Smartphone flashlight-triggered covalent organic framework nanozyme activity: A universal scheme for visual point-of-care testing

Owing to the advancement of interdisciplinary concepts, for example, wearable electronics, bioelectronics, and intelligent sensing, during the microelectronics industrial revolution, nowadays, extensively mature wearable sensing devices have become new favorites in the noninvasive human healthcare industry. The combination of wearable sensing devices with bionics is driving frontier developments in various fields, such as personalized medical monitoring and flexible electronics, due to the superior biocompatibilities and diverse sensing mechanisms. It is noticed that the integration of desired functions into wearable device materials can be realized by grafting biomimetic intelligence. Therefore, herein, the mechanism by which biomimetic materials satisfy and further enhance system functionality is reviewed. Next, wearable artificial sensory systems that integrate biomimetic sensing into portable sensing devices are introduced, which have received significant attention from the industry owing to their novel sensing approaches and portabilities. To address the limitations encountered by important signal and data units in biomimetic wearable sensing systems, two paths forward are identified and current challenges and opportunities are presented in this field. In summary, this review provides a further comprehensive understanding of the development of biomimetic wearable sensing devices from both breadth and depth perspectives, offering valuable guidance for future research and application expansion of these devices.

Biomimetic Wearable Sensors: Emerging Combination of Intelligence and Electronics.

Most current redox-type nanozyme-based colorimetric sensing platforms are susceptible to interference from the reductant when using chromogenic probe, and the unstable H2O2 used in the peroxidase-like nanozyme-based systems is prone to difficulty in sensing signal reproducibility, while peroxidase-like nanozyme with oxidase-mimicking activity is easy to bring background interference by O2. Since the strong structural designability of covalent organic frameworks (COFs) endows them great application value in the sensing fields, therefore, we envision the construction a COF oxidase-like nanozyme-based controllable sensing system that integrates self-reporting, self-correcting and light-responsive functions to avoid these affects. Herein, 3-nitrotyrosine (3-NT) biomarker was selected as model analyte. 1,3,5-triformylphloroglucinol (Tp) and 3,6-diaminoacridine (DA) were acted as building monomers of the multifunctional COF nanozyme (termed as TpDA). Owing to the excellent light-responsive oxidase-mimicking property of TpDA, 3-NT can be efficiently oxidized, the inner filter effect (IFE) between TpDA and the 3-NT oxidation product greatly quenches the intrinsic fluorescence of TpDA, making it a controllable self-reporting system for fluorescence turn-off sensing 3-NT. Additionally, the excessive reactive oxygen species (ROS) that generated continuously during photocatalysis can resist the interference of endogenous reductants. This study not only provides new insights to avoid the interference of H2O2, background and reductants from conventional redox-type nanozyme-based colorimetric systems but also opens avenues to rational construct versatile COF nanozyme-based sensor.

Three-in-one covalent organic framework nanozyme: Self-reporting, self-correcting and light-responsive for fluorescence sensing 3-nitrotyrosine

Metal-organic frameworks (MOFs) have been widely used as nanozymes with a great development prospect due to their unique advantages. It is known that the current Fe-based or Cu-based MOF, etc., exhibits the catalytic activity of nanozymes through the Fenton catalytic reaction. And the conversion efficiency of the Fe3+/Fe2+ or Cu2+/Cu+ cycle is key to the catalytic activity. Therefore, we proposed a novel co-catalytic method to promote the reaction rate of the rate-limiting step of Cu2+/Cu+ conversion in the Fenton reaction of Cu2+/H2O2 to enhance the catalytic activity of the nanozymes. As a proof of concept, the MoCu-2MI nanozyme with high catalytic activity was successfully synthesized using Mo-doped Cu-2MI (2-methylimidazole). By using 3,3',5,5'-tetramethylbenzidine (TMB) as the chromogenic substrate, MoCu-2MI exhibited higher peroxidase-like activity than pure Cu-2MI. Then, it was confirmed that the newly introduced Mo played a crucial co-catalytic role by characterizing the possible catalytic mechanism. Specifically, Mo acted as a co-catalyst to accelerate the electron transfer in the system, and then promote the Cu2+/Cu+ cycle in the Cu-Fenton reaction, which was conducive to accelerating the production of a large number of reactive oxygen species (ROS) from H2O2, and finally improve the activity. Ultimately, a biosensor platform combined with MoCu-2MI and cholesterol oxidase realized the one-step colorimetric detection of cholesterol in the range of 2-140 μM with the detection limit as low as 1.2 μM. This study provides a new strategy for regulating the activity of MOF nanozymes.

Enhanced peroxidase-like activity of MOF nanozymes by co-catalysis for colorimetric detection of cholesterol.

Prospects and challenges for the application of salty and saltiness-enhancing peptides in low-sodium meat products.

Colorimetric detection of creatinine based on specifically modulating the peroxidase-mimicking activity of Cu-Fenton system.

Thanks to the gustatory system, humans can experience the flavors in foods and drinks while avoiding the intake of some harmful substances. Although great advances in the fields of biotechnology, microfluidics, and nanotechnologies have been made in recent years, this astonishing recognition system can hardly be replaced by any artificial sensors designed so far. Here, taste organoids are coupled with an extracellular potential sensor array to form a novel bioelectronic organoid and developed a taste organoids‐on‐a‐chip system (TOS) for highly mimicking the biological sense of taste ex vivo with high stability and repeatability. The taste organoids maintain key taste receptors expression after the third passage and high cell viability during 7 days of on‐chip culture. Most importantly, the TOS not only distinguishs sour, sweet, bitter, and salt stimuli with great specificity, but also recognizes varying concentrations of the stimuli through an analytical method based on the extraction of signal features and principal component analysis. It is hoped that this bioelectronic tongue can facilitate studies in food quality controls, disease modelling, and drug screening.

Mimicking the Biological Sense of Taste In Vitro Using a Taste Organoids‐on‐a‐Chip System

The past decade has witnessed tremendous progress achieved in taste research, while few studies focus on interactions among taste compounds. Indeed, sweeteners and acidulants are commonly used food additives, and sweet-sour mixtures always provide improved tastes. For example, sensory studies have shown that sourness suppresses sweetness. However, the degree of sweetness suppression by sourness is difficult to evaluate quantitatively and objectively. Therefore, we propose a biohybrid tongue that is constructed by integrating mammalian gustatory epithelium with a microelectrode array chip. The taste quality and intensity information is coded in time-frequency patterns of local field potential. Different response patterns evoked by sweet and sour stimuli are observed, and the response is dose-dependent. Then, interaction effects of sourness against sweetness are quantified. The results indicate that suppression of sweetness by sourness occurs by increasing sourness concentrations. In summary, this study provides a powerful new tool for quantitative evaluation of sweet, sour, and their binary taste interactions that mimic the mammalian taste system.

Biohybrid Tongue for Evaluation of Taste Interaction between Sweetness and Sourness.

Humans perceive the world through five senses, of which olfaction is the oldest evolutionary sense that enables the detection of chemicals in the external environment. Recent progress in bioinspired electronics has boosted the development of artificial sensory systems. Here, a biohybrid olfactory system is proposed by integrating living mammals with implantable flexible neural electrodes, to employ the outstanding properties of mammalian olfactory system. In olfactory perception, the peripheral organ-olfactory epithelium (OE) projects axons into the olfactory relay station-olfactory bulb (OB). The olfactory information encoded in the neural activity is recorded from both OE and OB simultaneously using flexible neural electrodes. Results reveal that spontaneous slow oscillations (<12 Hz) in both OE and OB closely follow respiration. This respiration-locked rhythm modulates the amplitude of fast oscillations (>20 Hz), which are associated with odor perception. Further, by extracting the characteristics of odor-evoked oscillatory signals, responses of different odors are identified and classified with 80% accuracy. This study demonstrates for the first time that the flexible electrode enables chronic stable electrophysiological recordings of the peripheral and central olfactory system in vivo. Overall, the method provides a novel neural interface for olfactory biosensing and cognitive processing.

Long-Term Flexible Neural Interface for Synchronous Recording of Cross-Regional Sensory Processing along the Olfactory Pathway.

Many mammalian tissues adopt a specific cellular arrangement under stress stimulus that enables their unique function. However, conventional 3D (three-dimensional) encapsulation often fails to recapitulate the complexities of these arrangements, thus motivating the need for advanced cellular arrangement approaches. Here, an original 3D pre-stress bioprinting approach of directed tissues under the synergistic effect of static sustained tensile stress and molecular chain orientation, with an aid of slow crosslinking in bioink, is developed. The semi-crosslinking state of the designed bioink exhibits excellent elasticity for applying stress on the cells during the sewing-like process. After bioprinting, the bioink gradually forms complete crosslinking and keeps the applied stress force to induce cell-orientated growth. More importantly, multiple cell types can be arranged directionally by our approach, while the internal stress of the hydrogel filament is also adjustable. In addition, compared with conventional bioprinted skin, the 3D pre-stress bioprinted skin results in a better wound healing effect due to promoting the angiogenesis of granulation tissue. This study provides a prospective strategy to engineer skeletal muscles, as well as tendons, ligaments, vascular networks, or combinations thereof in the future. This article is protected by copyright. All rights reserved.

3D Pre-stress Bioprinting of Directed Tissues.

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