In situ infrared, Raman and X-ray spectroscopy for the mechanistic understanding of hydrogen evolution reaction

Hydrogen production by water reduction reactions has received considerable attention because hydrogen is considered a clean-energy carrier,key for a sustainable energy future.Computational methods have been widely used to study the reaction mechanism of the hydrogen evolution reaction(HER),but the calculation results need to be supported by experimental results and direct evidence to confirm the mechanistic insights.In this review,we discuss the fundamental principles of the in situ spectroscopic strategy and a theoretical model for a mechanistic understanding of the HER.In addition,we investigate recent studies by in situ Fourier transform infrared(FTIR),Raman spectroscopy,and X-ray absorption spectroscopy(XAS) and cover new findings that occur at the catalyst-electrolyte interface during HER.These spectroscopic strategies provide practical ways to elucidate catalyst phase,reaction intermediate,catalyst-electrolyte interface,intermediate binding energy,metal valency state,and coordination environment during HER.

Microstructures and micromechanical behaviors of high -entropy alloys investigated by synchrotron X-ray and neutron diffraction techniques: A review

High-entropy alloys(HEAs)possess outstanding features such as corrosion resistance,irradiation resistance,and good mechan-ical properties.A few HEAs have found applications in the fields of aerospace and defense.Extensive studies on the deformation mech-anisms of HEAs can guide microstructure control and toughness design,which is vital for understanding and studying state-of-the-art structural materials.Synchrotron X-ray and neutron diffraction are necessary techniques for materials science research,especially for in situ coupling of physical/chemical fields and for resolving macro/microcrystallographic information on materials.Recently,several re-searchers have applied synchrotron X-ray and neutron diffraction methods to study the deformation mechanisms,phase transformations,stress behaviors,and in situ processes of HEAs,such as variable-temperature,high-pressure,and hydrogenation processes.In this review,the principles and development of synchrotron X-ray and neutron diffraction are presented,and their applications in the deformation mechanisms of HEAs are discussed.The factors that influence the deformation mechanisms of HEAs are also outlined.This review fo-cuses on the microstructures and micromechanical behaviors during tension/compression or creep/fatigue deformation and the application of synchrotron X-ray and neutron diffraction methods to the characterization of dislocations,stacking faults,twins,phases,and intergrain/interphase stress changes.Perspectives on future developments of synchrotron X-ray and neutron diffraction and on research directions on the deformation mechanisms of novel metals are discussed.

Functional Confirmation Using a Medical X-Ray System of a Semiconductor Survey Meter

In recent years, semiconductor survey meters have been developed and are in increasing demand worldwide. This study determined if it is possible to use the X-ray system installed in each medical facility to calculate the time constant of a semiconductor survey meter and confirm the meter’s function. An additional filter was attached to the medical X-ray system to satisfy the standards of N-60 to N-120, more copper plates were added as needed, and the first and second half-value layers were calculated to enable comparisons of the facility’s X-ray system quality with the N-60 to N-120 quality values. Next, we used a medical X-ray system to measure the leakage dose and calculate the time constant of the survey meter. The functionality of the meter was then checked and compared with the energy characteristics of the meter. The experimental results showed that it was possible to use a medical X-ray system to reproduce the N-60 to N-120 radiation quality values and to calculate the time constant from the measured results, assuming actual leakage dosimetry for that radiation quality. We also found that the calibration factor was equivalent to that of the energy characteristics of the survey meter.

Assessing efficacy of standard impregnation techniques on die-cast aluminum alloys using X-ray micro-CT

Utilizing lightweight Al alloys in various industrial applications requires achieving precise pressure tightness and leak requirements.Vacuum pressure impregnation(VPI)with thermosetting polymers is commonly used to address leakage defects in die-cast Al alloys.In this study,the efficacy of the VPI technique in sealing alloy parts was investigated using a combination of nondestructive micro X-ray computed tomography(micro XCT)and a standard leak test.The results demonstrate that the commonly used water leak test is insufficient for determining the sealing performance.Instead,micro XCT shows distinct advantages by enabling more comprehensive analysis.It reveals the presence of a low atomic number impregnates sealant within casting defects,which has low grey contrast and allows for visualizing primary leakage paths in 3D.The effective atomic number of impregnated resin is 6.75 and that of Al alloy is 13.69 by dual-energy X-ray CT.This research findings will contribute to enhancing the standard VPI process parameters and the properties of impregnating sealants to improve quality assurance for impregnation in industrial metals.

Intensity correlation properties of x-ray beams split with Laue diffraction

Beam splitting is one of the main approaches to achieving x-ray ghost imaging, and the intensity correlation between diffraction beam and transmission beam will directly affect the imaging quality. In this paper, we investigate the intensity correlation between the split x-ray beams by Laue diffraction of stress-free crystal. The analysis based on the dynamical theory of x-ray diffraction indicates that the spatial resolution of diffraction image and transmission image are reduced due to the position shift of the exit beam. In the experimental setup, a stress-free crystal with a thickness of hundredmicrometers-level is used for beam splitting. The crystal is in a non-dispersive configuration equipped with a double-crystal monochromator to ensure that the dimension of the diffraction beam and transmission beam are consistent. A correlation coefficient of 0.92 is achieved experimentally and the high signal-to-noise ratio of the x-ray ghost imaging is anticipated.Results of this paper demonstrate that the developed beam splitter of Laue crystal has the potential in the efficient data acquisition of x-ray ghost imaging.

Theoretical characterization of the adsorption configuration of pyrrole on Si(100)surface by x-ray spectroscopy

The possible configurations of pyrrole absorbed on a Si(100)surface have been investigated by x-ray photoelectron spectroscopy(XPS)and near-edge x-ray absorption fine structure(NEXAFS)spectra.The C-1s XPS and NEXAFS spectra of these adsorption configurations have been calculated by using the density functional theory(DFT)method and fullcore hole(FCH)approximation to investigate the relationship between the adsorption configurations and the spectra.The result shows that the XPS and NEXAFS spectra are structurally dependent on the configurations of pyrrole absorbed on the Si(100)surface.Compared with the XPS,the NEXAFS spectra are relatively sensitive to the adsorption configurations and can accurately identify them.The NEXAFS decomposition spectra produced by non-equivalent carbon atoms have also been calculated and show that the spectral features vary with the diverse types of carbon atoms and their structural environments.

High-precision X-ray characterization for basic materials in modern high-end integrated circuit

Semiconductor materials exemplify humanity's unwavering pursuit of enhanced performance,efficiency,and functionality in electronic devices.From its early iterations to the advanced variants of today,this field has undergone an extraordinary evolution.As the reliability requirements of integrated circuits continue to increase,the industry is placing greater emphasis on the crystal qualities.Consequently,conducting a range of characterization tests on the crystals has become necessary.This paper will examine the correlation between crystal quality,device performance,and production yield,emphasizing the significance of crystal characterization tests and the important role of high-precision synchrotron radiation X-ray topography characterization in semiconductor analysis.Finally,we will cover the specific applications of synchrotron radiation characterization in the development of semiconductor materials.

基于X-rayμCT技术的玉米干燥损伤定量研究

应力裂纹是玉米干燥损伤的主要形式,一些微裂纹无法肉眼观察但影响玉米的机械强度、发芽率以及活力等。为此,利用X-rayμCT技术对不同干燥条件下玉米进行扫描,使用深度学习算法分割与胚乳密度相近的胚区域并结合软件对玉米内部物性特征参数进行提取,提出了一种新的玉米内部损伤定量评价方法。结合定量研究结果提出的玉米干燥损伤模型,可为玉米损伤预测提供新思路。

SMILE soft X-ray Imager flight model CCD370 pre-flight device characterisation

Throughout the SMILE mission the satellite will be bombarded by radiation which gradually damages the focal plane devices and degrades their performance.In order to understand the changes of the CCD370s within the soft X-ray Imager,an initial characterisation of the devices has been carried out to give a baseline performance level.Three CCDs have been characterised,the two flight devices and the flight spa re.This has been carried out at the Open University in a bespo ke cleanroom measure ment facility.The results show that there is a cluster of bright pixels in the flight spa re which increases in size with tempe rature.However at the nominal ope rating tempe rature(-120℃) it is within the procure ment specifications.Overall,the devices meet the specifications when ope rating at -120℃ in 6 × 6 binned frame transfer science mode.The se rial charge transfer inefficiency degrades with temperature in full frame mode.However any charge losses are recovered when binning/frame transfer is implemented.

胸腹部平扫CT值用于机会性筛查骨质疏松的可行性

目的:基于定量CT(QCT)探讨胸部常规kVp平扫和腹部能谱GSI平扫下椎体CT值用于机会性筛查骨质疏松的可行性。方法:前瞻性收集接受胸腹部平扫的患者431例,胸部CT扫描采用常规120 kVp,腹部扫描采用能谱(GSI)模式。对胸腹部扫描重叠的T11~L1椎体进行分析。使用QCT骨密度测量工作站测得胸部常规120 kVp下T11~L1椎体的骨密度(BMD),同时分别测量胸部120 kVp与腹部GSI扫描70 keV单能量下T11~L1椎体的CT值。采用组内相关系数(ICC)评估数据测量的一致性,Spearman相关性检验分析椎体BMD值与CT值之间的相关性。不同椎体间CT值差异采用Friedman秩和检验。参考QCT诊断标准,将椎体分为骨质疏松、骨量减少和骨量正常组,采用Kruskal-Wallis比较三组间及组内CT值差异。组内120 kVp-CT值和GSI-CT值采用Wilcoxon秩和检验。以T11~L1椎体BMD均值行骨质状态判定,采用受试者操作特征(ROC)曲线分析椎体CT值评估骨质状态的诊断效能。结果:椎体BMD与120 kVp-CT值和GSI-CT值均呈正相关(r=0.976、0.963,P<0.001)。120 kVp和GSI下T11~L1椎体CT值依次为T11[144.00(72.00)、158.00(79.00)]、T12[137.00(67.00)、150.00(76.00)]、L1[128.00(67.00)、137.00(74.00)],不同椎体及椎体内差异均有统计学意义(P<0.001)。431例患者共1293个椎体,骨量正常组椎体496个、骨量减少组椎体415个、骨质疏松组椎体382个。120 kVp和GSI下骨量正常、骨量减少和骨质疏松组椎体CT值依次为[181.50(43.67)、199.65(48.57)]、[132.20(18.50)、144.00(23.00)]和[87.75(22.20)、93.30(27.20)],不同骨质状态组间椎体CT值差异有统计学意义(P<0.05),且各组组内椎体GSI-CT值均高于椎体120 kVp-CT值(P<0.05)。120 kVp-CT值与GSI-CT值诊断骨量减少的AUC分别为0.976、0.967,差异无统计学意义(P=0.0937);诊断骨质疏松的AUC均为1.000,差异无统计学意义(P=1.000)。结论:胸部常规120 kVp及腹部GSI平扫CT值均可用于机会性筛查骨质疏松,诊断效能良好。

Exploring battery material failure mechanisms through synchrotron X-ray characterization techniques

Rechargeable battery cycling performance and related safety have been persistent concerns.It is crucial to decipher the capacity fading induced by electrode material failure via a range of techniques.Among these,synchrotron-based X-ray techniques with high flux and brightness play a key role in understanding degradation mechanisms.In this comprehensive review,we summarize recent advancements in degra-dation modes and mechanisms that were revealed by synchrotron X-ray methodologies.Subsequently,an overview of X-ray absorption spectroscopy and X-ray scattering techniques is introduced for charac-terizing failure phenomena at local coordination atomic environment and long-range order crystal struc-ture scale,respectively.At last,we envision the future of exploring material failure mechanism.

Automated Algorithms for Detecting and Classifying X-Ray Images of Spine Fractures

This paper emphasizes a faster digital processing time while presenting an accurate method for identifying spinefractures in X-ray pictures. The study focuses on efficiency by utilizing many methods that include picturesegmentation, feature reduction, and image classification. Two important elements are investigated to reducethe classification time: Using feature reduction software and leveraging the capabilities of sophisticated digitalprocessing hardware. The researchers use different algorithms for picture enhancement, including theWiener andKalman filters, and they look into two background correction techniques. The article presents a technique forextracting textural features and evaluates three picture segmentation algorithms and three fractured spine detectionalgorithms using transformdomain, PowerDensity Spectrum(PDS), andHigher-Order Statistics (HOS) for featureextraction.With an emphasis on reducing digital processing time, this all-encompassing method helps to create asimplified system for classifying fractured spine fractures. A feature reduction program code has been built toimprove the processing speed for picture classification. Overall, the proposed approach shows great potential forsignificantly reducing classification time in clinical settings where time is critical. In comparison to other transformdomains, the texture features’ discrete cosine transform (DCT) yielded an exceptional classification rate, and theprocess of extracting features from the transform domain took less time. More capable hardware can also result inquicker execution times for the feature extraction algorithms.

Gas microchannel plate-pixel detector for X-ray polarimetry

POLAR-2 is a gamma-ray burst(GRB)polarimeter that is designed to study the polarization in GRB radiation emissions,aiming to improve our knowledge of related mechanisms.POLAR-2 is expected to utilize an on-board polarimeter that is sensitive to soft X-rays(2-10 keV),called low-energy polarization detector.We have developed a new soft X-ray polari-zation detector prototype based on gas microchannel plates(GMCPs)and pixel chips(Topmetal).The GMCPs have bulk resistance,which prevents charging-up effects and ensures gain stability during operation.The detector is composed of low outgassing materials and is gas-sealed using a laser welding technique,ensuring long-term stability.A modulation factor of 41.28%±0.64% is obtained for a 4.5 keV polarized X-ray beam.A residual modulation of 1.96%±0.58% at 5.9 keV is observed for the entire sensitive area.

Optimized online filter stack spectrometer for ultrashort X-ray pulses

Currently,with the advent of high-repetition-rate laser-plasma experiments,the demand for online diagnosis for the X-ray spectrum is increasing because the laser-plasma-generated X-ray spectrum is very important for characterizing electron dynamics and applications.In this study,scintillators and silicon PIN(P-type–intrinsic-N-type semiconductor)diodes were used to construct a wideband online filter stack spectrometer.The X-ray sensor and filter arrangement was optimized using a genetic algorithm to minimize the condition number of the response matrix.Consequently,the unfolding error was significantly reduced based on numerical experiments.The detector responses were quantitatively calibrated by irradiating the scintillator and PIN diode with various nuclides and comparing the measuredγ-ray peaks.A prototype 15-channel spectrometer was developed by integrating an X-ray detector with front-and back-end electronics.The prototype spectrometer could record X-ray pulse signals at a repetition rate of 1 kHz.Furthermore,an optimized spectrometer was employed to record the real-time spectra of laser-driven bremsstrahlung sources.This optimized spectrometer offers a compact solution for spectrum diagnostics of ultrashort X-ray pulses,exhibiting improved accuracy in terms of spectrum measurements and repetition rates,and could be widely used in next-generation high-repetition-rate high-power laser facilities.

Quick-scanning X-ray absorption fine structure beamline at SSRF

The layout and characteristics of the hard X-ray spectroscopy beamline(BL11B)at the Shanghai synchrotron radiation facility are described herein.BL11B is a bending-magnet beamline dedicated to conventional and millisecond-scale quick-scanning X-ray absorption fine structures.It is equipped with a cylindrical collimating mirror,a double-crystal monochromator comprising Si(111)and Si(311),a channel-cut quick-scanning Si(111)monochromator,a toroidal focusing mirror,and a high harmonics rejection mirror.It can provide 5-30 keV of X-rays with a photon flux of~5×10^(11)photons/s and an energy resolution of~1.31×10^(-4)at 10 keV.The performance of the beamline can satisfy the demands of users in the fields of catalysis,materials,and environmental science.This paper presents an overview of the beamline design and a detailed description of its performance and capabilities.

Atmospheric transmission algorithm for pulsed X-rays from high-altitude nuclear detonations based on scattering correction

In high-altitude nuclear detonations,the proportion of pulsed X-ray energy can exceed 70%,making it a specific monitoring signal for such events.These pulsed X-rays can be captured using a satellite-borne X-ray detector following atmospheric transmission.To quantitatively analyze the effects of different satellite detection altitudes,burst heights,and transmission angles on the physical processes of X-ray transport and energy fluence,we developed an atmospheric transmission algorithm for pulsed X-rays from high-altitude nuclear detonations based on scattering correction.The proposed method is an improvement over the traditional analytical method that only computes direct-transmission X-rays.The traditional analytical method exhibits a maximum relative error of 67.79% compared with the Monte Carlo method.Our improved method reduces this error to within 10% under the same conditions,even reaching 1% in certain scenarios.Moreover,its computation time is 48,000 times faster than that of the Monte Carlo method.These results have important theoretical significance and engineering application value for designing satellite-borne nuclear detonation pulsed X-ray detectors,inverting nuclear detonation source terms,and assessing ionospheric effects.

Population-based X-ray gastric cancer screening in Hiroshima prefecture, Japan

BACKGROUND X-ray gastric cancer(GC)screening has been shown to decrease mortality.Population-based X-ray GC screening has been performed in Hiroshima Prefe-cture,Japan,since 1983 but time trends and the efficacy of the method over 39 years have not been assessed.METHODS This was a population-based retrospective study.The data were derived from aggregated data of the Hiroshima Regional Health Medical Promotion Organization,including the number and rate of participants and those requiring esophagogastroduodenoscopies(EGDs),the number and rate of participants diagnosed as having GC,and the positive predictive value of the abnormal findings detected by X-ray and confirmed by EGDs.The number and rate of esophageal cancers were also collected.Further,the cost of detecting one GC was evaluated.RESULTS The number of participants has decreased during the last four decades,from 39925 in 1983 to 12923 in 2021.The rate of those requiring EGDs decreased significantly in recent years(P<0.001).The number of participants diagnosed as having GC has also declined,from 76 to 10 cases.However,the rate of cases diagnosed as GC among the participants remained around 0.1%.The positive predictive value increased significantly in recent years except during 1983-1991.The number and rate of accidentally detected esophageal cancers have risen recently,from 0%in 2008 to 0.02%in 2021,one-fifth of the diagnosis rate of GC.One GC diagnosis costs approximately 4200000 Japanese Yen(30000 United States Dollars)for the X-ray screenings and EGDs.CONCLUSION X-ray GC screening in Hiroshima has been efficient,but one challenge is the cost.Esophageal cancers may also need to be considered because they have gradually increased in recent years.

Metal-Halide Perovskite Submicrometer-Thick Films for Ultra-Stable Self-Powered Direct X-Ray Detectors

Metal-halide perovskites are revolutionizing the world of X-ray detectors,due to the development of sensitive,fast,and cost-effective devices.Self-powered operation,ensuring portability and low power consumption,has also been recently demonstrated in both bulk materials and thin films.However,the signal stability and repeatability under continuous X-ray exposure has only been tested up to a few hours,often reporting degradation of the detection performance.Here it is shown that self-powered direct X-ray detectors,fabricated starting from a FAPbBr_(3)submicrometer-thick film deposition onto a mesoporous TiO_(2)scaffold,can withstand a 26-day uninterrupted X-ray exposure with negligible signal loss,demonstrating ultra-high operational stability and excellent repeatability.No structural modification is observed after irradiation with a total ionizing dose of almost 200 Gy,revealing an unexpectedly high radiation hardness for a metal-halide perovskite thin film.In addition,trap-assisted photoconductive gain enabled the device to achieve a record bulk sensitivity of 7.28 C Gy^(−1)cm^(−3)at 0 V,an unprecedented value in the field of thin-film-based photoconductors and photodiodes for“hard”X-rays.Finally,prototypal validation under the X-ray beam produced by a medical linear accelerator for cancer treatment is also introduced.

Ultrahard X-ray multifunctional application beamline at the SSRF

The ultrahard X-ray multifunctional application beamline(BL12SW)is a phase-II beamline project at the Shanghai Syn-chrotron Radiation Facility.The primary X-ray techniques used at the beamline are high-energy X-ray diffraction and imaging using white and monochromatic light.The main scientific objectives of ultrahard X-ray beamlines are focused on two research areas.One is the study of the structural properties of Earth’s interior and new materials under extreme high-temperature and high-pressure conditions,and the other is the characterization of materials and processes in near-real service environments.The beamline utilizes a superconducting wiggler as the light source,with two diamond windows and SiC discs to filter out low-energy light(primarily below 30 keV)and a Cu filter assembly to control the thermal load entering the subsequent optical components.The beamline is equipped with dual monochromators.The first was a meridional bending Laue monochromator cooled by liquid nitrogen,achieving a full-energy coverage of 30-162 keV.The second was a sagittal bending Laue monochromator installed in an external building,providing a focused beam in the horizontal direction with an energy range of 60-120 keV.There were four experimental hutches:two large-volume press experimental hutches(LVP1 and LVP2)and two engineering material experimental hutches(ENG1 and ENG2).Each hutch was equipped with various near-real service conditions to satisfy different requirements.For example,LVP1 and LVP2 were equipped with a 200-ton DDIA press and a 2000-ton dual-mode(DDIA and Kawai)press,respectively.ENG1 and ENG2 provide in situ tensile,creep,and fatigue tests as well as high-temperature conditions.Since June 2023,the BL12SW has been in trial operation.It is expected to officially open to users by early 2024.

Insights into the hydrogen evolution reaction in vanadium redox flow batteries:A synchrotron radiation based X-ray imaging study

The parasitic hydrogen evolution reaction(HER)in the negative half-cell of vanadium redox flow batteries(VRFBs)causes severe efficiency losses.Thus,a deeper understanding of this process and the accompanying bubble formation is crucial.This benchmarking study locally analyzes the bubble distribution in thick,porous electrodes for the first time using deep learning-based image segmentation of synchrotron X-ray micro-tomograms.Each large three-dimensional data set was processed precisely in less than one minute while minimizing human errors and pointing out areas of increased HER activity in VRFBs.The study systematically varies the electrode potential and material,concluding that more negative electrode potentials of-200 m V vs.reversible hydrogen electrode(RHE)and lower cause more substantial bubble formation,resulting in bubble fractions of around 15%–20%in carbon felt electrodes.Contrarily,the bubble fractions stay only around 2%in an electrode combining carbon felt and carbon paper.The detected areas with high HER activity,such as the border subregion with more than 30%bubble fraction in carbon felt electrodes,the cutting edges,and preferential spots in the electrode bulk,are potential-independent and suggest that larger electrodes with a higher bulk-to-border ratio might reduce HER-related performance losses.The described combination of electrochemical measurements,local X-ray microtomography,AI-based segmentation,and 3D morphometric analysis is a powerful and novel approach for local bubble analysis in three-dimensional porous electrodes,providing an essential toolkit for a broad community working on bubble-generating electrochemical systems.