Under the right process conditions, nanoparticles can cluster together to form defined, dispersed structures, which can be termed supraparticles. Controlling the size, shape, and morphology of such entities is a central step in various fields of science and technology, ranging from colloid chemistry and soft matter physics to powder technology and pharmaceutical and food sciences. These diverse scientific communities have been investigating formation processes and structure/property relations of such supraparticles under completely different boundary conditions. On the fundamental side, the field is driven by the desire to gain maximum control of the assembly structures using very defined and tailored colloidal building blocks, whereas more applied disciplines focus on optimizing the functional properties from rather ill-defined starting materials. With this review article, we aim to provide a connecting perspective by outlining fundamental principles that govern the formation and functionality of supraparticles. We discuss the formation of supraparticles as a result of colloidal properties interplaying with external process parameters. We then outline how the structure of the supraparticles gives rise to diverse functional properties. They can be a result of the structure itself (emergent properties), of the colocalization of different, functional building blocks, or of coupling between individual particles in close proximity. Taken together, we aim to establish structure-property and process-structure relationships that provide unifying guidelines for the rational design of functional supraparticles with optimized properties. Finally, we aspire to connect the different disciplines by providing a categorized overview of the existing, diverging nomenclature of seemingly similar supraparticle structures.
In the course of globalization, tracking of material supply chains and product protection against counterfeiting is a topic of increasing relevance. The labeling of raw materials or product components with encoded microstructures may therefore ensure their reliable and tamper-proof identification. In this work, luminescent lanthanide doped calcium fluoride nanoparticles with characteristic optical properties are assembled to micrometer-sized supraparticles via spray-drying. By wise selection of these nanoscale building blocks, it is possible to create spectrally encoded microparticles. Their code relies on the relative emission intensities of the different luminescent nanoparticles and their concentration ratios within the supraparticle. Due to this strategy, we offer a nanoscale modular approach for an easily adjustable and simple creation of ratiometric luminescence-encoded microparticles for the tamper-proof marking of objects.
Marking and identification of materials is becoming increasingly important due to complex global resource and supply chains. Luminescent particle‐based markers have come to the forefront due to their small dimensions and their ability to be integrated in diverse materials. However, light‐absorbing materials can hardly be marked by these particles, thus leading to insufficient recycling rates of, e.g., black plastics. In this work, microparticles with a unique magnetic fingerprint are tailored by modification of their nanoparticle building blocks. This fingerprint tailoring is achieved either by combination of magnetic building blocks with nonmagnetic ones in the supraparticles or, alternatively, by surface modification of the building blocks. An easy‐to‐use device, based on the principle of magnetic particle spectroscopy (MPS), is established to resolve the magnetic fingerprint information. This facilitates the employment of magnetic supraparticles as markers for product tracking and identification. As a proof of concept, it is shown that such particles enable the marking of black plastic.
“Communicating particles” are reported that combine an identification (ID) taggant and a temperature recorder in one single entity—a micron‐scaled supraparticle. The optical information carriers within the hybrid inorganic‐organic supraparticles are three different types of luminescent nanoparticles, which can be read‐out using single‐wavelength excitation. These three nanoparticle types are assembled into a core‐satellite structure via a two‐step droplet evaporation technique. The core is built‐up from Tb3+ and Eu3+‐doped nanophosphors, providing an environmentally stable ID that is easily tunable through ratiometric spectral coding. This core is surrounded by organic, dye‐doped polymer nanoparticle satellites, acting as thermal‐history‐recorders of their environment. Exposed to a threshold temperature, the luminescence of the utilized 7‐diethylamino‐4‐methylcoumarin‐doped polymer nanoparticles is irreversibly quenched. This “turn‐off ” signal response is attributed to conformational changes in the dyes’ excited state and an alteration of their molecular environment, respectively, triggered by the polymer nanoparticles’ glass transition. Thus, the sensitivity of the temperature recorder can be configured over a wide temperature range by varying the dye‐hosting polymer. At the same time, the ID of the particle, stemming from its inorganic building blocks, stays unaffected, thus stable against thermal changes. The idea of communicating particles introduces a promising concept for smart additives.
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