Enhanced Label-Free Photoelectrochemical Strategy for Pollutant Detection: Using Surface Oxygen Vacancies-Enriched BiVO4 Photoanode.

Label-free photoelectrochemical sensors have the advantages of high sensitivity and a simple electrode structure. However, its performance is greatly limited due to the photoactive materials' weak photoactivity and poor stability. Herein, a robust homogeneous photoelectrochemical (PEC) aptasensor has been constructed for atrazine (ATZ) based on photoetching (PE) surface oxygen vacancies (Ov)-enriched Bismuth vanadate (BiVO4) (PE-BVO). The surface of the Ov improves the carrier separation ability of BiVO4, thus providing a superior signal substrate for the sensor. A thiol molecular layer self-assembled on PE-BVO acts as a blocker, while 2D graphene acts as a signal-on probe after release from the aptamer-graphene complex. The fabricated sensor has a wide linear detection range of 0.5 pM to 10.0 nM and a low detection limit of 0.34 pM (S/N = 3) for ATZ. In addition, it can efficiently work in a wide pH range (3-13) and high ionic strength (∼6 M Na+), which provides promising opportunities for detecting environmental pollutants under complex conditions.

Central China as LGM plant refugia: Insights from biome reconstruction for palaeoclimate information.

The demonstration of survival of forest stands in relatively stable refugia during cold glacial stages has offered an increased understanding of the response of vegetation to climate change, but also provides insight into considerations for the conversation of biodiversity hotspots. However, refugia studies in China remain in question due to the lack of plant macrofossils, especially those of endemic and relict species. Palynology, while more broad brush, provides a method for exploring whether refugia occur, and can provide some details of palaeovegetation composition and temporal dynamics. Here, three pollen records derived from subalpine wetlands in central China, spanning the Last Glacial Maximum (LGM), have been coupled with biome and mean annual precipitation (MAP) reconstructions to identify the presence of trees that endured cold climate. The results indicated that some forest, including temperate deciduous broadleaf forest and cool mixed forest, survived the LGM at the three locations, and was thus at odds with the hypothesis that forests were replaced by herbs and grasses in central China at that time. Refugia favored by protection from cold air drainage and the availability of adequate water can explain the survival of the trees during otherwise harsh episodes. Our findings are consistent with other records from central China that argue for tree dominated refugia during the LGM.

Microfluidic Chip-Assisted Upconversion Luminescence Biosensing Platform for Point-of-Care Virus Diagnostics.

Epidemics caused by multiple viruses continue to emerge, which have brought a terrible impact on human society. Identification of viral infections with high sensitivity and portability is of significant importance for the screening and management of diseases caused by viruses. Herein, a microfluidic chip (MFC)-assisted upconversion luminescence biosensing platform is designed and fabricated for point-of-care virus detection. Upconversion nanoparticles with excellent stability are successfully synthesized as luminescent agents for optical signal generation in the portable virus diagnostic platform. The relevant investigation results illustrate that the MFC-assisted virus diagnostic platform possesses outstanding performance such as good integration, high sensitivity (1.12 pg mL-1), ease of use, and portability. In addition, clinical sample test result verifies its more prominent virus diagnostic properties than commercially available rapid test strips. All of these thrilling capabilities imply that the designed portable virus diagnostic platform has great potential for future virus detection applications.

Generation and enhancement of the sum sideband under double radiation pressure.

A theoretical scheme to enhance the sum sideband generation (SSG) via double radiation pressure is proposed. In this scheme, both sides of the double-cavity system are driven by red and blue detuned pump lasers and frequency components are generated at the sum sideband through optomechanical nonlinear interaction. The results show that the efficiency of SSG can be improved with orders of magnitude. We further investigate the properties of SSG in resolved and unresolved sideband regimes. The efficiencies of upper sum sideband generation (USSG) and lower sum sideband generation (LSSG) are the equivalent in the unresolved sideband regime when the threshold condition is satisfied. It is worth noting that with the increase of the ratio between the dissipation rate of the cavity field and the decay rate of the mechanical resonator (MR), the amplitude of the LSSG can be superior to that of the USSG. Our scheme may provide a potential application in realizing the measurement of high-precision weak forces and quantum-sensitive sensing.

Rapid point-of-care detection of SARS-CoV-2 RNA with smartphone-based upconversion luminescence diagnostics.

Accurate COVID-19 screening via molecular technologies is still hampered by bulky instrumentation, complicated procedure, high cost, lengthy testing time, and the need for specialized personnel. Herein, we develop point-of-care upconversion luminescence diagnostics (PULD), and a streamlined smartphone-based portable platform facilitated by a ready-to-use assay for rapid SARS-CoV-2 nucleocapsid (N) gene testing. With the complementary oligo-modified upconversion nanoprobes and gold nanoprobes specifically hybridized with the target N gene, the luminescence resonance energy transfer effect leads to a quenching of fluorescence intensity that can be detected by the easy-to-use diagnostic system. A remarkable detection limit of 11.46 fM is achieved in this diagnostic platform without the need of target amplification, demonstrating high sensitivity and signal-to-noise ratio of the assay. The capability of the developed PULD is further assessed by probing 9 RT-qPCR-validated SARS-CoV-2 variant clinical samples (B.1.1.529/Omicron) within 20 min, producing reliable diagnostic results consistent with those obtained from a standard fluorescence spectrometer. Importantly, PULD is capable of identifying the positive COVID-19 samples with superior sensitivity and specificity, making it a promising front-line tool for rapid, high-throughput screening and infection control of COVID-19 or other infectious diseases.

A perspective from the past in conservation of plant biodiversity in central China.

Biodiversity has increasingly come under threat from human activity everywhere on Earth. China, with over 33,000 species of vascular plants, is a megadiverse region, in part because of its diversity in topography and climates. One of its most extensive biomes is broadleaved evergreen/warm mixed forest which dominates eastern Asia and Central China. There is some debate about how glacial/interglacial cycles across the Quaternary had an impact on this biome. There were certainly broad scale changes in distribution of many key species. Here, we examine the four palaeoecological records from Central China that contain both LGM and Mid-Holocene vegetation records and consider the degree of biodiversity in Central China with the aim of developing a broad overview of the history on plants in the region. It is clear that in the mountainous regions of Central China, many taxa survived the LGM in situ, showing that there was enough stable habitat to support key species. Some mountainous areas have high degrees of endemism which suggests that fragmentation of populations across glacial/interglacial cycles may have been an important component in favoring speciation. The consideration of past records and modern species distributions have significance in selecting conservation areas.

Multiplexed detection of SARS-CoV-2 based on upconversion luminescence nanoprobe/MXene biosensing platform for COVID-19 point-of-care diagnostics.

Multiplexed detection is essential in biomedical sciences since it is more efficient and accurate than single-analyte detection. For an accurate early diagnosis of COVID-19, a multiplexed detection strategy is required to avoid false negatives with the existing gold standard assay. Nb2CTx nanosheets were found to efficiently quench the fluorescence emission of lanthanide-doped upconversion luminescence nanoparticles at wavelengths ranging from visible to near-infrared spectrum. Using this broad-spectrum quencher, we developed a label-free FRET-based biosensor for rapid and accurate detection of SARS-CoV-2 RNA. To target ORF and N genes, two types of oligo-modified lanthanide-doped upconversion nanoparticles can be used simultaneously to identify-two sites in one assay via upconversion fluorescence enhancement intensity measurement with detection limits of 15 pM and 914 pM, respectively. Moreover, with multisite cross-validation, this multiplexed and sensitive biosensor is capable of simultaneous and multicolor analysis of two gene fragments of SARS-CoV-2 Omicron variant within minutes in a single homogeneous solution, which significantly improves the detection efficiency. The diagnosis result via our assay is consistent with the PCR result, demonstrating its application in the rapid and accurate screening of multiple genes of SARS-CoV-2 and other infectious diseases.

Rapid and ultrasensitive detection of SARS-CoV-2 spike protein based on upconversion luminescence biosensor for COVID-19 point-of-care diagnostics.

Here, we firstly introduce a detection system consisting of upconversion nanoparticles (UCNPs) and Au nanorods (AuNRs) for an ultrasensitive, rapid, quantitative and on-site detection of SARS-CoV-2 spike (S) protein based on Förster resonance energy transfer (FRET) effect. Briefly, the UCNPs capture the S protein of lysed SARS-CoV-2 in the swabs and subsequently they are bound with the anti-S antibodies modified AuNRs, resulting in significant nonradiative transitions from UCNPs (donors) to AuNRs (acceptors) at 480 nm and 800 nm, respectively. Notably, the specific recognition and quantitation of S protein can be realized in minutes at 800 nm because of the low autofluorescence and high Yb-Tm energy transfer in upconversion process. Inspiringly, the limit of detection (LOD) of the S protein can reach down to 1.06 fg mL-1, while the recognition of nucleocapsid protein is also comparable with a commercial test kit in a shorter time (only 5 min). The established strategy is technically superior to those reported point-of-care biosensors in terms of detection time, cost, and sensitivity, which paves a new avenue for future on-site rapid viral screening and point-of-care diagnostics.

Self-powered aptasensor for picomole level pollutants based on a novel enzyme-free photofuel cell.

Atrazine (ATZ) is a highly toxic chlorine-containing aromatic structural triazine endocrine disruptor. Due to its chemical stability and electrochemical inertness, it is of great challenge and significance to establish a simple, portable, and in situ electrochemical sensor for ATZ. In the present work, a self-powered aptasensor (SPA) based on a novel enzyme-free photofuel cell (PFC) is successfully developed for ATZ for the first time. The designed SPA is constructed by the Ti-Fe-O nanotubes/nickel hydroxide (Ti-Fe-O NTs/Ni(OH)2) photoanode and Au/aptamer (Au/Apt) cathode, responsible for the spontaneous generation of electrons and specific recognition of ATZ, respectively. It is worth noting that Ti-Fe-O NTs on the photoanode can exhibit good visible-light absorption property, and modified Ni(OH)2 further enhances the photo-generated carrier separation and improves the output power generation of the SPA. The recognition is set at the cathode to ensure the detection of ATZ and the anti-interference ability. Under the separation mode, the constructed SPA has a high output power (390 µW cm-2), much better than most previous reports. It can further show specific recognition of ATZ with prominent sensitivity and a limit of detection (LOD) as low as 5.4 pM. Moreover, it has been applied to the real water sample analysis with satisfactory results. A promising self-powered sensing platform based on an enzyme-free PFC has therefore been provided for picomole level pollutants with high sensitivity and outstanding selectivity.

Advances in upconversion luminescence nanomaterial-based biosensor for virus diagnosis.

Various infectious viruses have been posing a major threat to global public health, especially SARS-CoV-2, which has already claimed more than six million lives up to now. Tremendous efforts have been made to develop effective techniques for rapid and reliable pathogen detection. The unique characteristics of upconversion nanoparticles (UCNPs) pose numerous advantages when employed in biosensors, and they are a promising candidate for virus detection. Herein, this Review will discuss the recent advancement in the UCNP-based biosensors for virus and biomarkers detection. We summarize four basic principles that guide the design of UCNP-based biosensors, which are utilized with luminescent or electric responses as output signals. These strategies under fundamental mechanisms facilitate the enhancement of the sensitivity of UCNP-based biosensors. Moreover, a detailed discussion and benefits of applying UCNP in various virus bioassays will be presented. We will also address some obstacles in these detection techniques and suggest routes for progress in the field. These progressions will undoubtedly pose UCNP-based biosensors in a prominent position for providing a convenient, alternative approach to virus detection.

One-Step, DNA-Programmed, and Flash Synthesis of Anisotropic Noble Metal Nanostructures on MXene.

Precise morphological control over anisotropic noble metal nanoparticles (ANPs) is one of the key issues in the nano-research field owing to their unique optoelectronic, magnetic, mechanical, and catalytic properties. Although nanostructures fabricated by the directed assembly of adsorbate have been widely demonstrated recently, facile yet universal synthesis of nanocrystal with tunable morphologies, green templates, no seeds, and high yield remains challenging. Herein, we develop a versatile method, allowing for the rapid, one-step, seedless, surfactant-free synthesis of a noble metal nanostructure with tunable anisotropy on MXene in a sequence-dependent manner through a single-DNA molecular regulator. Based on the mild reducibility of MXene and the selective affinity of the DNA to the specific facets in the crystals, oriented aggregations and the growth of ANPs (Au, Pt, Pd) can be achieved and the resulting asymmetric morphology from polyhedrons, or flowers, or nanoplates to dendrites is observed. The ability to align such ANPs on the MXene surface is expected to lead to improved photothermal effect and surface-enhanced Raman scattering. Furthermore, our work makes the fabrication of the ANPs or ANP-MXene heterostructure easier, stimulating further explorations of physical, chemical, and biological applications.

Enzyme-Free Molecularly Imprinted and Graphene-Functionalized Photoelectrochemical Sensor Platform for Pollutants.

In this work, a label-free nonenzymatic photoelectrochemical (PEC) sensor is successfully developed for the detection of a typical pollutant, microcystin-LR (MC-LR), based on a visible-light-responsive alloy oxide, with highly ordered and vertically aligned Ti-Fe-O nanotubes (NTs) as substrates. Ti-Fe-O NTs consisting mainly of TiO2 and atomically doped Fe2O3 are in situ prepared on a Ti-Fe alloy by electrochemical anodic oxidation. Using a simple electrochemical deposition technique, reduced graphene oxide (RGO) could be grown onto Ti-Fe-O NTs, exhibiting significant bifunctions. It not only provides an ideal microenvironment for functionalization of molecularly imprinted polymers (MIPs) on the surface but also serves as the PEC signal amplification element because of its outstanding conductivity for photons and electrons. The designed MIP/RGO/Ti-Fe-O NT PEC sensor exhibits high sensitivity toward MC-LR with a limit of detection as low as 10 pM. High selectivity toward MC-LR is also proven for the sensor. A promising detection platform not only for MC-LR but also for other pollutants has therefore been provided.

Pathogenic Virus Detection by Optical Nanobiosensors.

The novel coronavirus pandemic is sweeping the world and causing global crises. The lack of effective methods of early diagnosis and accurate detection may result in severe infection as well as mortality. Therefore, it is urgently required that rapid, selective, and accurate techniques for detecting pathogenic viruses are developed. Nanotechnology-based biosensors are finding many applications in biological detection, which may address these issues and realize direct detection of molecular targets in real time. Among various nanoplatforms, optical nanobiosensors have aroused much interest due to their inherent advantages of high sensitivity and direct readout. In this review, a summary of recent progress on the optical biosensors based on nanotechnology for pathogenic virus detection is provided, with focus on quantum dots (QDs), upconversion nanoparticles (UCNPs), noble metal nanoparticles, and organic fluorescent molecules-based nanoprobes and chemiluminescence assays. These representative studies demonstrate appealing performance as biosensors and hold great promise for clinical diagnosis.

Fluoride-Free 2D Niobium Carbide MXenes as Stable and Biocompatible Nanoplatforms for Electrochemical Biosensors with Ultrahigh Sensitivity.

Recently, 2D niobium carbide MXene has drawn vast attention due to its merits of large surface area, good metallic conductivity, and tunable band gap, making it desirable for various applications. However, the usage of highly toxic fluoride-containing etchant and quite long etching time in the conventional synthesis route has greatly hindered further exploration of MXene, especially restricting its biomedical application. Herein, novel fluoride-free Nb2CT x nanosheets are prepared by a facile strategy of electrochemical etching (E-etching) exfoliation. Taking advantage of rapid aluminum clearance, excellent chemical stability, and biocompatibility from the MXene by E-etching, fluoride-free Nb2CT x /acetylcholinesterase-based biosensors are constructed for phosmet detection with the limit of detection down to 0.046 ng mL-1. The fabricated Nb2CT x -based biosensor is superior to the counterpart from hydrofluoric acid-etched Nb2CT x , indicating that fluoride-free MXene can enhance the enzyme activity and electron transfer in the biosensor. The results prove that the fluorine-free MXene shows promise for developing biosensors with high performance of ultrahigh sensitivity and selectivity. It is highly expected that the fluoride-free MXene as a stable and biocompatible nanoplatform has great potential to be expanded to many other biomedical fields.

Croconaine nanoparticles with enhanced tumor accumulation for multimodality cancer theranostics.

A novel nanoparticle self-assembled by polyethylene glycol (PEG) modified croconaine dye (CR780) is presented for photoacoustic (PA)/near-infrared (NIR) fluorescence imaging-guided photothermal therapy (PTT). The simple PEGylation made CR780 amphiphilic, and led to their self-assembly into well-defined and uniform nanostructures with size tunable by controlling the assembly conditions. The CR780-PEG5K not only displayed the strength of small molecules (including rapid distribution to different organs, fast renal clearance and minimal accumulation to normal tissues), but also demonstrated the advantages of nanomaterials (including high physiological stability, multimodal theranostic ability, high tumor accumulation and retention). These facilely synthesized molecular nanoprobes showed great clinical translation potential as a versatile theranostic agent.