NIR-II Imaging and Sandwiched Plasmonic Biosensor for Ultrasensitive Intraoperative Definition of Tumor-Invaded Lymph Nodes.

Radical lymphadenectomy remains the cornerstone of preventing tumor metastasis through the lymphatic system. Current surgical resection of lymph nodes (LNs) based on fluorescence-guided surgery (FGS) suffers from low sensitivity/selectivity with only qualitative information, hampering accurate intraoperative decision-making. Herein, we develop a modularized theranostic system including NIR-II FGS and a sandwiched plasmonic chip (SPC). Intraoperative NIR-II FGS and detection of tumor-positive lymph nodes were performed on the gastric tumor to determine the feasibility of the modularized theranostic system in defining LN metastasis. Under the NIR-II imaging window, the orthotopic tumor and sentinel lymph nodes (SLNs) were successfully excised without ambient light interference in the operating room. Importantly, the SPC biosensor achieved 100% sensitivity and 100% specificity for tumor markers and realized rapid and high-throughput intraoperative SLN detection. We propose the synergetic design of combining the NIR-II FGS and suitable biosensor will substantially improve the efficiency of cancer diagnosis and therapy follow-up.

Three-Dimensional Histological Electrophoresis for High-Throughput Cancer Margin Detection in Multiple Types of Tumor Specimens.

Accurate identification of tumor margins during cancer surgeries relies on a rapid detection technique that can perform high-throughput detection of multiple suspected tumor lesions at the same time. Unfortunately, the conventional histopathological analysis of frozen tissue sections, which is considered the gold standard, often demonstrates considerable variability, especially in many regions without adequate access to trained pathologists. Therefore, there is a clinical need for a multitumor-suitable complementary tool that can accurately and high-throughput assess tumor margins in every direction within the surgically resected tissue. We herein describe a high-throughput three-dimensional (3D) histological electrophoresis device that uses tumor-specific proteins to identify and contour tumor margins intraoperatively. Testing on seven cell-line xenograft models and human cervical cancer models (representing five types of tissues) demonstrated the high-throughput detection utility of this approach. We anticipate that the 3D histological electrophoresis device will improve the accuracy and efficiency of diagnosing a wide range of cancers.

Naked-Eye Readable Microarray for Rapid Profiling of Antibodies against Multiple SARS-CoV-2 Variants.

Novel high-throughput protein detection technologies are critically needed for population-based large-scale SARS-CoV-2 antibody detection as well as for monitoring quality and duration of immunity against virus variants. Current protein microarray techniques rely heavily on labeled transduction methods that require sophisticated instruments and complex operations, limiting their clinical potential, particularly for point-of-care (POC) applications. Here, we developed a label-free and naked-eye readable microarray (NRM) based on a thickness-sensing plasmon ruler, enabling antibody profiling within 30 min. The NRM chips provide 100% accuracy for neutralizing antibody detection by efficiently screening antigen types and experimental conditions and allow for the profiling of antibodies against multiple SARS-CoV-2 variants in clinical samples. We further established a flexible "barcode" NRM assay with a simple tape-based operation, enabling an effective smartphone-based readout and analysis. These results demonstrate new strategies for high-throughput protein detection and highlight the potential of novel protein microarray techniques for realistic clinical applications.

Reinforced Blood-Derived Protein Hydrogels Enable Dual-Level Regulation of Bio-Physiochemical Microenvironments for Personalized Bone Regeneration with Remarkable Enhanced Efficacy.

Physiological microenvironment engineering has shown great promise in combating a variety of diseases. Herein, we present the rational design of reinforced and injectable blood-derived protein hydrogels (PDA@SiO2-PRF) composed of platelet-rich fibrin (PRF), polydopamine (PDA), and SiO2 nanofibers that can act as dual-level regulators to engineer the microenvironment for personalized bone regeneration with high efficacy. From the biophysical level, PDA@SiO2-PRF with high stiffness can withstand the external loading and maintaining the space for bone regeneration in bone defects. Particularly, the reinforced structure of PDA@SiO2-PRF provides bone extracellular matrix (ECM)-like functions to stimulate osteoblast differentiation via Yes-associated protein (YAP) signaling pathway. From the biochemical level, the PDA component in PDA@SiO2-PRF hinders the fast degradation of PRF to release autologous growth factors in a sustained manner, providing sustained osteogenesis capacity. Overall, the present study offers a dual-level strategy for personalized bone regeneration by engineering the biophysiochemical microenvironment to realize enhanced osteogenesis efficacy.

Ultrabright Renal-Clearable Cyanine-Protein Nanoprobes for High-Quality NIR-II Angiography and Lymphography.

The renal-clearable aspect of imaging agent with minimum toxicity issues and side effects is essential for clinical translation, yet clinical near-infrared-I/II (NIR-I/II) fluorophores with timely renal-clearance pathways are very limited. Herein, we rationally develop the cyanine-protein composite strategy through covalent bonding of ß-lactoglobulin (ß-LG) and chloride-cyanine dye to produce a brilliant and stable NIR-I/II fluorophore (e.g., ß-LG@IR-780). The ß-LG acts as a protecting shell with small molecular weight (18.4 kDa) and ultrasmall size (<5 nm), thus endowing the ß-LG@IR-780 with excellent biocompatibility and renal excretion. Our ß-LG@IR-780 probe enables noninvasive and precise NIR-II visualization of the physiological and pathological conditions of the vascular and lymphatic drainage system, facilitating intraoperative imaging-guided surgery and postoperative noninvasive monitoring. The minimum accumulation of our probes in the main organs improves the overall biosafety. This study provides a facile methodology for new-generation NIR-II fluorophores and largely improves the brightness and pharmacokinetics of small molecular dyes.

Thickness-Sensing Sandwiched Plasmonic Biosensors Enable Label-Free Naked-Eye Antibody Quantification.

Clinical serology assays for detecting the antibodies of the virus are time-consuming, are less sensitive/selective, or rely on sophisticated detection instruments. Here, we develop a sandwiched plasmonic biosensor (SPB) for supersensitive thickness-sensing via utilizing the distance-dependent electromagnetic coupling in sandwiched plasmonic nanostructures. SPBs quantitatively amplify the thickness changes on the nanoscale range (sensitivity: ∼2% nm-1) into macroscopically visible signals, thereby enabling the rapid, label-free, and naked-eye detection of targeted biomolecular species (via the thickness change caused by immunobinding events). As a proof of concept, this assay affords a broad dynamic range (7 orders of magnitude) and a low LOD (∼0.3 pM), allowing for the extremely accurate SARS-CoV-2 antibody quantification (sensitivity/specificity: 100%/∼99%, with a portable optical fiber device). This strategy is suitable for high-throughput multiplexed detection and smartphone-based sensing at the point-of-care, which can be expanded for various sensing applications beyond the fields of viral infections and vaccination.

Co-occurrence of Moyamoya syndrome and Kartagener syndrome caused by the mutation of DNAH5 and DNAH11: a case report.

BACKGROUND: Kartagener syndrome is an autosomal recessive inherited disorder of primary ciliary dyskinesia. Moyamoya syndrome refers to a moyamoya angiopathy associated with other neurological and/or extra-neurological symptoms, or due to a well identified acquired or inherited cause. We herein reported a case of a 48-year-old woman who was favored the diagnosis of Kartagener syndrome and moyamoya syndrome. The whole genome sequencing and bioinformatics analysis showed a homozygotic nonsense mutation in the dynein, axonemal, heavy chain (DNAH) 5 gene, and heterozygotic missense mutation in the DNAH11 gene. This is the first report of the co-occurrence of the two rare diseases. CASE PRESENTATION: A case of a 48-year-old woman was presented with hemiplegia and slurred speech. The magnetic resonance imaging of the brain confirmed acute cerebral infarction in the right basal ganglia region, semi-oval center, insular lobe, and frontal parietal lobe. The electrocardiogram showed inverted "P" waves in L1 and AVL on left-sided chest leads and computed tomography scan of the chest showed bronchiectasis changes, cardiac shadow and apex on the right side, and situs inversus of aortic arch position. The digital subtraction angiography showed inversion of the aortic arch, and bilateral internal carotid arteries are occluded from the ophthalmic segment. The clinical, radiological, and laboratory findings made the diagnosis of Kartagener syndrome and moyamoya syndrome. The whole genome sequencing and bioinformatics analysis showed a homozygotic nonsense mutation in DNAH5 gene, and heterozygotic missense mutation in the DNAH11 gene. CONCLUSION: The combined mutation of DNAH5 and DNAH11 may lead to the overlapping dysfunction of motile and nonmotile cilia, which contribute to the co-occurrence of Kartagener syndrome and moyamoya syndrome. Our report deserves further confirm by more case reports.

Enhanced High-Temperature Dielectric Properties of Poly(aryl ether sulfone)/BaTiO3 Nanocomposites via Constructing Chemical Crosslinked Networks.

Heat-resistant and crosslinked polymers/ceramic composites have been prepared and investigated for enhancing high-temperature dielectric properties to adapt the development of advanced electric and electronic systems. Here, a series of crosslinkable heat-resistant poly(arylene ether sulfone)s (DPAES) with large dipole units of -SO2 - are designed and synthesized as matrix, which are blended with BaTiO3 (BT) nanoparticles to fabricate crosslinked polymer composites for boosting high-temperature dielectric properties. The results show that BT/c-DPAES possess great dielectric stability at measured frequency and temperature. Meanwhile, the discharged energy density and efficiency of BT/c-DPAES composites are higher than that of BT/DPAES at high temperatures, e.g., 10 vol% BT/c-DPAES has a discharged energy density of 1.7 J cm-3 and efficiency of 73%, increasing by 42% and 128% in contrast to BT/DPAES, respectively. The enhanced high-temperature energy storage properties can be attributed to the construction of a crosslinked polymer network, reducing leakage current density of composites.

A Flexible Polymer Nanofiber-Gold Nanoparticle Composite Film for Solar-Thermal Seawater Desalination.

Interfacial solar-thermal conversion has broad application prospects in solar driven steam generation, seawater desalination, sewage purification, and other fields. For a wide range of applications, high-efficiency interfacial solar-thermal conversion materials with the feature of being lightweight, flexible, and easy to scale up at the same time are significantly valued. Herein, a strategy for the preparation of solar-thermal poly (4-vinylpyridine) (P4VP) nanofiber-gold nanoparticle (Au NP) composite film (PGCF) is reported. Combining with the flexible and lightweight P4VP nanofibers, these absorbed Au NPs enable better solar-thermal conversion efficiency. Accordingly, the PGCF provides high-performance interfacial solar-driven steam generation, with 77% solar-heat conversion efficiency under the power density of 3.4 kW m-2 , which shows stable output (3.4 kg m-2 h-1 ) in the application of solar-driven seawater desalination. In addition, PGCF is light in weight, flexible, and suitable for scalable commercial production, enabling PGCF broad application prospects in the field of light-to-heat conversion.

Effects of trisodium phosphate treatment after harvest on storage quality and sucrose metabolism in jujube fruit.

BACKGROUND: Trisodium phosphate (TSP), generally recognized as safe (GRAS), could control postharvest diseases and maintain fruit quality. However, changes of fruit quality and sucrose metabolism in harvested jujube after TSP treatment remain largely unknown. In the current study, jujube fruit (cv. sanxing) was used to study the effects of TSP on storage quality and sucrose metabolism during storage at 20 ± 2 °C with 40-50% relative humidity (RH). RESULTS: The results showed that 0.5 g L-1 TSP treatment reduced weight loss and reduced sugar content, suppressed the reduction of fruit firmness, maintained ascorbic acid (AsA) content and inhibited respiratory rate of jujube fruit. In addition, TSP treatment also reduced acid invertase (AI) and neutral invertase (NI) activities in sucrose metabolism in jujube fruit. Sucrose synthase-cleavage (SS-c), sucrose synthase-synthesis (SS-s) and sucrose phosphate synthase (SPS) activities were also suppressed by TSP treatment. CONCLUSION: Treatment with TSP could effectively reduce enzymes activities in sucrose metabolism and maintain storage quality of jujube fruit during storage. © 2019 Society of Chemical Industry.

Ordered Micro/Nanostructures with Geometric Gradient: From Integrated Wettability "Library" to Anisotropic Wetting Surface.

Geometric gradients within ordered micro/nanostructures exhibit unique wetting properties. Well-defined and ordered microsphere arrays with geometric gradient (OMAGG) are successfully fabricated through combining colloidal lithography and inclined reactive ion etching (RIE). During the inclined RIE, the graded etching rates in vertical direction of etcher chamber are the key to generating a geometric gradient. The OMAGG can be used as an effective mask for the preparation of micro/nanostructure arrays with geometric gradient by selective RIE. Through this strategy, a well-defined wettability "library" with graded silicon cone arrays is fabricated, and the possibility of screening one desired "book" from the designated wettability "library" is demonstrated. Meanwhile, the silicon cone arrays with geometric gradient (SCAGG) can be applied to control the wetting behavior of water after being modified by hydrophilic or hydrophobic chemical groups. Based on this result, a temperature-responsive wetting substrate is fabricated by modifying poly n-isopropyl acrylamide (PNIPAM) on the SCAGG. These wettability gradients have great potential in tissue engineering, microfluidic devices, and integrated sensors.

Autonomous Control of Fluids in a Wide Surface Tension Range in Microfluidics.

In this paper, we report the preparation of anisotropic wetting surfaces that could control various wetting behaviors of liquids in a wide surface tension range (from water to oil), which could be employed as a platform for controlling the flow of liquids in microfluidics (MFs). The anisotropic wetting surfaces are chemistry-asymmetric "Janus" silicon cylinder arrays, which are fabricated via selecting and regulating the functional groups on the surface of each cylinder unit. Liquids (in a wide surface tension range) wet in a unidirectional manner along the direction that was modified by the group with large surface energy. Through introducing the Janus structure into a T-shaped pattern and integrating it with an identical T-shaped poly(dimethylsiloxane) microchannel, the as-prepared chips can be utilized to perform as a surface tension admeasuring apparatus or a one-way valve for liquids in a wide surface tension range, even oil. Furthermore, because of the excellent ability in controlling the flowing behavior of liquids in a wide surface tension range in an open system or a microchannel, the anisotropic wetting surfaces are potential candidates to be applied both in open MFs and conventional MFs, which would broaden the application fields of MFs.

Unidirectional Wetting of Liquids on "Janus" Nanostructure Arrays under Various Media.

We report the unidirectional wetting behavior of liquids (water and oil) on Janus silicon cylinder arrays (Si-CAs) under various media (air, water, and oil). The Janus cylinders were prepared by chemical modification of nanocylinders with different molecules on two sides. Through adjusting surface energies of the modified molecules, the as-prepared surfaces could control the wetting behavior of different types of liquids under various media. We discuss the regularity systematically and propose a strategy for preparing anisotropic wetting surfaces under arbitrary media. That is, to find two surface modification molecules with different surface energies, one of the molecules is easy to be wetted by the liquid under the corresponding media, while the other one is difficult. Additionally, by introducing thermal-responsive polymer brushes onto one part of Janus Si-CAs, the surfaces show thermal-responsive anisotropic wetting property under various media. We believe that due to the excellent unidirectional wettability under various media, the Janus surfaces could be applied in water/oil transportation, oil-repellent and self-cleaning coatings, water/oil separation, microfluidics, and so on.

Thermal-Responsive Anisotropic Wetting Microstructures for Manipulation of Fluids in Microfluidics.

We show morphology-patterned stripes modified by thermal-responsive polymer for smartly guiding flow motion of fluid in chips. With a two-step modification process, we fabricated PNIPAAm-modified Si stripes on silicon slides, which were employed as substrates for fluid manipulation in microchannels. When the system temperature switches between above and below the lower critical solution temperature (LCST) of PNIPAAm, the wettability of the substrates also switches between strong anisotropy and weak anisotropy, which resulted in anisotropic (even unidirectional) flow and isotropic flow behavior of liquid in microchannels. The thermal-responsive flow motion of fluid in the chip is influenced by the applied pressure, the thickness of PNIPAAm, and dimension of the microchannels. Moreover, we measured the feasible applied pressure scopes under different structure factors. Because of the excellent reversibility and quick switching speed, the chip could be used as a thermal-responsive microvalve. Through tuning the system temperature and adding the assistant gas, we realized successive "valve" function. We believe that the practical and simple chip could be widely utilized in medical detection, immunodetection, protein analysis, and cell cultures.

Wrinkled single-layer graphenes fabricated by silicon nanopillar arrays.

The degree of crumpling affects the optoelectronic properties of graphene, which are very important for the performance of graphene-based devices and materials. In this article, we report an approach to tune the formation of wrinkles on single-layer graphene (SLG) by silicon nanopillar (SNP) arrays. By using gold nanoparticles as an etching mask, SNP arrays with different heights could be prepared by tuning the duration of etching. The formation of wrinkles on these SNP arrays was studied systematically. We found that thermal treatment could lead to a wrapping behavior of graphene around SNP arrays, which was accompanied by the emergence of many more wrinkles. Controllable wettability, conductivity and transmittance were demonstrated. This ability to tune wrinkles using SNP arrays can be employed to engineer the fabrication of graphene-related devices and other optoelectronic applications.

Controlling flow behavior of water in microfluidics with a chemically patterned anisotropic wetting surface.

We report the flow behavior of water in microfluidic systems based on a chemically patterned anisotropic wetting surface. When water flows inside a microchannel on top of a micropatterned surface with alternating hydrophilic/hydrophobic stripes, it exhibits an anisotropic flowing characteristic owing to the anisotropic wettability; thus, the patterned surface acts as a microvalve for the microfluidic system. The anisotropic flow of water is influenced by the microscale features of the patterns and the dimensions of the microchannels. Furthermore, by reasonably combining the patterned surface and microchannel together, we realize the transportation of water in a microchannel along a "virtual" wall, which is the boundary of the hydrophilic and hydrophobic area. We believe that the chemically patterned surfaces could be an alternative strategy to control the flow behavior of water in microfluidic channels.

Responsive etalon based on PNIPAM@SiO2 composite spacer with rapid response rate and excellent repeatability for sensing application.

In this paper, we demonstrate a responsive etalon fabricated through combining colloidal lithography and surface-initiated atom-transfer radical polymerization (SI-ATRP). The responsive etalon is simply constructed with one responsive spacer sandwiched by two reflective layers, and the middle responsive spacer is constructed by grafting thermo-responsive poly(N-isopropylacrylamide) (PNIPAM) brushes on a SiO2 nanosphere array. The etalon possesses one single interference peak in the visible region, and the interference peak changes sensitively against the concentration of the external stimulant (water vapor) or the temperature of the system, owing to the responsiveness of the PNIPAM brush. Importantly, the as-prepared etalon shows a rapid response rate and excellent stability, and it is also handy to realize the miniaturization and integration of the responsive etalon based on a conventional micro-fabrication method. These features all make the as-prepared responsive etalon an attractive candidate for future sensing applications. We believe such responsive etalons are promising for the fabrication of smart photonic materials and optical sensors that may be useful in tissue engineering, medical diagnosis, public security, and biochip areas.

Bioinspired multifunctional vanadium dioxide: improved thermochromism and hydrophobicity.

Vanadium dioxide (VO2) films with moth-eye nanostructures have been fabricated to enhance the thermochromic properties with different periodicity (d) to achieve antireflection (AR). It is revealed that the films with smaller d (210 and 440 nm) could increase both the luminous transmission (Tlum) and infrared transmission (TIR) at 25 and 90 °C, as the d is smaller than the given wavelength and the gradient refractive index produces antireflection. The average Tlum and TIR of VO2 increase with decreasing d. Compared with the planar film, the AR sample with periodicity of 210 nm and thickness of 140 nm can offer approximately 10% enhancement of Tlum and 24.5% increase in solar modulation (ΔTsol). With the addition of hydrophobic overcoat on the patterned VO2, ∼120° contact angle could be achieved. The present approach can tailor the optical transmittance in different wavelengths at high and low temperature together with self-cleaning, opening new avenues for producing hydrophobic VO2 with enhanced thermochromic properties for smart window applications.

A Hemoglobin Bionics-Based System for Combating Antibiotic Resistance in Chronic Diabetic Wounds via Iron Homeostasis Regulation.

Owing to the increased tissue iron accumulation in patients with diabetes, microorganisms may activate high expression of iron-involved metabolic pathways, leading to the exacerbation of bacterial infections and disruption of systemic glucose metabolism. Therefore, an on-demand transdermal dosing approach that utilizes iron homeostasis regulation to combat antimicrobial resistance is a promising strategy to address the challenges associated with low administration bioavailability and high antibiotic resistance in treating infected diabetic wounds. Here, it is aimed to propose an effective therapy based on hemoglobin bionics to induce disturbances in bacterial iron homeostasis. The preferred "iron cargo" is synthesized by protoporphyrin IX chelated with dopamine and gallium (PDGa), and is delivered via a glucose/pH-responsive microneedle bandage (PDGa@GMB). The PDGa@GMB downregulates the expression levels of the iron uptake regulator (Fur) and the peroxide response regulator (perR) in Staphylococcus aureus, leading to iron nutrient starvation and oxidative stress, ultimately suppressing iron-dependent bacterial activities. Consequently, PDGa@GMB demonstrates insusceptibility to genetic resistance while maintaining sustainable antimicrobial effects (>90%) against resistant strains of both S. aureus and E. coli, and accelerates tissue recovery (<20 d). Overall, PDGa@GMB not only counteracts antibiotic resistance but also holds tremendous potential in mediating microbial-host crosstalk, synergistically attenuating pathogen virulence and pathogenicity.

Cation-π interactions enabled water-stable perovskite X-ray flat mini-panel imager.

Sensitive and stable perovskite X-ray detectors are attractive in low-dosage medical examinations. The high sensitivity, tunable chemical compositions, electronic dimensions, and low-cost raw materials make perovskites promising next-generation semiconductors. However, their ionic nature brings serious concerns about their chemical and water stability, limiting their applications in well-established technologies like crystal polishing, micro-processing, photolithography, etc. Herein we report a one-dimensional tryptamine lead iodide perovskite, which is stable in water for several months as the strong cation-π interactions between organic cations. The one-dimensional and two-dimensional tryptamine lead iodide perovskite tablets are switchable through thermal-annealing or water-soaking treatments to relax microstrains. The water-stable and microstrain-free one-dimensional perovskite tablets yield a large sensitivity of 2.5 × 106 µC Gyair-1 cm-2 with the lowest detectable dose rate of 5 nGyair s-1. Microelectrode arrays are realized by surface photolithography to construct high-performance X-ray flat mini-panels with good X-ray imaging capability, and a record spatial resolution of 17.2 lp mm-1 is demonstrated.