一氧化二氮的光解动力学:O(^(1)D)+N_(2)(X^(1)∑_(g)^(+))产物通道

由于一氧化二氮(N_(2)O)在大气化学中的重要性,本文使用时间切片的离子速度成像技术重新研究了一氧化二氮在紫外吸收区域的光解离动力学.采用单色光测量了203.814nm和205.472nm光解产物O(^(1)D)的离子影像,以及采用双色光记录了从200到220nm范围八个光解波长下解离产物O(^(1)D)的图像.产物N_(2)(X^(1)∑_(g)^(+))碎片的转动态分布和各向异性参数的信息可以从图像中获取:实验结果表明,N_(2)产物的转动态分布发生反转,最大值在J≈70.随着N_(2)转动量子数J增加,各向异性参数β表现出两次显著的下降.根据前人的理论计算[J,Chem.Phys.136,044314(2012)],初始线性构型的轴向反冲程度的不同导致了β随J的变化.然而,在高J区域,非绝热跃迁之后的基态势能面上存在额外的扭矩,从而引起额外的转动激发和较低的β值.采用真空紫外单光子电离O(^(1)D)原子的双色实验能够准确地获得产物的转动态分布和角分布.该工作加深了对三原子分子光解机制的进一步理解.

Switching CO_(2) Electroreduction Selectivity Between C_(1) and C_(2) Hydrocarbons on Cu Gas-Diffusion Electrodes

Regulating the selectivity toward a target hydrocarbon product is still the focus of CO_(2)electroreduction.Here,we discover that the original surface Cu species in Cu gas-diffusion electrodes plays a more important role than the surface roughness,local pH,and facet in governing the selectivity toward C_(1)or C_(2)hydrocarbons.The selectivity toward C_(2)H_(4) progressively increases,while CH_(4) decreases steadily upon lowering the Cu oxidation species fraction.At a relatively low electrodeposition voltage of 1.5 V,the Cu gas-diffusion electrode with the highest Cu^(δ+)/Cu^(0)ratio favors the pathways of∗CO hydrogenation to form CH_(4) with maximum Faradaic efficiency of 65.4%and partial current density of 228 mA cm^(−2)at−0.83 V vs RHE.At 2.0 V,the Cu gas-diffusion electrode with the lowest Cu^(δ+)/Cu^(0)ratio prefers C-C coupling to form C_(2)+products with Faradaic efficiency topping 80.1%at−0.75 V vs RHE,where the Faradaic efficiency of C_(2)H_(4) accounts for 46.4%and the partial current density of C_(2)H_(4) achieves 279 mA cm^(−2).This work demonstrates that the selectivity from CH_(4) to C_(2)H_(4) is switchable by tuning surface Cu species composition of Cu gas-diffusion electrodes.

Effects of laser energy on the surface quality and properties of electrodeposited zinc-nickel-molybdenum coatings

As a substitute for toxic cadmium coatings in the aerospace industry,zinc-nickel coatings have excellent application prospects,and their properties can be improved by adding molybdenum.In this study,laser-assisted electrodeposition is used to improve the surface quality and properties of Zn–Ni–Mo coatings,with investigation of how laser energy in the range of 0–21.1μJ affects their element content,surface morphology,crystal phase,microhardness,residual internal stress,and corrosion resistance.The laser irradiation accelerates the electrodeposition,refines the grain size,improves the hydrogen adsorption,and reduces the residual tensile stress,and a laser energy of 15.4μJ gives the highest Ni and Mo contents and the lowest Zn content,as well as the optimum surface morphology,microhardness,residual internal stress,and corrosion resistance of the coating.

Employing MXene as a matrix for loading amorphous Si generated upon lithiation towards enhanced lithium-ion storage

Although Si-based nanomaterials provide incomparable lithium ion storage ability in theory, it suffers from low initial Coulombic efficiency, electrical disconnection, and fracture due to huge volume changes after extended cycles. As a result, it leads to a severe capacity fading and an increase in internal impedance. Herein, Ti-elemental MXene was employed as a matrix for the intermediate product of Si electrodes. The boundary between the inner core of pristine Si and its outer shell of amorphous Li x Si alloy was reconstructed. Smaller amorphous aggregates were observed in the MXene&Si hybrid electrode after 500 cycles by using transmission electron microscopy. Consequently, an enhanced specific capacity was achieved as MXene as a matrix enables loading amorphous Si.

Extraordinary mechanical properties of AZ61 alloy processed by ECAP with 160° channel angle and EPT

AZ61 Mg alloy with homogeneous refined microstructure and exceptional mechanical properties was obtained by the combined technology of equal-channel angular pressing(ECAP)and electropulsing treatment(EPT)in this paper.Based on an ECAP die with an intersection angle of 160,the lower temperature is particularly adapted for AZ61 alloy to be deformed,in which accompanied by high accumulated defects density.The recrystallization of EPTed samples during different stages indicated that the recrystallization behavior of the deformed Mg alloy was mainly affected by the processing time and duration of EPT.Compared to those of the as-received samples,the average grain size of the EPTed samples was refined from 89μm to 1.0μm,accordingly the yields stress(YS)and ultimate tensile strength(UTS)were increased from 100 MPa and 260 MPa to 330 MPa and 448 MPa,respectively.The mechanisms of microstructure transformation and the reinforced mechanical properties were analyzed based on the strain of single ECAP,cumulative storage energy and the athermal effect of EPT.

Morphology-Controlled Growth of A1N One-Dimensional Nanostructures

Aluminum nitride （AIN） nanowires, serrated nanoribbons, and nanoribbons were selectively obtained through a simple chloride assisted chemical vapor deposition process. The morphologies of the products could be controlled by adjusting the deposition position and the flux of the reactant gas. The morphologies and structures of the AIN products were investigated in detail. The formation mechanism of the as-prepared different morphologies of AIN one-dimensional （ID） nanostructures was discussed on the basis of the experimental results.

Probing dark matter particles from evaporating primordial black holes via electron scattering in the CDEX-10 experiment

Dark matter(DM)is a major constituent of the Universe.However,no definite evidence of DM particles(denoted as“χ”)has been found in DM direct detection(DD)experiments to date.There is a novel concept of detectingχfrom evaporating primordial black holes(PBHs).We search forχemitted from PBHs by investigating their interaction with target electrons.The examined PBH masses range from 1×10^(15)to 7×10^(16)g under the current limits of PBH abundance fPBH.Using 205.4 kg·day data obtained from the CDEX-10 experiment conducted in the China Jinping Underground Laboratory,we exclude theχ-electron(χ-e)elastic-scattering cross sectionσ_(χe)~5×10^(-29)cm^(2)forχwith a mass■keV from our results.With the higher radiation background but lower energy threshold(160 eV),CDEX-10 fills a part of the gap in the previous work.If(m_(χ),σ_(χe))can be determined in the future,DD experiments are expected to impose strong constraints on fPBHfor large MPBHs.

Anti-corrosion performance of Si-surface-alloying NdFeB magnets obtained with magnetron sputtering and thermal diffusion

Si alloying in the surface layer of NdFeB magnets was realized by thermal diffusion combined with magnetron sputtering.The surface composition,phase structure and morphology of NdFeB(S-Si)specimens were characterized by an X-ray diffractometer,an X-ray photoelectron spectrometer and a field emission scanning electron microscope,respectively.The corrosion resistance of bare NdFeB(S-Si)was analyzed by static full immersion corrosion test and electrochemical experiments.Effects of sputtering and thermal diffusion on the microstructure and corrosion resistance of the surface layer were studied.Results show that surface alloying layer can effectively improve the corrosion resistance of bare NdFeB with the optimized static total immersion corrosion test time in NdFeB(1S-Si)-800 of 36 h,which is much longer than that of the pristine NdFeB(less than 0.5 h).The E_(corr)of NdFeB(1S-Si)-800 positively shifts from-1.05 to-0.92 V,indicating that the corrosion tendency is obviously lower.The J_(corr)is1.45×10^(-6)A/cm^(2)which is 2 orders of magnitude lower than that of the pristine NdFeB(5.25×10^(-4)A/cm^(2)).The intergranular composite oxides existing in Nd-rich phase contribute to the enhancement of corrosion resistance of Si-surface-alloying NdFeB.

多环芳烃污染土壤微生物修复研究进展

多环芳烃是我国土壤环境质量标准中要求严格管控的一类持久性有机污染物,利用微生物技术修复有机污染土壤具有绿色、经济等突出特点,应用前景广泛。目前多学科的协同发展和新技术的研究应用,为多环芳烃土壤微生物转化机制与污染生态过程等方面带来了新的认识,同时对修复技术的实际应用与调控提供了新的思考方向。本文以多环芳烃污染土壤微生物修复为主体,从污染土壤微生物修复应用技术、多环芳烃微生物降解特征、土壤体系污染物归趋规律与微生物作用及土壤污染微生物群落响应与研究技术等方面进行综合评述,并针对现存应用技术瓶颈和理论空白作进一步思考和展望。

Activated carbon coated palygorskite as adsorbent by activation and its adsorption for methylene blue

An activation process for developing the surface and porous structure of palygorskite/carbon（PG/C） nanocomposite using ZnC l2 as activating agent was investigated. The obtained activated PG/C was characterized by X-ray diffraction（XRD）, Fourier transform infrared spectroscopy（FTIR）, field-emission scanning electron microscopy（SEM）, and Brunauer-Emmett-Teller analysis（BET） techniques. The effects of activation conditions were examined,including activation temperature and impregnation ratio. With increased temperature and impregnation ratio, the collapse of the palygorskite crystal structure was found to accelerate and the carbon coated on the surface underwent further carbonization. XRD and SEM data confirmed that the palygorskite structure was destroyed and the carbon structure was developed during activation. The presence of the characteristic absorption peaks of C_C and C-H vibrations in the FTIR spectra suggested the occurrence of aromatization. The BET surface area improved by more than 11-fold（1201 m2/g for activated PG/C vs. 106 m2/g for PG/C） after activation, and the material appeared to be mainly microporous. The maximum adsorption capacity of methylene blue onto the activated PG/C reached 351 mg/g. The activated PG/C demonstrated better compressive strength than activated carbon without palygorskite clay.

Study on preparation and properties of CeO_2/epoxy resin composite coating on sintered NdFeB magnet

The CeO2/epoxy resin composite coating was deposited on NdFeB substrate by cathode electrophoresis method for enhancing the anticorrosion and anti-wear performances. The morphologies and structures were characterized by a scanning electron microscope and an X-ray diffractometer. The micro hardness of the composite coating was evaluated by a microhardness tester. The corrosive behaviors of the coatings were studied by potentiodynamic polarization curve, electrochemical impedance spectroscopy and neutral salt spray tests. The concentration of CeO2 nanoparticles（NPs） in the electrophoresis bath was optimized according to the coating structures and anticorrosion performances. The results show that CeO2 NPs can enhance the microhardness of the composite coatings. Moreover, the nanoparticles disperse uniformly in the matrix when the concentration is lower than 30 g/L. The microhardness of CeO2/epoxy resin（30 g/L） composite coating is about 63% higher than that of the blank epoxy resin coating. And the NSS time of the CeO2/epoxy resin（30 g/L） composite coated sample can reach 1248 h.Meanwhile, the composite coatings possess no deteriorate influence on the magnetic properties of NdFeB substrates. The anticorrosion mechanisms of the composite coatings on the NdFeB substrate are deeply discussed.

Microstructure evolution and mechanical anisotropy of M50 steel ball bearing rings during multi-stage hot forging

This study aimed to explore the evolution of flow lines and microstructures of M50-steel bearing ring and the anisotropy of its tensile mechanical properties after Multi-Stage Hot Forging(MSHF) and subsequent spheroidizing annealing(MSHFA). To this end, the present study mainly employed stereo microscopy, Optical Metallurgical Microscopy(OMM), Scanning Electron Microscopy(SEM), and Electron Backscatter Diffraction(EBSD) to characterize and analyze the workpiece at each processing stage of MSHF while performing microhardness measurement and uniaxial tensile experiment to test and analyze the mechanical properties of the workpiece. Macro-structure observation showed that the simulation results of flow lines at each stage were consistent with the experimental results. Microscopic observation showed that, after MSHF, deformation gradually became less significant along the outward radial direction of the bearing ring. After MSHFA,the microstructures of the bearing ring became uniform, whereas primary carbides did not dissolve.The mechanical properties were better in the axial direction(AD) than in the radial(RD) and circumferential directions(CD) after MSHF due to the smaller grain width. After MSHFA, the mechanical properties in the ADs and CDs were better than those in the RDs, which was due to the large cross-sectional area of carbides along the flow-line direction.

First results on ^(76)Ge neutrinoless double beta decay from CDEX-1 experiment

We report the first results on 76Ge neutrinoless double beta decay from stage one of the China dark-matter experiment （CDEX）. A p-type point-contact high-purity germanium detector with a mass of 994g has been installed to detect neutrinoless double beta decay events, as well as to directly detect dark matter particles. An exposure of 304kgd has been analyzed over a wide spectral band from 500keV to 3MeV. The average event rate obtained was about 0.012 counts per keV per kg per day over the 2.039MeV energy range. The half-life of76Ge neutrinoless double beta decay derived based on this result is 70v2〉6.4× 1022 yr （90%C.L.）. An upper limit on the effective Majorana-neutrino mass of 5.0eV has been achieved.

Facile and environment friendly synthesis of hierarchical BiOCl flowery microspheres with remarkable photocatalytic properties

A facile and environment friendly approach to synthesis of unique hierarchical BiOCl flowery microspheres(FMs)using a biodegradable surfactant polyvinyl alcohol(PVA)was reported herein for the first time.Compared to the BiOCl nanosheets synthesized in the absence of PVA,hierarchical BiOCl FMs consist of large amounts of interwoven polycrystalline nanosheets that assemble into a porous flowery structure.The formation mechanism of the hierarchical BiOCl FMs was also proposed,whereby PVA was believed to play a key role in the crystal growth and the formation of the final microstructures.Compared with TiO2-P25 and BiOCl nanosheets,hierarchical BiOCl FMs displayed remarkably enhanced photocatalytic activity,and20 mg of BiOCl FMs could completely degrade 50 mL of methyl orange solution(20 mg/L)within 30 min under UVlight irradiation.According to the comprehensive analysis,it can be concluded that the larger specific surface area,porosity,suitable band gap,and the enhanced light absorption capacity may contribute to the remarkably enhanced photocatalytic activity.This facile and green approach to fabricating hierarchical BiOCl FMs would give vital clues to develop new route for synthesizing other hierarchical structured materials.

Exceptional mechanical properties of AZ31 alloy wire by combination of cold drawing and EPT

A 0.66 mm-diameter AZ31 alloy wire with ultimate tensile strength of 400 MPa and elongation of 28.5%was successfully prepared via the combination of cold-drawing and electropulsing treatment processing(EPT).Microstructure observation showed that the grain size of EPTed samples was refined to about 1μm and the basal texture strength with maxima texture index was weakened to 7.18.EPT can significantly accelerate recrystallization by enhancing the mobility of dislocation and atomic diffusion due to the coupling of the thermal and athermal effects.Finally,uniform ultrafine-grained structure was obtained in the EPTed samples by static recrystallization completed in a very short time(30 s)at relatively low temperature(433 K).

First experimental constraints on WIMP couplings in the effective field theory framework from CDEX

We present weakly interacting massive particles(WIMPs) search results performed using two approaches of effective field theory from the China Dark Matter Experiment(CDEX), based on the data from both CDEX-1B and CDEX-10 stages. In the nonrelativistic effective field theory approach, both time-integrated and annual modulation analyses were used to set new limits for the coupling of WIMP-nucleon effective operators at 90% confidence level(C.L.) and improve over the current bounds in the low mχregion. In the chiral effective field theory approach, data from CDEX-10 were used to set an upper limit on WIMP-pion coupling at 90% C.L. We for the first time extended the limit to the m_(χ)<6 GeV/c^(2) region.

Densification and anticorrosion performances of vacuum evaporated aluminium coatings on NdFeB magnets

Al coated NdFeB magnets obtained by vacuum evaporation technique were densified by high energy ball milling method.The surface morphology,metal composition and micro structure of the coatings were characterized by scanning electron microscopy,X-ray diffraction and X-ray photoelectron spectroscopy,respectively.The anticorrosive properties were investigated by potentiodynamic polarization curves and neutral salt spray test.The pores in the Al coatings of columnar crystals(Al) induced by the evaporation technique,were apparently filled in the following ball milling process,leading to the densification of Al coatings and the evident improvement of the anticorrosive performances.When treated with ball milling for 30 min,the sample achieves the best anticorrosive performances with the self-corrosion potential of-0.87 V,self-corrosion current density of 1.65 μA/cm^(2) and the neutral salt spray(NSS) time of 144 h(red rust).The improvement of the anticorro sive performances of vacuum evaporated Al coating mainly lies in the densification effect of the coating,which depends on different loading conditions of ball milling process.

High detectivity photodetectors based on perovskite nanowires with suppressed surface defects

Solution-processable,single-crystalline perovskite nanowires are ideal candidates for developing low-cost photodetectors,but their detectivities are limited due to a high level of unintentional defects.Through the surfaceinitiated solution-growth method,we fabricated high-quality,single-crystalline,defects-suppressed MAPbI_(3) nanowires,which possess atomically smooth side surfaces with a surface roughness of 0.27 nm,corresponding to a carrier lifetime of 112.9 ns.By forming ohmic MAPbI_(3)∕Au contacts through the dry contact method,highperformance metal–semiconductor–metal photodetectors have been demonstrated with a record large linear dynamic range of 157 dB along with a record high detectivity of 1.2×10^(14) Jones at an illumination power density of 5.5 nW∕cm^(2).Such superior photodetector performance metrics are attributed to,first,the defects-suppressed property of the as-grown MAPbI_(3) nanowires,which leads to a quite low noise current in the dark,and second,the ohmic contact between MAPbI_(3) and Au interfaces,which gives rise to an improved responsivity compared with the Schottky contact counterpart.The realized high-performance MAPbI_(3) nanowire photodetector advances the development of low-cost photodetectors and has potential applications in weak-signal photodetection.

Fe-(9~11)Cr-Y_(2)O_(3)作为ITER结构材料的制备与表征

采用传统的机械合金(MA)和放电等离子体烧结(SPS)工艺成功制备了Fe-(9~11)Cr二元合金及纳米氧化物弥散强化(ODS)合金,利用扫描电子显微镜(SEM)、X射线衍射仪(XRD)对MA粉末的形貌和物相进行分析,用能量色散谱(EDS)、显微维氏硬度仪、光学显微镜、透射电子显微镜(TEM)对合金样品进行表征。结果表明,在转速为300 r/min,球料比为10:1的条件下,MA粉末受到磨球与罐子内壁的撞击,晶粒尺寸不断细化,在40 h粉末晶粒尺寸减小至约16.1 nm趋于稳定。SPS烧结后晶粒尺寸无明显增大,各微量元素均匀分布在基体中。二元合金样品的维氏硬度随Cr含量增加而增大。10CrY合金样品经腐蚀液侵蚀后可粗略看到晶界呈均匀分布。ODS合金样品存在大量的纳米析出相,平均颗粒尺寸约30 nm。

Microstructure and mechanical behavior of Mg-5Zn matrix influenced by particle deformation zone

The effect of particle deformation zone(PDZ) on the microstructure and mechanical properties of SiC_(p)/Mg-5Zn composites was studied.Meanwhile,the work hardening and so ftening behavior of SiC_(p)/Mg-5Zn composites influenced by PDZ size were analyzed and discussed using neutron diffraction under in-situ tensile deformation.The evolution of FWHM(full width at half maximum) extracted from the diffraction pattern of SiC_(p)/Mg-5Zn composites was used to interpret the modification of dislocation density during in-situ tension,which discovered the effect of dislocation on the work hardening behavior of SiC_(p)/Mg-5Zn composites.In addition,the tensile stress reduction(△P_i) values during in-situ tension test were calculated to analyze the effect of PDZ size on the softening behavior of SiC_(p)/Mg-5Zn composites.The results show that the work hardening rate of SiC_(p)/Mg-5Zn composites increased with the enlargement of PDZ size,which was attributed to the grain size of SiC_(p)/Mg-5Zn composites increased with the enlargement of PDZ size.Moreover,the stress reduction(△P_i) values increased continuously during in-situ tensile for SiC_(p)/Mg-5Zn composites due to the increased stored energy produced during plastic deformation,which provided a driving force for the softening effect.However,the effect of grain size on the softening behavior is greater than that of the stored energy,which led to the tensile stress reduction(△P_i) values of P30(d_(PDZ)=30 μm)-SiC_(p)/Mg-5Zn composite were higher than that of P60(d_(PDZ)=60 μm)-SiC_(p)/Mg-5Zn composite when the ε_(ri) were 0.25,0.5,0.75 and 1,respectively.