Establishing and testing a robot-based platform to enable the automated production of nanoparticles in a flexible and modular way.

Robotic systems facilitate relatively simple human-robot interaction for non-robot experts, providing the flexibility to implement different processes. In this context, shorter process times, as well as an increased product and process quality could be achieved. Robots short time-consuming processes, take over ergonomically unfavorable tasks and work efficiently all the time. In addition, flexible production is possible while maintaining or even increasing safety. This study describes the successful development of a dual-arm robot-based modular infrastructure and the establishment of an automated process for the reproducible production of nanoparticles. As proof of concept, a manual synthesis protocol for silica nanoparticle preparation with a diameter of about 200 nm as building blocks for photonic crystals was translated into a fully automated process. All devices and components of the automated system were optimized and adapted according to the synthesis requirements. To demonstrate the benefit of the automated nanoparticle production, manual (synthesis done by lab technicians) and automated syntheses were benchmarked. To this end, different processing parameters (time of synthesis procedure, accuracy of dosage etc.) and the properties of the produced nanoparticles were compared. We demonstrate that the use of the robot not only increased the synthesis accuracy and reproducibility but reduced the personnel time and costs up to 75%.

Spray-Dried Photonic Balls with a Disordered/Ordered Hybrid Structure for Shear-Stress Indication.

Optical microscale shear-stress indicator particles are of interest for the in situ recording of localized forces, e.g., during 3D printing or smart skins in robotic applications. Recently developed particle systems are based on optical responses enabled by integrated organic dyes. They thus suffer from potential chemical instability and cross-sensitivities toward humidity or temperature. These drawbacks can be circumvented using photonic balls as shear-stress indicator particles, which employ structural color as the element to record forces. Here, such photonic balls are prepared from silica and iron oxide nanoparticles via the scalable and fast spray-drying technique. Process parameters to create photonic balls with a disordered core and an ordered particle structure toward the exterior of the supraparticles are reported. This hybrid disordered-ordered structure is responsible for a color loss of the indicator particles during shear-stress application because of irreversible structural destruction. By adjusting the primary silica particle sizes, nearly all colors of the visible spectrum can be achieved and the sensitivity of the response to shear stress can be adjusted.

Optically Sensitive and Magnetically Identifiable Supraparticles as Indicators of Surface Abrasion.

Identifying and ensuring the integrity of products plays an important role in today's globalized world. Miniaturized information taggants in the packaging surface are therefore required to monitor the product itself instead of applying external labels. Ideally, multiple types of information are stored in such additives. In this work, micrometer-sized core-shell particles (supraparticles) were developed to provide material surfaces with both an identifier and a surface abrasion indication functionality. The core of the supraparticles contains iron oxide nanoparticles that allow identification of the surface with a spectral magnetic code resolved by magnetic particle spectroscopy. The fluorescent silica nanoparticles in the supraparticle shell can be abraded by mechanical stress and resolved by fluorescence spectroscopy. This provides information about the mechanical integrity of the system. The application as surfaces, that contain several types of information in one supraparticle, was demonstrated here by incorporating such bifunctional supraparticles as additives in a surface coating.

Supraparticles with a Mechanically Triggerable Color-Change-Effect to Equip Coatings with the Ability to Report Damage.

Small scratches and abrasion cause damage to packaging coatings. Albeit often invisible to the human eye, such small defects in the coating may ultimately have a strong negative impact on the whole system. For instance, gases may penetrate the coating and consequently the package barrier, thus leading to the degradation of sensitive goods. Herein, the indicators of mechanical damage in the form of particles are reported, which can readily be integrated into coatings. Shear stress-induced damage is indicated by the particles via a color change. The particles are designed as core-shell supraparticles. The supraparticle core is based on rhodamine B dye-doped silica nanoparticles, whereas the shell is made of alumina nanoparticles. The alumina surface is functionalized with a monolayer of a perylene dye. The resulting core-shell supraparticle system thus contains two colors, one in the core and one in the shell part of the architecture. Mechanical damage of this structure exposes the core from the shell, resulting in a color change. With particles integrated into a coating lacquer, mechanical damage of a coating can be monitored via a color change and even be related to the degree of oxygen penetration in a damaged coating.

A Simple Model Setup Using Spray-Drying Principles and Fluorescent Silica Nanoparticles to Evaluate the Efficiency of Facemask Materials in Terms of Virus Particle Retention.

Herein, a simple model setup is presented to spray fine liquid droplets containing nanoparticles in an air stream transporting this toward a filter material. The nanoparticles are made of silica and tagged with a fluorescent dye in order to render the trace of the particles easily visible. The silica nanoparticles, in a first approximation, mimic virus (severe acute respiratory syndrome coronavirus 2) particles. The setup is used to evaluate different tissues, nowadays, in times of the coronavirus pandemic, commonly used as facemasks, with regard to their particle retention capability. The setup enables adjusting different "breathing scenarios" by adjusting the gas flow speed and, thereby, to compare the filter performance for these scenarios. The effective penetration of particles can be monitored via fluorescence intensity measurements and is visualized via scanning electron micrographs and photographs under UV light. Ultimately, a strong increase of particle penetration in various mask materials as function of flow speed of the droplets is observed and an ultimate retention is only observed for FFP3 and FFP2 masks.

Kinetic and spectroscopic responses of pH-sensitive nanoparticles: influence of the silica matrix.

Intracellular pH sensing with fluorescent nanoparticles is an emerging topic as pH plays several roles in physiology and pathologic processes. Here, nanoparticle-sized pH sensors (diameter far below 50 nm) for fluorescence imaging have been described. Consequently, a fluorescent derivative of pH-sensitive hydroxypyrene with pK a = 6.1 was synthesized and subsequently embedded in core and core-shell silica nanoparticles via a modified Stöber process. The detailed fluorescence spectroscopic characterization of the produced nanoparticles was carried out for retrieving information about the environment within the nanoparticle core. Several steady-state and time-resolved fluorescence spectroscopic methods hint to the screening of the probe molecule from the solvent, but it sustained interactions with hydrogen bonds similar to that of water. The incorporation of the indicator dye in the water-rich silica matrix neither changes the acidity constant nor dramatically slows down the protonation kinetics. However, cladding by another SiO2 shell leads to the partial substitution of water and decelerating the response of the probe molecule toward pH. The sensor is capable of monitoring pH changes in a physiological range by using ratiometric fluorescence excitation with λ ex = 405 nm and λ ex = 488 nm, as confirmed by the confocal fluorescence imaging of intracellular nanoparticle uptake.