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Ab initio calculations are used to theoretically study the intermolecular aza-Wittig reaction. This provides a new way in the synthesizing of amino acids.

The use of chemical ionization mass spectrometry to provide an efficient means to study intermediate radicals formed in the reactions of toluene is described. The kinetics reaction mechanisms of aromatic hydrocarbons in the atmosphere can thus be investigated.

Gold as a hydrogen-sensing electrode for in situ measurement of dissolved H2 in aqueous solutions under extreme conditions is reported. The dissolved H2 sensor, constructed with a Au-based sensing element and coupled with a YSZ/HgO/Hg electrode, is well suited for determining dissolved H2 concentrations of aqueous fluids at elevated temperatures and pressures. The Au electrode is made of Au wire mounted in a quartz bar, which can be pressurized and heated in the high-pressure and -temperature conditions. The Au-YSZ sensor has been tested for its potential response to the concentrations of dissolved H2 in fluids by using a flow-through reactor at high temperatures up to 400 °C and pressures to 38 MPa. Good sensitivity and linear response between the hydrogen concentrations in the fluids and the H2 sensor potentials are reported for hydrogen gas in the concentration range of 0.1-0.001 M H2 in aqueous fluids at temperatures up to 340 °C and 30 MPa. Nernstian response of the cell potential to dissolved H2 in fluids was determined at 340 °C and 30 MPa, described as follows: ΔE =0.9444 + 0.0603 log mH2 The experimental results indicate that the Au-YSZ/HgO/Hg cell can be used to measure the solubility of H2 in aqueous fluid at temperatures and pressures near to the critical state of water. Thus, this type of Au hydrogen sensor could be easily used for in situ measurement of H2 in hydrothermal fluids in a high-pressure vessel, or at midocean ridge, due to its structure of compression resistance. [ABSTRACT FROM AUTHOR]

The assembly of small water clusters (H2O)n, n = 1−6, on a graphite surface is studied using a density functional tight-binding method complemented with an empirical van der Waals force correction, with confirmation using second-order Møller−Plesset perturbation theory. It is shown that the optimized geometry of the water hexamer may change its original structure to an isoenergy one when interacting with a graphite surface in some specific orientation, while the smaller water cluster will maintain its cyclic or linear configurations (for the water dimer). The binding energy of water clusters interacting with graphite is dependent on the number of water molecules that form hydrogen bonds, but is independent of the water cluster size. These physically adsorbed water clusters show little change in their IR peak position and leave an almost perfect graphite surface. [ABSTRACT FROM AUTHOR]

In the current work, lychee pulp was subjected to Lactiplantibacillus plantarum ATCC 14917 fermentation, leading to a substantial increase (2.32-2.67-fold) in water-soluble polysaccharides (WSP). Concurrently, a significant degradation occurred in water-insoluble polysaccharides (WISP) composed of glucose (28.73%), arabinose (28.25%), galacturonic acid (25.07%), and galactose (11.00%). To clarify polysaccharide conversion and its relevant mechanism, carbohydrate-active enzyme encoding sequences in the L. plantarum ATCC 14917 genome and structural alterations of two polysaccharide fractions were dissected. By integrating the transcriptional assay, prokaryotic expression, and enzymic hydrolysis, three endoglucanases were demonstrated to catalyze WISP degradation, leading to WSP accumulation during lychee pulp fermentation with L. plantarum ATCC 14917. Reductions in proportions of galactose and galacturonic acid in WSPs were partly attributed to the actions of multiple galactosidases. These findings provide an enzyme-based explanation for WSP accumulation during Lactobacillus fermentation and serve as a practical foundation for directional polysaccharide conversion.

Photoelectrochemical (PEC) water splitting for hydrogen production is a promising technology for sustainable energy generation. In this work, we introduce Nd sites boost the PEC performance of Fe 2 O 3 photoanodes through a precise gas-phase cation exchange process, which substitutes surface Fe atoms with Nd. The incorporation of Nd significantly enhances charge transfer properties, increases carrier concentration, and reduces internal resistance, leading to a substantial increase in photocurrent density from 0.44 to 0.92 mA cm -2 at 1.23 V RHE . Further enhancement of catalytic activity was achieved by depositing a NiCo(OH) x layer and a photocurrent density of 1.15 mA cm -2 at 1.23 V RHE were obtained. Theoretical calculations corroborate these experimental results, revealing that Nd doping narrows the bandgap, improves charge separation efficiency, and lowers the reaction potential barrier, thereby accelerating water oxidation kinetics. These findings underscore the effectiveness of surface cation exchange and targeted metallic element doping in overcoming the intrinsic limitations of Fe 2 O 3 , providing a viable pathway for developing high-performance PEC systems for efficient hydrogen production.

The trade-off between the performances of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) presents a challenge in designing high-performance aqueous rechargeable zinc-air batteries (a-r-ZABs) due to sluggish kinetics and differing reaction requirements. Accurate control of the atomic and electronic structures is crucial for the rational design of efficient bifunctional oxygen electrocatalysts. Herein, we designed a Sn-Co/RuO 2 trimetallic oxide utilizing dual-active sites and tin (Sn) regulation strategy by dispersing Co (for ORR) and auxiliary Sn into the near-surface and surface of RuO 2 (for OER) to enhance both ORR and OER performances. Both theoretical calculations and advanced dynamic monitoring experiments revealed that the auxiliary Sn effectively regulated the atomic/electronic environment of Ru and Co dual-active sites, which optimized the *OOH/*OH adsorption behavior and promoted the release of the final products, thus breaking the reaction limits. Therefore, the as-designed Sn-Co/RuO 2 catalysts exhibited superb bifunctional performance with an oxygen potential difference (Δ E ) of 0.628 V and negligible activity degradation after 200,000 (ORR) or 20,000 (OER) CV cycles. The a-r-ZABs based on the Sn-Co/RuO 2 catalyst exhibited a higher performance at a wide temperature range of -30 to 65 °C. They demonstrated an ultralong lifespan of 138 days (20,000 cycles) at 5 mA cm -2 , 39.7 times higher than that of Pt/C + IrO 2 coupled catalysts at a low temperature of -20 °C. Additionally, they maintained an initial power density of 85.8% after long-term tests, significantly outperforming previously reported catalysts. More importantly, the a-r-ZABs also showed excellent stability of 766.45 h (about 4598 cycles) at a high current density of 10 mA cm -2 .

Kerogen is a key source of hydrocarbon production through hydraulic fracturing. However, the direct correlation between the molecular structure and mechanical properties remains unclear. Here, we employ four-dimensional scanning transmission electron microscopy (4D-STEM) to reveal heterogeneities defined by the orientation of π-π stacking domains and amorphous regions in kerogen. We observed that the morphologies of π-π stacking domains vary with kerogen maturity, ranging from small, randomly oriented grains to larger, continuous structures. Furthermore, we conduct in situ 4D-STEM tensile testing to visualize the strain distribution across these structural heterogeneities and elucidate the governing deformation mechanisms of kerogen. Our results demonstrate different mechanical responses within kerogen, suggesting that π-π stacking domains contribute to brittleness, while amorphous regions promote ductility. We believe this innovative approach to assessing the correlation between local structural order and the mechanical properties of kerogen could lead to improved geological models for optimizing the hydraulic fracturing efficiency.

As natural agonists of the stimulator of interferon genes (STING), cyclic dinucleotides (CDNs) have been identified as promising immunotherapies that trigger a potent immune response against tumors. However, the low stability, rapid clearance, inadequate cellular uptake, and inefficient cytosol localization heavily hinder the therapeutic efficacy of the hydrophilic and negatively charged 2', 3'-cyclic-GMP-AMP (cGAMP). How to efficiently deliver cGAMP into the endoplasmic reticulum (ER) to activate STING for immune priming remains challenging. Here, we report a pH-responsive and guanidinium-rich STING nanoagonist (nPGSA) for cytosol delivery of cGAMP. Compared with free cGAMP, nPGSA achieves up to a 37.4-fold enhancement of cellular internalization. The pH-sensitive and guanidinium-functional design facilitates quick release and endosome escape, thus enabling precise ER targeting of cGAMP and 33.9-fold amplification of STING sensibilization. Furthermore, through the modulation of tumor-associated macrophage (TAM) polarization, nPGSA elicits a potent antigen-specific cellular immune response and sustained tumor regression in melanoma- and neuroblastoma-bearing mice. Our study provides a promising strategy for the delivery of cGAMP, and it offers insights into the function of cGAMP in modulating the tumor immune microenvironment for cancer immunotherapy.

Diffusion is a ubiquitous process that is strongly correlated with concentration. Based on developed three-dimensional free energy and a continuous-time random-walk coarse-graining method, we found the optimal diffusion pathway under confinement, determined all diffusional energy barriers, and identified the major units of zeolite where molecular diffusion is limited. Interestingly, a novel diffusion mechanism was determined in the nanopore of a zeolite catalyst by molecular dynamics simulation, pulsed field gradient, and 2D exchange spectroscopy (EXSY) NMR experiments. We describe a "molecular self-gating effect" that effectively predominates the diffusion process in cage-type (e.g., RHO and MER) zeolites through a "traffic jam" and a "smooth traffic" process. Initially, transport is hindered by molecules forming a gate (traffic jam); then, as the number of molecules reaches a certain threshold, diffusion increases rapidly due to the synergistic collisions of aggregated molecules upon the gate (smooth traffic). This unique diffusion behavior is observed here for the first time and illustrates a microscopic mechanism dictated by the molecular self-gating effect in a confined space. The exploitable diffusion disclosed herein should shed new light on the fundamental understanding of transport, as well as enrich diffusion behavior under confinement.

Nitrogen-containing organic compounds (NOCs) in frost serve as a critical pathway for atmospheric nitrogen deposition, significantly impacting the biogeochemical cycles of nitrogen. However, the molecular characteristics of NOCs in frost and their deposition fluxes are scarcely studied. In this work, frost samples, collected in rural Northeast China in the winter of 2023, were analyzed using nontargeted ultrahigh performance liquid chromatography-orbitrap mass spectrometry (UHPLC-Orbitrap MS) to reveal their content in nitrogen-containing organic compounds (NOCs) and explore their wet deposition fluxes. The average number of assigned molecular formulas were lager on hazy days compared to nonhazy days for both water-soluble (WSOM) and water-insoluble organic matter (WISOM) in frost (3114 vs. 1934 for WSOM and 3042 vs . 2224 for WISOM in electrospray ionization (ESI-); 6921 vs . 5954 for WSOM and 6629 vs. 5547 in ESI+). Specifically, the number proportions of CHON were 35.6-49.9% (724-1517) and 47-51.1% (2686-3388) in the ESI- and ESI+ modes, respectively. Nitrophenol (C 6 H 5 NO 3 ) and methyl nitrophenol (C 7 H 7 NO 4 ) were the most abundant NOCs, with wet deposition fluxes (at maximum average concentrations) of 22.2 and 21.2 μg m -2 ·h -1 , respectively. On hazy days, the deposition fluxes of nitrophenol compounds reached up to 1.73 times that of nonhazy days, indicating significant ambient nitrogen deposition during the haze episode. This deposition flux positively correlated with PM 2.5 concentration, implying the important role of atmospheric particulates in influencing NOC deposition through frost. These findings highlight the susceptibility of frost to capturing NOCs from the atmosphere, potentially impacting nitrogen cycling in ecosystems.

Lomefloxacin (LOM) is an efficacious antibiotic that might lead to liver damage and other adverse reactions if consumed over an extended period. Hence, this study proposed a DNAzyme-mediated DNA walker as a signal amplifier in combination with a substantial quantity of Au nanoparticle (NP)-loaded hydrogen-bonded organic frameworks (HOFs) as a surface-enhanced Raman scattering (SERS) substrate to accomplish the highly sensitive detection of LOM in food. Crucially, due to their high specific surface area and strong adsorption capacity, HOFs act as an ideal substrate for the in situ growth of a large amount of Au NPs, which exhibit a robust and uniform SERS enhancement. Once the target LOM was presented, the DNAzyme was activated to start the DNA walker and produce single DNA in abundance, which further triggered the catalytic hairpin assembly (CHA) cycle. In addition, the multi-interstitial core-shell structure of Au@Ag@4-nitrobenzenethiol (4-NTP)@Au@Hp3 produced more SERS "hot spots" and significantly amplified the local electromagnetic field, with HOF@Au synergistically strengthening the Raman signal of 4-NTP. Using this principle, this sensor achieved the ultrasensitive detection of LOM through the "signal on" strategy, with a detection limit as low as 4.62 × 10 -14 mol/L. This strategy explored a meaningful innovative path for the design of a novel SERS biosensor for the sensitive and selective detection of antibiotics in food.

In clinical practice, mini-screws of titanium-6-aluminum-4-vanadium alloy with an extra low interstitial (ELI) grade (Ti-6Al-4V ELI) are widely used as orthodontic anchorages. However, in orthodontic treatment, Ti-6Al-4V mini-screw failure because of peri-implantitis is a major challenge. To prevent damage caused by peri-implantitis, we developed a novel Ti-6Al-4V disc/screw coated with poly(lactide- co -glycolide) incorporating fisetin, a naturally occurring flavonoid with anti-inflammatory and antiosteoclastogenic/osteogenic properties. Sustained fisetin release from the Ti-6Al-4V disc and its anti-inflammatory and antiosteoclastogenic/osteogenic differentiation properties were demonstrated using in vitro cell culture experiment. In addition, in a rat model of peri-implantitis, sustained fisetin release from the Ti-6Al-4V screw suppressed inflammation progression, reduced alveolar bone resorption, and stabilized screw movement. These findings highlight sustained fisetin-release Ti-6Al-4V screws as a promising strategy for enhancing orthodontic mini-screw stability and success through peri-implantitis prevention.

Electronic nose (E-nose) has been applied many times for exhale biomarker detection for lung cancer, which is a leading cause of cancer-related mortality worldwide. These noninvasive breath testing techniques can be used for the early diagnosis of lung cancer patients and help improve their five year survival. However, there are still many key challenges to be addressed, including accurately identifying the kind of volatile organic compounds (VOCs) biomarkers in human-exhaled breath and the concentrations of these VOCs, which may vary at different stages of lung cancer. Recent research has mainly focused on E-nose based on a metal oxide semiconductor sensor array with proposed single gas qualitative and quantitative algorithms, but there are few breakthroughs in the detection of multielement gaseous mixtures. This work proposes two hybrid deep-learning models that combine the Transformer and CNN algorithms for the identification of VOC types and the quantification of their concentrations. The classification accuracy of the qualitative model reached 99.35%, precision reached 99.31%, recall was 99.00%, and kappa was 98.93%, which are all higher than those of the comparison algorithms, like AlexNet, MobileNetV3, etc. The quantitative model achieved an average R 2 of 0.999 and an average RMSE of only 0.109 on the mixed gases. Otherwise, the parameter count and FLOPs of only 0.7 and 50.28 M, respectively, of the model proposed in this work were much lower than those of the comparison models. The detailed experiments demonstrated the potential of our proposed models for screening patients with early stage lung cancer.

Diabetic wounds are highly susceptible to bacterial infection, which can lead to the formation of bacterial biofilms, making diabetic wound healing a major challenge. In this study, a composited microneedle that incorporated drug-loaded conjugated polymer nanoparticles and basic fibroblast growth factor was prepared to eliminate biofilms and promote vascular regeneration. This microneedle released minocycline under near-infrared (NIR) light, effectively penetrating bacterial biofilms. The photothermal properties of the conjugated polymers, combined with the antibacterial action of minocycline, contribute to the eradication of biofilms and the elimination of drug-resistant bacteria. Moreover, it regulated the wound microenvironment by reducing the level of oxidative stress, as well as the production of inflammatory factors at the wound site. Meanwhile, it effectively boosted cell migration and promoted angiogenesis to accelerate diabetic wound healing. This composited microneedle for biofilm elimination represents a promising approach for promoting diabetic wound healing.

Real-time monitoring of dynamic microvesicles (MVs), vesicles associated with living cells, is of great significance in deeply understanding their origin, transport, and function. However, specific labeling MVs poses a challenge due to the lack of unique biomarkers that differentiate them from other cellular compartments. Here, we present a strategy to selectively label MVs by evaluating a series of lipid layer-sensitive cationic indolium-coumarin fluorescent probes (designated as IC-C n , with n ranging from 1 to 18) that feature varying aliphatic side chains (C n H 2 n +1 ). Through in situ cell imaging and analysis, we found that IC-C n location is highly related to their lipophilicities and the phospholipid layer hydrophobic microenvironments in cellular compartments. In detail, IC-C1 and IC-C2 specifically localize MVs both inside and outside cells. In contrast, IC-C3, IC-C4, and IC-C5 label cellular MVs and mitochondria but with distinct fluorescence lifetimes. Using these probes strategically, we have discovered that, in addition to the biogenesis of MVs from plasma membranes and damaged mitochondria, newly formed MVs can undergo fusion and fission processes. Moreover, mitochondria-derived MVs, beyond being released from parent cells, can fuse with lysosomes to facilitate the removal of dysfunctional mitochondria. The work not only provides new insights into MV physiology but also inspires the design strategies for probes used in specific labeling in cell studies.

Selenopeptides can be ideal dietary selenium (Se) supplements for humans. Currently, rice is not used much as a source of selenopeptides. Here, we executed the selenopeptidomics analysis of selenium-enriched rice protein hydrolysates using the full MS-dd-MS2 acquisition method and identified selenopeptides, including L{Se-Met}AK and other selenopeptides. Specifically, selenomethionine (SeMet) replaced methionine (Met) in the rice protein-Oryzain alpha chain (EC: 3.4.22) and generated a selenopeptide L{Se-Met}AK (molecular formula: C 20 H 38 N 5 O 5 Se) during subsequent protein hydrolysis. This selenopeptide was in 425-428 amino acid residues of the Oryzain alpha chain. Thermal processing led to selenopeptide cleavage, which affected the efficient retention of selenopeptides. Activation energy ( E a ) was used to locate the quality control markers in the thermal degradation of selenopeptides. Therefore, this study established the thermal degradation rate equation for the selenopeptide L{Se-Met}AK at 100 °C, 110 and 120 °C; and identified the pyrolysis products, including L{Se-Met}A, LMA, LMAK, K 1 , and K 2 , involving C-N cleavage on the amide bond of alanine and lysine, C-Se bond cleavage and C-N cleavage on the amide bond of alanine and Met; the fit coefficients of the thermal reaction models were ≥0.9248, which could accurately quantify the real-time pyrolysis kinetic process; and LMAK had a lower E a of 88.20 kJ/mol, which made it easier to produce. In summary, LMAK can be used as a quality control marker in the pyrolysis process, providing technical support for the efficient retention of selenopeptides.

Volatile organic compounds (VOCs) play a key role in plant communication with other organisms in the natural environment. However, the regulatory role of the phytohormone ethylene in volatile production in plants remains unclear. In this study, we demonstrated that the application of an ethylene precursor and amplification of ethylene signaling make rice plants more attractive to brown planthopper (BPH) females for feeding and oviposition. A combination of transcriptome and VOCs analyses indicated that overexpression of OsEIL1 , a master transcription factor in the ethylene pathway, influences the transcript levels of several terpene synthase genes as well as the production of volatile terpenes. Further investigation revealed that the expression of the limonene synthase gene, OsTPS19 , was down-regulated in OsEIL1 -overexpressing rice plants, leading to a decrease in limonene production and release. Genetic analysis confirmed the essential role of limonene in the OsEIL1-mediated attractiveness of rice plants to BPH. Our findings provide new perspectives for understanding the role of ethylene signaling in volatile-mediated plant-insect interactions.

Single-crystal Au(111), renowned for its chemically inert surface, long-range "herringbone" reconstruction, and high electrical conductivity, has long served as an exemplary template in diverse fields, e.g. , crystal epitaxy, electronics, and electrocatalysis. However, commercial Au(111) products are high-priced and limited to centimeter sizes, largely restricting their broad applications. Herein, a low-cost, high-reproducible method is developed to produce 4 in. Au(111) single crystals from commercial Au foils, via an abnormal grain growth process. This methodology involves the initial preparation of a (100)-textured Au polycrystalline foil, followed by the evolution and continuous expansion of an Au(111) abnormal grain through one-site stress loading and stress-relief annealing in an Ar/H 2 atmosphere. Theoretical simulations indicate that stress/strain and high-temperature treatments in the H 2 atmosphere induce an intermediate disordered state, facilitating the evolution from polycrystalline Au(100) foil to single-crystal Au(111) foil. Furthermore, the resulting Au(111) foils have been utilized as model substrates for the oriented growth of two-dimensional transition metal dichalcogenides and their heterostructures with graphene. This work hereby puts forward an effective approach for large-scale, cost-effective production of metal single crystals, potentially revolutionizing their applications across various fields, from materials sciences to electronics and catalysis.

Treatment of tumor brain metastases remains challenging due to the ineffectiveness of drugs in crossing the blood-brain barrier (BBB). Here, we proposed a potential strategy to target and modulate the meningeal lymphatic system for immunotherapy of breast cancer brain metastases (BCBM) through peripheral administration. CT/fluorescence dual-modality imaging demonstrated that the phospholipid nanoprobe (α-PLNPs) through intracisternal magna injection effectively labeled and long-range tracked the meningeal lymphatic pathway from meningeal lymphatic vessels (MLVs) to periphery drainage cervical lymph nodes (CLNs). Interestingly, the reverse pathway from CLNs to MLVs was also successfully labeled with α-PLNPs through cervical subcutaneous injection, facilitating the noninvasive delivery of immunomodulators to the meningeal lymphatics. Given this, we used melittin-carrying α-M-PLNPs to trigger the modulation of the meningeal lymphatic reverse pathway, which effectively prevents BCBM and prolongs the survival of mice through activating the antigen-presenting cells in the CLNs and promoting the migration of CD8 + T cells into the metastatic brain tumors. This study highlights the potential of the meningeal lymphatic reverse pathway for the immunotherapy of BCBM, which holds great promise for central nervous system disease therapy without the need for drug delivery via BBB.

Metal nanoclusters (NCs), owing to their atomic precision and unique molecule-like properties, have gained widespread attention for applications ranging from catalysis to bioimaging. In recent years, proteins, with their hierarchical structures and diverse functionalities, have emerged as good candidates for functionalizing metal NCs, rendering metal NC-protein conjugates with combined and even synergistically enhanced properties featured by both components. In this Perspective, we explore key questions regarding why proteins serve as complementary partners for metal NCs, the methodologies available for conjugating proteins with metal NCs, and the characterization techniques necessary to elucidate the structures and interactions within this emerging bionano system. We also highlight the emerging applications of metal NC-protein conjugates in biomedicine, catalysis, and biosensing in which the hybrid conjugates demonstrate remarkable performance. Furthermore, key challenges hampering further development of metal NC-protein conjugates, which include understanding binding mechanisms, expanding the diversity of proteins used for conjugation, and exploiting the individual roles of metal NCs and proteins within the hybrid systems, are discussed. This Perspective aims to systemize current synthetic methodologies and design principles for metal NC-protein conjugates, adding to their acceptance in precision nanotechnology.

With the rapid development of modern industry, traditional lubricants often require a variety of additives to be used in conjunction with each other, which not only increases the cost but also causes a waste of resources. Therefore, the development of a lubricant additive with both a dyeing function and an antiwear and friction reduction performance can more effectively meet the industrial needs. Cerium sulfide (Ce 2 S 3 ), with its excellent photostability, weather resistance, thermal stability, and nontoxicity, shows great potential as an environmentally friendly pigment. However, traditional methods for synthesizing Ce 2 S 3 are typically hindered by high-temperature requirements and potential toxicity issues, which limits the broad application of Ce 2 S 3 in lubricants. To overcome these limitations, this study employed a liquid-phase method under mild conditions to synthesize oleylamine-modified, wrinkle-free Ce 2 S 3 nanosheets (OA-Ce 2 S 3 NSs). The antiwear and friction-reducing properties of OA-Ce 2 S 3 NSs in poly alpha-olefin-6 base oils were evaluated under various friction conditions with a four-ball tribometer. Experimental results indicate that OA-Ce 2 S 3 NSs significantly enhance the friction-reducing and antiwear performance of lubricants by forming a physical adsorption film and an ultra thick tribochemical reaction film (with a typical thickness of 350 nm and a maximum thickness of up to 700 nm) on the friction surface. Furthermore, the study elucidates the lubrication mechanism of OA-Ce 2 S 3 NSs and proposes their sliding mechanism on friction surfaces. This research highlights the potential of Ce 2 S 3 nanosheets as lubricant additives and provides future directions for optimizing their synthesis and multifunctional applications, offering new insights into the field of lubrication science.

Existing miniaturized spectral imagers have mutual restrictions among spatial, temporal, and spectral resolutions, making them inadequate to meet practical needs. Here, we demonstrate a spatiotemporal filter array chip to tackle the trade-off among the three resolutions for miniaturized hyperspectral imaging. A 2 × 2 Fabry-Perot filter array is embedded inside a tunable liquid crystal spectral modulator, increasing the number of filtering channels spatiotemporally in hardware, which empowers the spectral imager with high spatial, temporal, and spectral resolutions simultaneously. The tunable filter is of transmission type with the advantages of easy fabrication and large modulation. Experimental results show the proposed spectral imager has a spectral resolution of around 0.5 nm in the visible range, with a frame rate of 60 Hz and a spatial resolution of up to 25 lp/mm without postinterpolation. The proposed filter gives the best balanced performance for spectral imaging in terms of spatial, temporal, and spectral resolutions.

The intercalated two-dimensional (2D) transition metal dichalcogenides (TMDCs) have attracted much attention for their designable structures and novel properties. Among this family, host materials with low symmetry such as 1T' phase TMDCs are particularly interesting because of their potentials in inducing unconventional phenomena. However, such systems typically have low quality and poor stability, hindering further study of the structure-property relationship and applications. In this work, we intercalated Cu into 1T' MoS 2 with high crystallinity and high thermal stability up to ∼300 °C. We identified the distribution and arrangement of Cu intercalators for the first time, and the results show that Cu intercalators occupy partially the tetrahedral interstices aligned with Mo sites. The obtained Cu-1T' MoS 2 exhibits an insulating hopping transport behavior with a large temperature coefficient of resistance reaching -4∼-2%·K -1 . This work broadens the artificial intercalated structure library and promotes the structure design and property modulation of layered materials.

Previous studies on natural samples of pampaloite (AuSbTe) revealed the crystal structure of a potentially cleavable and/or exfoliable material, while studies on natural and synthetic montbrayite (Sb-containing Au 2 Te 3 ) claimed various chemical compositions for this low-symmetry compound. Few investigations of synthetic samples have been reported for both materials, leaving much of their chemical, thermal, and electronic characteristics unknown. Here, we investigate the stability, electronic properties, and synthesis of the gold antimony tellurides AuSbTe and Au 1.9 Sb 0.46 Te 2.64 (montbrayite). Differential thermal analysis and in situ powder X-ray diffraction revealed that AuSbTe is incongruently melting, while Au 1.9 Sb 0.46 Te 2.64 is congruently melting. Calculations of the band structures and four-point resistivity measurements showed that AuSbTe is a semiconductor and Au 1.9 Sb 0.46 Te 2.64 a metal. Various synthesis attempts confirmed the limited stable chemical composition of Au 1.9 Sb 0.46 Te 2.64 , identified successful methods to synthesize both compounds, and highlighted the challenges associated with single-crystal synthesis of AuSbTe.

A palladium-catalyzed tandem reaction of 1-(2-iodophenyl)-3-arylprop-2-yn-1-ones and 1-(2-azidophenyl)propargyl ethers is developed to provide the rapid construction of a fused polycyclic indenone-indole scaffold under mild conditions. The reaction proceeds via a highly ordered process involving Sonogashira coupling, propargyl-allenyl isomerization, allene-azide cycloaddition, denitrogenation, and diradical coupling. The proposed reaction mechanism is supported by experimental and computational studies.

Two series of polycyclic aromatic hydrocarbon isomers ( PT-2 and PT-3 , and P2T-V and P2T-C ) were designed and synthesized by isomerically fusing phenanthrene with thiophene and thieno[3,2- b ]thiophene, respectively. All of the new target molecules were confirmed by single-crystal X-ray analysis, and it was found that the solid-state packing can be effectively modulated through a combination of π-extended and isomeric fused strategies. Meanwhile, compared with thiophene ring-terminated isomers PT-2 and PT-3 , both having a V-shaped geometry and showing no obvious self-assembly behavior, π-extended unit thieno[3,2- b ]thiophene-terminated isomer P2T-V displays a V-shaped structure with moderate self-assembly properties and isomer P2T-C exhibits a C-shaped configuration with further enhanced self-assembly properties.

Improving interfacial stability between cathode active material (CAM) and solid electrolyte (SE) is vital for developing high-performance all-solid-state batteries (ASSBs), with compatibility issues among the cell components representing a major challenge. CAM surface coating with a chemically inert ion conductor is a promising approach to suppress side reactions occurring at the cathode interfaces. Another strategy to mitigate mechanical degradation involves utilizing single-crystalline particle morphologies. Their more robust bulk structure and lower tortuosity for charge transport, compared to polycrystalline (PC) CAMs, can significantly enhance cyclability in ASSBs. Herein, we coated a LiNbO 3 protective layer onto the free surface of quasi single-crystalline LiNi 0.83 Co 0.12 Mn 0.05 O 2 (SC83) particles. Pellet-stack ASSB cells using the LiNbO 3 @SC83 CAM and argyrodite Li 6 PS 5 Cl as SE showed a capacity retention of 88% after 1000 cycles at the 1 C rate, compared to only 71% for the uncoated counterpart and far superior to that of LiNbO 3 @PC83 (30%). The effectiveness of LiNbO 3 coating and the SC-NCM nature in mitigating electro-chemo-mechanical degradation was studied by combining modeling and physical/electrochemical characterizations. We demonstrate that the capacity decay at fast charge is due primarily to the mechanical degradation of CAM particles, while it is strongly determined by CAM|SE interfacial reactions under slow-charging conditions.

Inspired by ancient trilobites, novel curved microlens arrays (CMLAs) were designed. Direct, fast, and low-cost CMLAs with two focal planes were fabricated using ultraprecision machining technology and hot embossing technology. We designed four pairs of artificial compound eyes (ACEs) composed of large and small lenses with four different curvatures to achieve focusing and imaging on two focal planes. A test system was constructed to capture the first-order and second-order images for each level of the ACEs. Additionally, we analyzed the deformation patterns in the first-order and second-order images. The wide field of view (FOV) value was 68°, which aligns with the theoretical prediction. The focusing performance was also investigated, and the experimental results indicate that each lens achieves uniform focusing within the FOV range. These results confirm that microlens arrays with two focal planes possess advanced imaging and focusing capabilities, enabling a wide depth-of-field function. This opens new avenues for the development of advanced detectors and optical imaging devices.

Switchable selectivity achieved by altering reaction conditions within the same photocatalytic system offers great advantages for sustainable chemical transformations and renewable energy conversion. In this study, we investigate an efficient photocatalytic methanol dehydrogenation with controlled selectivity by varying the concentration of nickel cocatalyst, using zinc indium sulfide nanocrystals as a semiconductor photocatalyst, which enables the production of either formaldehyde or ethylene glycol with high selectivity. Control experiments revealed that formaldehyde is initially generated and can either serve as a terminal product or intermediate in producing ethylene glycol, depending on the nickel concentration in the solution. Mechanistic studies suggest a unique role of ionic nickel as an additional photoelectron competitor that can significantly influence selectivity, alongside its well-established function as a hydrogen evolution reaction cocatalyst under photocatalytic conditions. The demonstrated switchable selectivity provides a new tool for producing diverse products from methanol, while advancing the understanding of cocatalyst behavior for versatile catalytic performance.

For Zn metal batteries, the Zn anode faces several challenges, including Zn dendrites, hydrogen evolution, and corrosion. These issues are closely related to the Zn deposition process at the electrode/electrolyte interface. Herein, we propose interfacial engineering to protect the Zn anode and induce homogeneous deposition using conjugated cyclized polyacrylonitrile (cPAN) polymer nanofibers. It works as a hydrophobic protective layer that inhibits contact with H 2 O molecules, thus reducing side reactions and enhancing the anticorrosion property. Also, with abundant zincophilic sites on cPAN nanofibers via coordination chemistry, Zn 2+ ion transport is promoted and homogeneous dendrite-free Zn deposition is obtained. As a result, the cPAN-coated Zn (cPAN@Zn) anode demonstrates high coulombic efficiency of over 99.9%, high cycling stability of over 2000 h at 1 mA cm -2 , long cycling of over 16 000 cycles at 10 mA cm -2 , and excellent kinetics with a low overpotential below 0.15 V at 50 mA cm -2 . This work provides novel insights into organic interfacial engineering via conjugated polymers in aqueous rechargeable Zn energy storage systems.

Continuous and reagentless biomolecular detection technologies are bringing an evolutionary influence on disease diagnostics and treatment. Aptamers are attractive as specific recognition probes because they are capable of regeneration without washing. Unfortunately, the affinity and dissociation kinetics of the aptamers developed to date show an inverse relationship, preventing continuous and reagentless detection of protein targets due to their low dissociation rates. Here, we describe an in vitro aptamer isolation strategy that enriches quick-response, high-affinity bivalent protein-binding aptamers. The method is general, as evidenced by the isolation of aptamers targeting thrombin and human serum albumin. We then demonstrated the excellent regeneration capability of the isolated thrombin aptamers using biolayer interferometry. The sensors instantly responded to alternating concentration changes of thrombin at nanomolar levels (200-500 nM), reaching highly consistent equilibrium signals within 10 s. In contrast, the well-known thrombin-binding aptamers, TBA-15 and TBA-29, were not capable of regeneration. Our study provides a simple means to obtain quick-response, high-affinity protein-binding aptamers. It can also be used for the isolation of aptamer pairs, which has been demonstrated to be quite challenging. Our study also provides insights into the rational design of aptamers to control their binding thermodynamics and kinetics.

The emergence of mobile colistin resistance gene mcr-1 has attracted global attention. The prevalence of mcr-1 -positive Escherichia coli (MCRPEC) in humans largely decreased following the ban of colistin as an animal growth promoter in China. However, the prevalence of MCRPEC in the hospital environment and the relationship between disinfectants and mcr-1 remain unclear. We found that MCRPEC prevalence was low in the feces of healthy humans attending physical examinations in six hospitals (4.6%, 71/1532) but high in hospital wastewater (50.0%, 27/54). mcr-1 was mainly located on IncI2 (63.0% in wastewater and 62.0% in feces) and IncHI2 plasmids (18.5% in wastewater and 21.1% in feces). High similarity of the mcr-1 context and its carrying plasmids was observed in human and wastewater MCRPEC, with several isolates clustering together. The coexistence of the ESBL gene bla CTX-M with mcr-1 occurred in 19.7% of IncI2 plasmids. Notably, 60.0% of IncHI2 plasmids exhibited co-occurrence of mcr-1 with the disinfectant resistance gene (DRG) qacE Δ 1 , conferring resistance to quaternary ammonium compounds (QACs). We revealed that QACs, rather than the other two types of disinfectants─ ortho -phthalaldehyde (OPA) and povidone-iodine (PVP-I)─select for plasmids carrying both qacE Δ 1 and mcr-1 and elevate their conjugative transfer frequency. Monitoring of DRGs in MCRPEC and managing disinfectant use are urgently needed in healthcare settings to mitigate the spread of colistin resistance from hospital environments to inpatients.

Accurate imaging evaluations of pre- and post-treatment of cardiovascular diseases are pivotal for effective clinical interventions and improved patient outcomes. However, current imaging methods lack real-time monitoring capabilities with a high contrast and resolution during treatments. This study introduces PEGylated ultrasmall iron oxide nanoparticles (PUSIONPs), which have undergone comprehensive safety evaluations, boasting an r 1 value of 6.31 mM -1 s -1 , for contrast-enhanced magnetic resonance angiography (MRA). Systematic comparisons against common clinical methods in rabbits reveal that PUSIONPs-enhanced MRA exhibited improved vascular contrast, clearer vascular boundaries, and superior vessel resolution. Moreover, owing to their nanosize, PUSIONPs demonstrate significantly prolonged blood circulation compared to small molecular contrast agents such as Magnevist and Ultravist. This extended circulation enables captivating real-time monitoring of thrombolysis treatment for up to 4 h in rabbit models postsingle contrast agent injection. Additionally, in larger animal models such as beagles and Bama minipigs, PUSIONPs-enhanced MRA also showcases superior contrast effects, boundary delineation, and microvessel visualization, underscoring their potential to transform cardiovascular imaging, particularly in real-time monitoring and high-resolution visualization during treatment processes.

The formation of non-ion conducting byproducts on zinc anode is notoriously detrimental to aqueous zinc-ion batteries (AZIBs). Herein, we successfully transform a representative detrimental byproduct, crystalline zinc hydroxide sulfate (ZHS) to fast-ion conducting solid-electrolyte interphase (SEI) via amorphization and fluorination induced by suspending CaF 2 nanoparticles in dilute sulfate electrolytes. Distinct from widely reported nonhomogeneous organic-inorganic hybrid SEIs that exhibit structural and chemical instability, the designed single-phase SEI is homogeneous, mechanically robust, and chemically stable. These characteristics of the SEI facilitate the prevention of zinc dendrite growth and reduction of capacity loss during long-term cycling. Importantly, AZIB full cells based on this SEI-forming electrolyte exhibit exceptional stability over 20,000 cycles at 3 A/g with a charging voltage of 2.2 V without short circuits and electrolyte dry-out. This work suggests avenues for designing SEIs on a metal anode and provides insights into associated SEI chemistry.