Biomarkers are crucial biological indicators in medical diagnostics and therapy. However, the process of biomarker discovery and validation is hindered by a lack of standardized protocols for analytical studies, storage and sample collection. Wearable chemical sensors provide a real-time, non-invasive alternative to typical laboratory blood analysis, and are an effective tool for exploring novel biomarkers in alternative body fluids, such as sweat, saliva, tears and interstitial fluid. These devices may enable remote at-home personalized health monitoring and substantially reduce the healthcare costs. This Review introduces criteria, strategies and technologies involved in biomarker discovery using wearable chemical sensors. Electrochemical and optical detection techniques are discussed, along with the materials and system-level considerations for wearable chemical sensors. Lastly, this Review describes how the large sets of temporal data collected by wearable sensors, coupled with modern data analysis approaches, would open the door for discovering new biomarkers towards precision medicine. 

/pdf/wearable-chemical-sensors-for-biomarker-discovery-in-the-1hkxiyze.pdf

Wearable chemical sensors for biomarker discovery in the omics era

Molecular imprinting technology (MIT) produces artificial binding sites with precise complementarity to substrates and thereby is capable of exquisite molecular recognition. Over five decades of evolution, it is predicted that the resulting host imprinted materials will overtake natural receptors for research and application purposes, but in practice, this has not yet been realized due to the unsustainability of their life cycles (i.e., precursors, creation, use, recycling, and end‐of‐life). To address this issue, greenificated molecularly imprinted polymers (GMIPs) are a new class of plastic antibodies that have approached sustainability by following one or more of the greenification principles, while also demonstrating more far‐reaching applications compared to their natural counterparts. In this review, the most recent developments in the delicate design and advanced application of GMIPs in six fast‐growing and emerging fields are surveyed, namely biomedicine/therapy, catalysis, energy harvesting/storage, nanoparticle detection, gas sensing/adsorption, and environmental remediation. In addition, their distinct features are highlighted, and the optimal means to utilize these features for attaining incredibly far‐reaching applications are discussed. Importantly, the obscure technical challenges of the greenificated MIT are revealed, and conceivable solutions are offered. Lastly, several perspectives on future research directions are proposed.

Greenificated Molecularly Imprinted Materials for Advanced Applications

While the current smartwatches and cellphones can readily track mobility and vital signs, a new generation of wearable devices is rapidly developing to enable users to monitor their health parameters at the molecular level. Within this emerging class of wearables, microneedle-based transdermal sensors are in a prime position to play a key role in synergizing the significant advantages of dermal interstitial fluid (ISF) as a rich source of clinical indicators and painless skin pricking to allow the collection of real-time diagnostic information. While initial efforts of microneedle sensing focused on ISF extraction coupled with either on-chip analysis or off-chip instrumentation, the latest trend has been oriented toward assembling electrochemical biosensors on the tip of microneedles to allow direct continuous chemical measurements. In this context, significant advances have recently been made in exploiting microneedle-based devices for real-time monitoring of various metabolites, electrolytes, and therapeutics and toward the simultaneous multiplexed detection of key chemical markers; yet, there are several grand challenges that still exist. In this review, we outline current progress, recent trends, and new capabilities of microneedle-empowered sensors, along with the current unmet challenges and a future roadmap toward transforming the latest innovations in the field to commercial products.

Lab under the Skin: Microneedle Based Wearable Devices.

Soft wearable devices for deep-tissue sensing

In recent years, an innovative transdermal delivery technology has attracted great interest for its ability to distribute therapeutics and cosmeceuticals for several applications, including vaccines, drugs, and biomolecules for skin-related problems. The advantages of microneedle patch technology have been extensively evaluated in the latest literature; hence, the academic publications in this area are rising exponentially. Like all new technologies, the microneedle patch application has great potential but is not without limitations. In this review, we will discuss the possible limitations by highlighting the areas where a great deal of improvements are required. Emphasising these concerns early on should help scientists and technologists to address the matters in a timely fashion and to use their resources wisely.

Microneedles in Drug Delivery: Progress and Challenges

The detection and quantification of protein biomarkers in interstitial fluid is hampered by challenges in its sampling and analysis. Here we report the use of a microneedle patch for fast in vivo sampling and on-needle quantification of target protein biomarkers in interstitial fluid. We used plasmonic fluor-an ultrabright fluorescent label-to improve the limit of detection of various interstitial fluid protein biomarkers by nearly 800-fold compared with conventional fluorophores, and a magnetic backing layer to implement conventional immunoassay procedures on the patch and thus improve measurement consistency. We used the microneedle patch in mice for minimally invasive evaluation of the efficiency of a cocaine vaccine, for longitudinal monitoring of the levels of inflammatory biomarkers, and for efficient sampling of the calvarial periosteum-a challenging site for biomarker detection-and the quantification of its levels of the matricellular protein periostin, which cannot be accurately inferred from blood or other systemic biofluids. Microneedle patches for the minimally invasive collection and analysis of biomarkers in interstitial fluid might facilitate point-of-care diagnostics and longitudinal monitoring.

/pdf/microneedle-patch-for-the-ultrasensitive-quantification-of-pcl47i6dyo.pdf

Microneedle patch for the ultrasensitive quantification of protein biomarkers in interstitial fluid.

Solar-driven desalination, which involves the conversion of solar energy to heat for freshwater generation, has been recognized as an attractive and sustainable desalination technology to alleviate freshwater shortage. In particular, photothermally driven membrane distillation (PMD) is a highly promising solar-driven desalination technology, especially in remote regions and disaster-struck communities, where no power infrastructure or waste heat from industrial plants is available. MXene, more specifically Ti3C2Tx, with excellent photothermal properties, easy processability, and electrical conductivity offers a great opportunity for realizing highly efficient, stable and multifunctional PMD membranes. Herein, we realize a MXene composite aerogel comprised of hydroxyapatite nanowires and poly(vinyl alcohol) with high thermal efficiency (61%) and water flux (0.72 kg m−2 h−1) under 0.8 sun irradiation (0.8 kW m−2), representing the first validation of highly efficient MXene-based PMD systems in treating ambient saline water. Owing to the strong interfacial interaction (i.e., hydrogen bonding) between the building blocks, the MXene composite aerogel with high porosity (up to 91%) exhibited excellent mechanical stability. This highly interconnected porous network offers low resistance to vapor transport and low thermal conductivity, which minimizes conductive heat transfer across the aerogel, thus maximizing the thermal efficiency. Furthermore, the outstanding bactericidal activity induced by solar irradiation or electric potential makes the MXene composite aerogel a highly attractive candidate for PMD in the real world.

MXene aerogel for efficient photothermally driven membrane distillation with dual-mode antimicrobial capability

Novel methods that enable sensitive, accurate and rapid detection of RNA would not only benefit fundamental biological studies but also serve as diagnostic tools for various pathological conditions, including bacterial and viral infections and cancer. Although highly sensitive, existing methods for RNA detection involve long turn-around time and extensive capital equipment. Here, an ultrasensitive and amplification-free RNA quantification method is demonstrated by integrating CRISPR-Cas13a system with an ultrabright fluorescent nanolabel, plasmonic fluor. This plasmonically enhanced CRISPR-powered assay exhibits nearly 1000-fold lower limit-of-detection compared to conventional assay relying on enzymatic reporters. Using a xenograft tumor mouse model, it is demonstrated that this novel bioassay can be used for ultrasensitive and quantitative monitoring of cancer biomarker (lncRNA H19). The novel biodetection approach described here provides a rapid, ultrasensitive, and amplification-free strategy that can be broadly employed for detection of various RNA biomarkers, even in resource-limited settings.

Plasmonically Enhanced CRISPR/Cas13a-Based Bioassay for Amplification-Free Detection of Cancer-Associated RNA

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Microneedle patch for the ultrasensitive quantification of protein biomarkers in interstitial fluid.

MXene aerogel for efficient photothermally driven membrane distillation with dual-mode antimicrobial capability

Plasmonically Enhanced CRISPR/Cas13a-Based Bioassay for Amplification-Free Detection of Cancer-Associated RNA