氨(NH_(3))作为重要的化学品和能源储存介质,需求量与日俱增.本文旨在通过电化学硝酸根还原反应(NO_(3)^(−)RR),将NO_(3)^(−)转化为NH3,不仅解决了NO_(3)^(−)引起的环境污染问题,又可以满足对NH_(3)的迫切需求.然而,NO_(3)^(−)RR涉及多...氨(NH_(3))作为重要的化学品和能源储存介质,需求量与日俱增.本文旨在通过电化学硝酸根还原反应(NO_(3)^(−)RR),将NO_(3)^(−)转化为NH3,不仅解决了NO_(3)^(−)引起的环境污染问题,又可以满足对NH_(3)的迫切需求.然而,NO_(3)^(−)RR涉及多个电子和质子转移过程,其中,NO_(2)^(−)是NO_(3)^(−)活化转化和深度还原合成NH_(3)的重要中间体.酞菁铜(CuPc)能够高效地活化转化NO_(3)^(−)为NO_(2)^(−),但在低过电位时无法有效地将NO2−还原为NH3,难以获得较高的氨法拉第效率(FENH3)和分电流密度.而氮配位的铁单原子催化剂(FeNC)则有较好的NO_(2)^(−)吸附活化特性.因此,利用双组分催化剂之间的协同作用以实现高效NO_(3)^(−)RR的活性和选择性是本文的主要研究思路.本文设计了CuPc/FeNC串联催化剂,利用CuPc和FeNC对NO_(3)^(−)和NO_(2)^(−)的吸附活化能力的差异,实现了高效的协同催化转化.X射线衍射、高角环形暗场扫描透射电镜、X射线光电子能谱及X射线吸收谱结果表明,FeNC催化剂中Fe原子均匀分布于ZIF-8热解后的基底.通过将FeNC和CuPc负载于气体扩散电极,在流动电解池中完成NO_(3)^(−)RR.CuPc/FeNC催化剂在较低电势区间中能够实现接近100%的NH3法拉第效率,同时在−0.57 V vs.RHE时达到273 mA cm–2的NH3分电流密度,并且在整个电势范围内有效地抑制了NO_(2)^(–)聚集.与单组分催化剂CuPc和FeNC对比结果表明,在−0.53 V vs.RHE时,CuPc/FeNC催化剂表现出较高的FE(NH_(3))/FE(NO_(2)^(−))比值,是CuPc催化剂的50倍;同时CuPc/FeNC催化剂上NH3分电流密度是FeNC催化剂的1.5倍.进一步研究了NO_(3)^(–)RR中的串联反应机制,其中FeNC催化剂表现出较高的NO_(2)^(–)RR活性,并且有效抑制了析氢反应.此外,CuPc/FeNC催化剂和FeNC催化剂在NO_(2)^(−)RR中表现出类似的NH3分电流密度,这表明在NO_(3)^(−)RR中,CuPc/FeNC催化剂性能的提高来源于FeNC位点能够进一步还原CuPc位点产生的NO_(2)^(–).理论计算结果表明,FeNC比CuPc表现出更强的NO_(2)^(–)吸附活化能力,说明NO_(2)^(−)在FeNC上更容易进行加氢还原.NO_(3)^(−)RR反应全路径分析结果表明,对于^(*)NO_(3)还原到*NO2过程,CuPc相对于FeNC位点具有明显降低的反应自由能,说明CuPc有利于NO_(2)^(−)的生成;而FeNC位点在后续的^(*)NO_(2)还原合成^(*)NH_(3)过程中具有更低的反应自由能,这与实验结果一致.一系列非原位和原位表征证明了CuPc催化剂在高电位下存在少量金属颗粒析出,与CuPc催化剂在高电位下NH_(3)分电流密度快速增加结果一致.综上,本工作中CuPc和FeNC催化剂之间的协同作用弥补了各自的不足,通过串联反应机制,在低过电位下有效增加了NH_(3)的法拉第效率和电流密度,实现了高效的协同催化转化,为设计和合成高效催化剂提供了新思路.展开更多
The stability of the microstructure and mechanical properties of the pre-hardened sheets during the pre-hardening forming(PHF)process directly determines the quality of the formed components.The microstructure stabili...The stability of the microstructure and mechanical properties of the pre-hardened sheets during the pre-hardening forming(PHF)process directly determines the quality of the formed components.The microstructure stability of the pre-hardened sheets was in-vestigated by differential scanning calorimetry(DSC),transmission electron microscopy(TEM),and small angle X-ray scattering(SAXS),while the mechanical properties and formability were analyzed through uniaxial tensile tests and formability tests.The results in-dicate that the mechanical properties of the pre-hardened alloys exhibited negligible changes after experiencing 1-month natural aging(NA).The deviations of ultimate tensile strength(UTS),yield strength(YS),and sheet formability(Erichsen value)are all less than 2%.Also,after different NA time(from 48 h to 1 month)is applied to alloys before pre-hardening treatment,the pre-hardened alloys possess stable microstructure and mechanical properties as well.Interestingly,with the extension of NA time before pre-hardening treatment from 48 h to 1 month,the contribution of NA to the pre-hardening treatment is limited.Only a yield strength increment of 20 MPa is achieved,with no loss in elongation.The limited enhancement is mainly attributed to the fact that only a limited number of clusters are transformed into Guinier-Preston(GP)zones at the early stage of pre-hardening treatment,and the formation ofθ''phase inhibits the nucleation and growth of GP zones as the precipitated phase evolves.展开更多
Fruitlet calyx shedding in pear plants is apparently regulated via numerous pathways that involve both environmental triggers and phytohormones cues such as auxin. In this study, we found at 10 days after full bloom (...Fruitlet calyx shedding in pear plants is apparently regulated via numerous pathways that involve both environmental triggers and phytohormones cues such as auxin. In this study, we found at 10 days after full bloom (DAFB) higher levels of indoleacetic acid (IAA) and tryptophan (Trp) in calyx persistence fruitlet (CPF) than calyx shedding fruitlet (CSF) ofDanshan Suli’ pear (Pyrus bretschneideri Rhed.). Consisting with this, the activity of indolealdehyde oxidase (IAAIdO), which promotes IAA synthesis, was remarkably increased, and that of peroxidase(POD), which degrades IAA, dropped markedly in CPF but not in CSF. Further, qRT-PCR results revealed that most of 31 PbrARFs (encoding auxin response factors) in Pyrus bretschneideri were highly expressed in CPF, whereas PbrARF4, PbrARF24 and PbrARF26 were significantly downregulated in CPF vis-a-vis CSF. Phylogenetic analysis revealed that 6 PbrARFs clustered in the group III, where PbrARF4 showed the closest affinity with AtARF1 that promotes organ abscission, indicating a putative role of PbrARF4 in mediating the process of calyx shedding in pear. In fact, the ectopic overexpression of PbrARF4 in Solanum lycopersicum resulted in an earlier-formed and deeper abscission layer (AL) in the transgenic plants, whose calyxes were more prone to wilt at the mature red stage (MR) compared with the control plants (wild-type). More importantly, expression levels of the abscission genes SILS and Sl Cel2 in transgenic plants overexpressing PbrARF4 were significantly upregulated in comparation with the WT, whereas those of Sl BI and Sl TAPG2 were considerably inhibited. Further, PbrJOINTLESS and PbrIDA,the two genes related to calyx shedding in pear, were up-regulated more in CSF than CPF. The findings contribute to a better understanding of PbrARFs involved in fruitlet calyx shedding of pear, which could prove beneficial to improving the quality of pear fruit.展开更多
Electrocatalysis is a process dealing with electrochemical reactions in the interconversion of chemical energy and electrical energy.Precise synthesis of catalytically active nanostructures is one of the key challenge...Electrocatalysis is a process dealing with electrochemical reactions in the interconversion of chemical energy and electrical energy.Precise synthesis of catalytically active nanostructures is one of the key challenges that hinder the practical application of many important energy‐related electrocatalytic reactions.Compared with conventional wet‐chemical,solid‐state and vapor deposition synthesis,electrochemical synthesis is a simple,fast,cost‐effective and precisely controllable method for the preparation of highly efficient catalytic materials.In this review,we summarize recent progress in the electrochemical synthesis of catalytic materials such as single atoms,spherical and shaped nanoparticles,nanosheets,nanowires,core‐shell nanostructures,layered nanomaterials,dendritic nanostructures,hierarchically porous nanostructures as well as composite nanostructures.Fundamental aspects of electrochemical synthesis and several main electrochemical synthesis methods are discussed.Structure‐performance correlations between electrochemically synthesized catalysts and their unique electrocatalytic properties are exemplified using selected examples.We offer the reader with a basic guide to the synthesis of highly efficient catalysts using electrochemical methods,and we propose some research challenges and future opportunities in this field.展开更多
Simultaneously achieving high activity,selectivity and stability for electrochemical CO_(2)reduction reaction(CO_(2)RR)remains great challenges.Herein,a phosphorus-modified Sn/Sn Oxcore/shell(P-Sn/SnO_x)catalyst,deriv...Simultaneously achieving high activity,selectivity and stability for electrochemical CO_(2)reduction reaction(CO_(2)RR)remains great challenges.Herein,a phosphorus-modified Sn/Sn Oxcore/shell(P-Sn/SnO_x)catalyst,derived from in situ electrochemical reduction of an amorphous Sn(HPO_(4))_(2) pre-catalyst,exhibits high CO_(2)RR performance.The total Faradaic efficiency(FE)of C_(1) products is close to 100%in a broad potential range from-0.49 to-1.02 V vs.reversible hydrogen electrode,and a total current density of 315.0 m A cm^(-2)is achieved.Moreover,the P-Sn/SnO_(x) catalyst maintains a formate FE of~90%for 120 h.Density functional theory calculations suggest that the phosphorus-modified Sn/SnO_(x) core/shell structure effectively facilitates formate production by enhancing CO_(2)adsorption and improving free energy profile of formate formation.展开更多
一氧化氮电还原反应将工业废气转化为有价值的氨,表现出极具潜力的应用前景.在本工作中,我们合成了具有高比表面积和丰富缺陷的氧化铜纳米片催化剂,在流动池中氨法拉第效率达到92.1%,在-0.2 V vs.RHE时,一氧化氮电还原电流密度和氨的生...一氧化氮电还原反应将工业废气转化为有价值的氨,表现出极具潜力的应用前景.在本工作中,我们合成了具有高比表面积和丰富缺陷的氧化铜纳米片催化剂,在流动池中氨法拉第效率达到92.1%,在-0.2 V vs.RHE时,一氧化氮电还原电流密度和氨的生产速率分别达到1.1 A cm^(-2)和7356μmol cm^(-2)h^(-1).在电流密度超过400 m A cm-2时,氨法拉第效率在50小时保持在80%以上.准原位X射线光电子能谱和原位X射线吸收光谱结果表明氧化铜纳米片在一氧化氮电还原过程中被电化学还原成单质铜.与铜纳米颗粒相比,氧化铜纳米片展现出较高的电化学表面积和一氧化氮电还原的内在活性.展开更多
Purpose The high-energy photon source(HEPS)is the first fourth-generation synchrotron photon source in China(Jiang et al.in Sci Sin Phys Mech Astron 44:1075-1094,2014).The strip electrode and its power supply provide ...Purpose The high-energy photon source(HEPS)is the first fourth-generation synchrotron photon source in China(Jiang et al.in Sci Sin Phys Mech Astron 44:1075-1094,2014).The strip electrode and its power supply provide necessary hardware support for correcting the magnetic field of the wiggler as reported by Zhao and Yin(Particle accelerator technology,Higher Education Press,Beijing,2006).The design of the conventional power supply for accelerators,with a large output current and high output voltage,making it easy to achieve high stability of the output current.The strip electrode power supply poses difficulties in achieving high stability due to its small output current and voltage.Because of size limitations,as well as the requirements of the power architecture,there are currently no commercial products for this type of power supply.Methods Designed and developed 32 strip electrode power supplies.Considering the large number of power supplies and limited space,a rack structure design was adopted,placing all power supplies in one rack.The main circuit of the power supply adopts a full bridge transformation structure(Chao et al.in Radiat Detect Technol Methods 6:470-478,2022),and the control scheme adopts full digital control based on FPGA(Long and Cheng in At Energy Sci Technol 43:780-784,2009).The power supply has two control modes:local operation and remote operation as reported by Lu(Particle accelerator technology,Hunan University,Changsha,2010).Results The test shows that all power supplies meet the indicator requirements,with a stability of less than 100 ppm.Conclusions The strip electrode power supply can effectively correct the multipole integral field error and improve the integral field performance of the wiggler.展开更多
The application of reliability analysis and reliability sensitivity analysis methods to complicated structures faces two main challenges:small failure probability(typical less than 10-5)and time-demanding mechanical m...The application of reliability analysis and reliability sensitivity analysis methods to complicated structures faces two main challenges:small failure probability(typical less than 10-5)and time-demanding mechanical models.This paper proposes an improved active learning surrogate model method,which combines the advantages of the classical Active Kriging–Monte Carlo Simulation(AK-MCS)procedure and the Adaptive Linked Importance Sampling(ALIS)procedure.The proposed procedure can,on the one hand,adaptively produce a series of intermediate sampling density approaching the quasi-optimal Importance Sampling(IS)density,on the other hand,adaptively generate a set of intermediate surrogate models approaching the true failure surface of the rare failure event.Then,the small failure probability and the corresponding reliability sensitivity indices are efficiently estimated by their IS estimators based on the quasi-optimal IS density and the surrogate models.Compared with the classical AK-MCS and Active Kriging–Importance Sampling(AK-IS)procedure,the proposed method neither need to build very large sample pool even when the failure probability is extremely small,nor need to estimate the Most Probable Points(MPPs),thus it is computationally more efficient and more applicable especially for problems with multiple MPPs.The effectiveness and engineering applicability of the proposed method are demonstrated by one numerical test example and two engineering applications.展开更多
Understanding the connection between brain and behavior in animals requires precise monitoring of their behaviors in three-dimensional(3-D)space.However,there is no available three-dimensional behavior capture system ...Understanding the connection between brain and behavior in animals requires precise monitoring of their behaviors in three-dimensional(3-D)space.However,there is no available three-dimensional behavior capture system that focuses on rodents.Here,we present MouseVenue3D,an automated and low-cost system for the efficient capture of 3-D skeleton trajectories in markerless rodents.We improved the most time-consuming step in 3-D behavior capturing by developing an automatic calibration module.Then,we validated this process in behavior recognition tasks,and showed that 3-D behavioral data achieved higher accuracy than 2-D data.Subsequently,MouseVenue3D was combined with fast high-resolution miniature two-photon microscopy for synchronous neural recording and behavioral tracking in the freely-moving mouse.Finally,we successfully decoded spontaneous neuronal activity from the 3-D behavior of mice.Our findings reveal that subtle,spontaneous behavior modules are strongly correlated with spontaneous neuronal activity patterns.展开更多
Bone defects are always accompanied by inflammation due to excessive reactive oxygen species(ROS)in injured regions,which greatly impedes the regeneration of bone tissues.Although many conductive polymers have been de...Bone defects are always accompanied by inflammation due to excessive reactive oxygen species(ROS)in injured regions,which greatly impedes the regeneration of bone tissues.Although many conductive polymers have been developed to scavenge ROS,they are typically non-degradable under physiological conditions,making them unsuitable for in vivo applications.Biodegradable polyorganophosphazenes(POPPs)may serve as potent ROS-scavenging biomaterials owing to their versatile chemical structures and ease of functionalization.Herein,a PATGP-type electroactive polyphosphazene with side groups of aniline tetramer and glycine ethyl ester was compared to conventional poly(lactic-co-glycolic acid)(PLGA)in regenerating bone tissues.To conduct in vitro and in vivo evaluations,three kinds of electrospun nanofibrous meshes were prepared:PLGA,PLGA/PATGP blend,and PLGA/PATGP core–shell nanofibers.Among them,PLGA/PATGP core–shell nanofibers outperform the blend and PLGA nanofibers in terms of scavenging ROS,promoting osteogenic differentiation,and accelerating neo-bone formation.The continuous PATGP shell on the PLGA/PATGP core–shell nanofiber surface could apparently provide more significant modulation effects on cellular behaviors than the PLGA/PATGP blend nanofibers with PATGP dispersed in the PLGA matrix.Therefore,the core–shell structured PLGA/PATGP nanofibers were envisioned as a promising candidate scaffold for bone tissue engineering.Additionally,the core–shell design paved the way for biomedical applications of functional POPPs in combination with other polymeric biomaterials,without phase separation or difficulty of increasing the molecular weights of POPPs.展开更多
Significant progress on electrocatalytic CO2 reduction reaction (CO2RR) has been achieved in recent years.However,the research and development of electrolyzer device for CO2RR is scarce.Here we use anion exchange memb...Significant progress on electrocatalytic CO2 reduction reaction (CO2RR) has been achieved in recent years.However,the research and development of electrolyzer device for CO2RR is scarce.Here we use anion exchange membrane to develop zerogap electrolyzers for CO2RR.The electrochemical properties of the electrolyzers with Pd/C and Cu cathodes are investigated.The Pd/C cathode shows a current density of 200 mA cm^-2with CO Faradaic efficiency of 98%and energy efficiency of 48.8%,while the Cu cathode shows a current density of 350 mA cm^-2with total CO2RR Faradaic efficiency of 81.9%and energy efficiency of 30.5%.This work provides a promising demonstration of CO2 electrolyzer using anion exchange membrane for CO2 electrolysis at industrial current densities.展开更多
In this paper,the images of tunnel surface are obtained by tunnel lining rapid inspection system,and tunnel crack forest dataset(TCFD)is established.The disaster characteristics of tunnel cracks are analyzed and summa...In this paper,the images of tunnel surface are obtained by tunnel lining rapid inspection system,and tunnel crack forest dataset(TCFD)is established.The disaster characteristics of tunnel cracks are analyzed and summarized.Solutions of tunnel crack segmentation(TCS)method are developed for the detection and recognition of cracks on tunnel lining.According to the image features of the tunnel lining and the optical principal of detection equipment,effective image pre-processing steps are carried out before crack extraction.The tunnel image of TCFD is divided into appropriate number of blocks to magnify the local features of tunnel cracks.Local threshold segmentation method is used to traverse the blocks successively,and the first target block with crack is obtained.The seed in the target block were obtained by adaptive localization method and mapped to the whole image.Region growing is performed through crack seed until complete tunnel crack is extracted.The results show that the precision,recall rate and F-measure of tunnel cracks under the TCS method can reach 92.58%,93.07%and 92.82%without strong interference.According to the binary images processed by TCS method,the projection images of different types of tunnel cracks and their respective laws are obtained.Furthermore,the TCS method is implemented and deployed as a GUI software application.展开更多
A strong animal survival instinct is to approach objects and situations that are of benefit and to avoid risk.In humans,a large proportion of mental disorders are accompanied by impairments in risk avoidance.One of th...A strong animal survival instinct is to approach objects and situations that are of benefit and to avoid risk.In humans,a large proportion of mental disorders are accompanied by impairments in risk avoidance.One of the most important genes involved in mental disorders is disrupted-in-schizophrenia-1(DISC1),and animal models in which this gene has some level of dysfunction show emotion-related impairments.However,it is not known whether DISC1 mouse models have an impairment in avoiding potential risks.In the present study,we used DISC1-N terminal truncation(DISC1-N^(TM))mice to investigate risk avoidance and found that these mice were impaired in risk avoidance on the elevated plus maze(EPM)and showed reduced social preference in a three-chamber social interaction test.Following EPM tests,c-Fos expression levels indicated that the nucleus accumbens(NAc)was associated with risk-avoidance behavior in DISC1-N^(TM)mice.In addition,in vivo electrophysiological recordings following tamoxifen administration showed that the firing rates of fast-spiking neurons(FS)in the NAc were significantly lower in DISC1-N^(TM)mice than in wild-type(WT)mice.In addition,in vitro patch clamp recording revealed that the frequency of action potentials stimulated by current injection was lower in parvalbumin(PV)neurons in the NAc of DISC1-N^(TM)mice than in WT controls.The impairment of risk avoidance in DISC1-N^(TM)mice was rescued using optogenetic tools that activated NAcPV neurons.Finally,inhibition of the activity of NAcPV neurons in PV-Cre mice mimicked the risk-avoidance impairment found in DISC1-N^(TM)mice during tests on the elevated zero maze.Taken together,our findings confirm an impairment in risk avoidance in DISC1-N^(TM)mice and suggest that reduced excitability of NAc^(PV) neurons is responsible.展开更多
Biological receptor-ligand adhesion governed by mammalian cells involves a series of mechanochemical pro-cesses that can realize reversible,loading rate-dependent specific interfacial bonding,and even exhibit a counte...Biological receptor-ligand adhesion governed by mammalian cells involves a series of mechanochemical pro-cesses that can realize reversible,loading rate-dependent specific interfacial bonding,and even exhibit a counterintuitive behavior called catch bonds that tend to have much longer lifetimes when larger pulling forces are applied.Inspired by these catch bonds,we designed a hydrogen bonding-meditated hydrogel made from acrylic acid-N-acryloyl glycinamide(AA-NAGA)copolymers and tannic acids(TA),which formed repeatable specific adhesion to polar surfaces in an ultra-fast and robust way,but hardly adhered to nonpolar materials.It demonstrated up to five-fold increase in shear adhesive strength and interfacial adhesive toughness with external loading rates varying from 5 to 500 mm min^(-1).With a mechanochemical coupling model based on Monte Carlo simulations,we quantitatively revealed the nonlinear dependence of rate-sensitive interfacial adhesion on external loading,which was in good agreement with the experimental data.Likewise,the developed hydrogels were biocompatible,possessed antioxidant and antibacterial properties and promoted wound healing.This work not only reports a stimuli-responsive hydrogel adhesive suitable for multiple biomedical applications,but also offers an innovative strategy for bionic designs of smart hydrogels with loading rate-sensitive specific adhesion for various emerging areas including flexible electronics and soft robotics.展开更多
背景颞叶癫痫(Temporal lobe epilepsy,TLE)是起源于海马和海马旁(Hippocampal and parahippocampal,HP-PHP)结构的自发性发作.剖自HP-PHP结构中发作传播的机制对于开发特异性的治疗靶点,进而更有效的治疗TLE至关重要.许多研究人员使用...背景颞叶癫痫(Temporal lobe epilepsy,TLE)是起源于海马和海马旁(Hippocampal and parahippocampal,HP-PHP)结构的自发性发作.剖自HP-PHP结构中发作传播的机制对于开发特异性的治疗靶点,进而更有效的治疗TLE至关重要.许多研究人员使用传统的膜片钳分析海马内嗅皮层(Hippocampalentorhinal cortex,HP-EC)脑切片以识别异常环路的发作传播路径.展开更多
Measuring eye movement is a fundamental approach in cognitive science as it provides a variety of insightful parameters that reflect brain states such as visual attention and emotions.Combining eye-tracking with multi...Measuring eye movement is a fundamental approach in cognitive science as it provides a variety of insightful parameters that reflect brain states such as visual attention and emotions.Combining eye-tracking with multimodal neural recordings or manipulation techniques is beneficial for understanding the neural substrates of cognitive function.Many commercially-available and custom-built systems have been widely applied to awake,head-fixed small animals.However,the existing eyetracking systems used in freely-moving animals are still limited in terms of their compatibility with other devices and of the algorithm used to detect eye movements.Here,we report a novel system that integrates a general-purpose,easily compatible eye-tracking hardware with a robust eye feature-detection algorithm.With ultra-light hardware and a detachable design,the system allows for more implants to be added to the animal's exposed head and has a precise synchronization module to coordinate with other neural implants.Moreover,we systematically compared the performance of existing commonly-used pupil-detection approaches,and demonstrated that the proposed adaptive pupil feature-detection algorithm allows the analysis of more complex and dynamic eye-tracking data in freemoving animals.Synchronized eye-tracking and electroencephalogram recordings,as well as algorithm validation under five noise conditions,suggested that our system is flexibly adaptable and can be combined with a wide range of neural manipulation and recording technologies.展开更多
文摘氨(NH_(3))作为重要的化学品和能源储存介质,需求量与日俱增.本文旨在通过电化学硝酸根还原反应(NO_(3)^(−)RR),将NO_(3)^(−)转化为NH3,不仅解决了NO_(3)^(−)引起的环境污染问题,又可以满足对NH_(3)的迫切需求.然而,NO_(3)^(−)RR涉及多个电子和质子转移过程,其中,NO_(2)^(−)是NO_(3)^(−)活化转化和深度还原合成NH_(3)的重要中间体.酞菁铜(CuPc)能够高效地活化转化NO_(3)^(−)为NO_(2)^(−),但在低过电位时无法有效地将NO2−还原为NH3,难以获得较高的氨法拉第效率(FENH3)和分电流密度.而氮配位的铁单原子催化剂(FeNC)则有较好的NO_(2)^(−)吸附活化特性.因此,利用双组分催化剂之间的协同作用以实现高效NO_(3)^(−)RR的活性和选择性是本文的主要研究思路.本文设计了CuPc/FeNC串联催化剂,利用CuPc和FeNC对NO_(3)^(−)和NO_(2)^(−)的吸附活化能力的差异,实现了高效的协同催化转化.X射线衍射、高角环形暗场扫描透射电镜、X射线光电子能谱及X射线吸收谱结果表明,FeNC催化剂中Fe原子均匀分布于ZIF-8热解后的基底.通过将FeNC和CuPc负载于气体扩散电极,在流动电解池中完成NO_(3)^(−)RR.CuPc/FeNC催化剂在较低电势区间中能够实现接近100%的NH3法拉第效率,同时在−0.57 V vs.RHE时达到273 mA cm–2的NH3分电流密度,并且在整个电势范围内有效地抑制了NO_(2)^(–)聚集.与单组分催化剂CuPc和FeNC对比结果表明,在−0.53 V vs.RHE时,CuPc/FeNC催化剂表现出较高的FE(NH_(3))/FE(NO_(2)^(−))比值,是CuPc催化剂的50倍;同时CuPc/FeNC催化剂上NH3分电流密度是FeNC催化剂的1.5倍.进一步研究了NO_(3)^(–)RR中的串联反应机制,其中FeNC催化剂表现出较高的NO_(2)^(–)RR活性,并且有效抑制了析氢反应.此外,CuPc/FeNC催化剂和FeNC催化剂在NO_(2)^(−)RR中表现出类似的NH3分电流密度,这表明在NO_(3)^(−)RR中,CuPc/FeNC催化剂性能的提高来源于FeNC位点能够进一步还原CuPc位点产生的NO_(2)^(–).理论计算结果表明,FeNC比CuPc表现出更强的NO_(2)^(–)吸附活化能力,说明NO_(2)^(−)在FeNC上更容易进行加氢还原.NO_(3)^(−)RR反应全路径分析结果表明,对于^(*)NO_(3)还原到*NO2过程,CuPc相对于FeNC位点具有明显降低的反应自由能,说明CuPc有利于NO_(2)^(−)的生成;而FeNC位点在后续的^(*)NO_(2)还原合成^(*)NH_(3)过程中具有更低的反应自由能,这与实验结果一致.一系列非原位和原位表征证明了CuPc催化剂在高电位下存在少量金属颗粒析出,与CuPc催化剂在高电位下NH_(3)分电流密度快速增加结果一致.综上,本工作中CuPc和FeNC催化剂之间的协同作用弥补了各自的不足,通过串联反应机制,在低过电位下有效增加了NH_(3)的法拉第效率和电流密度,实现了高效的协同催化转化,为设计和合成高效催化剂提供了新思路.
基金supported by the National Natural Science Foundation of China (Nos.52075400 and 52275368)the 111 Project (No.B17034)+1 种基金the Key Research and Development Program of Hubei Province,China (Nos.2021BAA200 and 2022AAA001)the Independent Innovation Projects of the Hubei Longzhong Laboratory (No.2022ZZ-04)。
文摘The stability of the microstructure and mechanical properties of the pre-hardened sheets during the pre-hardening forming(PHF)process directly determines the quality of the formed components.The microstructure stability of the pre-hardened sheets was in-vestigated by differential scanning calorimetry(DSC),transmission electron microscopy(TEM),and small angle X-ray scattering(SAXS),while the mechanical properties and formability were analyzed through uniaxial tensile tests and formability tests.The results in-dicate that the mechanical properties of the pre-hardened alloys exhibited negligible changes after experiencing 1-month natural aging(NA).The deviations of ultimate tensile strength(UTS),yield strength(YS),and sheet formability(Erichsen value)are all less than 2%.Also,after different NA time(from 48 h to 1 month)is applied to alloys before pre-hardening treatment,the pre-hardened alloys possess stable microstructure and mechanical properties as well.Interestingly,with the extension of NA time before pre-hardening treatment from 48 h to 1 month,the contribution of NA to the pre-hardening treatment is limited.Only a yield strength increment of 20 MPa is achieved,with no loss in elongation.The limited enhancement is mainly attributed to the fact that only a limited number of clusters are transformed into Guinier-Preston(GP)zones at the early stage of pre-hardening treatment,and the formation ofθ''phase inhibits the nucleation and growth of GP zones as the precipitated phase evolves.
基金supported by the China Agriculture Research System (Grant No.CARS-28-14)。
文摘Fruitlet calyx shedding in pear plants is apparently regulated via numerous pathways that involve both environmental triggers and phytohormones cues such as auxin. In this study, we found at 10 days after full bloom (DAFB) higher levels of indoleacetic acid (IAA) and tryptophan (Trp) in calyx persistence fruitlet (CPF) than calyx shedding fruitlet (CSF) ofDanshan Suli’ pear (Pyrus bretschneideri Rhed.). Consisting with this, the activity of indolealdehyde oxidase (IAAIdO), which promotes IAA synthesis, was remarkably increased, and that of peroxidase(POD), which degrades IAA, dropped markedly in CPF but not in CSF. Further, qRT-PCR results revealed that most of 31 PbrARFs (encoding auxin response factors) in Pyrus bretschneideri were highly expressed in CPF, whereas PbrARF4, PbrARF24 and PbrARF26 were significantly downregulated in CPF vis-a-vis CSF. Phylogenetic analysis revealed that 6 PbrARFs clustered in the group III, where PbrARF4 showed the closest affinity with AtARF1 that promotes organ abscission, indicating a putative role of PbrARF4 in mediating the process of calyx shedding in pear. In fact, the ectopic overexpression of PbrARF4 in Solanum lycopersicum resulted in an earlier-formed and deeper abscission layer (AL) in the transgenic plants, whose calyxes were more prone to wilt at the mature red stage (MR) compared with the control plants (wild-type). More importantly, expression levels of the abscission genes SILS and Sl Cel2 in transgenic plants overexpressing PbrARF4 were significantly upregulated in comparation with the WT, whereas those of Sl BI and Sl TAPG2 were considerably inhibited. Further, PbrJOINTLESS and PbrIDA,the two genes related to calyx shedding in pear, were up-regulated more in CSF than CPF. The findings contribute to a better understanding of PbrARFs involved in fruitlet calyx shedding of pear, which could prove beneficial to improving the quality of pear fruit.
文摘Electrocatalysis is a process dealing with electrochemical reactions in the interconversion of chemical energy and electrical energy.Precise synthesis of catalytically active nanostructures is one of the key challenges that hinder the practical application of many important energy‐related electrocatalytic reactions.Compared with conventional wet‐chemical,solid‐state and vapor deposition synthesis,electrochemical synthesis is a simple,fast,cost‐effective and precisely controllable method for the preparation of highly efficient catalytic materials.In this review,we summarize recent progress in the electrochemical synthesis of catalytic materials such as single atoms,spherical and shaped nanoparticles,nanosheets,nanowires,core‐shell nanostructures,layered nanomaterials,dendritic nanostructures,hierarchically porous nanostructures as well as composite nanostructures.Fundamental aspects of electrochemical synthesis and several main electrochemical synthesis methods are discussed.Structure‐performance correlations between electrochemically synthesized catalysts and their unique electrocatalytic properties are exemplified using selected examples.We offer the reader with a basic guide to the synthesis of highly efficient catalysts using electrochemical methods,and we propose some research challenges and future opportunities in this field.
基金supported by the National Key R&D Program of China (2021YFA1501503)the National Natural Science Foundation of China (22125205,22002155,22002158,92045302)+5 种基金the“Transformational Technologies for Clean Energy and Demonstration”Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21070613)the Fundamental Research Funds for the Central Universities (20720220008)the China Postdoctoral Science Foundation (2019M661142)the Natural Science Foundation of Liaoning Province (2021-MS-022)the High-Level Talents Innovation Project of Dalian City (2020RQ038)the support from the Photon Science Center for Carbon Neutrality。
文摘Simultaneously achieving high activity,selectivity and stability for electrochemical CO_(2)reduction reaction(CO_(2)RR)remains great challenges.Herein,a phosphorus-modified Sn/Sn Oxcore/shell(P-Sn/SnO_x)catalyst,derived from in situ electrochemical reduction of an amorphous Sn(HPO_(4))_(2) pre-catalyst,exhibits high CO_(2)RR performance.The total Faradaic efficiency(FE)of C_(1) products is close to 100%in a broad potential range from-0.49 to-1.02 V vs.reversible hydrogen electrode,and a total current density of 315.0 m A cm^(-2)is achieved.Moreover,the P-Sn/SnO_(x) catalyst maintains a formate FE of~90%for 120 h.Density functional theory calculations suggest that the phosphorus-modified Sn/SnO_(x) core/shell structure effectively facilitates formate production by enhancing CO_(2)adsorption and improving free energy profile of formate formation.
基金supported by the National Key R&D Program of China (2023YFA1508002)the National Natural Science Foundation of China (22125205 and 92015302)+2 种基金the Fundamental Research Funds for the Central Universities (20720220008)Dalian National Laboratory for Clean Energy (DNL201923)the Photon Science Center for Carbon Neutrality。
文摘一氧化氮电还原反应将工业废气转化为有价值的氨,表现出极具潜力的应用前景.在本工作中,我们合成了具有高比表面积和丰富缺陷的氧化铜纳米片催化剂,在流动池中氨法拉第效率达到92.1%,在-0.2 V vs.RHE时,一氧化氮电还原电流密度和氨的生产速率分别达到1.1 A cm^(-2)和7356μmol cm^(-2)h^(-1).在电流密度超过400 m A cm-2时,氨法拉第效率在50小时保持在80%以上.准原位X射线光电子能谱和原位X射线吸收光谱结果表明氧化铜纳米片在一氧化氮电还原过程中被电化学还原成单质铜.与铜纳米颗粒相比,氧化铜纳米片展现出较高的电化学表面积和一氧化氮电还原的内在活性.
文摘Purpose The high-energy photon source(HEPS)is the first fourth-generation synchrotron photon source in China(Jiang et al.in Sci Sin Phys Mech Astron 44:1075-1094,2014).The strip electrode and its power supply provide necessary hardware support for correcting the magnetic field of the wiggler as reported by Zhao and Yin(Particle accelerator technology,Higher Education Press,Beijing,2006).The design of the conventional power supply for accelerators,with a large output current and high output voltage,making it easy to achieve high stability of the output current.The strip electrode power supply poses difficulties in achieving high stability due to its small output current and voltage.Because of size limitations,as well as the requirements of the power architecture,there are currently no commercial products for this type of power supply.Methods Designed and developed 32 strip electrode power supplies.Considering the large number of power supplies and limited space,a rack structure design was adopted,placing all power supplies in one rack.The main circuit of the power supply adopts a full bridge transformation structure(Chao et al.in Radiat Detect Technol Methods 6:470-478,2022),and the control scheme adopts full digital control based on FPGA(Long and Cheng in At Energy Sci Technol 43:780-784,2009).The power supply has two control modes:local operation and remote operation as reported by Lu(Particle accelerator technology,Hunan University,Changsha,2010).Results The test shows that all power supplies meet the indicator requirements,with a stability of less than 100 ppm.Conclusions The strip electrode power supply can effectively correct the multipole integral field error and improve the integral field performance of the wiggler.
基金supported by National Natural Science Foundation of China(Nos.51905430,51608446)the Fundamental Research Fund for Central Universities(No.3102018zy011)+1 种基金the supports of Alexander von Humboldt Foundation of Germanythe Top International University Visiting Program for Outstanding Young scholars of Northwestern Polytechnical University。
文摘The application of reliability analysis and reliability sensitivity analysis methods to complicated structures faces two main challenges:small failure probability(typical less than 10-5)and time-demanding mechanical models.This paper proposes an improved active learning surrogate model method,which combines the advantages of the classical Active Kriging–Monte Carlo Simulation(AK-MCS)procedure and the Adaptive Linked Importance Sampling(ALIS)procedure.The proposed procedure can,on the one hand,adaptively produce a series of intermediate sampling density approaching the quasi-optimal Importance Sampling(IS)density,on the other hand,adaptively generate a set of intermediate surrogate models approaching the true failure surface of the rare failure event.Then,the small failure probability and the corresponding reliability sensitivity indices are efficiently estimated by their IS estimators based on the quasi-optimal IS density and the surrogate models.Compared with the classical AK-MCS and Active Kriging–Importance Sampling(AK-IS)procedure,the proposed method neither need to build very large sample pool even when the failure probability is extremely small,nor need to estimate the Most Probable Points(MPPs),thus it is computationally more efficient and more applicable especially for problems with multiple MPPs.The effectiveness and engineering applicability of the proposed method are demonstrated by one numerical test example and two engineering applications.
基金the Key Area R&D Program of Guangdong Province,China(2018B030338001 and 2018B030331001)the National Key R&D Program of China(2018YFA0701403)+11 种基金the National Natural Science Foundation of China(31500861,31630031,91732304,and 31930047)Chang Jiang Scholars Program,the International Big Science Program Cultivating Project of the Chinese Academy of Science(CAS172644KYS820170004)the Strategic Priority Research Program of the CAS(XDB32030100)the Youth Innovation Promotion Association of the CAS(2017413)the CAS Key Laboratory of Brain Connectome and Manipulation(2019DP173024)Shenzhen Government Basic Research Grants(JCYJ20170411140807570,JCYJ20170413164535041)the Science,Technology and Innovation Commission of Shenzhen Municipality(JCYJ20160429185235132)a Helmholtz-CAS Joint Research grant(GJHZ1508)Guangdong Provincial Key Laboratory of Brain Connectome and Behavior(2017B030301017)the Ten Thousand Talent Program,the Guangdong Special Support Program,Key Laboratory of Shenzhen Institute of Advanced Technology(2019DP173024)the Shenzhen Key Science and Technology Infrastructure Planning Project(ZDKJ20190204002).
文摘Understanding the connection between brain and behavior in animals requires precise monitoring of their behaviors in three-dimensional(3-D)space.However,there is no available three-dimensional behavior capture system that focuses on rodents.Here,we present MouseVenue3D,an automated and low-cost system for the efficient capture of 3-D skeleton trajectories in markerless rodents.We improved the most time-consuming step in 3-D behavior capturing by developing an automatic calibration module.Then,we validated this process in behavior recognition tasks,and showed that 3-D behavioral data achieved higher accuracy than 2-D data.Subsequently,MouseVenue3D was combined with fast high-resolution miniature two-photon microscopy for synchronous neural recording and behavioral tracking in the freely-moving mouse.Finally,we successfully decoded spontaneous neuronal activity from the 3-D behavior of mice.Our findings reveal that subtle,spontaneous behavior modules are strongly correlated with spontaneous neuronal activity patterns.
基金The authors acknowledge financial support from the National Key R&D Program of China(2018YFE0194400)the National Natural Science Foundation of China(51873013)Guangdong Basic and Applied Basic Research Foundation(2020A1515111182).
文摘Bone defects are always accompanied by inflammation due to excessive reactive oxygen species(ROS)in injured regions,which greatly impedes the regeneration of bone tissues.Although many conductive polymers have been developed to scavenge ROS,they are typically non-degradable under physiological conditions,making them unsuitable for in vivo applications.Biodegradable polyorganophosphazenes(POPPs)may serve as potent ROS-scavenging biomaterials owing to their versatile chemical structures and ease of functionalization.Herein,a PATGP-type electroactive polyphosphazene with side groups of aniline tetramer and glycine ethyl ester was compared to conventional poly(lactic-co-glycolic acid)(PLGA)in regenerating bone tissues.To conduct in vitro and in vivo evaluations,three kinds of electrospun nanofibrous meshes were prepared:PLGA,PLGA/PATGP blend,and PLGA/PATGP core–shell nanofibers.Among them,PLGA/PATGP core–shell nanofibers outperform the blend and PLGA nanofibers in terms of scavenging ROS,promoting osteogenic differentiation,and accelerating neo-bone formation.The continuous PATGP shell on the PLGA/PATGP core–shell nanofiber surface could apparently provide more significant modulation effects on cellular behaviors than the PLGA/PATGP blend nanofibers with PATGP dispersed in the PLGA matrix.Therefore,the core–shell structured PLGA/PATGP nanofibers were envisioned as a promising candidate scaffold for bone tissue engineering.Additionally,the core–shell design paved the way for biomedical applications of functional POPPs in combination with other polymeric biomaterials,without phase separation or difficulty of increasing the molecular weights of POPPs.
基金This work was supported by the National Key R&D Program of China(2016YFB0600901)the National Natural Science Foundation of China(21573222,91545202)+4 种基金Dalian National Laboratory for Clean Energy(DNL180404,DNL201924)Dalian Institute of Chemical Physics(DMTO201702)Dalian Outstanding Young Scientist Foundation(2017RJ03)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17020200)the CAS Youth Innovation Promotion(Y201938).
文摘Significant progress on electrocatalytic CO2 reduction reaction (CO2RR) has been achieved in recent years.However,the research and development of electrolyzer device for CO2RR is scarce.Here we use anion exchange membrane to develop zerogap electrolyzers for CO2RR.The electrochemical properties of the electrolyzers with Pd/C and Cu cathodes are investigated.The Pd/C cathode shows a current density of 200 mA cm^-2with CO Faradaic efficiency of 98%and energy efficiency of 48.8%,while the Cu cathode shows a current density of 350 mA cm^-2with total CO2RR Faradaic efficiency of 81.9%and energy efficiency of 30.5%.This work provides a promising demonstration of CO2 electrolyzer using anion exchange membrane for CO2 electrolysis at industrial current densities.
基金This research is supported by the Fundamental Research Funds for the Central Universities,China(300102120301)Natural Science Basic Research Plan in Shaanxi Province of China(2021JQ-216)Scientific Innovation Practice Project of Postgraduates of Chang'an University(300103714017).
文摘In this paper,the images of tunnel surface are obtained by tunnel lining rapid inspection system,and tunnel crack forest dataset(TCFD)is established.The disaster characteristics of tunnel cracks are analyzed and summarized.Solutions of tunnel crack segmentation(TCS)method are developed for the detection and recognition of cracks on tunnel lining.According to the image features of the tunnel lining and the optical principal of detection equipment,effective image pre-processing steps are carried out before crack extraction.The tunnel image of TCFD is divided into appropriate number of blocks to magnify the local features of tunnel cracks.Local threshold segmentation method is used to traverse the blocks successively,and the first target block with crack is obtained.The seed in the target block were obtained by adaptive localization method and mapped to the whole image.Region growing is performed through crack seed until complete tunnel crack is extracted.The results show that the precision,recall rate and F-measure of tunnel cracks under the TCS method can reach 92.58%,93.07%and 92.82%without strong interference.According to the binary images processed by TCS method,the projection images of different types of tunnel cracks and their respective laws are obtained.Furthermore,the TCS method is implemented and deployed as a GUI software application.
基金This work was supported by the National Natural Science Foundation of China(31671116,31761163005,31800881,and 91132306)the International Big Science Program Cultivation Project of Chinese Academy of Sciences(172644KYS820170004)+3 种基金the External Cooperation Program of the Chinese Academy of Sciences(172644KYSB20160057)Science and Technology Program of Guangzhou Municipality(202007030001)the Key-Area Research and Development Program of Guangdong Province(2018B030331001 and 2018B03033600)Shenzhen Government Basic Research Grants(JCYJ20200109115405930 and JCYJ20200109150717745).
文摘A strong animal survival instinct is to approach objects and situations that are of benefit and to avoid risk.In humans,a large proportion of mental disorders are accompanied by impairments in risk avoidance.One of the most important genes involved in mental disorders is disrupted-in-schizophrenia-1(DISC1),and animal models in which this gene has some level of dysfunction show emotion-related impairments.However,it is not known whether DISC1 mouse models have an impairment in avoiding potential risks.In the present study,we used DISC1-N terminal truncation(DISC1-N^(TM))mice to investigate risk avoidance and found that these mice were impaired in risk avoidance on the elevated plus maze(EPM)and showed reduced social preference in a three-chamber social interaction test.Following EPM tests,c-Fos expression levels indicated that the nucleus accumbens(NAc)was associated with risk-avoidance behavior in DISC1-N^(TM)mice.In addition,in vivo electrophysiological recordings following tamoxifen administration showed that the firing rates of fast-spiking neurons(FS)in the NAc were significantly lower in DISC1-N^(TM)mice than in wild-type(WT)mice.In addition,in vitro patch clamp recording revealed that the frequency of action potentials stimulated by current injection was lower in parvalbumin(PV)neurons in the NAc of DISC1-N^(TM)mice than in WT controls.The impairment of risk avoidance in DISC1-N^(TM)mice was rescued using optogenetic tools that activated NAcPV neurons.Finally,inhibition of the activity of NAcPV neurons in PV-Cre mice mimicked the risk-avoidance impairment found in DISC1-N^(TM)mice during tests on the elevated zero maze.Taken together,our findings confirm an impairment in risk avoidance in DISC1-N^(TM)mice and suggest that reduced excitability of NAc^(PV) neurons is responsible.
基金National Natural Science Foundation of China(Grant nos.11972001,11972002,12072001 and 91848201)Beijing Natural Science Foundation(Grant no.Z200017)National Key Research and Development Program of China(Grant no.2021YFA1000201).
文摘Biological receptor-ligand adhesion governed by mammalian cells involves a series of mechanochemical pro-cesses that can realize reversible,loading rate-dependent specific interfacial bonding,and even exhibit a counterintuitive behavior called catch bonds that tend to have much longer lifetimes when larger pulling forces are applied.Inspired by these catch bonds,we designed a hydrogen bonding-meditated hydrogel made from acrylic acid-N-acryloyl glycinamide(AA-NAGA)copolymers and tannic acids(TA),which formed repeatable specific adhesion to polar surfaces in an ultra-fast and robust way,but hardly adhered to nonpolar materials.It demonstrated up to five-fold increase in shear adhesive strength and interfacial adhesive toughness with external loading rates varying from 5 to 500 mm min^(-1).With a mechanochemical coupling model based on Monte Carlo simulations,we quantitatively revealed the nonlinear dependence of rate-sensitive interfacial adhesion on external loading,which was in good agreement with the experimental data.Likewise,the developed hydrogels were biocompatible,possessed antioxidant and antibacterial properties and promoted wound healing.This work not only reports a stimuli-responsive hydrogel adhesive suitable for multiple biomedical applications,but also offers an innovative strategy for bionic designs of smart hydrogels with loading rate-sensitive specific adhesion for various emerging areas including flexible electronics and soft robotics.
基金supported in part by the National Key R&D Program of China(2021ZD0203902 and 2018YFA0701403)the Key Area R&D Program of Guangdong Province(2018B030338001 and 2018B030331001)+9 种基金the National Natural Science Foundation of China(31500861,31630031,91732304,and 31930047)the Chang Jiang Scholars Program and the Ten Thousand Talent Program,the International Big Science Program Cultivating Project of the Chinese Academy of Science(CAS)(172644KYS820170004)the Strategic Priority Research Program of the CAS(XDB32030100)the Youth Innovation Promo-tion Association of the CAS(2017413)Shenzhen Government Basic Research Grants(JCYJ20170411140807570,JCYJ20170413164535041)the Science,Technology and Innovation Commission of Shenzhen Municipality(JCYJ20160429185235132)a Helmholtz-CAS joint research grant(GJHZ1508)the Guangdong Provincial Key Laboratory of Brain Connectome and Behavior(2017B030301017)the Guangdong Special Support Program,the Key Laboratory of the CAS(2019DP173024)the Shenzhen Key Science and Technology Infrastructure Planning Project(ZDKJ20190204002)。
文摘Measuring eye movement is a fundamental approach in cognitive science as it provides a variety of insightful parameters that reflect brain states such as visual attention and emotions.Combining eye-tracking with multimodal neural recordings or manipulation techniques is beneficial for understanding the neural substrates of cognitive function.Many commercially-available and custom-built systems have been widely applied to awake,head-fixed small animals.However,the existing eyetracking systems used in freely-moving animals are still limited in terms of their compatibility with other devices and of the algorithm used to detect eye movements.Here,we report a novel system that integrates a general-purpose,easily compatible eye-tracking hardware with a robust eye feature-detection algorithm.With ultra-light hardware and a detachable design,the system allows for more implants to be added to the animal's exposed head and has a precise synchronization module to coordinate with other neural implants.Moreover,we systematically compared the performance of existing commonly-used pupil-detection approaches,and demonstrated that the proposed adaptive pupil feature-detection algorithm allows the analysis of more complex and dynamic eye-tracking data in freemoving animals.Synchronized eye-tracking and electroencephalogram recordings,as well as algorithm validation under five noise conditions,suggested that our system is flexibly adaptable and can be combined with a wide range of neural manipulation and recording technologies.