Information-providing magnetic supraparticles: particle designs to record environmental stimuli with readout by magnetic particle spectroscopy

This data publication is based on the metadata and datasets underlying the manuscript: Information-providing magnetic supraparticles: particle designs to record environmental stimuli with readout by magnetic particle spectroscopy Abstract: The ability to gather information about materials and products, such as their origin, physicochemical properties or history of experienced environmental stimuli, is valuable for quality control, predictive maintenance, delivery tracking, recycling, and more. Integrating additives capable of recording and storing information into materials offers a flexible approach to create "materials intelligence". Common strategies utilize luminescent markers or DNA sequences that enable object identification and environmental impact monitoring. In contrast to optical methods limited to surface-level analysis, magnetic fields penetrate materials, enabling non-destructive readout even from the inside of opaque or multi-component objects. While magnetic particle technologies have traditionally been used for biosensing and imaging with highly sensitive instruments like magnetic resonance imaging, these methods are unsuitable for quick, on-site analysis of macroscopic objects. During the last decade, magnetic particle spectroscopy (MPS) has emerged as a faster and more accessible characterization technique. MPS measures the magnetic response of particles in ambient conditions under alternating fields, offering high temporal resolution (~1–10 seconds) and more geometric freedom than other magnetometry techniques. Magnetic nanoparticles are a widely studied material class that have been synthesized and optimized, e.g., for various MPS-based application scenarios and to obtain fundamental understanding of magnetic particle systems. Supraparticles (SPs) represent the next structural hierarchy level as they are composed of one or multiple types of (magnetic) nanoparticles in a defined particulate structure. By ingenious control of structure and composition of such SPs, we have shown that various kinds of information can be obtained from them upon readout with MPS. In this article, we present SP design concepts facilitating to obtain information about environmental stimuli (e.g., temperature, moisture, UV light, chemical gasses) based on irreversible spectral magnetic signal changes upon readout with MPS. Initially, the state of the art on nanoparticles, which provide information by stimulus-induced agglomeration, is summarized. Subsequently, SPs consisting of multiple different nanoparticle types and their capabilities to obtain information on environmental stimuli are considered. Specifically, the advantages of using one or more signal transducing magnetic nanoparticle types used in conjunction with one or more non-magnetic secondary materials susceptible to the desired environmental stimuli (sensitizer) are discussed. Finally, our latest findings on pronounced large-scale SP structure formation (millimeter-scale) through strongly-interacting SPs and their implications on the integration of SPs in macroscopic objects of interest are described. Each of the three structural hierarchy levels, namely nanoparticles, SPs, and the macroscopic object of interest, represents an opportunity on the material level to finetune magnetic interactions. However, since the magnetic interactions across these three structural hierarchy levels are interdependent, meaning changes at the nanoparticle level influence the interactions of SPs at the macroscopic level, their control and interpretation in MPS remain challenging and prone to misinterpretation. The application of magnetic SPs as information-providing additives for predictive maintenance, material reuse, recycling, and industrial digitization requires a thorough understanding of all three hierarchical levels. Only then, suitable materials and processes can be developed, turning challenges into opportunities for transforming passive matter into perceptual, information-providing systems through the integration of magnetic SPs.本数据出版物依托如下手稿的元数据与配套数据集：《提供信息的磁性超粒子（magnetic supraparticles）：通过磁性粒子光谱法（magnetic particle spectroscopy, MPS）读取以记录环境刺激的粒子设计》 摘要： 获取材料与产品相关信息——如其来源、理化性质或所经历的环境刺激历史——的能力，在质量管控、预测性维护、物流追踪、回收利用等诸多场景中均具有重要价值。将具备记录与存储信息能力的添加剂集成至材料中，为构建“材料智能”提供了灵活可行的方案。主流策略多采用发光标记物或DNA序列，以实现物体识别与环境影响监测。 与仅能开展表面分析的光学方法不同，磁场可穿透材料，即便对于不透明或多组分物体的内部，也能实现非破坏性的信息读取。尽管传统上磁性粒子技术借助磁共振成像（magnetic resonance imaging, MRI）等高灵敏度仪器应用于生物传感与成像，但此类方法并不适用于宏观物体的快速现场分析。近十年来，磁性粒子光谱法（magnetic particle spectroscopy, MPS）逐渐发展为一种更快速、更易操作的表征技术。MPS可在环境条件下的交变磁场中测量粒子的磁响应，具备约1~10秒的高时间分辨率，且相较于其他磁力测量技术，具有更高的几何自由度。 磁性纳米颗粒是一类被广泛研究的材料，已针对各类基于MPS的应用场景完成合成与优化，也为深入理解磁性粒子系统提供了基础。超粒子（supraparticles, SPs）则是更高一级的结构层级，它们由一种或多种（磁性）纳米颗粒以特定的粒子结构组装而成。通过精妙调控此类SPs的结构与组成，我们已证实可借助MPS读取从中获取多种类型的信息。 本文中，我们提出了一系列SP设计理念，可基于MPS读取时产生的不可逆光谱磁信号变化，获取环境刺激（如温度、湿度、紫外线、化学气体）相关的信息。本文首先综述了通过刺激诱导团聚来提供信息的纳米颗粒的现有研究进展。随后，本文探讨了由多种不同纳米颗粒组成的SPs，以及它们获取环境刺激信息的能力。具体而言，本文讨论了将一种或多种信号转导型磁性纳米颗粒，与一种或多种可响应目标环境刺激的非磁性辅助材料（敏化剂）结合使用的优势。最后，本文阐述了我们关于强相互作用SPs形成显著宏观尺度（毫米级）SP结构的最新研究发现，以及该发现对于将SPs集成至目标宏观物体中的启示。 纳米颗粒、SPs与目标宏观物体这三个结构层级，均可在材料层面为调控磁相互作用提供优化空间。然而，由于这三个结构层级间的磁相互作用相互关联——纳米颗粒层面的变化会影响SPs在宏观层面的相互作用——因此在MPS中对其进行调控与解读仍具有挑战性，且容易出现解读偏差。将磁性SPs作为提供信息的添加剂应用于预测性维护、材料复用、回收利用以及工业数字化等场景，需要对这三个层级均具备透彻的理解。唯有如此，才能开发出适配的材料与工艺，将挑战转化为机遇——通过集成磁性SPs，将被动物质转变为具备感知能力、可提供信息的系统。