p-d Orbital Hybridization Engineered Single-Atom Catalyst for Electrocatalytic Ammonia Synthesis

The rational design of metal single-atom catalysts(SACs)for electrochemical nitrogen reduction reaction(NRR)is challenging.Two-dimensional metal-organic frameworks(2DMOFs)is a unique class of promising SACs.Up to now,the roles of individual metals,coordination atoms,and their synergy effect on the electroanalytic performance remain unclear.Therefore,in this work,a series of 2DMOFs with different metals and coordinating atoms are systematically investigated as electrocatalysts for ammonia synthesis using density functional theory calculations.For a specific metal,a proper metal-intermediate atoms p-d orbital hybridization interaction strength is found to be a key indicator for their NRR catalytic activities.The hybridization interaction strength can be quantitatively described with the p-/d-band center energy difference(Δd-p),which is found to be a sufficient descriptor for both the p-d hybridization strength and the NRR performance.The maximum free energy change(ΔG_(max))andΔd-p have a volcanic relationship with OsC_(4)(Se)_(4)located at the apex of the volcanic curve,showing the best NRR performance.The asymmetrical coordination environment could regulate the band structure subtly in terms of band overlap and positions.This work may shed new light on the application of orbital engineering in electrocatalytic NRR activity and especially promotes the rational design for SACs.

Morphological and molecular evidence for natural hybridization between Sorbus pohuashanensis and S. discolor (Rosaceae)

In overlapping distribution areas of Sorbus pohuashanensis and S.discolor in North China(Mount Tuoliang,Mount Xiling and Mount Baihua),Sorbus indi-viduals were found with pink fruit,which have never been recorded for the flora of China.Fourteen morphological characters combined with four chloroplast DNA markers and internal transcribed spacer(ITS)were used to analyze the origin of the Sorbus individuals with pink fruits and their relationship to S.pohuashanensis and S.discolor.PCA,SDA and one-way(taxon)ANOVA of morphological characters provided convincing evidence of the hybrid ori-gin of Sorbus individuals with pink fruits based on a novel morphological character and many intermediate characters.Haplotype analysis based on four cpDNA markers showed that either S.pohuashanensis or S.discolor were maternal parents of Sorbus individuals with pink fruits.Incongru-ence of the position of Sorbus individuals with pink fruits between cpDNA and ITS in cluster trees supported by DNA sequence comparative analysis,implying former hybridiza-tion events between S.pohuashanensis and S.discolor.Mul-tiple hybridization events between S.pohuashanensis and S.discolor might have contributed to the generation of Sorbus individuals with pink fruits.This study has provided insights into hybridization between species of the same genus in sympatric areas,which is of great significance for the study of interspecific hybridization.

Cryptic diversity and rampant hybridization in annual gentians on the Qinghai-Tibet Plateau revealed by population genomic analysis

Understanding the evolutionary and ecological processes involved in population differentiation and speciation provides critical insights into biodiversity formation. In this study, we employed 29,865 single nucleotide polymorphisms(SNPs) and complete plastomes to examine genomic divergence and hybridization in Gentiana aristata, which is endemic to the Qinghai-Tibet Plateau(QTP) region. Genetic clustering revealed that G. aristata is characterized by geographic genetic structures with five clusters(West, East, Central, South and North). The West cluster has a specific morphological character(i.e., blue corolla) and higher values of FSTcompared to the remaining clusters, likely the result of the geological barrier formed by the Yangtze River. The West cluster diverged from the other clusters in the Early Pliocene;these remaining clusters diverged from one another in the Early Quaternary. Phylogenetic reconstructions based on SNPs and plastid data revealed substantial cyto-nuclear conflicts. Genetic clustering and D-statistics demonstrated rampant hybridization between the Central and North clusters,along the Bayankala Mountains, which form the geological barrier between the Central and North clusters. Species distribution modeling demonstrated the range of G. aristata expanded since the Last Interglacial period. Our findings provide genetic and morphological evidence of cryptic diversity in G. aristata, and identified rampant hybridization between genetic clusters along a geological barrier.These findings suggest that geological barriers and climatic fluctuations have an important role in triggering diversification as well as hybridization, indicating that cryptic diversity and hybridization are essential factors in biodiversity formation within the QTP region.

Enhanced and asymmetric signatures of hybridization at climatic margins: Evidence from closely related dioecious fig species

Hybridization plays a significant role in biological evolution. However, it is not clear whether ecological contingency differentially influences likelihood of hybridization, particularly at ecological margins where parental species may exhibit reduced fitnesses. Moreover, it is unknown whether future ecosystem change will increase the prevalence of hybridization. Ficus heterostyla and F. squamosa are closely related species co-distributed from southern Thailand to southwest China where hybridization, yielding viable seeds, has been documented. As a robust test of ecological factors driving hybridization, we investigated spatial hybridization signatures based on nuclear microsatellites from extensive population sampling across a widespread contact range. Both species showed high population differentiation and strong patterns of isolation by distance. Admixture estimates exposed asymmetric interspecific gene flow.Signatures of hybridization increase significantly towards higher latitude zones, peaking at the northern climatic margins. Geographic variation in reproductive phenology combined with ecologically challenging marginal habitats may promote this phenomenon. Our work is a first systematic evaluation of such patterns in a comprehensive, latitudinally-based clinal context, and indicates that tendency to hybridize appears strongly influenced by environmental conditions. Moreover, that future climate change scenarios will likely alter and possibly augment cases of hybridization at ecosystem scales.

Cryptic divergences and repeated hybridizations within the endangered “living fossil” dove tree(Davidia involucrata) revealed by whole genome resequencing

The identification and understanding of cryptic intraspecific evolutionary units(lineages) are crucial for planning effective conservation strategies aimed at preserving genetic diversity in endangered species.However, the factors driving the evolution and maintenance of these intraspecific lineages in most endangered species remain poorly understood. In this study, we conducted resequencing of 77 individuals from 22 natural populations of Davidia involucrata, a “living fossil” dove tree endemic to central and southwest China. Our analysis revealed the presence of three distinct local lineages within this endangered species, which emerged approximately 3.09 and 0.32 million years ago. These divergence events align well with the geographic and climatic oscillations that occurred across the distributional range.Additionally, we observed frequent hybridization events between the three lineages, resulting in the formation of hybrid populations in their adjacent as well as disjunct regions. These hybridizations likely arose from climate-driven population expansion and/or long-distance gene flow. Furthermore, we identified numerous environment-correlated gene variants across the total and many other genes that exhibited signals of positive evolution during the maintenance of two major local lineages. Our findings shed light on the highly dynamic evolution underlying the remarkably similar phenotype of this endangered species. Importantly, these results not only provide guidance for the development of conservation plans but also enhance our understanding of evolutionary past for this and other endangered species with similar histories.

Scale-space effect and scale hybridization in image intelligent recognition of geological discontinuities on rock slopes

Geological discontinuity(GD)plays a pivotal role in determining the catastrophic mechanical failure of jointed rock masses.Accurate and efficient acquisition of GD networks is essential for characterizing and understanding the progressive damage mechanisms of slopes based on monitoring image data.Inspired by recent advances in computer vision,deep learning(DL)models have been widely utilized for image-based fracture identification.The multi-scale characteristics,image resolution and annotation quality of images will cause a scale-space effect(SSE)that makes features indistinguishable from noise,directly affecting the accuracy.However,this effect has not received adequate attention.Herein,we try to address this gap by collecting slope images at various proportional scales and constructing multi-scale datasets using image processing techniques.Next,we quantify the intensity of feature signals using metrics such as peak signal-to-noise ratio(PSNR)and structural similarity(SSIM).Combining these metrics with the scale-space theory,we investigate the influence of the SSE on the differentiation of multi-scale features and the accuracy of recognition.It is found that augmenting the image's detail capacity does not always yield benefits for vision-based recognition models.In light of these observations,we propose a scale hybridization approach based on the diffusion mechanism of scale-space representation.The results show that scale hybridization strengthens the tolerance of multi-scale feature recognition under complex environmental noise interference and significantly enhances the recognition accuracy of GD.It also facilitates the objective understanding,description and analysis of the rock behavior and stability of slopes from the perspective of image data.

Manipulating d-d orbital hybridization induced by Mo-doped Co_(9)S_(8) nanorod arrays for high-efficiency water electrolysis

Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic performance.Herein,we demonstrate an ingenious d-d orbital hybridization concept to construct Mo-doped Co_(9)S_(8) nanorod arrays aligned on carbon cloth(CC)substrate(abbreviated as Mo-Co_(9)S_(8)@CC hereafter)as a high-efficiency bifunctional electrocatalyst toward water electrolysis.It has experimentally and theoretically validated that the 4d-3d orbital coupling between Mo dopant and Co site can effectively optimize the H_(2)O activation energy and lower H^(*)adsorption energy barrier,thereby leading to enhanced hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activities.Thanks to the unique electronic and geometrical advantages,the optimized Mo-Co_(9)S_(8)@CC with appropriate Mo content exhibits outstanding bifunctional performance in alkaline solution,with the overpotentials of 75 and 234 mV for the delivery of a current density of 10 mA cm^(-2),small Tafel slopes of 53.8 and 39.9 mV dec~(-1)and long-term stabilities for at least 32 and 30 h for HER and OER,respectively.More impressively,a water splitting electrolylzer assembled by the self-supported Mo-Co_(9)S_(8)@CC electrode requires a low cell voltage of 1.53 V at 10 mA cm^(-2)and shows excellent stability and splendid reversibility,demonstrating a huge potential for affordable and scalable electrochemical H_(2) production.The innovational orbital hybridization strategy for electronic regulation herein provides an inspirable avenue for developing progressive electrocatalysts toward new energy systems.

Asymmetric orbital hybridization in Zn-doped antiperovskite Cu_(1-x)Zn_(x)NMn_(3)enables highly efficient electrocatalytic hydrogen production

Rational design of efficient and robust earth-abundant alkaline hydrogen evolution reaction(HER)catalysts is a key factor for developing energy conversion technologies.Currently,antiperovskite nitride CuNMn_(3)has garnered significant interest due to its remarkable properties such as negative/zero thermal expansion and magnetocaloric effects.However,when utilized as hydrogen evolution catalysts,it encounters large challenge resulting from excessively strong/weak interactions with adsorbed H on Mn/Cu active sites,which leads to low HER activity.In this study,we introduce an asymmetric orbital hybridization strategy in Zn-doped Cu_(1-x)Zn_(x)NMn_(3)by leveraging the localization of Zn electronic states to reconfigure the electronic structures of Cu and Mn,thereby reducing the energy barrier for water dissociation and optimizing Cu and Mn active sites for hydrogen adsorption and H_(2)production.Electrochemical evaluations reveal that Cu_(0.85)Zn_(0.15)NMn_(3)with x=0.15 demonstrates exceptional electrocatalytic activity in alkaline electrolytes.A low overpotential of 52 mV at 10 mA cm^(-2)and outstanding stability over a 150-h test period are achieved,surpassing commercial Pt/C.This research offers a novel strategy for enhancing HER performance by modulating asymmetric hybridization of electron orbitals between multiple metal atoms within a material structure.

Enhanced Redox Electrocatalysis in High‑Entropy Perovskite Fluorides by Tailoring d–p Hybridization

High-entropy catalysts featuring exceptional properties are,in no doubt,playing an increasingly significant role in aprotic lithium-oxygen batteries.Despite extensive effort devoted to tracing the origin of their unparalleled performance,the relationships between multiple active sites and reaction intermediates are still obscure.Here,enlightened by theoretical screening,we tailor a high-entropy perovskite fluoride(KCoMnNiMgZnF_(3)-HEC)with various active sites to overcome the limitations of conventional catalysts in redox process.The entropy effect modulates the d-band center and d orbital occupancy of active centers,which optimizes the d–p hybridization between catalytic sites and key intermediates,enabling a moderate adsorption of LiO_(2)and thus reinforcing the reaction kinetics.As a result,the Li–O2 battery with KCoMnNiMgZnF_(3)-HEC catalyst delivers a minimal discharge/charge polarization and long-term cycle stability,preceding majority of traditional catalysts reported.These encouraging results provide inspiring insights into the electron manipulation and d orbital structure optimization for advanced electrocatalyst.

An optimized protocol using Steedman’s wax for high-sensitivity RNA in situ hybridization in shoot apical meristems and flower buds of cucumber

In situ mRNA hybridization(ISH)is a powerful tool for examining the spatiotemporal expression of genes in shoot apical meristems and flower buds of cucumber.The most common ISH protocol uses paraffin wax;however,embedding tissue in paraffin wax can take a long time and might result in RNA degradation and decreased signals.Here,we developed an optimized protocol to simplify the process and improve RNA sensitivity.We combined embedding tissue in low melting-point Steedman’s wax with processing tissue sections in solution,as in the whole-mount ISH method in the optimized protocol.Using the optimized protocol,we examined the expression patterns of the CLAVATA3(CLV3)and WUSCHEL(WUS)genes in shoot apical meristems and floral meristems of Cucumis sativus(cucumber)and Arabidopsis thaliana(Arabidopsis).The optimized protocol saved 4–5 days of experimental period compared with the standard ISH protocol using paraffin wax.Moreover,the optimized protocol achieved high signal sensitivity.The optimized protocol was successful for both cucumber and Arabidopsis,which indicates it might have general applicability to most plants.

颈椎前路Hybrid手术和颈椎后路单开门椎管扩大成形术治疗多节段脊髓型颈椎病临床疗效分析

目的:分析颈椎前路Hybrid手术和颈椎后路单开门椎管扩大成形术(EODL)治疗多节段脊髓型颈椎病的疗效,探讨多节段脊髓型颈椎病患者手术方式的选择。方法:对2017年7月—2020年7月在首都医科大学附属北京中医医院手术治疗的70例多节段脊髓型颈椎病患者进行回顾性分析,根据手术方式不同,分为前路组35例和后路组35例,前路组患者行Hybrid手术[颈椎前路椎间盘切除融合术(ACDF)联合人工颈椎间盘置换术(ACDR)],后路组患者行EODL。记录2组患者住院时间、手术时间、术中出血量和术后引流量,通过日本骨科协会(JOA)评分、JOA改善率、颈椎残障功能指数(NDI)、疼痛视觉模拟评分(VAS)和术后满意度评分进行疗效评价,统计2组患者术后并发症发生情况。结果:与后路组比较,前路组患者术中出血量、术后引流量、住院时间和手术时间均明显减少(P<0.01),术前各项评分差异无统计学意义(P>0.05)。末次随访时,与后路组比较,前路组患者JOA评分和JOA改善率明显升高(P<0.01),NDI评分和VAS评分明显降低(P<0.01)。与术前比较,末次随访时2组患者JOA评分明显升高(P<0.01),NDI和VAS评分均明显降低(P<0.01)。按术后满意度评分评价,2组患者术后满意度均较高。2组患者术后并发症发生率比较差异无统计学意义(P>0.05)。结论:颈椎前路Hybrid手术和EODL在治疗多节段脊髓型颈椎病方面均取得了较为满意的疗效。Hybrid手术具有出血量少和手术时间短等优点,临床上应根据患者实际情况选择最适宜的术式。

Activation Redistribution Based Hybrid Asymmetric Quantization Method of Neural Networks

The demand for adopting neural networks in resource-constrained embedded devices is continuously increasing.Quantization is one of the most promising solutions to reduce computational cost and memory storage on embedded devices.In order to reduce the complexity and overhead of deploying neural networks on Integeronly hardware,most current quantization methods use a symmetric quantization mapping strategy to quantize a floating-point neural network into an integer network.However,although symmetric quantization has the advantage of easier implementation,it is sub-optimal for cases where the range could be skewed and not symmetric.This often comes at the cost of lower accuracy.This paper proposed an activation redistribution-based hybrid asymmetric quantizationmethod for neural networks.The proposedmethod takes data distribution into consideration and can resolve the contradiction between the quantization accuracy and the ease of implementation,balance the trade-off between clipping range and quantization resolution,and thus improve the accuracy of the quantized neural network.The experimental results indicate that the accuracy of the proposed method is 2.02%and 5.52%higher than the traditional symmetric quantization method for classification and detection tasks,respectively.The proposed method paves the way for computationally intensive neural network models to be deployed on devices with limited computing resources.Codes will be available on https://github.com/ycjcy/Hybrid-Asymmetric-Quantization.

基于Hybrid A^(*)算法的变压器声级巡检系统研究与设计

随着国内变电站数目逐步增加,采用固定式声级监测终端对变压器声级检测的方式已经满足不了日常检测的需求。为解决固定式声级监测终端方式成本高、维护复杂、设备利用率低等问题,该文率先提出了一种变压器声级巡检系统,并设计了最优声级巡检路径。通过场地定位传感器生成变压器场地栅格图信息,采用Hybrid A^(*)算法将场地栅格图信息生成符合国标所要求的最优声级巡检路径检测点;针对所开发的变压器声级巡检装置,采用生成的巡检路径对变压器进行声级测定作业,对测定的声级数据进行分析处理。测试结果表明,该文开发的系统与设计算法的变压器声级巡检时间、检测效率以及数据的采集准确性都优于固定式声级监测终端方式,系统完成变压器声级巡检全过程的成功率可达95%。

复杂建设环境下基于Hybrid A^(*)算法的铁路平面线形绿色优化设计

随着“双碳经济下绿色铁路”理念的兴起,将“绿色生态”融入到铁路平面线路优化已成为近年来的研究热点。本文以铁路建设成本与生态破坏成本的协同优化为目标,引入并改进了一种自动驾驶导航算法(Hybrid A^(*)算法),以适应复杂的铁路设计问题,同时考虑最小曲线半径、最大曲线半径、最短曲线长度、最短夹直线长度、缓和曲线长度等铁路线形约束。研究结果表明:(1)改进后算法以离散网格方式整合外部环境因素,实现渐进式全局探索,获取接近全局最优的铁路线路设计结果;(2)该方法在复杂外部环境约束下,无需预设水平交点位置和数量,可自动生成符合线路-环境耦合约束的优化平面线路方案。

Enhancing rock fragmentation prediction in mining operations:A hybrid GWO-RF model with SHAP interpretability

In the mining industry,precise forecasting of rock fragmentation is critical for optimising blasting processes.In this study,we address the challenge of enhancing rock fragmentation assessment by developing a novel hybrid predictive model named GWO-RF.This model combines the grey wolf optimization(GWO)algorithm with the random forest(RF)technique to predict the D_(80)value,a critical parameter in evaluating rock fragmentation quality.The study is conducted using a dataset from Sarcheshmeh Copper Mine,employing six different swarm sizes for the GWO-RF hybrid model construction.The GWO-RF model’s hyperparameters are systematically optimized within established bounds,and its performance is rigorously evaluated using multiple evaluation metrics.The results show that the GWO-RF hybrid model has higher predictive skills,exceeding traditional models in terms of accuracy.Furthermore,the interpretability of the GWO-RF model is enhanced through the utilization of SHapley Additive exPlanations(SHAP)values.The insights gained from this research contribute to optimizing blasting operations and rock fragmentation outcomes in the mining industry.

Dual-ion carrier storage through Mg^(2+) addition for high-energy and long-life zinc-ion hybrid capacitor

Cation additives can efficiently enhance the total electrochemical capabilities of zinc-ion hybrid capacitors (ZHCs).However their energy storage mechanisms in zinc-based systems are still under debate.Herein,we modulate the electrolyte and achieve dual-ion storage by adding magnesium ions.And we assemble several Zn//activated carbon devices with different electrolyte concentrations and investigate their electrochemical reaction dynamic behaviors.The zinc-ion capacitor with Mg^(2+)mixed solution delivers 82 mAh·g^(-1)capacity at 1 A·g^(-1) and maintains 91%of the original capacitance after 10000 cycling.It is superior to the other assembled zinc-ion devices in single-component electrolytes.The finding demonstrates that the double-ion storage mechanism enables the superior rate performance and long cycle lifetime of ZHCs.

Electrostatic Interaction-directed Construction of Hierarchical Nanostructured Carbon Composite with Dual Electrical Conductive Networks for Zinc-ion Hybrid Capacitors with Ultrastability

Metal-organic framework(MOF)-derived carbon composites have been considered as the promising materials for energy storage.However,the construction of MOF-based composites with highly controllable mode via the liquid-liquid synthesis method has a great challenge because of the simultaneous heterogeneous nucleation on substrates and the self-nucleation of individual MOF nanocrystals in the liquid phase.Herein,we report a bidirectional electrostatic generated self-assembly strategy to achieve the precisely controlled coatings of single-layer nanoscale MOFs on a range of substrates,including carbon nanotubes(CNTs),graphene oxide(GO),MXene,layered double hydroxides(LDHs),MOFs,and SiO_(2).The obtained MOF-based nanostructured carbon composite exhibits the hierarchical porosity(V_(meso)/V_(micro)∶2.4),ultrahigh N content of 12.4 at.%and"dual electrical conductive networks."The assembled aqueous zinc-ion hybrid capacitor(ZIC)with the prepared nanocarbon composite as a cathode shows a high specific capacitance of 236 F g^(-1)at 0.5 A g^(-1),great rate performance of 98 F g^(-1)at 100 A g^(-1),and especially,an ultralong cycling stability up to 230000 cycles with the capacitance retention of 90.1%.This work develops a repeatable and general method for the controlled construction of MOF coatings on various functional substrates and further fabricates carbon composites for ZICs with ultrastability.

Regulatable Orthotropic 3D Hybrid Continuous Carbon Networks for Efficient Bi-Directional Thermal Conduction

Vertically oriented carbon structures constructed from low-dimen-sional carbon materials are ideal frameworks for high-performance thermal inter-face materials(TIMs).However,improving the interfacial heat-transfer efficiency of vertically oriented carbon structures is a challenging task.Herein,an orthotropic three-dimensional(3D)hybrid carbon network(VSCG)is fabricated by depositing vertically aligned carbon nanotubes(VACNTs)on the surface of a horizontally oriented graphene film(HOGF).The interfacial interaction between the VACNTs and HOGF is then optimized through an annealing strategy.After regulating the orientation structure of the VACNTs and filling the VSCG with polydimethylsi-loxane(PDMS),VSCG/PDMS composites with excellent 3D thermal conductive properties are obtained.The highest in-plane and through-plane thermal conduc-tivities of the composites are 113.61 and 24.37 W m^(-1)K^(-1),respectively.The high contact area of HOGF and good compressibility of VACNTs imbue the VSCG/PDMS composite with low thermal resistance.In addition,the interfacial heat-transfer efficiency of VSCG/PDMS composite in the TIM performance was improved by 71.3%compared to that of a state-of-the-art thermal pad.This new structural design can potentially realize high-performance TIMs that meet the need for high thermal conductivity and low contact thermal resistance in interfacial heat-transfer processes.

Hybrid手术对Stanford B型主动脉夹层疗效的研究进展

主动脉夹层主要通过使用假体移植物的开胸手术修复来治疗。在过去的10年里,胸主动脉腔内修复术(TEVAR)已成为一种创伤更小、潜在更安全的治疗方法。然而,单一的微创腔内修复术在缺乏足够的锚定区的Stanford B型主动脉夹层(TBAD)患者上有其局限性。因此,结合了外科手术及胸主动脉腔内修复术的Hy‐brid手术(或称为杂交手术),通过外科手段重建左颈总动脉和左锁骨下动脉的弓上分流术,再结合微创腔内修复术,显著减少患者在外科手术中并发症的发生率,且提高了那些常规胸主动脉腔内修复术缺乏理想锚定区患者的生存率。

A Review of Hybrid Cyber Threats Modelling and Detection Using Artificial Intelligence in IIoT

The Industrial Internet of Things(IIoT)has brought numerous benefits,such as improved efficiency,smart analytics,and increased automation.However,it also exposes connected devices,users,applications,and data generated to cyber security threats that need to be addressed.This work investigates hybrid cyber threats(HCTs),which are now working on an entirely new level with the increasingly adopted IIoT.This work focuses on emerging methods to model,detect,and defend against hybrid cyber attacks using machine learning(ML)techniques.Specifically,a novel ML-based HCT modelling and analysis framework was proposed,in which L1 regularisation and Random Forest were used to cluster features and analyse the importance and impact of each feature in both individual threats and HCTs.A grey relation analysis-based model was employed to construct the correlation between IIoT components and different threats.