Traditional quantitative colorimetric assays often rely on bulky laboratory instruments, such as UV-vis spectrophotometers and microplate readers. While smartphone-based point-of-need (PON) tools have emerged as alternatives, they are frequently limited by variation in ambient lighting and perspective distortion. To address these challenges, we developed a PON quantitative platform for colorimetric assays that integrates hydrogel (agarose based) coated filter paper as reaction "mini-disks", a handheld Wi-Fi scanner as the imaging tool, and a custom-designed app (universal for both smartphones and pads) for color analysis. Using two representative colorimetric assays, pH-differential colorimetric assay for anthocyanin and Ellman's assay for parathion methyl, we validated the performance of this new Wi-Fi scanning platform using conventional UV-vis spectrophotometry analysis. The results demonstrate that this integrated Wi-Fi scanning protocol promises a reliable, universal, low-cost, and convenient tool for on-site, quantitative colorimetric analysis in resource-limited settings.
CD3ζ-based chimeric antigen receptor macrophage (CAR-M) therapy for solid tumors is limited by complex viral-mediated genetic engineering and the challenge of maintaining a durable pro-inflammatory phenotype within the immunosuppressive tumor microenvironment. Here, we introduce a supramolecular glycoengineering strategy that bypasses genetic modification. By utilizing a novel metabolic labeling agent, Ac4ManNAda, we successfully install adamantane (Ada, a guest molecule) tags onto macrophage surfaces via native biosynthetic pathways to generate glycoengineered supramolecular macrophages (GSAR-M). This labeling not only significantly enhances recognition of β-cyclodextrin (β-CD, a host molecule)-tagged tumor cells via CD-Ada host-guest interactions but also, unexpectedly, acts as an intrinsic activator. It induces a sustained distinct activated state in GSAR-M, characterized by upregulated activation markers and enhanced migratory, phagocytic, and tumoricidal capacities. Furthermore, subsequent LPS stimulation of these cells (termed GSAR-M+) cooperatively amplifies F-actin content and pseudopodia formation, leading to superior tumor cell capture in vitro. In a murine 4T1 breast cancer model, this supramolecular glycoengineering strategy achieves profound tumor growth arrest and effectively remodels the immunosuppressive tumor microenvironment. This study establishes a streamlined, cost-effective, and non-viral engineering paradigm that integrates host-guest recognition with glycometabolic engineering, providing critical insights for the development of next-generation engineered immune cells in adoptive cell therapies.
With the rapid and widespread emergence of antibiotic-resistant bacteria, the development of novel and highly effective antibacterial strategies has become an urgent imperative. Graphene oxide‑silver nanoparticle composites (GOAg) represent a class of promising inorganic nano-antibacterial materials. However, GOAg rapidly undergoes aggregation in saline- or protein-containing physiological media, which severely hampers its antibacterial applications. Therefore, identifying an appropriate carrier for GOAg immobilization is urgently needed. In this study, a carboxymethyl chitosan-aldehyde sodium alginate (CMCS-ASA) hydrogel was employed as a matrix to encapsulate GOAg, thereby fabricating a CMCS-ASA-GOAg composite hydrogel. Comprehensive characterization demonstrated that the resulting composite hydrogel exhibited favorable swelling capacity, water-retention ability, injectability, self-healing performance, and optical transparency. Moreover, the hydrogel showed high drug encapsulation efficiency, appreciable loading capacity, and sustained-release behavior, enabling the continuous release of Ag+ for up to 27 days. The CMCS-ASA-GOAg composite hydrogel also exhibited excellent antibacterial activity and satisfactory biocompatibility. When the GOAg concentration reached 40 μg/mL, both the surface and interior of the hydrogel achieved bactericidal efficiencies exceeding 95% against Gram-negative and Gram-positive bacteria, while showing no obvious cytotoxicity toward mouse embryonic fibroblast cells. Collectively, these findings provide a new strategy and valuable reference for expanding the antibacterial applications of graphene-based nanomaterials.
From power lines and airplane wings to wind turbines, many devices and infrastructure would benefit from icephobicity, the ability for a material to shed ice, and thus avoid costly damages which disrupt critical aspects of daily life. Many existing icephobic materials suffer from durability issues simply due to weathering and contamination, which are often addressed by a related but distinct property: superhydrophobicity. Unfortunately, most superhydrophobic surfaces developed to date are not icephobic. Based on bench-top nanomolding of polydimethylsiloxane (PDMS) with optimized silicone oil content from crystalized polycarbonate (PC) template, we developed hierarchically structured silicone films (as a new class of slippery lubricant-infused porous surface, SLIPS) that are both superhydrophobic and supericephobic. In doing so, we effectively combine the properties of the lotus and pitcher plant; we explored how the morphology at nano/micrometer scale and the amount of silicone oil in our SLIPS can be tuned to balance wettability and ice shedding to achieve superhydrophobicity and supericephobicity simultaneously, with water contact angle as high as 171.2 ± 1.5° and ice adhesion strength as low as 11.5 ± 2.3 kPa (i.e., superior water repellency and ice shedding capability). While synergistically utilizing the properties of Nepenthes and Nelumbo nucifera, this new fabrication approach for SLIPS promises tremendous application potentials.
Barcode technology has gained significant attention in analytical and bioanalytical chemistry assays due to its high-throughput capability and rapid response. However, early studies primarily focused on the integration of barcode formatting without encoding and interpretation for multiplex assay reading. As a result, the full potential of barcode technology in enhancing assay efficiency and capability has not been fully realized. In this work, a Lego-based, Quick-Response (QR) code-formatted bioassay device has been designed and tested for the detection of disease biomarkers and other potential molecular targets of interest. Particularly the QR-coded device for multiplex immunoassays is consisted of 1 x 1 standard Lego bricks (either white or black), except for those in the "detection zones"; these are replaced by 3D-printed transparent Lego bricks with mini-vials at the center for performing assay reactions. This integrated smart device can be read with a standard barcode app, and the results are processed for semiquantitative readout. This Lego-assembled QR-coded assay device is capable of analyzing up to 24 samples simultaneously within 30 min, and its performance is demonstrated by simultaneously detecting a set of coronary heart disease markers, i.e., triglycerides, total cholesterol, and uric acid. The performance of this portable device meets biomedical testing standards, and its accuracy is validated by comparing real sample data with those obtained on an automatic immunoassay analyzer at hospital. We envision that the developed QR-coded Lego assay device promises a simple, accurate, and rapid platform methodology for point-of-care medical diagnosis and on-site chemical analysis.
Compared to pristine graphene, graphene oxide (GO) has intriguing advantages for biological applications, such as high compatibility and much improved solubility in an aqueous environment. In particular, the oxygen-containing functional groups on GO enable the highly stable covalent conjugation of biomolecules, which promotes its application for developing versatile functional devices. In this work, we explored an ultraviolet/ozone (UV/O3) treatment strategy to activate graphene-tape substrates (prepared by drop-casting graphene nanoplatelets on double-sided conductive carbon tapes) to achieve excellent bioconjugation capabilities. Our Fourier transform infrared spectroscopy (FTIR), wetting, and X-ray photoelectron spectroscopy (XPS) measurements confirmed the generation of high-density oxygen-containing functional groups on graphene-carbon tape, while the conductivity and electrochemical activity are merely influenced. Upon immobilizing amino-ferrocene (Fc-NH2) onto the UV/O3-activated graphene tape via carbodiimide cross-linking, a strong pair of redox peaks (corresponding to an Fc surface density over 8.0 × 10-9 mol/cm2) was observed, indicative of its "elevated" covalent conjugation capability. More remarkably, highly efficient conjugation of glucose oxidase on UV/O3-treated graphene tape was achieved, which demonstrated excellent catalytic activity, as confirmed by chronoamperometry. These results augment the great potential of UV/O3-activated graphene tape substrates for convenient fabrication of electroactive biofunctional devices with high performance.
In this work, we demonstrated the efficacy of combining covalent modification via the click reaction and benchtop machine-cutting of glass microfiber filters (GMFs) to fabricate microfluidic paper-based analytical devices (μPADs) for performing ultrasensitive fluorometric assays. This has been accomplished by activating the GMF surface through the self-assembly of propargyl-PEG3-triethoxysilane (PPTES) and the click reaction to immobilize fluorometric probes (i.e., 3-azido-7-hydroxycoumarin, A-7-HC). Specifically for making the device, mini-discs of GMF (d = 0.5 cm or any other shape and size) are machine-cut and treated with a low concentration of PPTES in dichloromethane, while the remainder of the original GMF substrate is rendered superhydrophobic by reacting with octadecyltrimethoxysilane (OTMS). Following the reassembly of the device, the Cu(I)-catalyzed alkyne-azide cycloaddition (CuAAC)-based assay is performed by introducing A-7-HC in the presence of different concentrations of copper standards. Coupling with smartphone imaging under customized LED irradiation, we showed that the assay sites (discs) are distinct and uniform (free of coffee-ring effect); the achieved limits of detection (9.2 ± 0.8 ppb) for copper are impressive in comparison with traditionally prepared devices (drop-casting reagents on photolithographically patterned GMF/paper). As we have validated the device with the results obtained with atomic absorption spectroscopy of commercial copper diary supplements, this work reveals the potential of combining covalent surface modification with benchtop patterning techniques to create flexible μPADs for performing quantitative colorimetric and fluorometric assays.
This study explored konjac composite gel with hypoglycemic properties. Kudzu root resistant starch (KRS) was added to enhance the gel's characteristics. Single-factor and orthogonal experiments optimized preparation conditions, revealing an optimal process: konjac semolina: water is 1:40 (w/v), 90 degrees C, KRS 2.00 g, alkali 18 %, stirring for 45 min. The water-holding capacity of the konjac composite gel prepared by this process reached 90.22 %, which is 15.81 % higher than that of pure konjac gel (74.41 %). Characterization of the composite gel by SEM, texture profile analysis, and sensory evaluation confirmed its enhanced quality. The reinforced network structure fundamentally improved the composite gel's textural properties. Its hardness, springiness, and chewiness reached 2.4, 1.1, and 1.2 times those of native KGM, respectively, resulting in an optimized mouthfeel. In vitro gastrointestinal digestion simulations were performed to assess the digestibility of the composite gels. The starch hydrolysis rates of the konjac composite gel were 1.338 % and 9.688 %. The composite gel exhibited significant alpha-amylase and alpha-glucosidase inhibitory activities (IR = 55.84 % and 48.78 %), indicating its potential as a functional food for glycemic control.
Cucurbit[7]uril (CB[7]), which is highly favorable for binding ferrocene (Fc) derivatives in solution and on the surface, has stood out as a promising electrochemical sensing motif due to its readily quantifiable redox responses. Given that understanding the complexation between CB[7] and drug candidates or steroids is crucial for pharmaceutical and steroidal applications, we report herein our electrochemical investigation to quantitate the affinity between surface-bound CB[7] and nonredox-active guests through competitive binding against ferrocene methanol (FcMeOH). The immobilization of the supramolecular host relies on the formation of azide-terminated alkanethiolate self-assembled monolayers (SAMs) on gold and subsequent copper(I)-catalyzed azide-alkyne cycloaddition (CuAAC) with alkyne-modified CB[7]. By incubating FcMeOH and subsequently a drug/steroid molecule, the competitive binding between CB[7]@drug/steroid and CB[7]@ferrocene complexes on the surface can be quantified with cyclic voltammetry, despite the nonredox-active nature of drug or steroid compounds. The formation constants of CB[7]@drug/steroid complexes are obtained with high accuracy, and a quantitative assay method is developed by establishing a linear relationship between the electrochemical signal and the guest concentration. Not only are the determined binding constants consistent with the literature values from conventional instrumental analyses (e.g., HPLC), but the obtained limits of detection (LODs) are also remarkable (i.e., from sub to low mu M range).
In this work, we have developed a portable laser scanning imaging system derived from Blu-ray disc technology for high-throughput biochip and sensor array characterization. This portable imaging system was constructed by adapting a standard Blu-ray drive to perform the scanning or imaging of an entire disc or interested regions. In addition, we have compiled a complete operating software program to process the raw data, generate the assay image, and perform quantitative analysis. Furthermore, the developed BD-LSI system was successfully applied to the quantitative detection of Anti-M & uuml;llerian hormone (AMH), which is an important biomarker of reproductive potential, in standard physiological buffers and serum samples. The achieved detection limit is as low as 18 pg/ mL with a dynamic range of up to 25 ng/mL, which meets the needs of clinical diagnosis. As validated by comparing with the Clinical Laboratory Improvement Amendments (CLIA) data on the same set of samples, the consistent results confirm that this BD-LSI system holds promise for multiplex on-site quantitative analysis at community clinics and even at home settings for self-monitoring of individual health.
Kidney-Specific Delivery In article number 2309949, Jinbin Liu, Ruibing Wang, and co-workers develop a series of ultrasmall NIR-II emitting gold nanocarriers, allowing for fine-tuning liver or kidney-specific delivery via altering the surface chemistry using cucurbit[7]uril and Cys-Arg-Gly-Asp peptide. Accordingly, the selected ultrasmall nanocarriers could facilitate kidney-targeted delivery in acute kidney injury mice, which significantly boosts drug accumulation at the site of injured kidneys, thereby achieving improved therapeutic results.
Plant-derived antibacterial agents are increasingly pivotal in mitigating the escalating threat posed by pathogenic microorganisms. Dihydromyricetin (DMY), a plant bioactive compound prevalent in Ampelopsis grossedentata, exhibits remarkable antibacterial properties. However, its poor solubility in water significantly hinders its application in antibacterial therapies, necessitating the exploration of suitable carriers for the loading and sustained release of DMY. In this study, a chitosan-based hydrogel was rapidly synthesized at 25 °C using carboxymethyl chitosan and sodium alginate as precursors, and then utilized for the encapsulation of DMY. The as-prepared hydrogel was characterized using scanning electron microscopy, Fourier-transform infrared spectroscopy, and thermogravimetric analysis, indicating its favorable swelling properties, injectability, transparency, and self-healing capabilities. Antibacterial assays demonstrated that both surface and internal of the hydrogel exhibited over 99 % inhibition against both Pseudomonas aeruginosa and Staphylococcus aureus when the DMY loading concentration reached 0.4 mg/mL. Furthermore, drug release studies demonstrated that the hydrogel effectively sustained the release of DMY for up to 130 h, irrespective of the acidic or alkaline aqueous solutions, as well as in phosphate-buffered saline. These findings provide novel insights and references for the synergistic antibacterial application of plant-derived agents in conjunction with hydrogels.
We have systematically investigated and found surprising superior catalytic activities of very short DNAzymes for copper(I)-catalyzed azide-alkyne cycloaddition (CuAAC), both in solution and on surface. As a key reaction of the "click chemistry" class, CuAAC is a highly efficient and specific covalent conjugation tool with demonstrated applications in organic synthesis, bioconjugation, and surface functionalization; however, it requires the presence of the Cu(I) catalyst, which is an unstable species in aqueous solutions. We show here that one ultrashort, 14-nucleotide-truncated fragment of an earlier in vitro selected DNAzyme (CLICK-17) shows a striking and superior catalytic activity toward the in trans CuAAC reaction in solution and on surface in the presence of either Cu(I) or Cu(II), at significantly lowered concentrations. These results obviate the need for long-sequence DNAzymes, selected out of the homogeneous solution phase, for application in complex surface environments.
Acetalization serves as both a synthesis tool for renewable cyclic acetal fuel additives and a protection strategy to improve selectivity in biomass conversion.
Commercial pH paper is a quick and simple tool for measuring a solution's acidity/basicity, but it only provides qualitative or semi-quantitative results, and the synthetic indicator dyes within can be toxic or carcinogenic. Although pH meters enable more accurate and quantitative analysis, they are less convenient to operate and are tedious to calibrate. This presents a need for an alternative pH testing method for applications where it is not easy or possible to use a pH meter, yet quantitative results are desired. We report herein the fabrication of a pH test strip made from superhydrophobic paper and agarose-anthocyanin film discs. In the proposed method, test strips are dipped into samples and then imaged with a portable scanner (or a smartphone). The color of the film is extracted with ImageJ software (or a mobile app), using the RGB color system. By generating a calibration curve relating the film color to the sample pH using standard buffer solutions, we are able to quantify the pH of beverages and other liquids with an accuracy and precision comparable to that of a pH meter. The test strips offer the same convenience as conventional pH paper, with the added capabilities of quantitation and multiplexed testing, which presents a practical tool for point-of-need pH analysis.
A microanalytical technique based on the photothermal effect in conjunction with back-scattering interferometry (BSI) using a single laser beam was developed for quantitative detection of heavy metals. After the chromogenic reaction of an analyte in a capillary tube, the photothermal effect induced by irradiation with the same laser beam leads to a change of the refractive index of the solution, which can be "quantified" using the BSI technique. For prove-of-concept, Cu(II) was chosen as the trial analyte, for which the solution changes to purplish through reacting with the chromogenic reagent; a single laser beam of 532 nm was adapted for both inducing the photothermal effect and realizing BSI detection. With as little as 1.0 μL solution, a limit of detection (LOD) of 0.10 mg/L for Cu(II) was achieved. In addition, the versatility of the technique was demonstrated by detecting other two heavy metal ions, Fe(II) and Cr(VI), with limits of detection of 0.06 mg/L and 0.04 mg/L, respectively. The demonstrated detection sensitivity, application versatility, and instrumentation simplicity of this new technique promises it as a practical tool for environmental monitoring and beyond.
The effect of molecular dipoles on charge transport across organic monolayer-modified metal-semiconductor junctions has been investigated systematically. We have prepared a new set of organic monolayers with varied terminal derivatization on crystalline silicon to construct molecular junctions using mercury drops as the top contact electrode. Although the surface and structural characterization indicated the high quality and uniformity of all these monolayers, the junctions (Hg/R-Si-) showed a diverse electrical performance. Beyond taking the most common theoretical approach to analyze these molecular junctions, that is, applying the thermionic emission model (TE) to calculate the barrier height (phi B) and ideality factor (eta), we have examined the contribution of the carrier generation-recombination (CGR) mechanism by fitting the experimental current-voltage curves. When eta is close to unity, the charge transport across these molecular junctions is dominated by TE; for eta values greater than unity, TE indeed remains the dominant current transport pathway, while CGR transport becomes significant.
Inorganic antibacterial nanomaterials play an increasingly important role in addressing the growing threat of drug-resistant bacteria. Graphene oxide-silver nanoparticles composite (GO-AgNPs), as a kind of inorganic nanomaterials, have excellent antibacterial properties, showing promising potential in biomedical field. However, GO-AgNPs are terribly prone to sedimentation due to aggregation in physiological solutions, along with its non-environmental issues during the synthesis process, seriously limits the antibacterial application of GO-AgNPs in the biomedical field. To solve this problem, herein, polyethylene glycol-graphene oxide-silver nanoparticles composite (GO-AgNPs-PEG) were prepared by modifying GO-AgNPs with polyethylene glycol to enhance their dispersion stability in physiological solutions. In addition, GO-AgNPs-PEG were prepared with using the natural product gallic acid as a reductant and stabilizer, exhibiting the characteristic of environmentally friendly. Meanwhile, the dispersion stability and antibacterial activity of GO-AgNPs-PEG were characterized by various technical methods, it was found that GO-AgNPs-PEG can be stably dispersed in a variety of physiological solutions (e.g., physiological saline, phosphate buffer solution, Luria-Bertani medium, Murashige and Skoog medium) for more than one week. Moreover, the antibacterial properties of GO-AgNPs-PEG in physiological solutions were significantly better than those of GO-AgNPs. Furthermore, it was discovered that the antibacterial mechanism of GO-AgNPs-PEG was probably associated to destroying the integrity of bacterial cell walls and membranes. The findings in this work can provide new ideas and references for the development of new inorganic antibacterial nanomaterials with stable dispersion in physiological solutions.
Herein, a smartphone-based portable reader with integrated optics for standard microtiter plates (96 wells) has been designed and demonstrated for high-throughput quantitation of validated biomarkers in serum. The customized optical attachment was simply constructed with a convex lens and a light source, by which the transmitted light through a 96-well microtiter plate was converged for imaging with a smartphone, so that accurate and wide-range reading of the plate can be achieved. More importantly, relying on the digitized colorimetric analysis of the obtained images, concentrations of various biomarkers can be determined directly using the customized mobile app. A set of validated biomarkers for inflammation and infection, C-reactive protein (CRP), serum amyloid A (SAA), and procalcitonin (PCT) have been quantitated with this new system; both the response ranges and limits of detection meet the requirement of clinical tests. The consistency with the results obtained using a commercial microplate reader proves its reliability and precision, augments its potential as a point-of-care diagnostic device for on-site testing or resource-limited settings.
pH determination and acid-base titrations areessentialexperiments performed by high school and university undergraduatestudents alike throughout their chemistry education. While these experimentsoften rely on conventional pH meters for quantification and pH teststrips or indicators for qualitative assessments, we demonstratedherein that a smartphone-based pH determination technique, performingdigital image analysis, particularly the determination of either thedominant wavelength or the RGB intensities, could readily replaceall but one conventional pH meter in a classroom setting. Using anin-house developed smartphone-based pH reading application (app),students were able to determine the pH and perform titrations usingpH strips and universal indicators, producing results matching thosedetermined with a standard pH meter. The app and its "variants"are available for download (https://tinyurl.com/2dashjyk and https://tinyurl.com/4d73wnxt), and no prior knowledge of coding or programing was required fromthe students. All that was needed was an Android 11 phone or tabletwith an Internet connection. Moreover, the students and instructors'reactions to the mobile app alike were very positive and showcasedthe need and interest for such inexpensive technology, which allowsfor the running of an entire class for pH determination of multiplereal-life samples or acid/base titration without using standard pHmeters.