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AUTHOR Schaffner, Manuel and R{"u}hs, Patrick A. and Coulter, Fergal and Kilcher, Samuel and Studart, Andr{'e} R.
Title 3D printing of bacteria into functional complex materials [Abstract]
Year 2017
Journal/Proceedings Science Advances
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Despite recent advances to control the spatial composition and dynamic functionalities of bacteria embedded in materials, bacterial localization into complex three-dimensional (3D) geometries remains a major challenge. We demonstrate a 3D printing approach to create bacteria-derived functional materials by combining the natural diverse metabolism of bacteria with the shape design freedom of additive manufacturing. To achieve this, we embedded bacteria in a biocompatible and functionalized 3D printing ink and printed two types of {textquotedblleft}living materials{textquotedblright} capable of degrading pollutants and of producing medically relevant bacterial cellulose. With this versatile bacteria-printing platform, complex materials displaying spatially specific compositions, geometry, and properties not accessed by standard technologies can be assembled from bottom up for new biotechnological and biomedical applications.
AUTHOR Marin, Maria Minodora and Gifu, Ioana Catalina and Pircalabioru, Gratiela Gradisteanu and Albu Kaya, Madalina and Constantinescu, Rodica Roxana and Alexa, Rebeca Leu and Trica, Bogdan and Alexandrescu, Elvira and Nistor, Cristina Lavinia and Petcu, Cristian and Ianchis, Raluca
Title Microbial Polysaccharide-Based Formulation with Silica Nanoparticles; A New Hydrogel Nanocomposite for 3D Printing [Abstract]
Year 2023
Journal/Proceedings Gels
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Natural polysaccharides are highly attractive biopolymers recommended for medical applications due to their low cytotoxicity and hydrophilicity. Polysaccharides and their derivatives are also suitable for additive manufacturing, a process in which various customized geometries of 3D structures/scaffolds can be achieved. Polysaccharide-based hydrogel materials are widely used in 3D hydrogel printing of tissue substitutes. In this context, our goal was to obtain printable hydrogel nanocomposites by adding silica nanoparticles to a microbial polysaccharide’s polymer network. Several amounts of silica nanoparticles were added to the biopolymer, and their effects on the morpho-structural characteristics of the resulting nanocomposite hydrogel inks and subsequent 3D printed constructs were studied. FTIR, TGA, and microscopy analysis were used to investigate the resulting crosslinked structures. Assessment of the swelling characteristics and mechanical stability of the nanocomposite materials in a wet state was also conducted. The salecan-based hydrogels displayed excellent biocompatibility and could be employed for biomedical purposes, according to the results of the MTT, LDH, and Live/Dead tests. The innovative, crosslinked, nanocomposite materials are recommended for use in regenerative medicine.
AUTHOR Katcharava, Zviadi and Marinow, Anja and Bhandary, Rajesh and Binder, Wolfgang H.
Title 3D Printable Composite Polymer Electrolytes: Influence of SiO2 Nanoparticles on 3D-Printability [Abstract]
Year 2022
Journal/Proceedings Nanomaterials
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We here demonstrate the preparation of composite polymer electrolytes (CPEs) for Li-ion batteries, applicable for 3D printing process via fused deposition modeling. The prepared composites consist of modified poly(ethylene glycol) (PEG), lithium bis(trifluoromethylsulfonyl)imide (LiTFSI) and SiO2-based nanofillers. PEG was successfully end group modified yielding telechelic PEG containing either ureidopyrimidone (UPy) or barbiturate moieties, capable to form supramolecular networks via hydrogen bonds, thus introducing self-healing to the electrolyte system. Silica nanoparticles (NPs) were used as a filler for further adjustment of mechanical properties of the electrolyte to enable 3D-printability. The surface functionalization of the NPs with either ionic liquid (IL) or hydrophobic alkyl chains is expected to lead to an improved dispersion of the NPs within the polymer matrix. Composites with different content of NPs (5%, 10%, 15%) and LiTFSI salt (EO/Li+ = 5, 10, 20) were analyzed via rheology for a better understanding of 3D printability, and via Broadband Dielectric Spectroscopy (BDS) for checking their ionic conductivity. The composite electrolyte PEG 1500 UPy2/LiTFSI (EO:Li 5:1) mixed with 15% NP-IL was successfully 3D printed, revealing its suitability for application as printable composite electrolytes.
AUTHOR Jonhson, Win and Xu, Xi and Bian, Ka and Xun, Yanran and Tan, Yong Hao and Chen, Zhe and Zhang, Danwei and Ding, Jun
Title 3D-Printed Hierarchical Ceramic Architectures for Ultrafast Emulsion Treatment and Simultaneous Oil-Water Filtration [Abstract]
Year 2022
Journal/Proceedings ACS Materials Lett.
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There is a critical need for energy-efficient water treatment processes as the world seeks to limit global warming below 1.5 °C. Gravity-driven mesh filtration presents a sustainable solution to treating oily wastewater and emulsions, which are byproducts of many human activities. The promise of a green alternative is getting closer with the development of 3D printing combined with reusable, recyclable, and ubiquitous materials such as silica to produce durable and recyclable filters with controllable mesh spacing. In this work, several filters were fabricated to separate oily water mixtures with a separation efficiency of 99% at high flow flux by coating 3D porous ceramic architectures with organosilanes. The proposed ceramic filters can also treat oil-in-water and water-in-oil surfactant-stabilized emulsions with high flow flux. This strategy to functionalize the 3D printed silica surface to form either hydrophobic or hydrophilic surfaces can open a new possibility for gravity-driven simultaneous oil-water separation. The first gravity-driven hierarchical auto-oil-water separator (HAOS) was introduced to separate an oily water mixture into two different containers using a combination of 3D printed hierarchical hydrophilic and hydrophobic filters without an additional postseparation step.
AUTHOR Demirörs, Ahmet F. and Poloni, Erik and Chiesa, Maddalena and Bargardi, Fabio L. and Binelli, Marco R. and Woigk, Wilhelm and de Castro, Lucas D. C. and Kleger, Nicole and Coulter, Fergal B. and Sicher, Alba and Galinski, Henning and Scheffold, Frank and Studart, André R.
Title Three-dimensional printing of photonic colloidal glasses into objects with isotropic structural color [Abstract]
Year 2022
Journal/Proceedings Nature Communications
Reftype Demirörs2022
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Structural color is frequently exploited by living organisms for biological functions and has also been translated into synthetic materials as a more durable and less hazardous alternative to conventional pigments. Additive manufacturing approaches were recently exploited for the fabrication of exquisite photonic objects, but the angle-dependence observed limits a broader application of structural color in synthetic systems. Here, we propose a manufacturing platform for the 3D printing of complex-shaped objects that display isotropic structural color generated from photonic colloidal glasses. Structurally colored objects are printed from aqueous colloidal inks containing monodisperse silica particles, carbon black, and a gel-forming copolymer. Rheology and Small-Angle-X-Ray-Scattering measurements are performed to identify the processing conditions leading to printed objects with tunable structural colors. Multimaterial printing is eventually used to create complex-shaped objects with multiple structural colors using silica and carbon as abundant and sustainable building blocks.
AUTHOR Rößler, Sina and Brückner, Andreas and Kruppke, Iris and Wiesmann, Hans-Peter and Hanke, Thomas and Kruppke, Benjamin
Title 3D Plotting of Silica/Collagen Xerogel Granules in an Alginate Matrix for Tissue-Engineered Bone Implants [Abstract]
Year 2021
Journal/Proceedings Materials
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Today, materials designed for bone regeneration are requested to be degradable and resorbable, bioactive, porous, and osteoconductive, as well as to be an active player in the bone-remodeling process. Multiphasic silica/collagen Xerogels were shown, earlier, to meet these requirements. The aim of the present study was to use these excellent material properties of silica/collagen Xerogels and to process them by additive manufacturing, in this case 3D plotting, to generate implants matching patient specific shapes of fractures or lesions. The concept is to have Xerogel granules as active major components embedded, to a large proportion, in a matrix that binds the granules in the scaffold. By using viscoelastic alginate as matrix, pastes of Xerogel granules were processed via 3D plotting. Moreover, alginate concentration was shown to be the key to a high content of irregularly shaped Xerogel granules embedded in a minimum of matrix phase. Both the alginate matrix and Xerogel granules were also shown to influence viscoelastic behavior of the paste, as well as the dimensionally stability of the scaffolds. In conclusion, 3D plotting of Xerogel granules was successfully established by using viscoelastic properties of alginate as matrix phase.
AUTHOR Lee, Mihyun and Bae, Kraun and Levinson, Clara and Zenobi-Wong, Marcy
Title Nanocomposite bioink exploits dynamic covalent bonds between nanoparticles and polysaccharides for precision bioprinting [Abstract]
Year 2020
Journal/Proceedings Biofabrication
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The field of bioprinting has made significant recent progress towards engineering tissues with increasing complexity and functionality. It remains challenging, however, to develop bioinks with optimal biocompatibility and good printing fidelity. Here, we demonstrate enhanced printability of a polymer-based bioink based on dynamic covalent linkages between nanoparticles (NPs) and polymers, which retains good biocompatibility. Amine-presenting silica NPs (ca. 45 nm) were added to a polymeric ink containing oxidized alginate (OxA). The formation of reversible imine bonds between amines on the NPs and aldehydes of OxA lead to significantly improved rheological properties and high printing fidelity. In particular, the yield stress increased with increasing amounts of NPs (14.5 Pa without NPs, 79 Pa with 2 wt% NPs). In addition, the presence of dynamic covalent linkages in the gel provided improved mechanical stability over 7 d compared to ionically crosslinked gels. The nanocomposite ink retained high printability and mechanical strength, resulting in generation of centimeter-scale porous constructs and an ear structure with overhangs and high structural fidelity. Furthermore, the nanocomposite ink supported both in vitro and in vivo maturation of bioprinted gels containing chondrocytes. This approach based on simple oxidation can be applied to any polysaccharide, thus the widely applicability of the method is expected to advance the field towards the goal of precision bioprinting.
AUTHOR Alison, Lauriane and Menasce, Stefano and Bouville, Florian and Tervoort, Elena and Mattich, Iacopo and Ofner, Alessandro and Studart, André R.
Title 3D printing of sacrificial templates into hierarchical porous materials [Abstract]
Year 2019
Journal/Proceedings Scientific Reports
Reftype Alison2019
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Hierarchical porous materials are widespread in nature and find an increasing number of applications as catalytic supports, biological scaffolds and lightweight structures. Recent advances in additive manufacturing and 3D printing technologies have enabled the digital fabrication of porous materials in the form of lattices, cellular structures and foams across multiple length scales. However, current approaches do not allow for the fast manufacturing of bulk porous materials featuring pore sizes that span broadly from macroscopic dimensions down to the nanoscale. Here, ink formulations are designed and investigated to enable 3D printing of hierarchical materials displaying porosity at the nano-, micro- and macroscales. Pores are generated upon removal of nanodroplets and microscale templates present in the initial ink. Using particles to stabilize the droplet templates is key to obtain Pickering nanoemulsions that can be 3D printed through direct ink writing. The combination of such self-assembled templates with the spatial control offered by the printing process allows for the digital manufacturing of hierarchical materials exhibiting thus far inaccessible multiscale porosity and complex geometries.
AUTHOR Rupp, Harald and Döhler, Diana and Hilgeroth, Philipp and Mahmood, Nasir and Beiner, Mario and Binder, Wolfgang H.
Title 3D Printing of Supramolecular Polymers: Impact of Nanoparticles and Phase Separation on Printability [Abstract]
Year 2019
Journal/Proceedings Macromolecular Rapid Communications
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Abstract 3D printing of linear and three-arm star supramolecular polymers with attached hydrogen bonds and their nanocomposites is reported. The concept is based on hydrogen-bonded supramolecular polymers, known to form nano-sized micellar clusters. Printability is based on reversible thermal- and shear-induced dissociation of a supramolecular polymer network, which generates stable and self-supported structures after printing, as checked via melt-rheology and X-ray scattering. The linear and three-arm star poly(isobutylene)s PIB-B2 (Mn = 8500 g mol −1), PIB-B3 (Mn = 16 000 g mol −1), and linear poly(ethylene glycol)s PEG-B2 (Mn = 900 g mol−1, 8500 g mol −1) are prepared and then probed by melt-rheology to adjust the viscosity to address the proper printing window. The supramolecular PIB polymers show a rubber-like behavior and are able to form self-supported 3D printed objects at room temperature and below, reaching polymer strand diameters down to 200–300 µm. Nanocomposites of PIB-B2 with silica nanoparticles (12 nm, 5–15 wt%) are generated, in turn leading to an improvement of their shape persistence. A blend of the linear polymer PIB-B2 and the three-arm star polymer PIB-B3 (ratio ≈ 3/1 mol) reaches an even higher structural stability, able to build free-standing structures.
AUTHOR Couck, Sarah and Saint-Remi, Julien Cousin and der Perre, Stijn Van and Baron, Gino V. and Minas, Clara and Ruch, Patrick and Denayer, Joeri F. M.
Title 3D-printed SAPO-34 monoliths for gas separation [Abstract]
Year 2018
Journal/Proceedings Microporous and Mesoporous Materials
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Abstract A 3D printing method (the Direct Ink writing, DIW, method) is applied to produce SAPO-34 zeolite based structured adsorbents with the shape of a honeycomb-like monolith. The use of the 3D printing technique gives this structure a well-defined and easily adaptable geometry. As binder material, methyl cellulose was used. The SAPO-34 monolith was characterized by SEM as well as Ar and Hg porosimetry. The CO2 adsorption affinity, capacity and heat of adsorption were determined by recording high pressure adsorption isotherms at different temperatures, using the gravimetric technique. The separation potential was investigated by means of breakthrough experiments with mixtures of CO2 and N2. The experimental selectivity of CO2/N2 separation was compared to the selectivity as predicted by the Ideal Adsorbed Solution Theory. A drop in capacity was noticed during the experiments and N2 capacities were close to zero or slightly negative due to the very low adsorption, meaning absolute selectivity values could not be determined. However, due to the low N2 capacity, experimental selectivity is estimated to be excellent as was predicted with IAST. While the 3D printing is found to be a practical, fast and flexible route to generate monolithic adsorbent structures, improvements in formulation are required in terms of sample robustness for handling purposes and heat transfer characteristics of the obtained monoliths during gas separation.
AUTHOR Lee, Mihyun and Bae, Kraun and Guillon, Pierre and Chang, Jin and Arlov, Øystein and Zenobi-Wong, Marcy
Title Exploitation of Cationic Silica Nanoparticles for Bioprinting of Large-Scale Constructs with High Printing Fidelity [Abstract]
Year 2018
Journal/Proceedings ACS Applied Materials and Interfaces
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Three-dimensional (3D) bioprinting allows the fabrication of 3D structures containing living cells whose 3D shape and architecture are matched to a patient. The feature is desirable to achieve personalized treatment of trauma or diseases. However, realization of this promising technique in the clinic is greatly hindered by inferior mechanical properties of most biocompatible bioink materials. Here, we report a novel strategy to achieve printing large constructs with high printing quality and fidelity using an extrusion-based printer. We incorporate cationic nanoparticles in an anionic polymer mixture, which significantly improves mechanical properties, printability, and printing fidelity of the polymeric bioink due to electrostatic interactions between the nanoparticles and polymers. Addition of cationic-modified silica nanoparticles to an anionic polymer mixture composed of alginate and gellan gum results in significantly increased zero-shear viscosity (1062%) as well as storage modulus (486%). As a result, it is possible to print a large (centimeter-scale) porous structure with high printing quality, whereas the use of the polymeric ink without the nanoparticles leads to collapse of the printed structure during printing. We demonstrate such a mechanical enhancement is achieved by adding nanoparticles within a certain size range (90%) and extracellular matrix secretion are observed for cells printed with nanocomposite inks. The design principle demonstrated can be applied for various anionic polymer-based systems, which could lead to achievement of 3D bioprinting-based personalized treatment.
AUTHOR Sommer, Marianne R. and Alison, Lauriane and Minas, Clara and Tervoort, Elena and Ruhs, Patrick A. and Studart, Andre R.
Title 3D printing of concentrated emulsions into multiphase biocompatible soft materials [Abstract]
Year 2017
Journal/Proceedings Soft Matter
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3D printing via direct ink writing (DIW) is a versatile additive manufacturing approach applicable to a variety of materials ranging from ceramics over composites to hydrogels. Due to the mild processing conditions compared to other additive manufacturing methods{,} DIW enables the incorporation of sensitive compounds such as proteins or drugs into the printed structure. Although emulsified oil-in-water systems are commonly used vehicles for such compounds in biomedical{,} pharmaceutical{,} and cosmetic applications{,} printing of such emulsions into architectured soft materials has not been fully exploited and would open new possibilities for the controlled delivery of sensitive compounds. Here{,} we 3D print concentrated emulsions into soft materials{,} whose multiphase architecture allows for site-specific incorporation of both hydrophobic and hydrophilic compounds into the same structure. As a model ink{,} concentrated emulsions stabilized by chitosan-modified silica nanoparticles are studied{,} because they are sufficiently stable against coalescence during the centrifugation step needed to create a bridging network of droplets. The resulting ink is ideal for 3D printing as it displays high yield stress{,} storage modulus and elastic recovery{,} through the formation of networks of droplets as well as of gelled silica nanoparticles in the presence of chitosan. To demonstrate possible architectures{,} we print biocompatible soft materials with tunable hierarchical porosity containing an encapsulated hydrophobic compound positioned in specific locations of the structure. The proposed emulsion-based ink system offers great flexibility in terms of 3D shaping and local compositional control{,} and can potentially help address current challenges involving the delivery of incompatible compounds in biomedical applications.
AUTHOR Baumann, Bernhard and Jungst, Tomasz and Stichler, Simone and Feineis, Susanne and Wiltschka, Oliver and Kuhlmann, Matthias and Lindén, Mika and Groll, Jürgen
Title Control of Nanoparticle Release Kinetics from 3D Printed Hydrogel Scaffolds [Abstract]
Year 2017
Journal/Proceedings Angewandte Chemie International Edition
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The convergence of biofabrication with nanotechnology is largely unexplored but enables geometrical control of cell-biomaterial arrangement combined with controlled drug delivery and release. As a step towards integration of these two fields of research, this study demonstrates that modulation of electrostatic nanoparticle–polymer and nanoparticle–nanoparticle interactions can be used for tuning nanoparticle release kinetics from 3D printed hydrogel scaffolds. This generic strategy can be used for spatiotemporal control of the release kinetics of nanoparticulate drug vectors in biofabricated constructs.
AUTHOR Kokkinis, Dimitri and Schaffner, Manuel and Studart, Andr{'{e}} R.
Title Multimaterial magnetically assisted 3D printing of composite materials
Year 2015
Journal/Proceedings Nature Communications
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