patch with microfluidic channels was obtained from the restored molds. The bioinspired origami structure endows the MN patch with a high degree of functional integration, including microfluidic channels and electrocircuits. The microfluidic channels combined with the pH value and glucose concentration indicators enable the patch with the capability of biomarker sensing detection. Porous structures, a temperature-responsive hydrogel, and a photothermal-sensitive agent are utilized to form a controllable drug release system on the MN patch. Meanwhile, MXene electrocircuits were printed on the MN patch for motion sensing. In addition, the ability of the MN patch to accelerate wound healing was demonstrated by a mouse model experiment with full-thickness skin wounds. These results indicate that the multifunctional 3D origami MN patch is a valuable intelligent strategy for wound management.     

Magnetically Driven Undulatory Microswimmers Integrating Multiple Rigid Segments

Mimicking biological locomotion strategies offers important possibilities and motivations for robot design and control methods. Among bioinspired microrobots, flexible microrobots exhibit remarkable efficiency and agility. These microrobots traditionally rely on soft material components to achieve undulatory propulsion, which may encounter challenges in design and manufacture including the complex fabrication processes and the interfacing of rigid and soft components. Herein, a bioinspired magnetically driven microswimmer that mimics the undulatory propulsive mechanism is proposed. The designed microswimmer consists of four rigid segments, and each segment is connected to the succeeding segment by joints. The microswimmer is fabricated integrally by 3D laser lithography without further assembly, thereby simplifying microrobot fabrication while enhancing structural integrity. Experimental results show that the microswimmer can successfully swim forward along guided directions via undulatory locomotion in the low Reynolds number (Re) regime. This work demonstrates for the first time that the flexible characteristic of microswimmers can be emulated by 3D structures with multiple rigid segments, which broadens possibilities in microrobot design. The proposed magnetically driven microswimmer can potentially be used in biomedical applications, such as medical diagnosis and treatment in precision medicine.     

Scalable Nanoshaping of Hierarchical Metallic Patterns with Multiplex Laser Shock Imprinting Using Soft Optical Disks

Large‐area patterning of metals in nanoscale has always been a challenge. Traditional microfabrication processes involve many high‐cost steps, including etching and high‐vacuum deposit, which limit the development of functional nanostructures, especially multiscale metallic patterns. Here, multiplex laser shock imprinting (MLSI) process is introduced to directly manufacture hierarchical micro/nanopatterns at a high strain rate on metallic surfaces using soft optical disks with 1D periodic trenches as molds. The unique metal/polymer layered structures in inexpensive soft optical disks make them strong candidates of molds for MLSI processes. The feasibility of MLSI on hard metals toward soft molds is studied using theoretical simulation. In addition, various types of hierarchical structures are fabricated via MLSI, and their optical reflectance can be modulated via a combination of depth (laser power density), width (types of molds), and angles (rotation between molds). The optical properties have been studied with surface plasmon polariton modes theory. This work opens a new way of manufacturing hierarchical micro/nanopatterns on metals, which is promising for future applications in fields of plasmonics and metasurfaces.     

A Multidrug Delivery Microrobot for the Synergistic Treatment of Cancer

Multidrug combination therapy provides an effective strategy for malignant tumor treatment. This paper presents the development of a biodegradable microrobot for on-demand multidrug delivery. By combining magnetic targeting transportation with tumor therapy, it is hypothesized that loading multiple drugs on different regions of a single magnetic microrobot can enhance a synergistic effect for cancer treatment. The synergistic effect of using two drugs together is greater than that of using each drug separately. Here, a 3D-printed microrobot inspired by the fish structure with three hydrogel components: skeleton, head, and body structures is demonstrated. Made of iron oxide (Fe₃O₄) nanoparticles embedded in poly(ethylene glycol) diacrylate (PEGDA), the skeleton can respond to magnetic fields for microrobot actuation and drug-targeted delivery. The drug storage structures, head, and body, made by biodegradable gelatin methacryloyl (GelMA) exhibit enzyme-responsive cargo release. The multidrug delivery microrobots carrying acetylsalicylic acid (ASA) and doxorubicin (DOX) in drug storage structures, respectively, exhibit the excellent synergistic effects of ASA and DOX by accelerating HeLa cell apoptosis and inhibiting HeLa cell metastasis. In vivo studies indicate that the microrobots improve the efficiency of tumor inhibition and induce a response to anti-angiogenesis. The versatile multidrug delivery microrobot conceptualized here provides a way for developing effective combination therapy for cancer.     

A preliminary study of cushion properties of a 3D printed thermoplastic polyurethane Kelvin foam

The cells in conventional packaging foams have random size and orientation, and the energy‐absorbing behaviour of these foams is determined by the collective contribution of different sizes of cells. In contrast to the random nature of stochastic foams, 3D printing technologies allow engineers to design and produce foams having engineered cellular structures. In this study, engineered cellular structures based on the classic Kelvin 1887 model were 3D printed in 30 × 30 × 30 mm thermoplastic polyurethane cubes with a repeating size of 216 unit cells. One hundred consecutive cyclic compression tests were performed to assess the 3D printed foam's resilience and energy absorption characteristics. The stress‐strain curve of the 3D printed thermoplastic polyurethane foam indicated viscoelastic behaviour and a Mullins effect indicative of resilient rubber. A long wave buckling mode was observed during cyclic compression cycles due to the Kelvin structure. The cushion factor computed from the stress‐strain curve was close to that of a metal spring with linear elasticity. The combination of the 3D printed foam's resilience, its much lower density than rubber, and the complete geometric freedom of the engineered cellular structures offer designers the potential to create high‐performance cushion materials tailored for packaging applications.     

3D‐Printed Biomimetic Super‐Hydrophobic Structure for Microdroplet Manipulation and Oil/Water Separation

Biomimetic functional surfaces are attracting increasing attention for various technological applications, especially the superhydrophobic surfaces inspired by plant leaves. However, the replication of the complex hierarchical microstructures is limited by the traditional fabrication techniques. In this paper, superhydrophobic micro‐scale artificial hairs with eggbeater heads inspired by Salvinia molesta leaf was fabricated by the Immersed surface accumulation three dimensional (3D) printing process. Multi‐walled carbon nanotubes were added to the photocurable resins to enhance the surface roughness and mechanical strength of the microstructures. The 3D printed eggbeater surface reveals interesting properties in terms of superhydrophobilicity and petal effect. The results show that a hydrophilic material can macroscopically behave as hydrophobic if a surface has proper microstructured features. The controllable adhesive force (from 23 μN to 55 μN) can be easily tuned with different number of eggbeater arms for potential applications such as micro hand for droplet manipulation. Furthermore, a new energy‐efficient oil/water separation solution based on our biomimetic structures was demonstrated. The results show that the 3D‐printed eggbeater structure could have numerous applications, including water droplet manipulation, 3D cell culture, micro reactor, oil spill clean‐up, and oil/water separation.     

Rise of cyborg microrobot: different story for different configuration

By integrating organic parts achieved through evolution and inorganic parts developed by human civilisation, the cyborg microrobot is rising by taking advantage of the high flexibility, outstanding energy efficiency, extremely exquisite structure in the natural components and the fine upgradability, nice controllability in the artefact parts. Compared to the purely synthetic microrobots, the cyborg microrobots, due to the exceptional biocompatibility and biodegradability, have already been utilised in in situ diagnosis, precise therapy and other biomedical applications. In this review, through a thorough summary of recent advances of cyborg microrobots, the authors categorise the cyborg microrobots into four major classes according to the configuration between biomaterials and artefact materials, i.e. microrobots integrated inside living cell, microrobots modified with biological debris, microrobots integrated with single cell and microrobots incorporated with multiple cells. Cyborg microrobots with the four types of configurations are introduced and summarised with the combination approaches, actuation mechanisms, applications and challenges one by one. Moreover, they conduct a comparison among the four different cyborg microrobots to guide the actuation force promotion, locomotion control refinement and future applications. Finally, conclusions and future outlook of the development and potential applications of the cyborg microrobots are discussed.Inspec keywords: medical robotics, cellular biophysics, mobile robots, molecular biophysics, polymers, microrobotsOther keywords: locomotion control refinement, actuation force promotion, combination approaches, biological debris, living cell, artefact materials, biomaterials, biomedical applications, biodegradability, exceptional biocompatibility, natural components, energy efficiency, human civilisation, purely synthetic microrobots, cyborg microrobot     

Polycarbonate Heat Molding for Soft Lithography

Soft lithography enables rapid microfabrication of many types of microsystems by replica molding elastomers into master molds. However, master molds can be very costly, hard to fabricate, vulnerable to damage, and have limited casting life. Here, an approach for the multiplication of master molds into monolithic thermoplastic sheets for further soft lithographic fabrication is introduced. The technique is tested with master molds fabricated through photolithography, mechanical micromilling as well as 3D printing, and the results are demonstrated. Microstructures with submicron feature sizes and high aspect ratios are successfully copied. The copying fidelity of the technique is quantitatively characterized and the microfluidic devices fabricated through this technique are functionally tested. This approach is also used to combine different master molds with up to 19 unique geometries into a single monolithic copy mold in a single step displaying the effectiveness of the copying technique over a large footprint area to scale up the microfabrication. This microfabrication technique can be performed outside the cleanroom without using any sophisticated equipment, suggesting a simple way for high‐throughput rigid monolithic mold fabrication that can be used in analytical chemistry studies, biomedical research, and microelectromechanical systems.     

Electro‐Assisted Bioprinting of Low‐Concentration GelMA Microdroplets

Low‐concentration gelatin methacryloyl (GelMA) has excellent biocompatibility to cell‐laden structures. However, it is still a big challenge to stably fabricate organoids (even microdroplets) using this material due to its extremely low viscosity. Here, a promising electro‐assisted bioprinting method is developed, which can print low‐concentration pure GelMA microdroplets with low cost, low cell damage, and high efficiency. With the help of electrostatic attraction, uniform GelMA microdroplets measuring about 100 μm are rapidly printed. Due to the application of lower external forces to separate the droplets, cell damage during printing is negligible, which often happens in piezoelectric or thermal inkjet bioprinting. Different printing states and effects of printing parameters (voltages, gas pressure, nozzle size, etc.) on microdroplet diameter are also investigated. The fundamental properties of low‐concentration GelMA microspheres are subsequently studied. The results show that the printed microspheres with 5% w/v GelMA can provide a suitable microenvironment for laden bone marrow stem cells. Finally, it is demonstrated that the printed microdroplets can be used in building microspheroidal organoids, in drug controlled release, and in 3D bioprinting as biobricks. This method shows great potential use in cell therapy, drug delivery, and organoid building.     

Magnetoactive Acoustic Metamaterials

Acoustic metamaterials with negative constitutive parameters (modulus and/or mass density) have shown great potential in diverse applications ranging from sonic cloaking, abnormal refraction and superlensing, to noise canceling. In conventional acoustic metamaterials, the negative constitutive parameters are engineered via tailored structures with fixed geometries; therefore, the relationships between constitutive parameters and acoustic frequencies are typically fixed to form a 2D phase space once the structures are fabricated. Here, by means of a model system of magnetoactive lattice structures, stimuli‐responsive acoustic metamaterials are demonstrated to be able to extend the 2D phase space to 3D through rapidly and repeatedly switching signs of constitutive parameters with remote magnetic fields. It is shown for the first time that effective modulus can be reversibly switched between positive and negative within controlled frequency regimes through lattice buckling modulated by theoretically predicted magnetic fields. The magnetically triggered negative‐modulus and cavity‐induced negative density are integrated to achieve flexible switching between single‐negative and double‐negative. This strategy opens promising avenues for remote, rapid, and reversible modulation of acoustic transportation, refraction, imaging, and focusing in subwavelength regimes.     

3D Printed High‐Performance Lithium Metal Microbatteries Enabled by Nanocellulose

Batteries constructed via 3D printing techniques have inherent advantages including opportunities for miniaturization, autonomous shaping, and controllable structural prototyping. However, 3D‐printed lithium metal batteries (LMBs) have not yet been reported due to the difficulties of printing lithium (Li) metal. Here, for the first time, high‐performance LMBs are fabricated through a 3D printing technique using cellulose nanofiber (CNF), which is one of the most earth‐abundant biopolymers. The unique shear thinning properties of CNF gel enables the printing of a LiFePO₄ electrode and stable scaffold for Li. The printability of the CNF gel is also investigated theoretically. Moreover, the porous structure of the CNF scaffold also helps to improve ion accessibility and decreases the local current density of Li anode. Thus, dendrite formation due to uneven Li plating/stripping is suppressed. A multiscale computational approach integrating first‐principle density function theory and a phase‐field model is performed and reveals that the porous structures have more uniform Li deposition. Consequently, a full cell built with a 3D‐printed Li anode and a LiFePO₄ cathode exhibits a high capacity of 80 mA h g^?1 at a charge/discharge rate of 10 C with capacity retention of 85% even after 3000 cycles.     

Three dimensional printed macroporous polylactic acid/hydroxyapatite composite scaffolds for promoting bone formation in a critical-size rat calvarial defect model

We have explored the applicability of printed scaffold by comparing osteogenic ability and biodegradation property of three resorbable biomaterials. A polylactic acid/hydroxyapatite (PLA/HA) composite with a pore size of 500 μm and 60% porosity was fabricated by three-dimensional printing. Three-dimensional printed PLA/HA, β-tricalcium phosphate (β-TCP) and partially demineralized bone matrix (DBM) seeded with bone marrow stromal cells (BMSCs) were evaluated by cell adhesion, proliferation, alkaline phosphatase activity and osteogenic gene expression of osteopontin (OPN) and collagen type I (COL-1). Moreover, the biocompatibility, bone repairing capacity and degradation in three different bone substitute materials were estimated using a critical-size rat calvarial defect model in vivo. The defects were evaluated by micro-computed tomography and histological analysis at four and eight weeks after surgery, respectively. The results showed that each of the studied scaffolds had its own specific merits and drawbacks. Three-dimensional printed PLA/HA scaffolds possessed good biocompatibility and stimulated BMSC cell proliferation and differentiation to osteogenic cells. The outcomes in vivo revealed that 3D printed PLA/HA scaffolds had good osteogenic capability and biodegradation activity with no difference in inflammation reaction. Therefore, 3D printed PLA/HA scaffolds have potential applications in bone tissue engineering and may be used as graft substitutes in reconstructive surgery.     

3D‐Printed Transparent Glass

Silica inks are developed, which may be 3D printed and thermally processed to produce optically transparent glass structures with sub‐millimeter features in forms ranging from scaffolds to monoliths. The inks are composed of silica powder suspended in a liquid and are printed using direct ink writing. The printed structures are then dried and sintered at temperatures well below the silica melting point to form amorphous, solid, transparent glass structures. This technique enables the mold‐free formation of transparent glass structures previously inaccessible using conventional glass fabrication processes.     

A New 3D Printing Strategy by Harnessing Deformation,Instability, and Fracture of Viscoelastic Inks

Direct ink writing (DIW) has demonstrated great potential as a multimaterial multifunctional fabrication method in areas as diverse as electronics, structural materials, tissue engineering, and soft robotics. During DIW, viscoelastic inks are extruded out of a 3D printer's nozzle as printed fibers, which are deposited into patterns when the nozzle moves. Hence, the resolution of printed fibers is commonly limited by the nozzle's diameter, and the printed pattern is limited by the motion paths. These limits have severely hampered innovations and applications of DIW 3D printing. Here, a new strategy to exceed the limits of DIW 3D printing by harnessing deformation, instability, and fracture of viscoelastic inks is reported. It is shown that a single nozzle can print fibers with resolution much finer than the nozzle diameter by stretching the extruded ink, and print various thickened or curved patterns with straight nozzle motions by accumulating the ink. A quantitative phase diagram is constructed to rationally select parameters for the new strategy. Further, applications including structures with tunable stiffening, 3D structures with gradient and programmable swelling properties, all printed with a single nozzle are demonstrated. The current work demonstrates that the mechanics of inks plays a critical role in developing 3D printing technology.     

3D Printing of Living Responsive Materials and Devices

3D printing has been intensively explored to fabricate customized structures of responsive materials including hydrogels, liquid‐crystal elastomers, shape‐memory polymers, and aqueous droplets. Herein, a new method and material system capable of 3D‐printing hydrogel inks with programed bacterial cells as responsive components into large‐scale (3 cm), high‐resolution (30 μm) living materials, where the cells can communicate and process signals in a programmable manner, are reported. The design of 3D‐printed living materials is guided by quantitative models that account for the responses of programed cells in printed microstructures of hydrogels. Novel living devices are further demonstrated, enabled by 3D printing of programed cells, including logic gates, spatiotemporally responsive patterning, and wearable devices.