Interlayer Delocalized Electrons Activate Basal Plane for Ultrahigh-Current-Density Hydrogen Evolution.

The basal plane of transition metal dichalcogenides (TMDCs) is inert for the hydrogen evolution reaction (HER) due to its low-efficiency charge transfer kinetics. We propose a strategy of filling the van der Waals (vdW) layer with delocalized electrons to enable vertical penetration of electrons from the collector to the adsorption intermediate vertically. Guided by density functional theory, we achieve this concept by incorporating Cu atoms into the interlayers of tantalum disulfide (TaS2). The delocalized electrons of d-orbitals of the interlayered Cu can constitute the charge transfer pathways in the vertical direction, thus overcoming the hopping migration through vdW gaps. The vertical conductivity of TaS2 increased by 2 orders of magnitude. The TaS2 basal plane HER activity was extracted with an on-chip microcell. Modified by the delocalized electrons, the current density increased by 20 times, reaching an ultrahigh value of 800 mA cm-2 at -0.4 V without iR compensation.

A novel laccase-like Cu-MOF for colorimetric differentiation and detection of phenolic compounds.

The development of convenient, fast, and cost-effective methods for differentiating and detecting common organic pollutant phenols has become increasingly important for environmental and food safety. In this study, a copper metal-organic framework (Cu-MOF) with flower-like morphology was synthesized using 2-methylimidazole (2-MI) as ligands. The Cu-MOF was designed to mimic the natural laccase active site and proved demonstrated excellent mimicry of enzyme-like activity. Leveraging the superior properties of the constructed Cu-MOF, a colorimetric method was developed for analyzing phenolic compounds. This method exhibited a wide linear range from 0.1 to 100 µM with a low limit of detection (LOD) of 0.068 µM. Besides, by employing principal component analysis (PCA), nine kinds of phenols was successfully distinguished and identified. Moreover, the combination of smartphones with RGB profiling enabled real-time, quantitative, and high-throughput detection of phenols. Therefore, this work presents a paradigm and offers guidance for the differentiation and detection of phenolic pollutants in the environment.

Intrinsic Defect-Driven Synergistic Synaptic Heterostructures for Gate-Free Neuromorphic Phototransistors.

The optoelectronic synaptic devices based on two-dimensional (2D) materials offer great advances for future neuromorphic visual systems with dramatically improved integration density and power efficiency. The effective charge capture and retention are considered as one vital prerequisite to realizing the synaptic memory function. However, the current 2D synaptic devices are predominantly relied on materials with artificially-engineered defects or intricate gate-controlled architectures to realize the charge trapping process. These approaches, unfortunately, suffer from the degradation of pristine materials, rapid device failure, and unnecessary complication of device structures. To address these challenges, an innovative gate-free heterostructure paradigm is introduced herein. The heterostructure presents a distinctive dome-like morphology wherein a defect-rich Fe7S8 core is enveloped snugly by a curved MoS2 dome shell (Fe7S8@MoS2), allowing the realization of effective photocarrier trapping through the intrinsic defects in the adjacent Fe7S8 core. The resultant neuromorphic devices exhibit remarkable light-tunable synaptic behaviors with memory time up to ≈800 s under single optical pulse, thus demonstrating great advances in simulating visual recognition system with significantly improved image recognition efficiency. The emergence of such heterostructures foreshadows a promising trajectory for underpinning future synaptic devices, catalyzing the realization of high-efficiency and intricate visual processing applications.

Endogenous mRNA-Powered and Spatial Confinement-Derived DNA Nanomachines for Ultrarapid and Sensitive Imaging of Let-7a.

DNA nanostructure-based signal amplifiers offer new tools for imaging intracellular miRNA. However, the inadequate kinetics and susceptibility to enzymatic hydrolysis of these amplifiers, combined with a deficient cofactor concentration within the intracellular environment, significantly undermine their operational efficiency. In this study, we address these challenges by encapsulating a localized target strand displacement assembly (L-SD) and a toehold-exchange endogenous-powered component (R-mRNA) within a framework nucleic acid (FNA) structure─20 bp cubic DNA nanocage (termed RL-cube). This design enables the construction of an endogenous-powered and spatial-confinement DNA nanomachine for ratiometric fluorescence imaging of intracellular miRNA Let-7a. The R-mRNA is designed to be specifically triggered by glyceraldehyde 3-phosphate dehydrogenase (GAPDH), an abundant cellular enzyme, and concurrently releases a component that can recycle the target Let-7a. Meanwhile, L-SD reacts with Let-7a to release a stem-loop beacon, generating a FRET signal. The spatial confinement provided by the framework, combined with the ample intracellular supply of GAPDH, imparts remarkable sensitivity (7.57 pM), selectivity, stability, biocompatibility, and attractive dynamic performance (2240-fold local concentration, approximately four times reaction rate, and a response time of approximately 7 min) to the nanomachine-based biosensor. Consequently, this study introduces a potent sensing approach for detecting nucleic acid biomarkers with significant potential for application in clinical diagnostics and therapeutics.

GeO2 Nanoparticles Decorated in Amorphous Carbon Nanofiber Framework as Highly Reversible Lithium Storage Anode.

Germanium oxide (GeO2) is a high theoretical capacity electrode material due to its alloying and conversion reaction. However, the actual cycling capacity is rather poor on account of suffering low electron/ion conductivity, enormous volume change and agglomeration in the repeated lithiation/delithiation process, which renders quite a low reversible electrochemical lithium storage reaction. In this work, highly amorphous GeO2 particles are uniformly distributed in the carbon nanofiber framework, and the amorphous carbon nanofiber not only improves the conduction and buffers the volume changes but also prevents active material agglomeration. As a result, the present GeO2 and carbon composite electrode exhibits highly reversible alloying and conversion processes during the whole cycling process. The two reversible electrochemical reactions are verified by differential capacity curves and cyclic voltammetry measurements during the whole cycling process. The corresponding reversible capacity is 747 mAh g-1 after 300 cycles at a current density of 0.3 A g-1. The related reversible capacities are 933, 672, 487 and 302 mAh g-1 at current densities of 0.2, 0.4, 0.8 and 1.6 A g-1, respectively. The simple strategy for the design of amorphous GeO2/carbon composites enables potential application for high-performance LIBs.

Dual-ligand lanthanide metal-organic framework probe for ratiometric fluorescence detection of mercury ions in wastewater.

By serving dipyridylic acid (DPA) and 2,5-dihydroxyterephthalic acid (DHTA) as the biligands, a novel lanthanide (Eu3+) metal-organic framework (MOF) namely Eu-DHTA/DPA was prepared for specific Hg2+ fluorescence determination. The dual-ligand approach can endows the resulting luminescent MOF with dual emission of ratiometric fluorescence and uniform size. Eu3+ produces intense red fluorescence when activated by the ligand DPA, while the other ligand DHTA produces yellow fluorescence. Under 273 nm excitation, the presence of Hg2+ in the monitoring environment causes an increase in the intensity of the DHTA fluorescence peak at 559 nm and a decrease in the intensity of the Eu3+ fluorescence peak at 616 nm. Hg2+ effectively quenches the fluorescence emission of the central metal Eu3+ in Eu-DHTA/DPA at 616 nm through a dynamic quenching effect. This recognition process occurs due to the coordination of Hg2+ with ligands such as benzene rings, carboxyl groups, and pyridine N in three-dimensional space. Hg2+ was detected by measuring the ratio between two fluorescence peaks (I559 nm/I616 nm) within the range 2-20 µM, achieving a remarkably low detection limit of 40 nM. The established ratiometric fluorescence method has been successfully applied to the determination of Hg2+ in industrial wastewater of complex composition. The method plays a crucial role in the rapid and sensitive monitoring of Hg2+ in real environmental samples. The recoveries ranged from 92.82% to 112.67% (n = 3) with relative standard deviations (RSD) below 4.8%. This study offers a convenient and effective method for constructing probes for Hg2+ monitoring, with practical applications in environmental monitoring.

Gate-voltage-modulated electrostatic interaction between the probe and the channel material of FET biosensors for detecting telomerase.

A gate-voltage-modulated strategy was proposed to improve the detection performance of telomerase. We comprehensively investigated the mechanism for the gate-voltage-modulated detection performance by modulating the electrostatic interaction between charges of a single-stranded DNA probe and electrons of the In2O3 channel. This gate-voltage-modulated interaction between the probe and the channel can potentially serve as a universal strategy for high-performance FET biosensors.

Interfacial engineered PANI/carbon nanotube electrode for 1.8 V ultrahigh voltage aqueous supercapacitors.

Flexible three-dimensional interconnected carbon nanotubes on the carbon cloth (3D-CNTs/CC) were obtained through simple magnesium reduction reactions. According to the Nernst equation, the cell voltage based on these pure carbon electrodes without any additives could reach 1.5 V due to the higher di-hydrogen evolution over potential in neutral 3.5 M LiCl electrolytes. In order to improve the electrochemical performance of the electrodes, 3D-CNTs/CC electrodes covered with polyaniline barrier layer (3D-PANI/CNTs/CC) were prepared byin situelectropolymerization using interfacial engineering method. The assembled symmetric supercapacitors display a broadened voltage of 1.8 V, high areal capacitance of 380 mF cm-2, outstanding areal energy density of 85.5µWh cm-2and 84% of its initial capacitance after 20 000 charge-discharge cycles. This work demonstrated that the interface engineering strategy provides a promising way to improve the energy density of carbon-based aqueous supercapacitors by widening the voltage and boosting the capacitance simultaneously.

P-doped porous carbon derived from walnut shell for zinc ion hybrid capacitors.

Zinc ion hybrid capacitors (ZHCs) are expected to be candidates for large-scale energy storage products due to their high power density and large energy density. Due to their low cost and stability, carbon materials are generally the first choice for the cathode of ZHCs, but they face a challenge in the serious self-discharge behavior. Herein, zinc ion hybrid capacitors with high-performance are successfully assembled using a porous carbon cathode derived from low-cost p-doped waste biomass and a commercial zinc foil anode. The p-doped walnut shell ZHCs delivered a specific capacity of 158.9 mA h g-1 with an energy density of 127.1 W h kg-1 at a low current density. More importantly, the device had outstanding anti-self-discharge characteristics (retaining 77.98% of its specific capacity after a 72 h natural self-discharge test) and long-term cycle stability (retaining 88.2% of its initial specific capacity after 15 000 cycles at 7.5 A g-1). This work presents guidance and support for the design and optimization of electrode materials for zinc ion supercapacitors and next-generation aqueous zinc ion energy storage performance.

High-capacity and ultrastable lithium storage in SnSe2-SnO2@NC microbelts enabled by heterostructures.

The ingenious design of high-performance tin-based lithium-ion batteries (LIBs) is challenging due to their poor conductivity and drastic volume change during continuous lithiation/delithiation cycles. Herein, we present a strategy to confine heterostructured SnSe2-SnO2 nanoparticles into macroscopic nitrogen-doped carbon microbelts (SnSe2-SnO2@NC) as anode materials for LIBs. The composites exhibit an excellent specific capacity of 436.3 mA h g-1 even at 20 A g-1 and an ultrastable specific capacity of 632.7 mA h g-1 after 2800 cycles at 5 A g-1. Density Functional Theory (DFT) calculations reveal that metallic SnSe2-SnO2 heterostructures endow the lithium atoms at the interface with high adsorption energy, which promotes the anchoring of Li atoms, and enhances the electrical conductivity of the anode materials. This demonstrates the superior Li+ storage performance of the SnSe2-SnO2@NC microbelts as anode materials.

Nanopatterning Technologies of 2D Materials for Integrated Electronic and Optoelectronic Devices.

With the reduction of feature size and increase of integration density, traditional 3D semiconductors are unable to meet the future requirements of chip integration. The current semiconductor fabrication technologies are approaching their physical limits based on Moore's law. 2D materials such as graphene, transitional metal dichalcogenides, etc., are of great promise for future memory, logic, and photonic devices due to their unique and excellent properties. To prompt 2D materials and devices from the laboratory research stage to the industrial integrated circuit-level, it is necessary to develop advanced nanopatterning methods to obtain high-quality, wafer-scale, and patterned 2D products. Herein, the recent development of nanopatterning technologies, particularly toward realizing large-scale practical application of 2D materials is reviewed. Based on the technological progress, the unique requirement and advances of the 2D integration process for logic, memory, and optoelectronic devices are further summarized. Finally, the opportunities and challenges of nanopatterning technologies of 2D materials for future integrated chip devices are prospected.

Label-free SERS strategy for rapid detection of capsaicin for identification of waste oils.

Identification of waste oils is challenging in the field of food safety due to the lack of common markers and straightforward analytical methods. Herein, we developed a novel label-free surface-enhanced Raman spectroscopy (SERS) strategy to identify waste oils using Ag nanoparticles solution (Ag NPs sol.) as a SERS substrate to significantly enhance the Raman signal of capsaicin marker molecule usually contained in the waste oils. The enhanced signal was directly detected by a portable Raman spectrometer with the limit of detection (LOD) of 2.9 µg L-1 within 10 min. Concentration-dependent SERS investigation showed the linear relationship between the SERS signal intensity of the characteristic peaks and the concentrations of capsaicin in the range of 10-2500 µg L-1 and the correlation coefficient was 0.9895. Our findings show the sensitivity, accessibility, and reliability of this method for the rapid identification of waste oils and furthermore for the practical applications in the field of food safety.

Iron vacancies engineering of FexC@NC hybrids toward enhanced lithium-ion storage properties.

Defect engineering have profound influence on the energy storage properties of electrode hybrids by adjusting their intrinsic electronic characteristics. For iron carbide based materials, however, the effect of defect (especially cation vacancies) toward their electrochemical performance are still unclear. Herein, the feasible and scalable synthesis of FexC@NC with 3D honeycomb-like carbon architecture and abundant Fe vacancies via template etching is reported. Such structure enable outstanding lithium-ion storage properties owing to hierarchical pores, improved intrinsic electrochemical activity, as well as the introduction of more active sites. As a result, the FexC@NC-2 presents a high reversible specific capacity of 1079 mAh g-1after 1000 cycles. Moreover, an excellent cycling stability can be achieved via maintaining a high-capacity retention (689 mAh g-1, 98.4%) over 1000 cycles at 5 A g-1. This study provides a feasible strategy for developing high-performance hybrids with hierarchical pore and rich defects structures.

Hierarchical Ni3S2nanorod@nanosheet arrays on Ni foam for high-performance supercapacitor.

We successfully designed and prepared hierarchical Ni3S2nanorod@nanosheet arrays on three-dimensional Ni foam via facile hydrothermal sulfuration. We conducted a series of time- and temperature-dependent experiments to determine the Ostwald ripening process of hierarchical Ni3S2nanorod@nanosheet arrays. The rationally hierarchical architecture creates an excellent supercapacitor electrode for Ni3S2nanorod@nanosheet arrays. The areal capacitance of this array reaches 5.5 F cm-2at 2 mA cm-2, which is much higher than that of Ni3S2nanosheet arrays (1.5 F cm-2). The corresponding asymmetric supercapacitor exhibits a wide potential window of 1.6 V and energy density up to 1.0 Wh cm-2when the proposed array is utilized as the positive electrode with activated carbon as the negative electrode. This electrochemical performance enhancement is attributable to the hierarchical structure and synergistic cooperation of macroporous Ni foam and well-aligned Ni3S2nanorod@nanosheet arrays. Our results represent a promising approach to the preparation of hierarchical nanorod@nanosheet arrays as high-performing electrochemical capacitors.

Rapid and Quantitative Detection of Aflatoxin B1 in Grain by Portable Raman Spectrometer.

Many foodstuffs are extremely susceptible to contamination with aflatoxins, in which aflatoxin B1 is highly toxic and carcinogenic. Therefore, it is crucial to develop a rapid and effective analytical method for detecting and monitoring aflatoxin B1 in food. Herein, a surface-enhanced Raman spectroscopic (SERS) method combined with QuEChERS (quick, easy, cheap-effective, rugged, safe) sample pretreatment technique was used to detect aflatoxin B1. Sample preparation was optimized into a one-step extraction method using an Au nanoparticle-based solution (Au sol) as the SERS detection substrate. An affordable portable Raman spectrometer was then used for rapid, label-free, quantitative detection of aflatoxin B1 levels in foodstuffs. This method showed a good linear log relationship between the Raman signal intensity of aflatoxin B1 in the 1-1000 µg L-1 concentration range with a limit of detection of 0.85 µg kg-1 and a correlation coefficient of 0.9836. Rapid aflatoxin B1 detection times of ∼10 min for wheat, corn, and protein feed powder samples were also achieved. This method has high sensitivity, strong specificity, excellent stability, is simple to use, economical, and is suitable for on-site detection, with good prospects for practical application in the field of food safety.

Electrochemically Induced Structural and Morphological Evolutions in Nickel Vanadium Oxide Hydrate Nanobelts Enabling Fast Transport Kinetics for High-Performance Zinc Storage.

Suitable intercalation cathodes and fundamental insights into the Zn-ion storage mechanism are the crucial factors for the booming development of aqueous zinc-ion batteries. Herein, a novel nickel vanadium oxide hydrate (Ni0.25V2O5·0.88H2O) is synthesized and investigated as a high-performance electrode material, which delivers a reversible capacity of 418 mA h g-1 with 155 mA h g-1 retained at 20 A g-1 and a high capacity of 293 mA h g-1 in long-term cycling at 10 A g-1 with 77% retention after 10,000 cycles. More importantly, multistep phase transition and chemical-state change during intercalation/deintercalation of hydrated Zn2+ are illustrated in detail via in situ/ex situ analytical techniques to unveil the Zn2+ storage mechanism of the hydrated and layered vanadium oxide bronze. Furthermore, morphological development from nanobelts to hierarchical structures during rapid ion insertion and extraction is demonstrated and a self-hierarchical process is correspondingly proposed. The unique evolutions of structure and morphology, together with consequent fast Zn2+ transport kinetics, are of significance to the outstanding zinc storage capacity, which would enlighten the mechanism exploration of the aqueous rechargeable batteries and push development of vanadium-based cathode materials.

Revegetation of a barren rare earth mine using native plant species in reciprocal plantation: effect of phytoremediation on soil microbiological communities.

Over-exploration of rare earth elements causes soil desertification and environmental degradation. However, the restoration of rare earth mine tailings requires the recovery of both vegetation and soil microbiota. Accordingly, the present study aimed to compare the efficacy of restoring mine tailings using organic compost and native plants (Miscanthus sinensis, Pinus massoniana, Bambusa textilis, or a mixture of all three). After three years, the mixed plantation harbored tenfold greater plant richness than that in the barren land. Among these, M. sinensis played a dominant role across all restored areas. The microbial communities of the soils were assessed using high-throughput 16S rDNA gene sequencing. A total of 34,870 16S rDNA gene sequences were obtained and classified into 15 bacterial phyla and 36 genera. The dominant genus across all the restored soils was Burkholderia, and the bacterial diversity of restored soils was greater than that of soils from either unrestored or natural (unexploited) areas, with the M. sinensis plantation yielding the greatest diversity. The effects of phytoremediation were mainly driven by changes in nutrient and metal contents. These results indicate that M. sinensis significantly improves phytoremediation and that mixed planting is ideal for restoring the soils of abandoned rare earth mines.

In-situ Grown SnO2 Nanospheres on Reduced GO Nanosheets as Advanced Anodes for Lithium-ion Batteries.

Nanostructured tin dioxide (SnO2) has emerged as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity (1494 mA h g-1) and excellent stability. Unfortunately, the rapid capacity fading and poor electrical conductivity of bulk SnO2 material restrict its practical application. Here, SnO2 nanospheres/reduced graphene oxide nanosheets (SRG) are fabricated through in-situ growth of carbon-coated SnO2 using template-based approach. The nanosheet structure with the external layer of about several nanometers thickness can not only accommodate the volume change of Sn lattice during cycling but also enhance the electrical conductivity effectively. Benefited from such design, the SRG composites could deliver an initial discharge capacity of 1212.3 mA h g-1 at 0.1 A g-1, outstanding cycling performance of 1335.6 mA h g-1 after 500 cycles at 1 A g-1, and superior rate capability of 502.1 mA h g-1 at 5 A g-1 after 10 cycles. Finally, it is believed that this method could provide a versatile and effective process to prepare other metal-oxide/reduced graphene oxide (rGO) 2D nanocomposites.

A 3D interconnected NH4Fe0.6V2.4O7.4@C nanocomposite with superior sodium storage properties.

A novel 3D interconnected NH4Fe0.6V2.4O7.4@C nanocomposite was in situ synthesized through a facile hydrothermal reaction at low temperature (98 °C), and its electrochemical performance as a cathode for sodium-ion batteries (SIBs) was investigated for the first time. Under the intercalation of Fe3+ and carbon-coating, as-prepared samples turned to 3D interconnected structures, which were composed of NH4Fe0.6V2.4O7.4 nanoparticles and carbon chains. The 3D interconnected NH4Fe0.6V2.4O7.4@0.5 wt%C nanocomposite exhibits a high discharge specific capacity of 306 mA h g-1 at a current density of 20 mA g-1 and a high-rate capacity of 130 mA h g-1 at 0.4 A g-1. The results of EIS and ex situ SEM indicated that the 3D interconnected NH4Fe0.6V2.4O7.4@0.5 wt%C nanocomposite possesses good electrical conductivity and structural stability. The ex situ XRD results suggest that NH4Fe0.6V2.4O7.4@0.5 wt%C undergoes a reversible insertion/de-insertion mechanism during a charge/discharge process. Our work demonstrates that the 3D interconnected NH4Fe0.6V2.4O7.4@C nanocomposite material could be considered as a potential cathode for sodium ion batteries.

Hard Carbon Wrapped Na3V2(PO4)3@C Porous Composite Extending Cycling Lifespan for Sodium-Ion Batteries.

Although the NASICON-type of Na3V2(PO4)3 is regarded as a potential cathode candidate for advanced sodium-ion batteries (SIBs), it has an undesirable rate performance and low cyclability, which are a result of its poor electronic conductivity. Here, we utilized conductive polyaniline (PANI) grown in situ to obtain the hard carbon-coated porous Na3V2(PO4)3@C composite (NVP@C@HC) with a typically simple and effective sol-gel process. Based on the restriction of double carbon layers, the NVP size decreases distinctly, which can curtail the sodium-ion diffusion distance and enhance the electronic conductivity. As expected, the product displays good discharge capacity (111.6 mA h g-1 at 1 C), outstanding rate capacity (60.4 mA h g-1 at 50 C), and remarkable cycling stability (63.3 mA h g-1 with a retention of 83.3% at 40 C over 3000 cycles). Also, it performs a long-term cycling capacity of 58.5 mA h g-1 exceeding 15 000 cycles at 20 C (with a capacity loss of 0.24% per cycle).