Synergy of Target-Induced Magnetic Network and Single-Drop Chromogenic System for Ultrasensitive "All-in-Tube" Detection of miRNA in Whole Blood.

The development of liquid biopsy methods for the accurate and reliable detection of miRNAs in whole blood is critical for the early diagnosis and monitoring of diseases. However, accurate quantification of miRNA expression levels remains challenging due to the complex matrix and low abundance of miRNAs in blood samples. Herein, we report a contactless signal output strategy with low background interference that ensures "zero-contact" between the reaction system and the colorimetry system. The designed target-induced magnetic ZnS/ZIF-90/ZnS network can serve as a unique signal amplifier and transducer. It releases hydrogen sulfide (H2S) gas in an acidic solution which can be concentrated in a droplet of only a few microliters in volume, etching the silver layer of Au@Ag nanostars (NSTs) in the droplet. This will lead to changes in the localized surface plasmon resonance signals of the NSTs. Finally, quantitative detection of let-7a is realized by measuring the offset value of the UV-vis absorption peak. Therefore, by virtue of the synergistic action of quadruple signal amplification methods, including catalytic hairpin assembly, ZnS/ZIF-90/ZnS, magnetic separation, and microextraction, the "All-in-Tube" ultrasensitive detection of low-abundance let-7a in whole blood is achieved with a detection limit as low as the aM level. In addition, the "zero-contact" signal output mode effectively solves the problem of complex matrix interference, demonstrating the great potential of this method for miRNA quantification in complex samples, such as whole blood.

Regulating the Sequence Structure of Conjugated Block Copolymers Enables Large-Area Single-Component Organic Solar Cells with High Efficiency and Stability.

Single-component organic solar cells (SCOSCs) based on conjugated block copolymers (CBCs) by covalently bonding a polymer donor and polymer acceptor become more and more appealing due to the formation of a favorable and stable morphology. Unfortunately, a deep understanding of the effect of the assembly behavior caused by the sequence structure of CBCs on the device performance is still missing. Herein, from the aspect of manipulating the sequence length and distribution regularity of CBCs, we synthesized a series of new CBCs, namely D18(20)-b-PYIT, D18(40)-b-PYIT and D18(60)-b-PYIT by two-pot polymerization, and D18(40)-b-PYIT(r) by traditional one-pot method. It is observed that precise manipulation of sequence length and distribution regularity of the polymer blocks fine-tunes the self-assembly of the CBCs, optimizes film morphology, improves optoelectronic properties, and reduces energy loss, leading to simultaneously improved efficiency and stability. Among these CBCs, the D18(40)-b-PYIT-based device achieves a high efficiency of 13.4 % with enhanced stability, which is an outstanding performance among SCOSCs. Importantly, the regular sequence distribution and suitable sequence length of the CBCs enable a facile film-forming process of the printed device. For the first time, the blade-coated large-area rigid/flexible SCOSCs are fabricated, delivering an impressive efficiency of 11.62 %/10.73 %, much higher than their corresponding binary devices.

Oligomer-Assisted Photoactive Layers Enable >18 % Efficiency of Organic Solar Cells.

Although ternary organic solar cells (OSCs) have unique advantages in improving device performance, the morphology assembly in the ternary-phase would be more uncertain or complex than that in the binary-phase. Here, we propose a new concept of oligomer-assisted photoactive layers for high-performance OSCs. The formed alloy-like phase of the oligomer : host polymer blend enabled the oligomer-assisted OSCs to fuse the advantages of both binary and ternary devices, exhibiting substantially enhanced performance and stability compared to the control devices. With the addition of oligomers, outstanding efficiencies of 17.33 % for a PM6 : Y6 device, 18.32 % for a PM6 : BTP-eC9 device, and 17.13 % for a PM6/Y6 pseudo-bilayer device were achieved, all of which are one of the highest values in their corresponding fields. The improved performance originated from the downshift energy levels, enhanced light absorption, optimized blend morphology, favorable charge dynamics, and reduced non-radiative energy loss.

Alkylsilyl Fused Ring-Based Polymer Donor for Non-Fullerene Solar Cells with Record Open Circuit Voltage and Energy Loss.

The energy loss (Eloss ), especially the nonradiative recombination loss and energetic disorder, needs to be minimized to improve the device performance with a small voltage (VOC ) loss. Urbach energy (EU ) of organic photovoltaic materials is related to energetic disorder, which can predict the Eloss of the corresponding device. Herein, a polymer donor (PBDS-TCl) with Si and Cl functional atoms for organic solar cells (OSCs) is synthesized. It can be found that the VOC and Eloss can be well manipulated by regulation of the energy level of the polymer donor and EU , which is dominated by the morphology. A low energetic disorder with an EU of 23.7 meV, a low driving force of 0.08 eV, and a low Eloss of 0.41 eV are achieved for the PBDS-TCl:Y6-based OSCs. Consequently, an impressive open circuit voltage (VOC ) of 0.92 V is obtained. To the best of knowledge, the VOC value and Eloss are both the record values for the Y6-based device. These results demonstrate that fine-tuning the polymer donor by functional atom modification on the side chain is a promising way to reduce EU and energy loss, as well as obtain small driving force and high VOC for highly efficient OSCs.

Highly coherent and multi-octave mid-infrared supercontinuum generations in a reverse-strip AlGaAs waveguide with three zero-dispersion wavelengths.

In this paper, a reverse-strip AlGaAs waveguide with three zero-dispersion wavelengths (ZDWs) is designed. The corresponding three ZDWs are located at 3.74, 6.56, and 8.89 µm. The nonlinearity coefficient of the proposed reverse-strip AlGaAs waveguide is calculated as 2.09W-1m-1 at wavelength 4.9 µm. The effects of pump pulse parameters, waveguide length, and noise coefficient on the nonlinear dynamics of supercontinuum (SC) generation are investigated. When the hyperbolic secant pump pulse with a wavelength of 4.9 µm, peak power of 900 W, and duration of 100 fs is launched into the proposed waveguide and propagated after a 3 mm length, highly coherent and multi-octave mid-infrared (MIR) SC spanning from 2.2 to 14.5 µm (more than 2.7 octaves, at -40dB level) is generated. Finally, a possible fabrication process of the reverse-strip AlGaAs waveguide is introduced. Our research results have important applications in MIR photonics, MIR spectroscopy, optical precision measurement, and more.

CA-CWA: Channel-Aware Contention Window Adaption in IEEE 802.11ah for Soft Real-Time Industrial Applications.

In 2016, the IEEE task group ah (TGah) released a new standard called IEEE 802.11ah, and industrial Internet of Things (IoT) is one of its typical use cases. The restricted access window (RAW) is one of the core MAC mechanisms of IEEE 802.11ah, which aims to address the collision problem in the dense wireless networks. However, in each RAW period, stations still need to contend for the channel by Distributed Coordination Function and Enhanced Distributed Channel Access (DCF/EDCA), which cannot meet the real-time requirements of most industrial applications. In this paper, we propose a channel-aware contention window adaption (CA-CWA) algorithm. The algorithm dynamically adapts the contention window based on the channel status with an external interference discrimination ability, and improves the real-time performance of the IEEE 802.11ah. To validate the real-time performance of CA-CWA, we compared CA-CWA with two other backoff algorithms with an NS-3 simulator. The results illustrate that CA-CWA has better performance than the other two algorithms in terms of packet loss rate and average delay. Compared with the other two algorithms, CA-CWA is able to support industrial applications with higher deadline constraints under the same channel conditions in IEEE 802.11ah.

Contrastive Unsupervised Representation Learning With Optimize-Selected Training Samples.

Contrastive unsupervised representation learning (CURL) is a technique that seeks to learn feature sets from unlabeled data. It has found widespread and successful application in unsupervised feature learning, with the design of positive and negative pairs serving as the type of data samples. While CURL has seen empirical successes in recent years, there is still room for improvement in terms of the pair data generation process. This includes tasks such as combining and re-filtering samples, or implementing transformations among positive/negative pairs. We refer to this as the sample selection process. In this article, we introduce an optimized pair-data sample selection method for CURL. This method efficiently ensures that the two types of sampled data (similar pair and dissimilar pair) do not belong to the same class. We provide a theoretical analysis to demonstrate why our proposed method enhances learning performance by analyzing its error probability. Furthermore, we extend our proof into PAC-Bayes generalization to illustrate how our method tightens the bounds provided in previous literature. Our numerical experiments on text/image datasets show that our method achieves competitive accuracy with good generalization bounds.

Acceptor-only oligomers with high coplanarity enable efficient and stable organic solar cells.

Acceptor-only oligomers are developed as guest components to construct oligomer-assisted active layers for high performance organic solar cells. Due to the high planarity and structural similarity with the host polymer donor, BDD-based acceptor-only oligomers formed an alloy phase with PM6 and optimized the phase morphology effectively, achieving a stable device displaying 18% efficiency.

Three-in-One Strategy Enables Single-Component Organic Solar Cells with Record Efficiency and High Stability.

Single-component organic solar cells (SCOSCs) with covalently bonding donor and acceptor are becoming increasingly attractive because of their superior stability over traditional multicomponent blend organic solar cells (OSCs). Nevertheless, the efficiency of SCOSCs is far behind the state-of-the-art multicomponent OSCs. Herein, by combination of the advantages of three-component and single-component devices, this work reports an innovative three-in-one strategy to boost the performance of SCOSCs. In this three-in-one strategy, three independent components (PM6, D18, and PYIT) are covalently linked together to create a new single-component active layer based on ternary conjugated block copolymer (TCBC) PM6-D18-b-PYIT by a facile polymerization. Precisely manipulating the component ratios in the polymer chains of PM6-D18-b-PYIT is able to broaden light utilization, promote charge dynamics, optimize, and stabilize film morphology, contributing to the simultaneously enhanced efficiency and stability of the SCOSCs. Ultimately, the PM6-D18-b-PYIT-based device exhibits a power conversion efficiency (PCE) of 14.89%, which is the highest efficiency of the reported SCOSCs. Thanks to the aggregation restriction of each component and chain entanglement in the three-in-one system, the PM6-D18-b-PYIT-based SCOSC displays significantly higher stability than the corresponding two-component (PM6-D18:PYIT) and three-component (PM6:D18:PYIT). These results demonstrate that the three-in-one strategy is facile and promising for developing SCOSCs with superior efficiency and stability.

From liquid to solid: A novel approach for utilizing sulfate reduction effluent through phase transition - Effluent-induced nanoscale zerovalent iron sulfidation.

This study investigated the use of sulfate reduction effluent (SR-effluent) to induce sulfidation on nanoscale zerovalent iron (nZVI). SR-effluent-modified nZVI achieved a 100% improvement in Cr(VI) removal from simulated groundwater, a result comparable to cases where other, more typical sulfur precursors (Na2S2O4, Na2S2O3, Na2S, K2S6, and S0) were used. Through a structural equation model analysis, amendment of nanoparticles' agglomeration (standardized path coefficient (std. path coeff.) = -0.449, p < 0.05) and hydrophobicity (std. path coeff. = 0.100, p < 0.05) and direct reaction between iron-sulfur compounds and Cr(VI) (std. path coeff. ranged from -0.195 to 0.322, p < 0.05) were primarily contributing to sulfidation-induced Cr(VI) removal enhancement. Regarding the property improvement of nZVI, the SR-effluent's corrosion radius played a crucial role in tuning the content and distribution of the iron-sulfur compounds based on the core-shell structure of the nZVI and the redox processes at the aqueous-solid interface.

Environmental Factors Affecting the Diversity and Composition of Environmental Microorganisms in the Shaoxing Rice Wine Producing Area.

Shaoxing rice wine is a notable exemplar of Chinese rice wine. Its superior quality is strongly correlated with the indigenous natural environment. The results indicated that Firmicutes (75%), Actinobacteria (15%), Proteobacteria (5%), and Bacteroidetes (3%) comprised the prevailing bacterial groups. Among the main bacterial genera, Lactobacillus was the most abundant, accounting for 49.4%, followed by Lactococcus (11.9%), Saccharopolyspora (13.1%), Leuconostoc (4.1%), and Thermoactinomyces (1.1%). The dominant fungal phyla were Ascomycota and Zygomycota. Among the dominant genera, Saccharomyces (59.3%) prevailed as the most abundant, followed by Saccharomycopsis (10.7%), Aspergillus (7.1%), Thermomyces (6.2%), Rhizopus (4.9%), Rhizomucor (2.2%), and Mucor (1.3%). The findings demonstrate that the structure of the bacterial and fungal communities remains stable in the environment, with their diversity strongly influenced by climatic conditions. The continuous fluctuations in environmental factors, such as temperature, air pressure, humidity, rainfall, and light, significantly impact the composition and diversity of microbial populations, particularly the dominant bacterial community.

Machine learning-driven 3D plasmonic cellulose sensor for in situ rapid SERS detection of bisphenol compounds in water sample.

Rapid component separation and accurate identification of bisphenols compounds (BPs) in real water sample remain an attractive challenge due to the trace amounts and structural similarities of BPs, and complexity of real samples. Here, we designed and synthesized chemically modified cellulose p-toluenesulfonate (CTSA) to encapsulate octadecylamine-modified gold nanoparticles (Au-ODA), obtaining 3D plasmonic cellulose (Au@CTSA). Simultaneously, by virtue of the high surface area in the 3D network of CTSA and the solvent volatile deposition, BPs in water were in situ extracted and concentrated in Au@CTSA microspheres. Since the 3D network of Au@CTSA supports the formation of "hotspots", the number of "hotspots" available is greatly improved, enabling excellent SERS detection of BPs. Based on the collected SERS spectra, machine learning was utilized to analyze the overall profile of BPs, which eliminated the subjective judgment of the concentration by the Au@CTSA sensor using a single characteristic peak. In this way, the accuracy of identification of BPs was significantly improved. The machine learning-driven Au@CTSA sensor realized the detection of traces bisphenol A (BPA), bisphenol S (BPS), and bisphenol F (BPF) in water sample, pushing quantitative detection of different concentrations of BPs and contributing facile indicators for water quality monitoring.

A bio-analytic nanoplatform based on Au post-functionalized CeFeO3 for the simultaneous determination of melatonin and ascorbic acid through photo-assisted electrochemical technology.

Both melatonin and ascorbic acid could perform an irreplaceable role in maintaining the ecological balance of the human body and fighting cardiovascular diseases. Herein, a dual-channel photo-assisted electrochemical sensor has been fabricated based on Au post-functionalized CeFeO3 nanospheres to simultaneously monitor melatonin and ascorbic acid for the first time. Briefly, CeFeO3 nanospheres are prepared through a hydrothermal and annealing process, and then the reduced Au nanoclusters are anchored on the surface of spheres to afford the CeFeO3@Au bi-nanospherical sensing probe. Impressively, the pre-fabricated sensor can produce a current signal 11% higher under light than that produced in a dark environment during the electrochemical measurements. Subsequently, the sensor fabricated by our strategy has achieved the simultaneous determination of melatonin and ascorbic acid with the wide detecting ranges of 1 nM-5 µM and 1 nM to 2 µM, and low detection limits of 0.8 nM and 0.4 nM by electrochemical measurements with the presence of the sunlight, and has shown satisfactory recoveries in the real sample measurements, demonstrating that the CeFeO3@Au bi-nanospherical sensing probe will be an auspicious candidate of advanced electrode material in photo-assisted electrochemical sensing applications.

The construction of molecularly imprinted electrochemical biosensor for selective glucose sensing based on the synergistic enzyme-enzyme mimic catalytic system.

It is generally accepted that glucose oxidase (GOx) shows unique specificity in ß-d-glucose catalysis. However, it has been found that GOx can catalyze diverse monosaccharides. Therefore, the sensing accuracy for glucose biosensors using GOx as probes will be largely compromised by the presence of other monosaccharides. Herein, multifunctional bi-nanospheres (Fe3O4@Au NCs), which show both peroxidase-like and catalase-like catalytic activities in different working conditions, are successfully constructed and served as desirable platform with huge surface area for the immobilization of large amount of GOx probes. In acidic environment, hydroxyl radicals could be generated via the cascaded catalysis of ß-d-glucose by Fe3O4@Au-GOx, and then employed to initiate the polymerization of boric acid derivative to prepare molecularly imprinted polymers (MIPs) on the surface of GOx using ß-d-glucose as template. Then, the molecularly imprinted GOx are immobilized on the surface of highly oriented pyrolytic graphite (HOPG) electrode and an electrochemical biosensor (Fe3O4@Au-GOx-HOPG) for glucose sensing is successfully obtained. Interestingly, the as-prepared biosensors could selectively detect glucose in the range of 10.0 µM - 5.0 mM with a LOD = 5.0 µM with the help of MIPs, which is comparable or better than other glucose sensors reported recently.

Random Copolymerization Strategy for Host Polymer Donor PM6 Enables Improved Efficiency Both in Binary and Ternary Organic Solar Cells.

Although breakthroughs have been made in organic solar cells (OSCs) in recent years, the power conversion efficiency (PCE) of OSCs still lags behind inorganic/perovskite solar cells. In this work, two terpolymers were synthesized by introducing the thieno[3,4-c]pyrrole-4,6-(5H)-dione (TPD) block into the host polymer donor PM6. Owing to the lower highest occupied molecular orbital energy level, wider light absorption, optimal molecular packing, and more desirable aggregation morphology by addition of the TPD, the PM6-TPD-5 % : Y6-based device displayed an improved PCE of 16.3 % with an enhanced open-circuit voltage (VOC ) of 0.860 V, relative to that of PM6-TPD-10 % : Y6 (PCE=14.8 %) and PM6 : Y6-based device (PCE=15.6 %). Interestingly, the VOC did not always increase in proportion to the third component. Besides, ternary OSCs based on PM6 : PM6-TPD-5 % : Y6 achieved a superior PCE of 17.1 %. This work demonstrated that random copolymerization is a feasible and effective strategy to further increase device performance, and the two polymers that possess similar structure and absorption in ternary devices can also obtain impressive efficiency.

Exploiting Novel Unfused-Ring Acceptor for Efficient Organic Solar Cells with Record Open-Circuit Voltage and Fill Factor.

Unfused-ring acceptors (UFAs) show bright application prospects in organic solar cells (OSCs) thanks to their easy synthesis, low cost, and good device performance. The selection of central-core building block and suitable side chain are the key factors to achieve high-performance UFAs. Current tremendous endeavors for the development of UFAs mainly concentrate on obtaining higher short-circuit current density (Jsc ), albeit accompanied by low open-circuit voltage (Voc ) and modest fill factor (FF). Herein, two novel A-D-A'-D-A type UFAs (BTCD-IC and BTCD-2FIC), which have the same new electron-withdrawing central-core dithieno[3',2':3,4;2'',3'':5,6]-benzo[1,2-c][1,2,5]thiadia-zole (DTBT) and cyclopentadithiophene unit (CPDT, substituted by 2-butyl-1-octyl alkyl chain) coupling with different terminals, were designed and synthesized. Two UFAs showed strong and broad light absorption in the wavelength range of 300-850 nm owing to the strong intramolecular charge transfer effect favorable by DTBT core. Compared with BTCD-IC, BTCD-2FIC with F-containing terminal group exhibited higher molar extinction coefficient, lower energy level, higher charge mobility, stronger crystallinity, more ordered molecular stacking, and better film morphology. As a result, when blended with donor polymer PBDB-T (poly[(2,6-(4,8-bis(5-(2-ethylhexyl)thiophen-2-yl)benzo[1,2-b:4,5-b']dithiophene)-co-(1,3-di(5-thiophene-2-yl)-5,7-bis(2-ethylhexyl)benzo[1,2-c:4,5-c']-dithiophene-4,8-dione)]), the BTCD-2FIC-based OSC achieved a superior power conversion efficiency (PCE) of 11.32 %, with a high Voc of 0.85 V, a Jsc of 18.24 mA cm-2 , and a FF of 73 %, than BTCD-IC-based OSC (PCE=8.96 %). Impressively, the simultaneously enhanced Voc and FF values of the PBDB-T:BTCD-2FIC device were the highest values of the A-D-A'-D-A-type UFAs. The results demonstrate the application of electron-withdrawing DTBT central-core unit in efficient UFAs provides meaningful molecular design guidance for high-performance OSCs.

Specific sensing of resorcin based on the hierarchical porous nanoprobes constructed by cuttlefish-derived biomaterials through differential pulse voltammetry.

The specific detection of resorcin from its isomers is a current research hotspot. Thus in our work, a ternary hierarchical porous nanoprobe has been constructed based on the combination of cuttlefish ink and bimetallic Au@Ag nanoclusters for the specific sensing of resorcin. Briefly, through electrostatic interaction, Au@Ag core-shell nanoclusters are immobilized on the surface of polydopamine extracted from cuttlefish, which is turned into nitrogen-doped porous carbon functionalized by bimetallic Au@Ag by topological transformation subsequently. Afterward, an electrochemical sensor is fabricated based on the nanoprobes for specifically determining resorcin in solution by differential pulse voltammetry, and the linear detection ranges of the sensor are 1-100 µM and 1.2-4 mM while the detection limit reaches 0.06 µM. Meanwhile, the sensing mechanism of resorcin by the pre-fabricated sensor is detailedly studied by density functional theory to obtain a clear electrochemical process. Besides, the selectivity, stability, plus reproducibility of the pre-fabricated sensor have been also tested, and the determinations for resorcin in real environmental water samples have also been performed with good recoveries, revealing the auspicious application potential in the environmental monitoring.

Fabrication of Cobaltous Sulfide Nanoparticle-Modified 3D MXene/Carbon Foam Hybrid Aerogels for All-Solid-State Supercapacitors.

MXene is a neoteric type of bidimensional (2D) transition metal carbide/nitride with broad application prospects, in particular with electrochemical energy storage. The electrochemical performance of MXene is unsatisfactory because it is easy to stack resulting in the difficulty of electrolyte penetration and ion transport. In this study, the cobaltous sulfide-modified 3D MXene/N-doped carbon foam (CoS@MXene/CF) hybrid aerogel is projected and manufactured via simple in situ growth and thermal annealing strategies. The capacitance of the as-fabricated 300-CMC-31:1 electrode material reaches 250 F g-1 (1 A g-1), which is obviously higher than those of MXene, CoS@CF, 400-CMC-31:1, 300-CMC-10:1, 300-CMC-50:1, CF, and MXene/CF electrode materials. Moreover, it can hold 97.5% of the original capacitance after 10,000 cycles and the internal resistance (Rs) is only 0.50 Ω. A green bulb can be lit by two all-solid asymmetric supercapacitors installed in series. The prepared CoS@MXene/CF hybrid aerogel exhibits promising potential for practical application in energy storage areas.

A molecularly imprinted nanoreactor with spatially confined effect fabricated with nano-caged cascaded enzymatic system for specific detection of monosaccharides.

Glucose oxidase (GOx), traditionally regarded as an oxidoreductase with high ß-D-glucose specificity, has been widely applied as sensing probe for ß-D-glucose detection. However, it is found that the specificity of GOx is not absolute and GOx cannot decern ß-D-glucose among its isomers such as xylose, mannose and galactose. The existence of the other monosaccharides in sensing system could compromise the sensitivity for ß-D-glucose, therefore, it is of great urgency to achieve the highly specific catalytic performance of GOx. Herein, porous metal-organic frameworks (MOF) are prepared as the host matrix for immobilization of both GOx and bovine hemoglobin (BHb), obtained a cascaded catalytic system (MOF@GOx@BHb) with both enhanced GOx activity and peroxidase-like activity owing to the spatially confined effect. Then, using ß-D-glucose as both template molecules and substances, hydroxyl radicals are produced continuously and applied for initiating the polymerization of molecular imprinting polymers (MIPs) on the surface of MOF@GOx@BHb. Impressively, the obtaining molecularly imprinted GOx (noted as MOF@GOx@BHb-MIPs) achieves the highly sensitive and specific detection of ß-D-glucose in the concentration range of 0.5-20 µM with the LOD = 0.4 µM (S/N = 3) by colorimetry. Similarly, MOF@GOx@BHb-MIPs are subsequently obtained using mannose, xylose and galactose as template molecules, respectively, and also show satisfied specific catalytic activity towards corresponding templates, indicating the effectiveness of the proposed strategy to achieve highly specific catalytic performance of GOx.

A novel AIE molecule as a hole transport layer enables efficient and stable perovskite solar cells.

A low-cost and efficient hole transport layer (HTL) material (TPE-CZ) with the aggregation-induced emission (AIE) effect has been synthesized. Due to the AIE effect, perovskite solar cells with TPE-CZ as the HTL deliver a higher power conversion efficiency (PCE) of 18% with better stability than those with the reference HTL (Spiro-OMeTAD).