Immune Checkpoint Reprogramming via Sequential Nucleic Acid Delivery Strategy Optimizes Systemic Immune Responses for Gastrointestinal Cancer Immunotherapy.

Monoclonal antibodies targeting immune checkpoints have been widely applied in gastrointestinal cancer immunotherapy. However, systemic administration of various monoclonal antibodies does not often result in sustained effects in reversing the immunosuppressive tumor microenvironment (TME), which may be due to the spatiotemporal dynamic changes of immune checkpoints. Herein, we reported a novel immune checkpoint reprogramming strategy for gastrointestinal cancer immunotherapy. It was achieved by the sequential delivery of siPD-L1 (siRNA for programmed cell death ligand 1) and pOX40L (plasmid for OX40 ligand), which were complexed with two cationic polymer brush-grafted carbon nanotubes (dense short (DS) and dense long (DL)) designed based on the structural characteristics of nucleic acids and brush architectures. Upon administrating DL/pOX40L for the first three dosages, then followed by DS/siPD-L1 for the next three dosages to the TME, it upregulated the stimulatory checkpoint OX40L on dendritic cells (DCs) and downregulated inhibitory checkpoint PD-L1 on tumor cells and DCs in a sequential reprogramming manner. Compared with other combination treatments, this sequential strategy drastically boosted the DCs maturation, and CD8+ cytotoxic T lymphocytes infiltration in tumor site. Furthermore, it could augment the local antitumor response and improve the T cell infiltration in tumor-draining lymph nodes to reverse the peripheral immunosuppression. Our study demonstrated that sequential nucleic acid delivery strategy via personalized nanoplatforms effectively reversed the immunosuppression status in both tumor microenvironment and peripheral immune landscape, which significantly enhanced the systemic antitumor immune responses and established an optimal immunotherapy strategy against gastrointestinal cancer.

Advancements and greenification potential of magnetic molecularly imprinted polymers for chromatographic analysis of veterinary drug residues in milk.

Milk, as a widely consumed nutrient-rich food, is crucial for bone health, growth, and overall nutrition. The persistent application of veterinary drugs for controlling diseases and heightening milk yield has imparted substantial repercussions on human health and environmental ecosystems. Due to the high demand, fresh consumption, complex composition of milk, and the potential adverse impacts of drug residues, advanced greener analytical methods are necessitated. Among them, functional materials-based analytical methods attract wide concerns. The magnetic molecularly imprinted polymers (MMIPs), as a kind of typical functional material, possess excellent greenification characteristics and potencies, and they are easily integrated into various detection technologies, which have offered green approaches toward analytes such as veterinary drugs in milk. Despite their increasing applications and great potential, MMIPs' use in dairy matrices remains underexplored, especially regarding ecological sustainability. This work reviews recent advances in MMIPs' synthesis and application as efficient sorbents for veterinary drug extraction in milk followed by chromatographic analysis. The uniqueness and effectiveness of MMIPs in real milk samples are evaluated, current limitations are addressed, and greenification opportunities are proposed. MMIPs show promise in revolutionizing green analytical procedures for veterinary drug detection, aligning with the environmental goals of modern food production systems.

Synthesis of green magnetic molecularly imprinted polymers for selective extraction of rifaximin in milk samples.

In this study, a new analytical method was developed using magnetic molecularly imprinted polymers (MMIPs) by employing eco-friendly supramolecular ternary deep eutectic solvents to synthesize these MMIPs for selective extraction of rifaximin. The characterization analysis and adsorption affinity investigation were conducted. The results showed fast adsorption (15 min) with high adsorption capacity (43.20 mg g-1) and selectivity for rifaximin. Various extraction parameters were optimized, achieving recoveries ranging from 86.67% to 99.47% in spiked milk samples using high-performance liquid chromatography (HPLC). The detection and quantification limits were 0.01 mg L-1 and 0.03 mg L-1, respectively. The method exhibited low RSDs (<4.70%) and excellent selectivity, with MMIPs reusable up to seven times with only a 10% performance loss. This study proposes a convenient and reliable method for trace-level rifaximin extraction from milk using eco-friendly MMIPs.

AI-assisted smartphone-based colorimetric biosensor for visualized, rapid and sensitive detection of pathogenic bacteria.

Accurate and effective detection is essential to against bacterial infection and contamination. Novel biosensors, which detect bacterial bioproducts and convert them into measurable signals, are attracting attention. We developed an artificial intelligence (AI)-assisted smartphone-based colorimetric biosensor for the visualized, rapid, sensitive detection of pathogenic bacteria by measuring the bacteria secreted hyaluronidase (HAase). The biosensor consists of the chlorophenol red-ß-D-galactopyranoside (CPRG)-loaded hyaluronic acid (HA) hydrogel as the bioreactor and the ß-galactosidase (ß-gal)-loaded agar hydrogel as the signal generator. The HAase degrades the bioreactor and subsequently determines the release of CPRG, which could further react with ß-gal to generate signal colors. The self-developed YOLOv5 algorithm was utilized to analyze the signal colors acquired by smartphone. The biosensor can provide a report within 60 min with an ultra-low limit of detection (LoD) of 10 CFU/mL and differentiate between gram-positive (G+) and gram-negative (G-) bacteria. The proposed biosensor was successfully applied in various areas, especially the evaluation of infections in clinical samples with 100% sensitivity. We believe the designed biosensor has the potential to represent a new paradigm of "ASSURED" bacterial detection, applicable for broad biomedical uses.

Modulation of Gut Microbial Metabolism by Cyanidin-3-O-Glucoside in Mitigating Polystyrene-Induced Colonic Inflammation: Insights from 16S rRNA Sequencing and Metabolomics.

Microplastics derived from plastic waste have emerged as a pervasive environmental pollutant with potential transfer and accumulation through the food chain, thus posing risks to both ecosystems and human health. The gut microbiota, tightly intertwined with metabolic processes, exert substantial influences on host physiology by utilizing dietary compounds and generating bacterial metabolites such as tryptophan and bile acid. Our previous studies have demonstrated that exposure to microplastic polystyrene (PS) disrupts the gut microbiota and induces colonic inflammation. Meanwhile, intervention with cyanidin-3-O-glucoside (C3G), a natural anthocyanin derived from red bayberry, could mitigate colonic inflammation by reshaping the gut bacterial composition. Despite these findings, the specific influence of gut bacteria and their metabolites on alleviating colonic inflammation through C3G intervention remains incompletely elucidated. Therefore, employing a C57BL/6 mouse model, this study aims to investigate the mechanisms underlying how C3G modulates gut bacteria and their metabolites to alleviate colonic inflammation. Notably, our findings demonstrated the efficacy of C3G in reversing the elevated levels of pro-inflammatory cytokines (IL-6, IL-1ß, and TNF-α) and the upregulation of mRNA expression (Il-6, Il-1ß, and Tnf-α) induced by PS exposure. Meanwhile, C3G effectively inhibited the reduction in levels (IL-22, IL-10, and IL-4) and the downregulation of mRNA expression (Il-22, Il-10, and Il-4) of anti-inflammatory cytokines induced by PS exposure. Moreover, PS-induced phosphorylation of the transcription factor NF-κB in the nucleus, as well as the increased level of protein expression of iNOS and COX-2 in the colon, were inhibited by C3G. Metabolisms of gut bacterial tryptophan and bile acids have been extensively implicated in the regulation of inflammatory processes. The 16S rRNA high-throughput sequencing disclosed that PS treatment significantly increased the abundance of pro-inflammatory bacteria (Desulfovibrio, norank_f_Oscillospiraceae, Helicobacter, and Lachnoclostridium) while decreasing the abundance of anti-inflammatory bacteria (Dubosiella, Akkermansia, and Alistipes). Intriguingly, C3G intervention reversed these pro-inflammatory changes in bacterial abundances and augmented the enrichment of bacterial genes involved in tryptophan and bile acid metabolism pathways. Furthermore, untargeted metabolomic analysis revealed the notable upregulation of metabolites associated with tryptophan metabolism (shikimate, l-tryptophan, indole-3-lactic acid, and N-acetylserotonin) and bile acid metabolism (3b-hydroxy-5-cholenoic acid, chenodeoxycholate, taurine, and lithocholic acid) following C3G administration. Collectively, these findings shed new light on the protective effects of dietary C3G against PS exposure and underscore the involvement of specific gut bacterial metabolites in the amelioration of colonic inflammation.

Ultrasensitive colorimetric detection of creatinine via its dual binding affinity for silver nanoparticles and silver ions.

Creatinine is an important biomarker for the diagnosis of chronic kidney disease (CKD). Recently, it has been reported that the concentration of salivary creatinine correlates well with the concentration of serum creatinine, which makes the former useful for the development of non-invasive and point-of-care (POC) detection for CKD diagnosis. However, there exists a technical challenge in the rapid detection of salivary creatinine at low concentrations of 3-18 µM when using the current kidney function test strips as well as the traditional methods employed in hospitals. Herein, we demonstrate a simple, sensitive colorimetric assay for the detection of creatinine with a limit-of-detection (LOD) down to the nanomolar level. Our approach utilises the dual binding affinity of creatinine for citrate-capped silver nanoparticles (Ag NPs) and Ag(i) ions, which can trigger the aggregation of Ag NPs and thus lead to the colour change of a sample. The quantitative detection of creatinine was achieved using UV-Vis spectroscopy with a LOD of 6.9 nM in artificial saliva and a linear dynamic range of 0.01-0.06 µM. This method holds promise to be further developed into a POC platform for the CKD diagnosis.

Cellular uptake and in vivo distribution of mesenchymal-stem-cell-derived extracellular vesicles are protein corona dependent.

Extracellular vesicles (EVs) derived from mesenchymal stem cells are promising nanotherapeutics in liver diseases due to their regenerative and immunomodulatory properties. Nevertheless, a concern has been raised regarding the rapid clearance of exogenous EVs by phagocytic cells. Here we explore the impact of protein corona on EVs derived from two culturing conditions in which specific proteins acquired from media were simultaneously adsorbed on the EV surface. Additionally, by incubating EVs with serum, simulating protein corona formation upon systemic delivery, further resolved protein corona-EV complex patterns were investigated. Our findings reveal the potential influences of corona composition on EVs under in vitro conditions and their in vivo kinetics. Our data suggest that bound albumin creates an EV signature that can retarget EVs from hepatic macrophages. This results in markedly improved cellular uptake by hepatocytes, liver sinusoidal endothelial cells and hepatic stellate cells. This phenomenon can be applied as a camouflage strategy by precoating EVs with albumin to fabricate the albumin-enriched protein corona-EV complex, enhancing non-phagocytic uptake in the liver. This work addresses a critical challenge facing intravenously administered EVs for liver therapy by tailoring the protein corona-EV complex for liver cell targeting and immune evasion.

Photothermal Ferrotherapy - Induced Immunogenic Cell Death via Iron-Based Ternary Chalcogenide Nanoparticles Against Triple-Negative Breast Cancer.

Triple-negative breast cancer (TNBC) is highly malignant and prone to recurrence and metastasis. Patients with TNBC have limited therapeutic options, often resulting in poor prognosis. Some new treatments for TNBC have been considered in the past decade, such as immunotherapy, photothermal therapy (PTT), and ferroptosis therapy, that allow the rapid and minimally invasive ablation of cancer. However, a multifunctional nanodrug system with more potent efficacy for TNBC is still needed. The use of iron-based ternary chalcogenide nanoparticles (NPs), namely AgFeS2 , is reported, which synergistically combines photothermal therapy, ferrotherapy, and immunotherapy in one system for the treatment of TNBC. AgFeS2 possesses excellent photothermal conversion performance for tumor near-infrared (NIR) phototherapy. Upon photoirradiation, these NPs generate heat, accelerate the release of iron ions, and effectively catalyze the Fenton reaction, resulting in cell apoptosis and ferroptosis. Additionally, AgFeS2 promotes the release of tumor-specific antigens and triggers an immune response via immunogenic cell death (ICD), thereby providing unique synergistic mechanisms for cancer therapy. The present study demonstrates the great potential of iron-based ternary chalcogenide as a new therapeutic platform for a combination of photothermal therapy, ferrotherapy, and immunotherapy for the suppression of TNBC.

Dynamic and Label-Free Sensing of Cardiomyocyte Responses to Nanosized Vesicles for Cardiac Oxidative Stress Injury Therapy.

Cardiac oxidative stress is a significant phenotype of myocardial infarction disease, a leading cause of global health threat. There is an urgent need to develop innovative therapies. Nanosized extracellular vesicle (nEV)-based therapy shows promise, yet real-time monitoring of cardiomyocyte responses to nEVs remains a challenge. In this study, a dynamic and label-free cardiomyocyte biosensing system using microelectrode arrays (MEAs) was constructed. Cardiomyocytes were cultured on MEA devices for electrophysiological signal detection and treated with nEVs from E. coli, gardenia, HEK293 cells, and mesenchymal stem cells (MSC), respectively. E. coli-nEVs and gardenia-nEVs induced severe paroxysmal fibrillation, revealing distinct biochemical communication compared to MSC-nEVs. Principal component analysis identified variations and correlations between nEV types. MSC-nEVs enhanced recovery without inducing arrhythmias in a H2O2-induced oxidative stress injury model. This study establishes a fundamental platform for assessing biochemical communication between nEVs and cardiomyocytes, offering new avenues for understanding nEVs' functions in the cardiovascular system.

Graphene Sensor Arrays for Rapid and Accurate Detection of Pancreatic Cancer Exosomes in Patients' Blood Plasma Samples.

Biosensors based on graphene field effect transistors (GFETs) have the potential to enable the development of point-of-care diagnostic tools for early stage disease detection. However, issues with reproducibility and manufacturing yields of graphene sensors, but also with Debye screening and unwanted detection of nonspecific species, have prevented the wider clinical use of graphene technology. Here, we demonstrate that our wafer-scalable GFETs array platform enables meaningful clinical results. As a case study of high clinical relevance, we demonstrate an accurate and robust portable GFET array biosensor platform for the detection of pancreatic ductal adenocarcinoma (PDAC) in patients' plasma through specific exosomes (GPC-1 expression) within 45 min. In order to facilitate reproducible detection in blood plasma, we optimized the analytical performance of GFET biosensors via the application of an internal control channel and the development of an optimized test protocol. Based on samples from 18 PDAC patients and 8 healthy controls, the GFET biosensor arrays could accurately discriminate between the two groups while being able to detect early cancer stages including stages 1 and 2. Furthermore, we confirmed the higher expression of GPC-1 and found that the concentration in PDAC plasma was on average more than 1 order of magnitude higher than in healthy samples. We found that these characteristics of GPC-1 cancerous exosomes are responsible for an increase in the number of target exosomes on the surface of graphene, leading to an improved signal response of the GFET biosensors. This GFET biosensor platform holds great promise for the development of an accurate tool for the rapid diagnosis of pancreatic cancer.

Assessing the greenification potential of cyclodextrin-based molecularly imprinted polymers for pesticides detection.

Cyclodextrins, with their unparalleled attributes of eco-friendliness, natural abundance, versatile utility, and facile functionalization, make a paramount contribution to the field of molecular imprinting. Leveraging the unique properties of cyclodextrins in molecularly imprinted polymers synthesis has revolutionized the performance of molecularly imprinted polymers, resulting in enhanced adsorption selectivity, capacity, and rapid extraction of pesticides, while also circumventing conventional limitations. As the concern for food quality and safety continues to grow, the need for standard analytical methods to detect pesticides in food and environmental samples has become paramount. Cyclodextrins, being non-toxic and biodegradable, present an attractive option for greener reagents in imprinting polymers that can also ensure environmental safety post-application. This review provides a comprehensive summary of the significance of cyclodextrins in molecular imprinting for pesticide detection in food and environmental samples. The recent advancements in the synthesis and application of molecularly imprinted polymers using cyclodextrins have been critically analyzed. Furthermore, the current limitations have been meticulously examined, and potential opportunities for greenification with cyclodextrin applications in this field have been discussed. By harnessing the advantages of cyclodextrins in molecular imprinting, it is possible to develop highly selective and efficient methods for detecting pesticides in food and environmental samples while also addressing the challenges of sustainability and environmental impact.

Self-Illuminating NIR-II Chemiluminescence Nanosensor for In Vivo Tracking H2 O2 Fluctuation.

Chemiluminescence (CL) imaging, as an excitation-free technique, exhibits a markedly improved signal-to-noise ratio (SNR) owing to the absence of an excitation light source and autofluorescence interference. However, conventional chemiluminescence imaging generally focuses on the visible and first near-infrared (NIR-I) regions, which hinders high-performance biological imaging due to strong tissue scattering and absorption. To address the issue, self-luminescent NIR-II CL nanoprobes with a second near-infrared (NIR-II) luminescence in the presence of hydrogen peroxide are rationally designed. A cascade energy transfer, including chemiluminescence resonance energy transfer (CRET) from the chemiluminescent substrate to NIR-I organic molecules and Förster resonance energy transfer (FRET) from NIR-I organic molecules to NIR-II organic molecules, occurs in the nanoprobes, contributing to NIR-II light with great efficiency and good tissue penetration depth. Based on excellent selectivity, high sensitivity to hydrogen peroxide, and long-lasting luminescence performance, the NIR-II CL nanoprobes are applied to detect inflammation in mice, showing a 7.4-fold enhancement in SNR compared with that of fluorescence.

Biomimetic integrated gustatory and olfactory sensing array based on HL-1 cardiomyocyte facilitating drug screening for tachycardia treatment.

The ectopic co-expression of taste and olfactory receptors in cardiomyocytes provides not only possibilities for the construction of biomimetic gustatory and olfactory sensors but also promising novel therapeutic targets for tachycardia treatment. Here, bitter taste and olfactory receptors endogenously expressed in HL-1 cells were verified by RT-PCR and immunofluorescence staining. Then HL-1 cardiomyocyte-based integrated gustatory and olfactory sensing array coupling with the microelectrode array (MEA) was first constructed for drugs screening and evaluation for tachycardia treatment. The MEA sensor detected the extracellular field potentials and reflected the systolic-diastolic properties of cardiomyocytes in real time in a label-free and non-invasive way. The in vitro tachycardia model was constructed using isoproterenol as the stimulator. The proposed sensing array facilitated potential drug screening for tachycardia treatment, such as salicin, artemisinin, xanthotoxin, and azelaic acid which all activated specific receptors on HL-1 cells. IC50 values for four potential drugs were calculated to be 0.0036 µM, 309.8 µM, 14.68 µM, and 0.102 µM, respectively. Visualization analysis with heatmaps and PCA cluster showed that different taste and odorous drugs could be easily distinguished. The mean inter-class Euclidean distance between different bitter drugs was 1.681, which was smaller than the distance between bitter and odorous drugs of 2.764. And the inter-class distance was significantly higher than the mean intra-class Euclidean distance of 1.172. In summary, this study not only indicates a new path for constructing novel integrated gustatory and olfactory sensors but also provides a powerful tool for the quantitative evaluation of potential drugs for tachycardia treatment.

Exploiting the potential of extracellular vesicles as delivery vehicles for the treatment of melanoma.

Melanoma, the most aggressive skin cancer that originated from genetic mutations in the melanocytes, is still a troublesome medical problem under the current therapeutic approaches, which include surgical resection, chemotherapy, photodynamic therapy, immunotherapy, biochemotherapy and targeted therapy. Nanotechnology has significantly contributed to the development of cancer treatment in the past few years, among which extracellular vesicles (EVs) are nanosized lipid bilayer vesicles secreted from almost all cells that play essential roles in many physiological and pathological processes. In terms of melanoma therapy, the unique physicochemical properties of EVs make them promising nanocarriers for drug transportation compared to other synthetic nanocarriers. Moreover, EVs can be further engineered to maximize their drug delivery potential. Herein, in this minireview, we gave a brief overview of EV-based drug delivery strategies for melanoma therapy, in which different therapeutics delivered via EVs were summarized. We also highlighted the current progress of the EV-based delivery platform for melanoma therapy in clinical trials. The obstacles to applying exosomes in clinical practice toward further translation of EVs melanoma therapy were also discussed at the end. In summary, EVs offer promising prospects for melanoma therapy, whilst the ways for unlocking EVs' full potential in melanoma therapies should be further investigated by solving relevant issues which hamper EVs-based melanoma therapy translation in the future.

On-chip integrated graphene aptasensor with portable readout for fast and label-free COVID-19 detection in virus transport medium.

Graphene field-effect transistor (GFET) biosensors exhibit high sensitivity due to a large surface-to-volume ratio and the high sensitivity of the Fermi level to the presence of charged biomolecules near the surface. For most reported GFET biosensors, bulky external reference electrodes are used which prevent their full-scale chip integration and contribute to higher costs per test. In this study, GFET arrays with on-chip integrated liquid electrodes were employed for COVID-19 detection and functionalized with either antibody or aptamer to selectively bind the spike proteins of SARS-CoV-2. In the case of the aptamer-functionalized GFET (aptasensor, Apt-GFET), the limit-of-detection (LOD) achieved was about 103 particles per mL for virus-like particles (VLPs) in clinical transport medium, outperforming the Ab-GFET biosensor counterpart. In addition, the aptasensor achieved a LOD of 160 aM for COVID-19 neutralizing antibodies in serum. The sensors were found to be highly selective, fast (sample-to-result within minutes), and stable (low device-to-device signal variation; relative standard deviations below 0.5%). A home-built portable readout electronic unit was employed for simultaneous real-time measurements of 12 GFETs per chip. Our successful demonstration of a portable GFET biosensing platform has high potential for infectious disease detection and other health-care applications.

Detection of Cancer-Derived Exosomes Using a Sensitive Colorimetric Aptasensor.

Exosomes are a type of extracellular vesicles that contain constituents including proteins, DNAs, and RNAs of the cells that secrete them. Cancerous exosomes are potential biomarkers for cancer diagnosis. Biosensors are useful analytical tools for quantification of biomarkers and targeted molecules. An aptasensor uses the aptamer as the biorecognition element to bind to the target and is one main type of biosensors that is promising for exosomes analysis and clinical cancer detection. The assay described in this chapter allows for reliable, sensitive, and specific detection of cancer-derived exosomes using a colorimetric aptasensor that is promising for point-of-care testing.

Polysaccharide-Based Hydrogels for Wound Dressing: Design Considerations and Clinical Applications.

Wound management remains a worldwide challenge. It is undeniable that patients with problems such as difficulties in wound healing, metabolic disorder of the wound microenvironment and even severely infected wounds etc. always suffer great pain that affected their quality of lives. The selection of appropriate wound dressings is vital for the healing process. With the advances of technology, hydrogels dressings have been showing great potentials for the treatment of both acute wounds (e.g., burn injuries, hemorrhage, rupturing of internal organs/aorta) and chronic wounds such as diabetic foot and pressure ulcer. Particularly, in the past decade, polysaccharide-based hydrogels which are made up with abundant and reproducible natural materials that are biocompatible and biodegradable present unique features and huge flexibilities for modifications as wound dressings and are widely applicable in clinical practices. They share not only common characteristics of hydrogels such as excellent tissue adhesion, swelling, water absorption, etc., but also other properties (e.g., anti-inflammatory, bactericidal and immune regulation), to accelerate wound re-epithelialization, mimic skin structure and induce skin regeneration. Herein, in this review, we highlighted the importance of tailoring the physicochemical performance and biological functions of polysaccharide-based hydrogel wound dressings. We also summarized and discussed their clinical states of, aiming to provide valuable hints and references for the future development of more intelligent and multifunctional wound dressings of polysaccharide hydrogels.

Detection of Glial Fibrillary Acidic Protein in Patient Plasma Using On-Chip Graphene Field-Effect Biosensors, in Comparison with ELISA and Single-Molecule Array.

Glial fibrillary acidic protein (GFAP) is a discriminative blood biomarker for many neurological diseases, such as traumatic brain injury. Detection of GFAP in buffer solutions using biosensors has been demonstrated, but accurate quantification of GFAP in patient samples has not been reported, yet in urgent need. Herein, we demonstrate a robust on-chip graphene field-effect transistor (GFET) biosensing method for sensitive and ultrafast detection of GFAP in patient plasma. Patients with moderate-severe traumatic brain injuries, defined by the Mayo classification, are recruited to provide plasma samples. The binding of target GFAP with the specific antibodies that are conjugated on a monolayer GFET device triggers the shift of its Dirac point, and this signal change is correlated with the GFAP concentration in the patient plasma. The limit of detection (LOD) values of 20 fg/mL (400 aM) in buffer solution and 231 fg/mL (4 fM) in patient plasma have been achieved using this approach. In parallel, for the first time, we compare our results to the state-of-the-art single-molecule array (Simoa) technology and the classic enzyme-linked immunosorbent assay (ELISA) for reference. The GFET biosensor shows competitive LOD to Simoa (1.18 pg/mL) and faster sample-to-result time (<15 min), and also it is cheaper and more user-friendly. In comparison to ELISA, GFET offers advantages of total detection time, detection sensitivity, and simplicity. This GFET biosensing platform holds high promise for the point-of-care diagnosis and monitoring of traumatic brain injury in GP surgeries and patient homes.

Tailoring the Architecture of Cationic Polymer Brush-Modified Carbon Nanotubes for Efficient siRNA Delivery in Cancer Immunotherapy.

The facile and controlled fabrication of homogeneously grafted cationic polymers on carbon nanotubes (CNTs) remains poorly investigated, which further hinders the understanding of interactions between functionalized CNTs with different nucleic acids and the rational design of appropriate gene delivery vehicles. Herein, we describe the controlled grafting of cationic poly(2-dimethylaminoethylmethacrylate) brushes on CNTs via surface-initiated atom transfer radical polymerization integrated with mussel-inspired polydopamine chemistry. The binding of nucleic acids with different brush-CNT hybrids discloses the highly architectural-dependent behavior with dense short brush-coated CNTs displaying the highest binding among all the other hybrids, namely, dense long, sparse long, and sparse short brush-coated CNTs. Additionally, different chemistries of the brush coatings were shown to influence the biocompatibility, cellular uptake, and silencing efficiency in vitro. This platform provides great flexibility for the design of polymer brush-CNT hybrids with precise control over their structure-activity relationship for the rational design of nucleic acid delivery systems.

Enhancing Structural Properties and Performance of Graphene-Based Devices Using Self-Assembled HMDS Monolayers.

The performance of graphene devices is often limited by defects and impurities induced during device fabrication. Polymer residue left on the surface of graphene after photoresist processing can increase electron scattering and hinder electron transport. Furthermore, exposing graphene to plasma-based processing such as sputtering of metallization layers can increase the defect density in graphene and alter the device performance. Therefore, the preservation of the high-quality surface of graphene during thin-film deposition and device manufacturing is essential for many electronic applications. Here, we show that the use of self-assembled monolayers (SAMs) of hexamethyldisilazane (HMDS) as a buffer layer during the device fabrication of graphene can significantly reduce damage, improve the quality of graphene, and enhance device performance. The role of HMDS has been systematically investigated using surface analysis techniques and electrical measurements. The benefits of HMDS treatment include a significant reduction in defect density compared with as-treated graphene and more than a 2-fold reduction of contact resistance. This surface treatment is simple and offers a practical route for improving graphene device interfaces, which is important for the integration of graphene into functional devices such as electronics and sensor devices.