Diabetes mellitus accompanies an abnormally high glucose level in the bloodstream. Early diagnosis and proper glycemic management of blood glucose are essential to prevent further progression and complications. Biosensor-based colorimetric detection has progressed and shown potential in portable and inexpensive daily assessment of glucose levels because of its simplicity, low-cost, and convenient operation without sophisticated instrumentation. Colorimetric glucose biosensors commonly use natural enzymes that recognize glucose and chromophores that detect enzymatic reaction products. However, many natural enzymes have inherent defects, limiting their extensive application. Recently, nanozyme-based colorimetric detection has drawn attention due to its merits including high sensitivity, stability under strict reaction conditions, flexible structural design with low-cost materials, and adjustable catalytic activities. This review discusses various nanozyme materials, colorimetric analytic methods and mechanisms, recent machine learning based analytic methods, quantification systems, applications and future directions for monitoring and managing diabetes.

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Nanozyme-based colorimetric biosensor with a systemic quantification algorithm for noninvasive glucose monitoring

Counterfeit medicines are a healthcare security problem, posing not only a direct threat to patient safety and public health but also causing heavy economic losses. Current anticounterfeiting methods are limited due to the toxicity of the constituent materials and the focus of secondary packaging level protections. We introduce an edible, imperceptible, and scalable matrix code of information representation and data storage for pharmaceutical products. This matrix code is digestible as it is composed of silk fibroin genetically encoded with fluorescent proteins produced by ecofriendly, sustainable silkworm farming. Three distinct fluorescence emission colors are incorporated into a multidimensional parameter space with a variable encoding capacity in a format of matrix arrays. This code is smartphone-readable to extract a digitized security key augmented by a deep neural network for overcoming fabrication imperfections and a cryptographic hash function for enhanced security. The biocompatibility, photostability, thermal stability, long-term reliability, and low bit error ratio of the code support the immediate feasibility for dosage-level anticounterfeit measures and authentication features. The edible code affixed to each medicine can serve as serialization, track and trace, and authentication at the dosage level, empowering every patient to play a role in combating illicit pharmaceuticals.

Edible Matrix Code with Photogenic Silk Proteins

Smart luminescent materials with tangible and reversible responses to external stimuli have gained popularity for multiple applications. However, impracticable stimuli and less adaptability render them unfit for real‐life applications. Here, a proton competitive binding‐based molecular system is reported, which demonstrates, both in solution and solid state, remarkable responses toward light illumination and temperature variation. Small change in solvent composition could result in remarkable variation in measurable temperature range at least from −80 to 60 °C. Combination of light illumination and temperature change enables multilevel anti‐counterfeiting, as well as construction of easy‐to‐use and high‐resolution liquid thermometers. The key components in the concerned molecular system are a newly designed fluorophore, NI‐CBN, a four‐coordinated boron derivative of naphthalimide (NI), and an organic fluoride salt that is tetrabutylammonium fluoride (TBAF). Reaction between NI‐CBN and TBAF yields a dynamic fluorophore, NI‐CBN‐F, which shows remarkable color change to the stimuli via proton migration between the imine group in NI‐CBN and the fluoride anion of the salt. Such responses enable the aforementioned advanced anti‐counterfeiting and visible temperature monitoring.

A Mild‐Stimuli‐Responsive Fluorescent Molecular System Enables Multilevel Anti‐Counterfeiting and Highly Adaptable Temperature Monitoring

Luminescence materials have gained extensive attention in anti‐counterfeiting owing to their unique superiorities. Visible‐near infrared (vis‐NIR) dual emission that combines naked‐eye visible light and concealed NIR light would provide a promising strategy for improving the covertness and secure anti‐counterfeiting effect. Here, two organic conjugated materials 4,4′‐(thieno[3,4‐c][1,2,5]thiadiazole‐4,6 diyl)bis(N,N‐bis(4‐(aldehyde)phenyl)aniline) (TTD‐TPA‐CHO) and 4,4′‐(thieno[3,4‐c][1,2,5]thiadiazole‐4,6 diyl)bis(N,N‐bis(phenyl)aniline) (TTD‐TPA) based on thieno[3,4‐c][1,2,5]thiadiazole (TT) have been developed, exhibiting vis‐NIR dual emissions by manipulating the charge transfer states. With the aid of self‐healing technique, stretchable and highly transparent TTD‐TPA‐CHO and TTD‐TPA containing self‐healing PDMS films are efficiently prepared to fabricate dual‐mode anti‐counterfeiting patterns for demonstrating the anti‐counterfeiting applications. Under UV light, the luminescent patterns in visible region can be read out by the naked eye, while the concealed information could be accessed by NIR detection devices. These results evidently suggest the important role of vis‐NIR dual emission in enhancing the stealth of encrypted information and the security level of anti‐counterfeiting. Hopefully, this work would promote the further development of vis‐NIR dual‐emission organic conjugated materials in anti‐counterfeiting techniques.

Thieno[3,4‐c][1,2,5]Thiadiazole‐Based Organic Conjugated Molecules with Visible and Near‐Infrared Dual Emissions for Luminescent Anti‐Counterfeiting Applications

Exploring high‐safety but convenient encryption and decryption technologies to combat threats of information leakage is urgently needed but remains a great challenge. Here, a synergistically time‐ and temperature‐resolved information coding/decoding solution based on functional photonic inks is demonstrated. Encrypted messages can be stored into multiple channels with dynamic‐color patterns, and information decryption is only enabled at appointed temperature and time points. Notably, the ink can be easily processed into quick‐response codes and multipixel plates. With high transparency and responsive color variations controlled by ink compositions and ambient temperatures, advanced 3D stacking multichannel coding and Morse coding techniques can be applied for multi‐information storage, complex anticounterfeiting, and information interference. This study paves an avenue for the design and development of dynamic photonic inks and complex encryption technologies for high‐end anticounterfeiting applications.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202206290

Sophisticated yet Convenient Information Encryption/Decryption Based on Synergistically Time‐/Temperature‐Resolved Photonic Inks

Counterfeit medicines are a fundamental healthcare problem, threatening patient safety and public health as well as causing economic damage. Online pharmacies and the ongoing pandemic have promoted medicine counterfeiting. However, the existing anticounterfeit methods are limited because of material toxicity, low security, and complicated fabrication. Here a dosage‐level security method is introduced that combines digital watermarking and physical printing at the material level. A set of requirements is designed to ensure the edibility, printability, imperceptibility, and robustness of cyber‐physical watermarking. An inkjet printer using safe food coloring is adapted to print a watermarked image on a recombinant luminescent silk protein taggant to enhance attack resistance. Machine learning of color accuracy recovers unavoidable color distortions during printing and acquisition, allowing robust smartphone readability. An edible watermarked taggant affixed to each individual medicine can offer anticounterfeit and authentication features at the dosage level, empowering every patient to aid in abating illicit medicines.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/adfm.202112479

Cyber‐Physical Watermarking with Inkjet Edible Bioprinting

Biocompatible fluorescent silk fibroin bioink for digital light processing 3D printing.

Bombyx mori is a key insect in the sericulture industry and one of the very important economic animals that are responsible for not only the livelihood of many farmers internationally but also expended biomedical use. The National Institute of Agricultural Sciences of the Rural Development Administration of Korea (NIAS, RDA, Korea) has been collecting silkworm resources with various phenotypic traits from the 1960s and established breeding lines for using them as genetic resources. And these breeding line strains have been used to develop suitable F1 hybrid strains for specific use. In this study, we report the whole-genome sequences of 37 breeding line B. mori strains established over the past 60 years, along with the description of their phenotypic characteristics with photos of developmental stages. In addition, we report the example phenotypic characteristics of the F1-hybrid strain using these breeding line strains. We hope this data will be used as valuable resources to the related research community for studying B. mori and similar other insects. 

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Whole-genome sequences of 37 breeding line Bombyx mori strains and their phenotypes established since 1960s

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K. Kim

Papers

Cyber‐Physical Watermarking with Inkjet Edible Bioprinting

Edible Matrix Code with Photogenic Silk Proteins

Biocompatible fluorescent silk fibroin bioink for digital light processing 3D printing.

Whole-genome sequences of 37 breeding line Bombyx mori strains and their phenotypes established since 1960s

Whole-genome sequences of 37 breeding line Bombyx mori strains and their phenotypes established since 1960s