Tobias M. Nargang

Three-dimensional printing of transparent fused silica glass

Glass is one of the most important high-performance materials used for scientific research, in industry and in society, mainly owing to its unmatched optical transparency, outstanding mechanical, chemical and thermal resistance as well as its thermal and electrical insulating properties. However, glasses and especially high-purity glasses such as fused silica glass are notoriously difficult to shape, requiring high-temperature melting and casting processes for macroscopic objects or hazardous chemicals for microscopic features. These drawbacks have made glasses inaccessible to modern manufacturing technologies such as three-dimensional printing (3D printing). Using a casting nanocomposite, here we create transparent fused silica glass components using stereolithography 3D printers at resolutions of a few tens of micrometres. The process uses a photocurable silica nanocomposite that is 3D printed and converted to high-quality fused silica glass via heat treatment. The printed fused silica glass is non-porous, with the optical transparency of commercial fused silica glass, and has a smooth surface with a roughness of a few nanometres. By doping with metal salts, coloured glasses can be created. This work widens the choice of materials for 3D printing, enabling the creation of arbitrary macro- and microstructures in fused silica glass for many applications in both industry and academia.

Liquid Glass: A Facile Soft Replication Method for Structuring Glass

Liquid glass is a photocurable amorphous silica nanocomposite that can be structured using soft replication molds and turned into glass via thermal debinding and sintering. Simple polymer bonding techniques allow the fabrication of complex microsystems in glass like microfluidic chips. Liquid glass is a step toward prototyping of glass microstructures at low cost without requiring cleanroom facilities or hazardous chemicals.

Rational design of a peptide capture agent for CXCL8 based on a model of the CXCL8:CXCR1 complex

Protein-capture agents are widely used for the detection, immobilization and isolation of proteins and are the foundation for the development of in vitro diagnostic chips. The chemokine CXCL8 is an interesting protein target due to its involvement in the human inflammatory response. We constructed a novel structural model of CXCL8 interaction with its G-protein coupled receptor CXCR1, taking into account previously reported experimental data. From this CXCL8:CXCR1 model complex, the interaction of CXCL8 with residues near the extracellular domains 3 and 4 of CXCR1 were used as a scaffold for the rational design of a peptide capture agent called ‘IL8RPLoops’. A molecular dynamics simulation of IL8RPLoops indicates a stable helical conformation consistent with the CXCR1 structure from which it was derived. CXCL8 capture in fluorescence-based assays on beads and on glass demonstrates that IL8RPLoops is an effective capture agent for CXCL8. Additionally, we found IL8RPLoops to be a potent inhibitor of CXCL8-induced neutrophil migration and CXCL8:CXCR1 association. A theoretical binding model for IL8RPLoops:CXCL8 is proposed, which shows the peptide predominantly interacting with CXCL8 via electrostatic contacts with the ELR motif at the CXCL8 N-terminus.

Functionalization of paper using photobleaching: A fast and convenient method for creating paper‐based assays with colorimetric and fluorescent readout

Lateral flow immunoassays (LFIA), where a protein–protein interaction can be monitored on a test strip by a color reaction, are of high interest in the field of point‐of‐care diagnostics due to their cost‐efficient production, portability, and ease of use. Despite their simple appearance, state‐of‐the‐art manufacturing of such test strips is not trivial since the strips comprise of several reaction zones: cellulose serves as hydrophilic support with excellent flow properties; and nitrocellulose is the membrane of choice for zones with immobilized biomolecules due to its hydrophobicity and thus preferable adhesion properties. These individual reaction zone membranes need to be joined together after fabrication. Variations in general membrane properties and production‐related lot‐to‐lot variations make it difficult to produce reliable tests with high reproducibility. In this paper, we present a facile and rapid method to immobilize antibodies directly onto cellulose by using maskless projection lithography. With this method it is possible to manufacture LFIA strips with individual reaction zones in a single material, i.e. cellulose.

Transparent, abrasion-insensitive superhydrophobic coatings for real-world applications

Superhydrophobic surfaces and surface coatings are of high interest for many applications in everyday life including non-wetting and low-friction coatings as well as functional clothing. Manufacturing of these surfaces is intricate since superhydrophobicity requires structuring of surfaces on a nano- to microscale. This delicate surface structuring makes most superhydrophobic surfaces very sensitive to abrasion and renders them impractical for real-life applications. In this paper we present a transparent fluorinated polymer foam that is synthesized by a simple one-step photoinitiated radical polymerization. We term this material “Fluoropor”. It possesses an inherent nano-/microstructure throughout the whole bulk material and is thus insensitive to abrasion as its superhydrophobic properties are not merely due to a thin-layer surface-effect. Due to its foam-like structure with pore sizes below the wavelength of visible light Fluoropor appears optically transparent. We determined contact angles, surface energy, wear resistance and Vickers hardness to highlight Fluoropor’s applicability for real-word applications.

Suspended Liquid Subtractive Lithography: One-step generation of 3D channel geometries in viscous curable polymer matrices

The miniaturization of synthesis, analysis and screening experiments is an important step towards more environmentally friendly chemistry, statistically significant biology and fast and cost-effective medicinal assays. The facile generation of arbitrary 3D channel structures in polymers is pivotal to these techniques. Here we present a method for printing microchannels directly into viscous curable polymer matrices by injecting a surfactant into the uncured material via a steel capillary attached to a 3D printer. We demonstrate this technique using polydimethylsiloxane (PDMS) one of the most widely used polymers for the fabrication of, e. g. microfluidic chips. We show that this technique which we term Suspended Liquid Subtractive Lithography (SLSL) is well suited for printing actuators, T-junctions and complex three dimensional structures. The formation of truly arbitrary channels in 3D could revolutionize the fabrication of miniaturized chips and will find broad application in biology, chemistry and medicine.

Suspended liquid subtractive lithography: printing three dimensional channels directly into uncured PDMS

Polydimethylsiloxane (PDMS) is one of the most widely used polymers for the generation of microfluidic chips. The standard procedures of soft lithography require the formation of a new master structure for every design which is timeconsuming and expensive. All channel generated by soft lithography need to be consecutively sealed by bonding which is a process that can proof to be hard to control. Channel cross-sections are largely restricted to squares or flat-topped designs and the generation of truly three-dimensional designs is not straightforward. Here we present Suspended Liquid Subtractive Lithography (SLSL) a method for generating microfluidic channels of nearly arbitrary three-dimensional structures in PDMS that do not require master formation or bonding and give circular channel cross sections which are especially interesting for mimicking in vivo environments. In SLSL, an immiscible liquid is introduced into the uncured PDMS by a capillary mounted on a 3D printer head. The liquid forms continuous “threads” inside the matrix thus creating void suspended channel structures.

Correction: Rational design of a peptide capture agent for CXCL8 based on a model of the CXCL8:CXCR1 complex

Correction for ‘Rational design of a peptide capture agent for CXCL8 based on a model of the CXCL8:CXCR1 complex’ by Dorothea Helmer et al., RSC Adv., 2015, 5, 25657–25668.

Structuring unbreakable hydrophobic barriers in paper

Hydrophobic barriers are one of the key elements of microfluidic paper based analytical devices (μPADs).μPADs are simple and cost efficient and they can be carried out without the need of high standard laboratories. To carry out such a test a method is needed to create stable hydrophobic barriers. Commonly used methods like printing wax or polystyrene have the major drawback that these barriers are stiff and break if bended which means they will no longer be able to retain a liquid sample. Here we present silanes to structure hydrophobic barriers via polycondensation and show a silanization method which combines the advantages of flexible silane/siloxane layers with the short processing times of UV-light based structuring. The barriers are created by using methoxy silanes which are mixed with a photo acid generator (PAG) as photoinitiator. Also a photosensitizer was given to the mixture to increase the effectiveness of the PAG. After the PAG is activated by UV-light the silane is hydrolyzed and coupled to the cellulose via polycondensation. The created hydrophobic barriers are highly stable and do not break if being bended.

Photolithographic structuring of soft, extremely foldable and autoclavable hydrophobic barriers in paper

Microfluidic paper-based analytical devices (μPADs) offer the possibility to carry out laboratory test on a piece of paper. This enables on-site monitoring in regions with scarce laboratory infrastructure but also promises cost savings for health care systems in highly-developed regions. One key element of all μPADs are hydrophobic barriers which control the liquid flow during the analysis. There are different approaches to generating hydrophobic barriers such as, e.g., wax or polymer printing as well as lithographic techniques. However, all of these introduce stiff barriers into the otherwise soft and foldable paper which significantly limits its handling. In almost all cases, once the paper is folded strongly the barriers break and are no longer able to retain a liquid sample. In this paper, we present a method for structuring hydrophobic barriers by a light-based approach making use of a light-controlled locally confined silanization. This method combines the advantages of photolithography and 3D printing in terms of process speed and flexibility with a chemical modification technique which locally modifies the wetting behaviour of the paper instead of applying a physical bulk barrier. This allows generating hydrophobic barriers which retain the flexibility of the paper and can be freely folded without losing their liquid-retaining properties even after as many as 50 fold cycles. The structures produced in this way are highly chemically stable and can even be autoclaved. We demonstrate the suitability of this method in bioanalytics using an enzymatic assay demonstrating that the silanization chemistry does not impair the biocompatibility of the substrate.