Machine Learning-assisted Rational Design of Si-rhodamine as Cathepsin-pH Activated Probe for Accurate Fluorescence Navigation.

High-performance fluorescent probes stand as indispensable tools in fluorescence-guided imaging, and are crucial for precise delineation of focal tissue while minimizing unnecessary removal of healthy tissue. Herein, we firstly proposed machine learning-assisted strategy to investigate the current available xanthene dyes, and constructed a quantitative prediction model to guide the rational synthesis of novel fluorescent molecules with desired pH responsivity. We successfully achieved two novel Si-rhodamine derivatives and constructed the Cathepsin/pH sequentially activated probe SiR-CTS-pH. The results reveal that SiR-CTS-pH exhibits higher signal-to-noise ratio of fluorescence imaging, compared to single pH or cathepsin-activate probe. Moreover, SiR-CTS-pH shows strong differentiation abilities for tumor cells and tissues and accurately discriminates the complex hepatocellular carcinoma tissues from normal ones, indicating its significant application potential in clinical practice. Therefore, the continuous development of xanthene dyes and the rational design of superior fluorescent molecules through Machine Learning-assisted model will broaden the path and provide more advanced methods to researchers. This article is protected by copyright. All rights reserved.

The nematode effector Mj-NEROSs interacts with Rieske's iron-sulfur protein influencing plastid ROS production to suppress plant immunity.

Root-knot nematodes (RKN; Meloidogyne species) are plant pathogens that introduce several effectors in their hosts to facilitate infection. The actual targets and functioning mechanism of these effectors largely remain unexplored. This study illuminates the role and interplay of the Meloidogyne javanica nematode effector ROS suppressor (Mj-NEROSs) within the host plant environment. Mj-NEROSs suppresses INF1-induced cell death as well as flg22-induced callose deposition and reactive oxygen species (ROS) production. A transcriptome analysis highlighted the downregulation of ROS-related genes upon Mj-NEROSs expression. NEROSs interacts with the plant Rieske's iron-sulfur protein (ISP) as shown by yeast-two-hybrid and bimolecular fluorescence complementation. Secreted from the subventral pharyngeal glands into giant cells, Mj-NEROSs localizes in the plastids where it interacts with ISP, subsequently altering electron transport rates and ROS production. Moreover, our results demonstrate that isp Arabidopsis thaliana mutants exhibit increased susceptibility to M. javanica, indicating ISP importance for plant immunity. The interaction of a nematode effector with a plastid protein highlights the possible role of root plastids in plant defense, prompting many questions on the details of this process.

Stereoscopic Polymer Network for Developing Mechanically Robust Flexible Perovskite Solar Cells with an Efficiency Approaching 25.

Flexible perovskite solar cells (pero-SCs) have the potential to overturn the application scenario of silicon photovoltaic technology. However, their mechanical instability severely impedes their practical applicability, and the corresponding intrinsic degradation mechanism remains unclear. In this study, the degradation behavior of flexible pero-SCs is systematically analyzed under mechanical stress and it is observed that the structural failure first occurs in the polycrystal perovskite film, then extend to interfaces. To suppress the structural failure, pentaerythritol triacrylate, a crosslinked molecule with three stereoscopic crosslink sites, is employed to establish a 3D polymer network in both the interface and bulk perovskite. This network reduced the Young's modulus of the perovskite and simultaneously enhanced the interfacial toughness. As a result, the formation of cracks and delamination, which occur under a high mechanical stress, is significantly suppressed in the flexible pero-SC, which consequently retained 92% of its initial power conversion efficiency (PCE) after 20 000 bending cycles. Notably, the flexible device also shows a record PCE of 24.9% (certified 24.48%).

Investigation on a mobile fire extinguishing approach using liquid carbon dioxide as inert medium for underground mine.

Injecting carbon dioxide is the most effective means of preventing and extinguishing fires in sealing hazardous areas, but the traditional method slowly and remotely injects carbon dioxide gas into the well after gasification on the ground, which is dependent on the complete mine pipe network without cooling effect. To inject liquid directly from the tank with vacuum interlayer and heat insulating powder for rapid inerting and cooling, a new approach using track mobile platform to go deep into the underground mine disaster area is proposed, so the liquid can be delivered to the nozzle at the end of DN40 large diameter pipe, and the continuous gasification jet can be realized. The experimental results show that: (1) The liquid volume in a tank of vacuum degree within 2.0 Pa and 200 mm interlayer reduced no more than 15.5% after 48 days; (2) Taking the pressure in the tank as the power source, because of environmental differences inside and outside the pipe after 100 m pressure holding delivery, the physical form of liquid and gas could be converted instantly; (3) The continuous discharge time without ice blocking for a tank full of 2 m3 liquid was about 10.5 min under 25 L dual mode nitrogen pressurization, which is 1/12 of injection time after ground gasification; (4) Based on the temperature decrease trend measured at different positions, the cooling characteristics on liquid gasification jet path are quantified, and the calculation formula of temperature changing with time on the center line of liquid gasification jet is obtained. Through this new approach, the integration of vacuum insulated storage, safe mobile transportation, and continuous and rapid release with large flow can be achieved for the liquid carbon dioxide.

Regulation of the d-band center of metal-organic frameworks for energy-saving hydrogen generation coupled with selective glycerol oxidation.

The hybrid electrolyzer coupled glycerol oxidation (GOR) with hydrogen evolution reaction (HER) is fascinating to simultaneously generate H2 and high value-added chemicals with low energy input, yet facing a challenge. Herein, Cu-based metal-organic frameworks (Cu-MOFs) are reported as model catalysts for both HER and GOR through doping of atomically dispersed precious and nonprecious metals. Remarkably, the HER activity of Ru-doped Cu-MOF outperformed a Pt/C catalyst, with its Faradaic efficiency for formate formation at 90% at a low potential of 1.40 V. Furthermore, the hybrid electrolyzer only needed 1.36 V to achieve 10 mA cm-2, 340 mV lower than that for splitting pure water. Theoretical calculations demonstrated that electronic interactions between the host and guest (doped) metals shifted downward the d-band centers (εd) of MOFs. This consequently lowered water adsorption and dissociation energy barriers and optimized hydrogen adsorption energy, leading to significantly enhanced HER activities. Meanwhile, the downshift of εd centers reduced energy barriers for rate-limiting step and the formation energy of OH*, synergistically enhancing the activity of MOFs for GOR. These findings offered an effective means for simultaneous productions of hydrogen fuel and high value-added chemicals using one hybrid electrolyzer with low energy input.

Development of a Melting Curve-Based Triple Eva Green Real-Time PCR Assay for Simultaneous Detection of Three Shrimp Pathogens.

Infections with Enterocytozoon hepatopenaei (EHP), infectious hypodermal and hematopoietic necrosis virus (IHHNV), and Decapod iridescent virus 1 (DIV1) pose significant challenges to the shrimp industry. Here, a melting curve-based triple real-time PCR assay based on the fluorescent dye Eva Green was established for the simultaneous detection of EHP, IHHNV, and DIV1. The assay showed high specificity, sensitivity, and reproducibility. A total of 190 clinical samples from Shandong, Jiangsu, Sichuan, Guangdong, and Hainan provinces in China were evaluated by the triple Eva Green real-time PCR assay. The positive rates of EHP, IHHNV, and DIV1 were 10.5%, 18.9%, and 44.2%, respectively. The samples were also evaluated by TaqMan qPCR assays for EHP, DIV1, and IHHNV, and the concordance rate was 100%. This illustrated that the newly developed triple Eva Green real-time PCR assay can provide an accurate method for the simultaneous detection of three shrimp pathogens.

Stress Dissipation Driven by Multi-Interface Built-In Electric Fields and Desert-Rose-Like Structure for Ultrafast and Superior Long-Term Sodium Ion Storage.

The kinetics and durability of conversion-based anodes greatly depend on the intrinsic stress regulating ability of the electrode materials, which has been significantly neglected. Herein, a stress dissipation strategy driven by multi-interface built-in electric fields (BEFs) and architected structure, is innovatively proposed to design ultrafast and long-term sodium ion storage anodes. Binary Mo/Fe sulfide heterostructured nanorods with multi-interface BEFs and staggered cantilever configuration are fabricated to prove our concept. Multi-physics simulations and experimental results confirm that the inner stress in multiple directions can be dissipated by the multi-interface BEFs at the micro-scale, and by the staggered cantilever structure at the macro-scale, respectively. As a result, our designed heterostructured nanorods anode exhibits superb rate capability (332.8 mAh g-1 at 10.0 A g-1 ) and durable cyclic stability over 900 cycles at 5.0 A g-1 , outperforming other metal chalcogenides. This proposed stress dissipation strategy offers a new insight for developing stable structures for conversion-based anodes.

Nitrogen and Sulfur Co-Doped Carbon-Coated Ni3 S2 /MoO2 Nanowires as Bifunctional Catalysts for Alkaline Seawater Electrolysis.

Bifunctional catalysts have inherent advantages in simplifying electrolysis devices and reducing electrolysis costs. Developing efficient and stable bifunctional catalysts is of great significance for industrial hydrogen production. Herein, a bifunctional catalyst, composed of nitrogen and sulfur co-doped carbon-coated trinickel disulfide (Ni3 S2 )/molybdenum dioxide (MoO2 ) nanowires (NiMoS@NSC NWs), is developed for seawater electrolysis. The designed NiMoS@NSC exhibited high activity in alkaline electrolyte with only 52 and 191 mV overpotential to attain 10 mA cm-2 for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. Significantly, the electrolyzer (NiMoS@NSC||NiMoS@NSC) based on this bifunctional catalyst drove 100 mA cm-2 at only 1.71 V along with a robust stability over 100 h in alkaline seawater, which is superior to a platinum/nickel-iron layered double hydroxide couple (Pt||NiFe LDH). Theoretical calculations indicated that interfacial interactions between Ni3 S2 and MoO2 rearranged the charge at interfaces and endowed Mo sites at the interfaces with Pt-like HER activity, while Ni sites on Ni3 S2 surfaces at non-interfaces are the active centers for OER. Meanwhile, theoretical calculations and experimental results also demonstrated that interfacial interactions improved the electrical conductivity, boosting reaction kinetics for both HER and OER. This study presented a novel insight into the design of high-performance bifunctional electrocatalysts for seawater splitting.

In-situ reconstruction of rock-like 3D hierarchical MIL-53(Fe) self-supporting electrode with oxygen vacancy induced ultra-long stable and efficient water oxidation.

The exploitation of efficient, stable and cheap electrocatalyst for oxygen evolution reaction (OER) is very significant to the development of energy technology. In this study, Fe-based metal-organic frameworks (MIL-53(Fe)) self-supporting electrode with a 3D hierarchical open structure was developed through a semi-sacrificial strategy. The self-supporting electrode exhibits an excellent OER performance with an overpotential of 328 mV at 100 mA cm-2 in 1 M KOH, which is superior than that of IrO2 catalyst. Importantly, the optimized self-supporting electrode could operate at 100 mA cm-2 for 520 h without visible decrease in activity. It was also found that the structure of MIL-53(Fe) was in-situ self-reconstructed into oxyhydroxides during OER process. However, the 3D hierarchical open structure assembled with nano-microstructures kept well, which ensured the long-term stability of our self-supporting electrode for OER. Furthermore, density functional theory (DFT) calculations reveal that the FeOOH with rich oxygen vacancy transformed from MIL-53(Fe) plays a key role for the OER catalytic activity. And, the uninterrupted formation of oxygen vacancy during OER process ensures the continuous OER catalytic activity, which is the original source for the ultra-long stability of the self-supporting electrode toward OER. This work explores the way for the construction of efficient self-supporting oxygen electrodes based on MOFs.

Volatile Perovskite Precursor Ink Enables Window Printing of Phase-Pure FAPbI3 Perovskite Solar Cells and Modules in Ambient Atmosphere.

Despite the great success of perovskite photovoltaics in terms of device efficiency and stability using laboratory-scale spin-coating methods, the demand for high-throughput and cost-effective solutions remains unresolved and rarely reported because of the complicated nature of perovskite crystallization. In this work, we propose a stable precursor ink design strategy to control the solvent volatilization and perovskite crystallization to enable the wide speed window printing (0.3 to 18.0 m/min) of phase-pure FAPbI3 perovskite solar cells (pero-SCs) in ambient atmosphere. The FAPbI3 perovskite precursor ink uses volatile acetonitrile (ACN) as the main solvent with DMF and DMSO as coordination additives is beneficial to improve the ink stability, inhibit the coffee rings, and the complicated intermediate FAPbI3 phases, delivering high-quality pin-hole free and phase-pure FAPbI3 perovskite films with large-scale uniformity. Ultimately, small-area FAPbI3 pero-SCs (0.062 cm2 ) and large-area modules (15.64 cm2 ) achieved remarkable efficiencies of 24.32 % and 21.90 %, respectively, whereas the PCE of the devices can be maintained at 23.76 % when the printing speed increases to 18.0 m/min. Specifically, the unencapsulated device exhibits superior operational stability with T90 >1350 h. This work represents a step towards the scalable, cost-effective manufacturing of perovskite photovoltaics with both high performance and high throughput.

Molecular Engineering of Sulfone-Xanthone Chromophore for Enhanced Fluorescence Navigation.

Enriching the palette of high-performance fluorescent dyes is vital to support the frontier of biomedical imaging. Although various rhodamine skeletons remain the premier type of small-molecule fluorophores due to the apparent high brightness and flexible modifiability, they still suffer from the inherent defect of small Stokes shift due to the nonideal fluorescence imaging signal-to-background ratio. Especially, the rising class of fluorescent dyes, sulfone-substituted xanthone, exhibits great potential, but low chemical stability is also pointed out as the problem. Molecular engineering of sulfone-xanthone to obtain a large Stokes shift and high stability is highly desired, but it is still scarce. Herein, we present the combination modification method for optimizing the performance of sulfone-xanthone. These redesigned fluorescent skeletons owned greatly improved stability and Stokes shift compared with the parent sulfone-rhodamine. To the proof of bioimaging capacity, annexin protein-targeted peptide LS301 was introduced to the most promising dyes, J-S-ARh, to form the tumor-targeted fluorescent probe, J-S-LS301. The resulting probe, J-S-LS301, can be an outstanding fluorescence tool for the orthotopic transplantation tumor model of hepatocellular carcinoma imaging and on-site pathological analysis. In summary, the combination method could serve as a basis for rational optimization of sulfone-xanthone. Overall, the chemistry reported here broadens the scope of accessible sulfone-xanthone functionality and, in turn, enables to facilitate the translation of biomedical research toward the clinical domain.

Regulation of the electronic structure of a RuNi/MoC electrocatalyst for high-efficiency hydrogen evolution in alkaline seawater.

Alkaline seawater electrolysis offers a way to generate hydrogen without carbon emissions. However, developing highly efficient catalysts that can sustain high performance and stability for the hydrogen evolution reaction (HER) in alkaline seawater is a formidable challenge. Here, a nanowire (NW) of a RuNi/MoC heterojunction embedded in N-doped carbon (RuNi/MoC@NC) was developed as a potent HER catalyst. The catalyst required only 21 mV at 10 mA cm-2 for HER in alkaline seawater, which surpasses 20% Pt/C. Moreover, using nickel foam (NF) as a catalyst carrier, an electrolyzer composed of RuNi/MoC@NC and nickel-iron layered double hydroxide (NiFe LDH) needed only 1.81 V at 500 mA cm-2 for full water splitting and showed long-term stability (over 500 h). Theoretical calculation revealed that the Ru and Ni sites in the catalyst had the optimal adsorption energy for hydrogen and water, respectively, which synergistically lowered the energy barrier for HER. This work offered an efficient method to design a highly effective HER catalyst for alkaline seawater splitting.

Interfacial Electron Regulation and Composition Evolution of NiFe/MoC Heteronanowire Arrays for Highly Stable Alkaline Seawater Oxidation.

In alkaline seawater electrolysis, the oxygen evolution reaction (OER) is greatly suppressed by the occurrence of electrode corrosion due to the formation of hypochlorite. Herein, a catalyst consisting of MoC nanowires modified with NiFe alloy nanoparticles (NiFe/MoC) on nickel foam (NF) is prepared. The optimized catalyst can deliver a large current density of 500 mA cm-2 at a very low overpotential of 366 mV in alkaline seawater, respectively, outperforming commercial IrO2 . Remarkably, an electrolyzer assembled with NiFe/MoC/NF as the anode and NiMoN/NF as the cathode only requires 1.77 V to drive a current density of 500 mA cm-2 for alkaline seawater electrolysis, as well as excellent stability. Theory calculation indicates that the initial activity of NiFe/MoC is attributed to increased electrical conductivity and decreased energy barrier for OER due to the introduction of Fe. We find that the change of the catalyst in the composition occurred after the stability test; however, the reconstructed catalyst has an energy barrier close to that of the pristine one, which is responsible for its excellent long-term stability. Our findings provide an efficient way to construct high-performance OER catalysts for alkaline seawater splitting.

Lignan intake and risk of cardiovascular disease and type 2 diabetes: a meta-analysis of prospective cohort studies.

We conducted a meta-analysis of 12 prospective cohort studies to further illuminate the associations of lignan intake with risk of cardiovascular disease (CVD) and type 2 diabetes mellitus (T2DM). Compared with the lowest intake, the highest intake of lignans was correlated with a decreased incidence of CVD (relative risk [RR]: 0.85, 95% confidence interval [CI]: 0.80-0.90) and T2DM (RR: 0.82, 95% CI: 0.68-0.99). The benefits of lignan intake in CVD prevention were consistent across subgroups. In dose-response analysis, the RR for every 500-µg/d increment in lignan intake was 0.83 (95% CI: 0.74-0.92) for CVD and 0.96 (95% CI: 0.95-0.98) for T2DM. Moreover, a curvilinear dose-response pattern was observed for both CVD (p for nonlinearity < 0.001) and T2DM (p for nonlinearity < 0.001) in relation to lignan intake. These results indicated that higher lignan intake may be associated, in a dose-dependent manner, with a lower risk of CVD and T2DM.

Rational Design of pH-Independent and High-Fidelity Near-Infrared Tunable Fluorescent Probes for Tracking Leucine Aminopeptidase In Vivo.

Accurate detection of target analytes and generation of high-fidelity fluorescence signals are particularly critical in life sciences and clinical diagnostics. However, the majority of current NIR-I fluorescent probes are vulnerable to pH effects resulting in signal distortion. In this work, a series of fluorescence-tunable and pH-independent probes are reported by combining optically tunable groups of unsymmetric Si-rhodamines and introducing the methoxy instead of the spiro ring on the benzene ring at position 9. To validate the concept, the leucine aminopeptidase response site was introduced into Si-2,6OMe-NH2 with the best optical properties to synthesize Si-LAP for monitoring the intrahepatic LAP in vivo. Therefore, the design approach may provide a new and practical strategy for designing innovative functional fluorescent probes and generating high-stability and high-fidelity fluorescent signals.

56-fs diode-pumped SESAM mode-locked Yb:YAl3(BO3)4 laser.

We report on the first sub-60 fs pulse generated from a diode-pumped SESAM mode-locked Yb-laser based on a non-centrosymmetric Yb:YAl3(BO3)4 crystal as a gain medium. In the continuous-wave regime, pumping with a spatially single-mode, fiber-coupled 976 nm InGaAs laser diode, the Yb:YAl3(BO3)4 laser generated 391 mW at 1041.7 nm with a slope efficiency as high as 65.1%, and a wavelength tuning across 59 nm (1019 to 1078 nm) was achieved. By implementing a commercial SESAM to initiate and sustain the soliton type mode-locking, and using only a 1 mm-thick laser crystal, the Yb:YAl3(BO3)4 laser delivered pulses as short as 56 fs at a central wavelength of 1044.6 nm with an average output power of 76 mW at a pulse repetition rate of ∼67.55 MHz. To the best of our knowledge, this result represents the shortest pulses ever achieved from Yb:YAB crystal.

Dual-Functional Z-Scheme TiO2 @MoS2 @NC Multi-Heterostructures for Photo-Driving Ultrafast Sodium Ion Storage.

Exploiting dual-functional photoelectrodes to harvest and store solar energy is a challenging but efficient way for achieving renewable energy utilization. Herein, multi-heterostructures consisting of N-doped carbon coated MoS2 nanosheets supported by tubular TiO2 with photoelectric conversion and electronic transfer interfaces are designed. When a photo sodium ion battery (photo-SIB) is assembled based on the heterostructures, its capacity increases to 399.3 mAh g-1 with a high photo-conversion efficiency of 0.71 % switching from dark to visible light at 2.0 A g-1 . Remarkably, the photo-SIB can be recharged by light only, with a striking capacity of 231.4 mAh g-1 . Experimental and theoretical results suggest that the proposed multi-heterostructures can enhance charge transfer kinetics, maintain structural stability, and facilitate the separation of photo-excited carriers. This work presents a new strategy to design dual-functional photoelectrodes for efficient use of solar energy.

Migration from Lysosome to Nucleus: Monitoring Lysosomal Alkalization-Related Biological Processes with an Aminofluorene-Based Probe.

Aberrant lysosomal alkalization is associated with various biological processes, such as oxidative stress, cell apoptosis, ferroptosis, etc. Herein, we developed a novel aminofluorene-based fluorescence probe named FAN to monitor the lysosomal alkalization-related biological processes by its migration from lysosome to nucleus. FAN possessed NIR emission, large Stokes shift, high pH stability, and high photostability, making it suitable for real-time and long-term bioimaging. As a lysosomotropic molecule, FAN can accumulate in lysosomes first and then migrate to the nucleus by right of its binding capability to DNA after lysosomal alkalization. In this manner, FAN was successfully used to monitor these physiological processes which triggered lysosomal alkalization in living cells, including oxidative stress, cell apoptosis, and ferroptosis. More importantly, at higher concentrations, FAN could also serve as a stable nucleus dye for the fluorescence imaging of the nucleus in living cells and tissues. This novel multifunctional fluorescence probe shows great promise for application in lysosomal alkalization-related visual research and nucleus imaging.

Highly efficiency production of D-allulose from inulin using curli fiber multi-enzyme cascade catalysis.

D-Allulose is a rare sugar with numerous physiological benefits and low caloric content, which can be obtained from inulin through enzymatic catalysis. In this study, we combined D-allulose 3-epimerase, exo- and endo-inulinases (EXINU and ENINU) with the NGTag/NGCatcher/CsgA system to accelerate D-allulose accumulation from inulin. Molecular dynamics simulations were used to screen linkers of appropriate length for ENINU. In vitro, we successfully observed the assembled NGCatcher_ENINU_CsgA, NGTag_EXINU, and DAERK fibers using fluorescent labelling with GFP, YFP, and mCherry. The optimal pH and temperature of the tagged variants were comparable to those of the wild-type, and the MD simulations showed that NGCatcher_ENINU_CsgA had improved stability in the working environment of EXINU. D-Allulose accumulation rate of the assembled enzymes cascade (NGCatcher_ENINU_CsgA/NGTag_EXINU_CsgA/DAERK) reached 0.25 g/L min-1 (1.25 mgD-allulose mgDAERK-1 min-1) at an inulin concentration of 100 g/L. The assembled system greatly improves the high-valued productions of rare sugars from cheap biomass.

Consistent 3D Hand Reconstruction in Video via Self-Supervised Learning.

We present a method for reconstructing accurate and consistent 3D hands from a monocular video. We observe that the detected 2D hand keypoints and the image texture provide important cues about the geometry and texture of the 3D hand, which can reduce or even eliminate the requirement on 3D hand annotation. Accordingly, in this work, we propose S2HAND, a self-supervised 3D hand reconstruction model, that can jointly estimate pose, shape, texture, and the camera viewpoint from a single RGB input through the supervision of easily accessible 2D detected keypoints. We leverage the continuous hand motion information contained in the unlabeled video data and explore S2HAND(V), which uses a set of weights shared S2HAND to process each frame and exploits additional motion, texture, and shape consistency constrains to obtain more accurate hand poses, and more consistent shapes and textures. Experiments on benchmark datasets demonstrate that our self-supervised method produces comparable hand reconstruction performance compared with the recent full-supervised methods in single-frame as input setup, and notably improves the reconstruction accuracy and consistency when using the video training data.