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Additive manufacturing (AM) has revolutionised the manufacturing industry, offering versatile capabilities for creating complex geometries directly from a digital design. Among the various 3D printing methods for polymers, vat photopolymerisation combines photochemistry and 3D printing. Despite the fact that single-epoxy 3D printing has been explored, the fabrication of multi-material bioderived epoxy thermosets remains unexplored. This study introduces the feasibility and potential of multi-material 3D printing by means of a dual-vat Digital Light Processing (DLP) technology, focusing on bioderived epoxy resins such as ELO (epoxidized linseed oil) and DGEVA (vanillin alcohol diglycidyl ether). By integrating different materials with different mechanical properties into one sample, this approach enhances sustainability and offers versatility for different applications. Through experimental characterisation, including mechanical and thermal analysis, the study demonstrates the ability to produce structures composed of different materials with tailored mechanical properties and shapes that change on demand. The findings underscore the promising technology of dual-vat DLP technology applied to sustainable bioderived epoxy monomers, allowing sustainable material production and complex structure fabrication.

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Modern additive manufacturing enables the simultaneous processing of different materials during the printing process. While multimaterial 3D printing allows greater freedom in part design, the prediction of the mix-material properties becomes challenging. One type of multimaterials are matrix-inclusion composites, where one material contains inclusions of another material. Aim of this study was to develop a method to predict the uniaxial Young's modulus and Poisson's ratio of material jetted matrix-inclusion composites by a combination of simulations and experimental data.Fifty samples from commercially available materials in their pure and matrix-inclusion mixed forms, with cubic inclusions, have been fabricated using material jetting and mechanically characterized by uniaxial tensile tests. Multiple simulation approaches have been assessed and compared to the measurement results in order to find and validate a method to predict the multimaterials' properties. Optical coherence tomography and microscopy was used to characterize the size and structure of the multimaterials, compared to the design.The materials exhibited Young's moduli in the range of 1.4 GPa to 2.5 GPa. The multimaterial mixtures were never as stiff as the weighted volume average of the primary materials (up to [Formula: see text] softer for 45% RGD8530-DM inclusions in VeroClear matrix). Experimental data could be predicted by finite element simulations by considering a non-ideal contact stiffness between matrix and inclusion ([Formula: see text] for RGD8530-DM, [Formula: see text] for RGD8430-DM), and geometries of the printed inclusions that deviated from the design (rounded edge radii of [Formula: see text]m). Not considering this would lead to a difference of the estimation result of up to [Formula: see text]MPa (44%), simulating an inclusion volume fraction of 45% RGD8530-DM.Prediction of matrix-inclusion composites fabricated by multimaterial jetting printing, is possible, however, requires a priori knowledge or additional measurements to characterize non-ideal contact stiffness between the components and effective printed geometries, precluding therefore a simple multimaterial modelling.

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Self-healing silicones that are able to restore functionalities and extend the lifetime of soft devices hold great potential in many applications. However, currently available silicones need to be triggered to self-heal or suffer from creep-induced irreversible deformation during use. Here, a platform is proposed to design and print silicone objects that are programmed at the molecular and architecture levels to achieve self-healing at room temperature while simultaneously resisting creep. At the molecular scale, dioxaborolanes moieties are incorporated into silicones to synthesize self-healing vitrimers, whereas conventional covalent bonds are exploited to make creep-resistant elastomers. When combined into architectured printed parts at a coarser length scale, the layered materials exhibit fast healing at room temperature without compromising the elastic recovery obtained from covalent polymer networks. A patient-specific vascular phantom and fluidic chambers are printed to demonstrate the potential of architectured silicones in creating damage-resilient functional devices using molecularly designed elastomer materials.

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Additive manufacturing (AM), which is based on the principle of layer-by-layer shaping and stacking of discrete materials, has shown significant benefits in the fabrication of complicated implants for tissue engineering (TE). However, many native tissues exhibit anisotropic heterogenous constructs with diverse components and functions. Consequently, the replication of complicated biomimetic constructs using conventional AM processes based on a single material is challenging. Multimaterial 3D and 4D bioprinting (with time as the fourth dimension) has emerged as a promising solution for constructing multifunctional implants with heterogenous constructs that can mimic the host microenvironment better than single-material alternatives. Notably, 4D-printed multimaterial implants with biomimetic heterogenous architectures can provide a time-dependent programmable dynamic microenvironment that can promote cell activity and tissue regeneration in response to external stimuli. This paper first presents the typical design strategies of biomimetic heterogenous constructs in TE applications. Subsequently, the latest processes in the multimaterial 3D and 4D bioprinting of heterogenous tissue constructs are discussed, along with their advantages and challenges. In particular, the potential of multimaterial 4D bioprinting of smart multifunctional tissue constructs is highlighted. Furthermore, this review provides insights into how multimaterial 3D and 4D bioprinting can facilitate the realization of next-generation TE applications.

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Lithium-ion batteries (LIBs) have significantly impacted the daily lives, finding broad applications in various industries such as consumer electronics, electric vehicles, medical devices, aerospace, and power tools. However, they still face issues (i.e., safety due to dendrite propagation, manufacturing cost, random porosities, and basic & planar geometries) that hinder their widespread applications as the demand for LIBs rapidly increases in all sectors due to their high energy and power density values compared to other batteries. Additive manufacturing (AM) is a promising technique for creating precise and programmable structures in energy storage devices. This review first summarizes light, filament, powder, and jetting-based 3D printing methods with the status on current trends and limitations for each AM technology. The paper also delves into 3D printing-enabled electrodes (both anodes and cathodes) and solid-state electrolytes for LIBs, emphasizing the current state-of-the-art materials, manufacturing methods, and properties/performance. Additionally, the current challenges in the AM for electrochemical energy storage (EES) applications, including limited materials, low processing precision, codesign/comanufacturing concepts for complete battery printing, machine learning (ML)/artificial intelligence (AI) for processing optimization and data analysis, environmental risks, and the potential of 4D printing in advanced battery applications, are also presented.

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BACKGROUND: Diabetic heel ulceration is a common, detrimental, and costly complication of diabetes. This study investigates a novel "graded-stiffness" offloading method, which consists of a heel support with increasing levels of stiffness materials to better redistribute plantar pressure for heel ulcer prevention and treatment. RESEARCH QUESTION: Is the novel "graded-stiffness" solution better able to redistribute heel pressure and reduce focal stress concentration areas of the heel? METHODS: Twenty healthy young men walked with four, 3D-printed, insole configurations. The configurations included the "graded-stiffness" insoles with and without an offloading hole under the heel tissue at risk for ulcerations and two conventional offloading supports of flat insoles with no offloading and simple holed offloading insoles. In-shoe plantar pressure was measured using the Pedar-X system. Peak pressure and pressure dose were measured at three heel regions: offloaded region, perimeter of offloaded region, and periphery region. RESULTS: The simple offloading configuration reduced pressure at the offloaded region; however, pressure at the perimeter of the offloading region significantly increased. With respect to ANOVA, the "graded-stiffness" offloading configurations were more effective than existing tested solutions in reducing and redistributing heel peak pressure and pressure dose, considering all heel regions. SIGNIFICANCE: The "graded-stiffness" offloading solution demonstrated a novel flexible and customized solution that can be manufactured on-demand through a precise selection of the graded-stiffness offloading location and material properties to fit the shape and size of the ulcer. This study is a follow-up in-vivo pilot study, in a healthy population group, to our previous computation modeling work that reported the efficiency of the "graded-stiffness" configuration, and which emphasizes its potential for streamlining and optimizing the prevention and treatment of diabetic heel ulcers.

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Diabetic heel ulceration is a serious, destructive, and costly complication of diabetes. In this study, a novel "graded-stiffness" offloading method was proposed. This method consists of heel support with multi-increasing levels of stiffness materials, to prevent and treat heel ulcers. A three-dimensional finite element model of the heel was used to evaluate the novel "graded-stiffness" orthotic device compared to two existing solutions: (1) an insole with a hole under the active ulcer and (2) an insole with a hole filled with a soft material (elastic modulus of 15 kPa). Volumetric exposure evaluation of internal tissues to stress was performed at two volume-of-interests: (1) the area of the heel soft tissues typically at high risk for ulceration, and (2) the soft tissues surrounding the high-risk area. The models predict that the "graded-stiffness" offloading solution is more effective than existing solutions in distributing and reducing heel internal loads, considering both volume-of-interests. Comparing different material gradient combinations for the offloading support reveals considerable variation of the heel stress distribution. In clinical practice, the "graded-stiffness" technological solution enables to form an adaptable and flexible system that can be customized to a specific patient, through adequate selection of the offloading materials, to fit the shape and size of the ulcer. This solution can be made as an off-the-shelf product or alternatively, be manufactured by-demand using 3D printing tools. The proposed novel practical offloading solution has the potential for streamlining and optimizing the prevention and treatment of diabetic heel ulcers.

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Additive manufacturing or 3D printing of materials is a prominent process technology which involves the fabrication of materials layer-by-layer or point-by-point in a subsequent manner. With recent advancements in additive manufacturing, the technology has excited a great potential for extension of simple designs to complex multi-material geometries. Vat photopolymerization is a subdivision of additive manufacturing which possesses many attractive features, including excellent printing resolution, high dimensional accuracy, low-cost manufacturing, and the ability to spatially control the material properties. However, the technology is currently limited by design strategies, material chemistries, and equipment limitations. This review aims to provide readers with a comprehensive comparison of different additive manufacturing technologies along with detailed knowledge on advances in multi-material vat photopolymerization technologies. Furthermore, we describe popular material chemistries both from the past and more recently, along with future prospects to address the material-related limitations of vat photopolymerization. Examples of the impressive multi-material capabilities inspired by nature which are applicable today in multiple areas of life are briefly presented in the applications section. Finally, we describe our point of view on the future prospects of 3D printed multi-material structures as well as on the way forward towards promising further advancements in vat photopolymerization.

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One-dimensional (1D) fibers have been widely used in composites reinforcement for microwave attenuation due to their outstanding mechanical and electromagnetic properties, especially in the axial direction. However, the precise control of fiber alignment in a polymer matrix remains a challenge. In this work, we successfully demonstrated the well-controlled alignment of silicon carbide nanowires (SiCNW) in a silicone matrix by using direct ink writing (DIW)-based 3D printing. It is proven that the printed multilayer material with fiber alignment could show a dramatic improvement in both reflection loss (RL) and effective attenuation bandwidth (EAB, RL < -10 dB). In particular, a uniaxial in-plane orientation is found to be the optimal alignment among other planar and also out-of-plane orientations. Benefiting from the optimized alignment, the 3D-printed SiC composite could show an EAB (∼6.4 GHz)1.6 times broader than that of the randomly mixed composite at the same thickness without alignment, associated with a minimum RL of -48 dB at 14.3 GHz. In addition, it is demonstrated that DIW could print different materials, such as SiCNW and multiwall carbon nanotube (MWCNT), in alternating layers for multiple-frequency-band attenuation benefiting from the distinct property of each material. Considering the one-step control of fiber alignment and material selectivity, DIW could play an important role in materials design for high-efficiency microwave attenuation.

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The mechanical behaviors of two multi-materials, DP590 (steel sheet)-A356 (cast aluminum alloy) and SS330 (steel sheet)-A5052 (aluminum sheet), were studied. A structural adhesive was used for the joining of steel and aluminum at adhesion strengths of 10, 22, and 30 MPa. To demonstrate that the three-point bending properties depend on the difference in strength between steel and aluminum and adhesion strength, optical microscopy (OM), scanning electron microscopy (SEM), and finite-element analysis (FEA) were performed. According to the results of the bending tests on both multi-materials under the same stacking conditions, the flexural stress increased with the improvement in the adhesion strength until interface separation or aluminum fracture. At the same adhesion strength, the DP590 (lower)-A356 (upper) and SS330 (upper)-A5052 (lower) configurations exhibited a tendency to decrease in the sudden stress drop due to aluminum fracture and interface separation. The bending results were analyzed through the FEA and the stress distribution as a function of the stacking and adhesion strength was confirmed.

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Currently, there are no straightforward methods to 3D print materials with nanoscale control over morphological and functional properties. Here, a novel approach for the fabrication of materials with controlled nanoscale morphologies using a rapid and commercially available Digital Light Processing 3D printing technique is demonstrated. This process exploits reversible deactivation radical polymerization to control the in-situ-polymerization-induced microphase separation of 3D printing resins, which provides materials with complex architectures controllable from the macro- to nanoscale, resulting in the preparation of materials with enhanced mechanical properties. This method does not require specialized equipment or process conditions and thus represents an important development in the production of advanced materials via additive manufacturing.

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Strong and well-engineered interfaces between dissimilar materials are a hallmark of natural systems but have proven difficult to emulate in synthetic materials, where interfaces often act as points of failure. In this work, curing reactions that are triggered by exposure to different wavelengths of visible light are used to produce multimaterial objects with tough, well-defined interfaces between chemically distinct domains. Longer-wavelength (green) light selectively initiates acrylate-based radical polymerization, while shorter-wavelength (blue) light results in the simultaneous formation of epoxy and acrylate networks through orthogonal cationic and radical processes. The improved mechanical strength of these interfaces is hypothesized to arise from a continuous acrylate network that bridges domains. Using printed test structures, interfaces were characterized through spatial resolution of their chemical composition, localized mechanical properties, and bulk fracture strength. This wavelength-selective photocuring of interpenetrating polymer networks is a promising strategy for increasing the mechanical performance of 3D-printed objects and expanding light-based additive manufacturing technologies.

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3D printing, formally known as additive manufacturing, creates complex geometries via layer-by-layer addition of materials. While 3D printing has been historically perceived as the static addition of build layers, 3D printing is now considered as a dynamic assembly process. In this context, here a new 3D printing process is reported that executes full degree-of-freedom (DOF) transformation (translating, rotating, and scaling) of each individual building layer while utilizing continuous fabrication techniques. Transforming individual building layers within the sequential layered manufacturing process enables dynamic transformation of the 3D printed parts on-the-fly, eliminating the time-consuming redesign steps. Preserving the locality of the transformation to each layer further enables the discrete conformal transformation, allowing objects such as vascular scaffolds to be optimally fabricated to properly fit within specific patient anatomy obtained from the magnetic resonance imaging (MRI) measurements. Finally, exploiting the freedom to control the orientation of each individual building layer, multimaterials, multiaxis 3D printing capability are further established for integrating functional modules made of dissimilar materials in 3D printed devices. This final capability is demonstrated through 3D printing a soft pneumatic gripper via heterogenous integration of rigid base and soft actuating limbs.

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3D printing technology has been extensively applied in the medical field, but the ability to replicate tissues that experience significant loads and undergo substantial deformation, such as the aorta, remains elusive. Therefore, this study proposed a method to imitate the mechanical characteristics of the aortic wall by 3D printing embedded patterns and combining two materials with different physical properties. First, we determined the mechanical properties of the selected base materials (Agilus and Dragonskin 30) and pattern materials (VeroCyan and TPU 95A) and performed tensile testing. Three patterns were designed and embedded in printed Agilus-VeroCyan and Dragonskin 30-TPU 95A specimens. Tensile tests were then performed on the printed specimens, and the stress-strain curves were evaluated. The samples with one of the two tested orthotropic patterns exceeded the tensile strength and strain properties of a human aorta. Specifically, a tensile strength of 2.15 ± 0.15 MPa and strain at breaking of 3.18 ± 0.05 mm/mm were measured in the study; the human aorta is considered to have tensile strength and strain at breaking of 2.0-3.0 MPa and 2.0-2.3 mm/mm, respectively. These findings indicate the potential for developing more representative aortic phantoms based on the approach in this study.

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Composite hydrogels have gained great attention as three-dimensional (3D) printing biomaterials because of their enhanced intrinsic mechanical strength and bioactivity compared to pure hydrogels. In most conventional printing methods for composite hydrogels, particles are preloaded in ink before printing, which often reduces the printability of composite ink with little mechanical improvement due to poor particle-hydrogel interaction of physical mixing. In contrast, the in situ incorporation of nanoparticles into a hydrogel during 3D printing achieves uniform distribution of particles with remarkable mechanical reinforcement, while precursors dissolved in inks do not influence the printing process. Herein, we introduced a "printing in liquid" technique coupled with a hybridization process, which allows 3D freeform printing of nanoparticle-reinforced composite hydrogels. A viscoplastic matrix for this printing system provides not only support for printed hydrogel filaments but also chemical reactants to induce various reactions in printed objects for in situ modification. Nanocomposite hydrogel scaffolds were successfully fabricated through this 3D freeform printing of hyaluronic acid (HAc)-alginate (Alg) hydrogel inks through a two-step crosslinking strategy. The first ionic crosslinking of Alg provided structural stability during printing, while the secondary crosslinking of photo-curable HAc improved the mechanical and physiological stability of the nanocomposite hydrogels. For in situ precipitation during 3D printing, phosphate ions were dissolved in the hydrogel ink and calcium ions were added to the viscoplastic matrix. The composite hydrogels demonstrated a significant improvement in mechanical strength, biostability, as well as biological performance compared to pure HAc. Moreover, the multi-material printing of composites with different calcium phosphate contents was achieved by adjusting the ionic concentration of inks. Our method greatly accelerates the 3D printing of various functional or hybridized materials with complex geometries through the design and modification of printing materials coupled with in situ post-printing functionalization and hybridization in reactive viscoplastic matrices.

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3D printing and bioprinting have become a key component in precision medicine. They have been used toward the fabrication of medical devices with patient-specific shapes, production of engineered tissues for in vivo regeneration, and preparation of in vitro tissue models used for screening therapeutics. In particular, vat polymerization-based 3D (bio)printing as a unique strategy enables more sophisticated architectures to be rapidly built. This progress report aims to emphasize the recent advances made in vat polymerization-based 3D printing and bioprinting, including new biomaterial ink formulations and novel vat polymerization system designs. While some of these approaches have not been utilized toward the combination with biomaterial inks, it is anticipated their rapid translation into biomedical applications.

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Distribution of multimaterials at arbitrary positions with nanoscale resolution and over a large area substrate is essential to future advances in functional graded materials. Such stringent requirements are highly beyond the reach of current techniques, although newly developed 3D printing technologies are addressed. Here, a radial gradient circle array film with the distribution accuracy up to ≈18 nm is fabricated by using microtopographic substrate. A mathematical model is developed to guide the distribution of position, size, shape, and type of materials on an arbitrary section for the given morphology of substrate. The periodic electrical and mechanical properties of the radial gradient circle film are identified, which can be beneficial for further functionalization and applications, such as gradient refractive index lenses, microcoils, and microantennas.

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At the core of additive manufacturing (3D printing) is the ability to rapidly print with multiple materials for arbitrary distribution with high resolution, which can remove challenges and limits of traditional assembly and enable us to make increasingly complex objects, especially exciting meta-materials. Here we demonstrate a simple and effective strategy to achieve nano-resolution printing of multiple materials for arbitrary distribution via layer-by-layer deposition on a special deposition surface. The established physical model reveals that complex distribution on a section can be achieved by vertical deformation of simple lamination of multiple materials. The deformation is controlled by a special surface of the mold and a contour-by-contour (instead of point-by-point) printing mode is revealed in the actual process. A large-scale concentric ring array with a minimum feature size below 50 nm is printed within less than two hours, verifying the capacity of high-throughput, high-resolution and rapidity of printing. The proposed printing method opens the way towards the programming of internal compositions of object (such as functional microdevices with multiple materials).

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Any object can be considered as a spatial distribution of atoms and molecules; in this sense, we can manufacture any object as long as the precise distribution of atoms and molecules is achieved. However, the current point-by-point methods to precisely manipulate single atoms and single molecules, such as the scanning tunneling microscope (STM), have difficulty in manipulating a large quantity of materials within an acceptable time. The macroscopic manipulation techniques, such as magnetron sputtering, molecular beam epitaxy, and evaporation, could not precisely control the distribution of materials. Herein, we take a step back and present a universal method of controlling the distribution of multimaterails during macroscopic manipulation via microtopography-guided substrates. For any given target distribution of multimaterials in a plane, the complicated lateral distribution of multimaterials was firstly transformed into a simple spatial lamellar body. Then, a deposition mathematical model was first established based on a mathematical transformation. Meanwhile, the microtopographic substrate can be fabricated according to target distribution based on the deposition mathematical model. Following this, the deposition was implemented on the substrate according to the designed sequence and thickness of each material, resulting in the formation of the deposition body on the substrate. Finally, the actual distribution was obtained on a certain section in the deposition body by removing the upside materials. The actual distribution can mimic the target one with a controllable accuracy. Furthermore, two experiments were performed to validate our method. As a result, we provide a feasible and scalable solution for controlling the distribution of multimaterials, and point out the direction of improving the position accuracy of each material. We may achieve real molecular manufacturing and nano-manufacturing if the position accuracy of distribution approaches the atomic level.

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A stereolithography-based bioprinting platform for multimaterial fabrication of heterogeneous hydrogel constructs is presented. Dynamic patterning by a digital micromirror device, synchronized by a moving stage and a microfluidic device containing four on/off pneumatic valves, is used to create 3D constructs. The novel microfluidic device is capable of fast switching between different (cell-loaded) hydrogel bioinks, to achieve layer-by-layer multimaterial bioprinting. Compared to conventional stereolithography-based bioprinters, the system provides the unique advantage of multimaterial fabrication capability at high spatial resolution. To demonstrate the multimaterial capacity of this system, a variety of hydrogel constructs are generated, including those based on poly(ethylene glycol) diacrylate (PEGDA) and gelatin methacryloyl (GelMA). The biocompatibility of this system is validated by introducing cell-laden GelMA into the microfluidic device and fabricating cellularized constructs. A pattern of a PEGDA frame and three different concentrations of GelMA, loaded with vascular endothelial growth factor, are further assessed for its neovascularization potential in a rat model. The proposed system provides a robust platform for bioprinting of high-fidelity multimaterial microstructures on demand for applications in tissue engineering, regenerative medicine, and biosensing, which are otherwise not readily achievable at high speed with conventional stereolithographic biofabrication platforms.

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