The electrocatalytic nitrate reduction to ammonia (NRA) involves complex multi-electron transfer steps and various intermediates, presenting significant challenges in reaction selectivity. Therefore, the development of cost-effective and high-efficiency electrocatalysts is critical. Herein, a bismuth-based Bi19S27Br3/TiO2 heterostructure was constructed via a facile hydrothermal strategy. The integration of Bi19S27Br3 with TiO2introduced abundant oxygen vacancies, which significantly enhanced the adsorption of NO3-. Furthermore, the construction of an n-n type heterojunction expanded the electrochemically active surface area and optimized the electron transfer pathway, thereby promoting charge separation efficiency. Consequently, the Bi19S27Br3/TiO2 catalyst delivered a high ammonia yield of 7.2 mg center dot h-1 center dot mgcat-1 at-0.9 V vs. RHE and a Faradaic efficiency of 86.5% at-0.8 V vs. RHE. These results demonstrate that the Bi19S27Br3/TiO2heterojunction is a promising candidate for ambient nitrate reduction.

ConspectusThe study of main-group molecules that mimic transition metal (TM) complexes in bond activation and catalysis has attracted considerable interest in recent decades. However, main-group elements lack the same electronic versatility that endows TM complexes with diverse reactivity patterns. This limitation has driven efforts to develop innovative strategies to harness and expand the reactivity of main-group compounds. Among these, leveraging cooperative effects between main-group centers has emerged as a particularly promising approach to fine-tune their reactivity, as exemplified by frustrated Lewis pairs (FLPs) and bimetallic main-group complexes. Despite these advances, examples of cooperative interactions involving multiple low-valent main-group element centers remain rare. Such cooperativity is of great interest because the presence of multiple low-valent centers facilitates enhanced multielectron transfer capabilities. Consequently, advancing the design and synthesis of multinuclear low-valent main-group compounds holds great promise for unlocking new reactivity in main-group chemistry.This Account details our studies of the synthesis of heavier tetrylene-stabilized low-valent main-group compounds and their applications in cooperative bond activation and catalysis. We describe the design of new types of multidentate silylene ligands and demonstrate their effectiveness in stabilizing boron(I) and aluminum(I) compounds, referred to as borylene and aluminylene, respectively. The cooperation between B(I)/Si(II) and Al(I)/Si(II) centers enables the cleavage of various bonds, including the N-H bond in aniline, the C=O bond in ketones and carbon dioxide, the N=O bond in nitrosoarenes, and the C≡O bond in carbon monoxide. These compounds serve as effective precatalysts for carbon dioxide reduction and the reductive coupling of nitrosoarenes to azoxyarenes, respectively. Using a bis(germylenyl)carborane ligand, we have isolated zerovalent group 14 compounds, such as stannylone and plumbylone. The cooperation between Sn(0)/Ge(II) and Pb(0)/Ge(II) centers enables multiple electron transfers to cleave the N=O bonds of nitrous oxide and nitro compounds. The stannylone acts as an efficient precatalyst for the deoxygenation of nitrous oxide and nitro compounds, leading to the formation of dinitrogen and hydrazines, respectively. These results provide a unique proof-of-concept, underscoring their potential as versatile platforms for challenging bond activation and catalysis.

The widespread occurrence of Pepper mild mottle virus (PMMoV) in aquatic environments presents substantial risks to agricultural safety and ecosystem integrity. This study reports the synthesis of an endogenous copper-modified biochar (ECu‑BC800) through one‑step pyrolysis of copper hyperaccumulator plant dayflower (Commelina communis L.) biomass for peroxymonosulfate (PMS) activation and efficient PMMoV inactivation. Systematic characterization revealed that the endogenous doping strategy enabled atomic-level dispersion of copper species as nanoclusters (< 2  nm) uniformly and stably embedded within the carbon‑nitrogen matrix, forming abundant Cu-N coordination structures and a Cu+ dominated valence state, along with a high specific surface area (98.7 m2/ g) and mesoporous structure. The ECu‑BC800/PMS system achieved rapid viral inactivation (achieving up to 5.1log10 reduction within 10 min), outperforming exogenously copper‑loaded biochar (Cu‑BC800) and pristine biochar (BC800). The system maintained good stability and adaptability across a wide pH range (3-9) and in various real water matrices, including tap water and river water. Mechanism studies showed that both radical (•SO4-, •OH and •O2-) and non‑radical (1O2) pathways contributed to inactivation. The catalyst maintained high activity over five cycles with negligible Cu leaching (0.012 mg/L). Transmission electron microscopy and infectivity assays confirmed severe structural damage and complete loss of viral infectivity. This work offers a sustainable and efficient strategy for controlling waterborne plant viruses in water.

Methylene blue (MB), typically regarded as a model dye pollutant, was repurposed as a multifunctional component to enhance the performance of metal-organic framework/cellulose nanofiber (MIL@CNF) membranes. By immobilizing MB into MIL, MB-MIL@CNF membranes were developed that integrated photosensitization, catalytic activity, and antifouling capability. The optimized MB-MIL@CNF membrane exhibited markedly enhanced water flux and achieved 93.71 % levofloxacin (LEVO) degradation under visible light irradiation, surpassing pristine MIL@CNF (59.95 %). Mechanistic studies revealed that MB acted as a photosensitizer and electronic modulator, broadening light absorption, facilitating charge transfer, and generating O-1(2) and O-center dot(2)- for efficient LEVO degradation. In addition, MB incorporation significantly improved antifouling performance through light-driven self-cleaning. Stability tests confirmed the strong adsorption of MB by MIL, without detectable leaching or secondary toxicity. Phytotoxicity assays further demonstrated that MB-MIL@CNF membranes not only eliminated LEVO-induced growth inhibition but also posed minimal ecological risk. This work transformed a conventional dye pollutant into a functional sensitizer, providing new insights into the synergistic design of sustainable, high-performance catalytic membranes for water purification.

Functional nanomaterials have been extensively applied to remediate cadmium (Cd) contaminated agricultural soil. In this study, the effects of surface-etched functionalized porous nanosilica (E-MPNS) on Cd bioavailability, the Cd fraction, Cd accumulation in vegetables, soil microorganisms, and soil quality were evaluated in detail in a pot experiment. The results showed that E-MPNS application at 1.0% significantly reduced the Cd bioavailability (DTPA-extractable Cd) from 2.35 mg·kg−1 to 0.97 mg·kg−1, the acid-soluble Cd decreased from 37.68% to 21.47% and the residual Cd increased from 14.31% to 45.76%. Simultaneously, the Cd content in edible parts of Chinese cabbage decreased from 1.01 mg·kg−1 to 0.19 mg·kg−1, with a maximum remediation efficiency of 81.19%. In addition, E-MPNS application elevated soil organic matter (from 12.81 g·kg−1 to 18.57 g·kg−1) and available silicon (from 147.88 mg·kg−1 to 341.11 mg·kg−1) contents. E-MPNS had no adverse effects on bacterial diversity and tended to increase bacterial richness. Notably, the soil ecosystem multifunctionality index increased from −0.91–0.11, indicating that the soil quality significantly improved. Cost-benefit analysis suggest that E-MPNS has a relatively low production cost of 26.39 $·kg−1. These findings indicate that E-MPNS is a promising candidate for Cd immobilization in agricultural soil and improvement of soil quality.

Dissolved black carbon (DBC), the mobile and reactive fraction released from biochar, can adsorb onto iron oxides and alter their photochemical reactivity, thereby influencing the photochemical transformation of coexisting organic pollutants. However, how DBC molecular composition, which varies with pyrolysis temperature, governs its interactions with different hematite facets, and how these interactions in turn affect organic pollutant photodegradation remains unclear. Herein, hematite nanocrystals exposing {001}, {100}, and {012} facets, and two DBCs pyrolyzed at 300 ℃ and 500 ℃ (DBC300 and DBC500), were employed to investigate DBC molecular fractionation and transformation, and their impacts on sunlight-driven tetracycline hydrochloride (TCH) photodegradation. FT-ICR MS analysis showed that the intrinsic molecular composition of DBC primarily determined its molecular fractionation and transformation, whereas hematite crystal facets mainly regulated the extent of these processes. DBC300 underwent adsorption coupled with more extensive molecular transformation, whereas DBC500 was dominated by adsorption-driven molecular fractionation. Distinct facet-dependent behaviors were observed, with {001}-dominated hematite nano-plates favoring adsorption-driven molecular fractionation, {100}-dominated hematite nano-rods exhibiting the highest surface area-normalized adsorption density, and {012}-exposed hematite nano-cubes showing the greatest potential for molecular transformation. Photodegradation experiments showed that DBC adsorption substantially inhibited TCH photodegradation on all hematite nanocrystals. Although the retained low-molecular-weight aromatic fractions slightly enhanced light harvesting, adsorbed high-MW and oxygen-rich DBC fractions primarily inhibited hematite photochemical reactivity by suppressing interfacial charge transfer and altering reactive intermediate generation. These findings highlight the role of mineral-organic interactions in regulating contaminant fate in iron-rich aquatic environments and reveal the emerging challenges associated with biochar applications.

Achieving synergy between ultra-high strength and plasticity in nanocrystalline metals remains a grand challenge, as they are typically plagued by intrinsic brittleness arising from catastrophic shear localization. Here, we overcome this limitation by engineering an oxide/nanocrystalline dual-phase (ONDP) architecture within a CoCrFeNiMn high-entropy alloy via rapid current-activated sintering. Guided by atomistic simulations and lattice misfit calculations, a high density of semi-coherent C15-Cr2MnO4 nanoprecipitates was successfully introduced via an ethylene glycol-assisted ball milling and sintering process. The fabricated alloy delivers a compressive yield strength of 4.5 GPa, which is among the highest values reported for nanocrystalline fcc metals/alloys tested by micropillar compression, while maintaining >30% uniform plasticity. Mechanistically, these semi-coherent oxides effectively suppress grain rotation and convert the nanocrystalline matrix into dislocation storage reservoirs, thereby avoiding strain localization and enabling pronounced strain hardening. This study establishes a scalable pathway for stabilizing nanostructures through O-induced dual-phase engineering, offering a blueprint for next-generation high-performance structural materials.

The creation of diverse heterogeneous interfaces is a key strategy for developing highly efficient electrocatalysts for the alkaline oxygen evolution reaction (OER). This paper reports an easy two-step synthesis of a trimetallic (NiCoFe) sulfide catalyst with a 0D-2D hybrid structure via a competitive co-deposition strategy. Unlike conventional hydrothermal or coprecipitation methods, this strategy enables the simultaneous formation of 0D nanoparticles and 2D nanosheets on carbon nanotubes (CNTs), achieving uniform dispersion and robust anchoring of the 0D nanoparticles on the 2D nanosheets, forming abundant and stable heterogeneous interfaces. This effectively prevents the agglomeration of 0D nanoparticles. Coupled with CNTs, an efficient electron transport network is established, significantly enhancing local charge transfer efficiency and intrinsic catalytic activity. The resulting catalyst exhibits an exceptionally low overpotential of 260 mV at 100 mA cm-2 for the OER in alkaline media. When employed in an anion exchange membrane water electrolyzer (AEMWE), it demonstrates remarkable durability, operating stably for over 500 h at a high current density of 65 °C, 100 mA cm-2 in 1 M KOH without performance decay. Using X-ray absorption fine structure (XAFS) spectroscopy, we demonstrated the electronic coupling mechanism at the interface between CNTs and the ternary metal sulfide. This work highlights the critical role of interface engineering and co-deposition competitive strategy in applications and preparation of 0D-2D sulfide catalysts, but also provides new insights into the rational design of advanced non-precious metal electrocatalysts.

Lakes play a pivotal role in the global carbon cycle and climate change mitigation by sequestering carbon. However, under combined human and climate pressures, it remains uncertain whether increased organic carbon burial flux (OCBF) necessarily corresponds to stable carbon sequestration. Here, we utilized MAOC% as the key indicator of organic carbon pool stability (OCPS), complemented by grain size and isotopic signatures from high resolution sedimentary records, to investigate the mechanisms underlying the decoupling between OCBF and OCPS in Dongting Lake. Results showed that OCBF and OCPS responded nonlinearly to sedimentary transitions, explaining 72% and 46% of their respective variance (p < 0.001). In East Dongting, OCBF peaked at 350.30 ± 253.51 g C m⁻² yr⁻¹, primarily driven by eutrophication enhanced autotrophic production. However, the rapid burial of labile organic matter likely overwhelmed the available capacity for stable mineral association, contributing to a marked decline in the proportion of mineral associated organic carbon (MAOC%). This imbalance ultimately weakened the OCPS. In contrast, West Dongting maintained a consistently high MAOC% (94.63%) due to sustained inputs of fine minerals from upstream channel scouring. This mineral supply promoted persistent organic mineral associations, resulting in continuously enhanced OCPS despite a relatively lower burial flux (250.60 ± 61.00 g C m⁻² yr⁻¹). These findings provide robust evidence that high OCBF does not necessarily indicate a stable carbon sink. We therefore emphasize that a multidimensional assessment framework integrating carbon flux and stability is essential for developing spatially differentiated and effective lake carbon management strategies.

Abstract Room-temperature mid- and far-infrared photodetectors are critical for next-generation sensing and communication, yet their development is severely hindered by the prohibitive cooling requirements of conventional state-of-the-art materials and the restricted 1200 nm cut-off wavelength of emerging earth-abundant absorbers like kesterite Cu2ZnSnSe4 (CZTSe). Herein, we propose a dual-site isovalent engineering paradigm of heavy-cation substitution coupled with light-anion compensation to shatter the intrinsic optoelectronic limits of CZTSe. Combining comprehensive first-principles calculations and macroscopic device simulations, we systematically investigate the Cu2ZnPbxSn1–xSe4–ySy solid solution series. The isomorphous substitution of Sn with bulky Pb atoms triggers a profound bandgap collapse down to an ultranarrow 0.042 eV via intense localized orbital reconstruction, successfully extending the absorption edge deep into the extreme far-infrared regime. Concurrently, gradient S alloying at the Se sites induces a uniform lattice contraction, which effectively relieves steric strain and precisely widens the bandgap, fundamentally suppressing the thermal generation-recombination dark currents inherent to narrow-bandgap architectures. Striking an optimal balance between bandgap engineering and carrier dynamics, the simulated room-temperature photodetector delivers a peak specific detectivity exceeding 1.5 × 1012 Jones and an unprecedented panchromatic response with a cut-off wavelength up to 29,500 nm. This synergistic compositional design strategy provides a robust atomic framework and a highly competitive material platform for the development of uncooled, ultra-broadband infrared optoelectronics.

Cell-free biosensing systems offer programmable, rapid, and low-cost molecular detection, which have been applied in nucleic acid assays frequently, but mostly rely on multiple enzymes and separate amplification steps which limit their application. In this study, using miRNA-21 as a model target, a single-tube, isothermal, cell-free biosensing platform that integrates SplintR ligase-mediated template assembly with T7 RNA polymerase-driven, product-assisted autocatalytic transcriptional cycling has been developed. The presence of target miRNA triggers the ligation of two DNA probes to form a functional transcription template, initiating the synthesis of light-up RNA aptamers through the cell-free system. The transcribed aptamer also re-enters the reaction as an RNA "splint", regenerating new templates and triggering additional transcription rounds, thereby establishing an autocatalytic signal amplification under constant conditions. The one-pot workflow does not require reverse transcription, thermocycling, or separate pre-amplification, minimizing hands-on steps and reducing contamination risk. The produced RNA aptamer can bind with a cognate fluorogenic dye to produce fluorescence signal and this can be used for target quantification. The platform achieves a detection limit of 0.52 pM with a linear range of 1 pM-1 μM, and demonstrates high specificity against closely related miRNA sequences. The proposed system was successfully applied to detect target in clinical serum samples, yielding satisfactory results. This work presents a rapid, sensitive, and easy-to-use strategy for miRNA quantification, offering a robust tool for point-of-care testing and liquid biopsy applications.

High-energy–density lithium metal batteries, either liquid or solid state, require ultrathin Li anodes, but their implementation is hindered by poor Li processability in fabrication and inhomogeneous Li plating behaviours upon cycling. This work addresses these challenges through a mask-patterned discrete array using a molten salt-derived Li nanocomposite. The screen-printing strategy circumvents the poor wettability of molten Li on copper that causes high Li|Cu contact angle and non-uniform Li spreading, thus fabricating ultrathin Li foils with equivalent thicknesses below 30 μm. Concurrently, the molten salt-derived inorganic nanoparticles in Li favour homogeneous Li deposition and induce inorganic-rich solid electrolyte interphase to jointly suppress active Li consumption. The resulting Li array (10–28 μm) anodes demonstrate remarkable performance in both liquid- and solid-state systems, achieving high energy densities up to 504 Wh kg−1/1071 Wh L−1 and stable cycling over 260 cycles with high-loading cathodes. This integrated approach resolves both fabrication and cycling challenges of ultrathin Li anodes and offers an alternative solution for high-performance liquid-/solid-state batteries.

Seahorse products face rampant counterfeiting due to their high value and low production. The determination of species-specific DNA sequences is a key factor in identifying species. A conserved genetic fragment in the seahorse genome has been identified as a specific marker. In this study, a novel cell-free transcription system-based fluorescence biosensor has been designed and applied for seahorse product authenticity identification. A toehold-mediated triplex DNA complex has been designed. Within this complex, a single-stranded DNA (ssDNA) component is designed to hybridize with two other incomplete template strands, forming a complete aptamer transcription template. The target seahorse DNA, which exhibits greater complementarity with the other two strands in the triplex complex, can displace the ssDNA upon its presence and trigger a strand displacement reaction. The released ssDNA can be removed using magnetic beads easily since it is modified with biotin. The absence of ssDNA in the system prevented the formation of the complete transcription template, which inhibited the recognition by T7 RNA polymerase and reduced subsequent RNA transcription through the cell-free transtcription system. The resultant reduction in RNA production diminishes its binding to fluorescent aptamers, leading to a decrease in the detected fluorescence signal. Under optimized assay conditions, the fluorescence signal difference exhibited a linear correlation with the logarithm of seahorse DNA concentration over the range of 150 pM to 35 nM, achieving a limit of detection (LOD) of 65 pM. The proposed system has good reproducibility and selectivity, and has been successfully applied to seahorse product identification.

Flexible piezoresistive pressure sensors integrating high sensitivity,broad linear detection range,and excellent stability are crucial for wearable electronics and human-machine interfaces.However,achieving a balanced improvement in these performance metrics remains a challenge.Herein,we propose and fabricate a high-performance flexible pressure sensor based on a chitosan/hydroxylated carbon nanotubes(CTS/CNTs-OH)composite fabric.Benefiting from the inherent antibacterial properties of chitosan and the synergistic effect with hydroxylated carbon nanotubes,the composite fabric and the sensor exhibit excellent antibacterial performance,which can effectively avoid sensor performance degradation and human skin discomfort caused by microbial growth in wearable scenarios.In addition,the chitosan-based fibrous network endows the sensor with good biocompatibility,breathability,and mechanical compliance,making it suitable for long-term skin-contact wearable applications.By optimizing the electrophoretic deposition process and the fabric layering structure,the sensor demonstrates outstanding overall performance:a broad detection range of up to 100 kPa,a maximum sensitivity of 0.151 kPa-1,and excellent linearity(R2>0.999)across a wide pressure range.Notably,the multilayer fabric architecture enables a continuous evolution of interfacial contact under external pressure,which contributes to the simultaneous achievement of high sensitivity and a wide linear sensing range.Under dynamic pressure testing,the sensor exhibits fast response(6 ms)and recovery(46 ms)times,and it is capable of detecting subtle pressures as low as 0.98 Pa.Such rapid response characteristics allow the sensor to accurately capture both static and dynamic mechanical stimuli associated with human motions.The sensor maintains highly stable electrical output after more than 8000 loading-unloading cycles at 100 kPa,confirming its remarkable mechanical durability.For practical demonstrations,relying on its excellent antibacterial and sensing properties,the sensor was successfully employed for real-time monitoring of various human motions.Combined with a deep learning model based on a convolutional neural network(CNN),it achieved high-accuracy classification of eight types of human activities,with an overall recognition accuracy exceeding 99%.These results highlight the strong compatibility between the proposed sensor and data-driven intelligent recognition algorithms.This work provides an effective material and structural design strategy for developing high-performance,wearable flexible sensing systems,especially suitable for the wearable electronics field requiring biocompatibility and antibacterial properties.

Large floodplain wetlands are increasingly affected by reservoir regulation, declining sediment supply, and vegetation succession, yet the relationships between water–sediment dynamics and wetland carbon stocks across spatial and temporal scales remain poorly understood. Using Landsat time-series imagery from 1994 to 2023 and field measurements, we assessed long-term vegetation succession and changes in soil carbon stocks (STC) and aboveground vegetation carbon stocks (VTC) in Dongting Lake wetlands. Over the past 30 years, extensive transitions occurred between Carex and Phragmites australis (P. australis) communities, with conversion from Carex to P. australis being the dominant pathway. Area-weighted carbon stocks increased by approximately 5.66 × 10⁶ Mg C overall despite substantial interannual fluctuations, and were consistently higher in East Dongting Lake than in West and South Dongting Lake. Flooding frequency showed the highest explanatory power for spatial variation in carbon stocks (q = 0.564), whereas sediment transport was significantly negatively correlated with interannual changes in both STC and VTC. Approximately 18.6% of the wetland area experienced declining carbon stocks and largely overlapped with vegetation degradation zones, indicating scale-dependent relationships between water–sediment dynamics and wetland carbon stocks. Wetland management should prioritize seasonal hydrological connectivity, strengthen monitoring of degraded areas, and adopt region-specific strategies according to local water and sediment conditions. This framework provides a reference for carbon-stock assessment and adaptive management in large floodplain wetlands affected by flow regulation and declining sediment supply.

Flexible sensors are widely used in emerging intelligent systems giving the ability to perceive and interact with complex environments through multimodal signals. However, most existing devices rely on spatially separated or independently acquired modalities, limiting synchronous perception, introducing crosstalk and hindering robust data fusion. Here we present a bio-inspired flexible bimodal sensor that integrates co-located photoelectric and pressure sensing within a vertically stacked architecture with intrinsically decoupled outputs. The device combines a SnSexSy/PTAA heterojunction for efficient broadband photodetection with a covalently interlocked polypropylene/functionalized carbon nanotube network for highly linear, sensitive pressure sensing, achieving good responsivity, low detection limits and minimal (<1%) cross-channel interference. By fusing multimodal signals, the sensor enables accurate object recognition, mapless robotic navigation in simulated fire and tracking soil moisture and light intensity for environmental monitoring. These results establish a material and architectural paradigm for synergistic bimodal sensing, with broad implications for embodied intelligence, human–machine interfaces and precision agriculture. A bio-inspired flexible bimodal sensor integrates co-located photoelectric and pressure sensing with decoupled outputs, enabling high-accuracy object recognition, autonomous robotic navigation and precision agricultural monitoring via synergistic data fusion.

To investigate the accumulation and potential risks of metal(loid)s in Flos Sophorae Immaturus (FSI) in a typical non-ferrous metal smelting region, fifty pairs of soil and FSI samples were collected from Jiyuan City to determine the metal(loid)s contents and evaluate their potential health risks to local FSI consumers. Results showed that the average contents of Pb, Cd, and As in the soil samples were 309.07, 5.33, and 54.37 mg/kg, with 2%, 10%, 16%, and 72% of these soils were unpolluted, slightly, moderately, and heavily polluted, respectively. Meanwhile, the contents of Pb, Cd, and As in FSI ranged from 0.75 to 41.90 mg/kg, 0.04-0.79 mg/kg, and 0.35-15.80 mg/kg, and had average contents of 4.62, 0.18, and 1.89 mg/kg, respectively. Approximately 85.8% of metal(loid)s in FSI were accumulated from soil, and the proportion of As accumulated from soil was the highest (95%), followed by Pb (84%) and Cd (79%). In addition, soil organic matter and available phosphorus were the main factors influencing metal(loid)s accumulation in FSI. Health risk assessment revealed that the average and 95% percentile non-carcinogenic risk index (for Cd and As) and total carcinogenic risk were all higher than the reference value. The margin of exposure analysis for Pb further revealed that merely exposure to Pb via FSI can also pose adverse effects on the health of children. These results indicate that the metal(loid)s in FSI pose serious potential health risks to local consumers.