We present a comprehensive study of the CO_(2)-CO interaction potential using a 9-dimensional(9D)potential energy surface(PES)constructed with the fundamental invariant-neural networks(FINN)method.The PES was generate...We present a comprehensive study of the CO_(2)-CO interaction potential using a 9-dimensional(9D)potential energy surface(PES)constructed with the fundamental invariant-neural networks(FINN)method.The PES was generated from 65330 CCSD(T)-F12a/aug-cc-pVTZ ab initio data points,with counterpoise correction,applied to eliminate basis set superposition error(BSSE).We performed quasi-classical trajectory simulations using this PES to investigate the rotational energy transfer dynamics.Our results reveal complex energy transfer mechanisms,with significant rotational excitation and relaxation dependent on collision energy and initial rotational states.The 9D PES provides a more accurate representation of the CO_(2)-CO system,offering new insights into molecular dynamics and interaction mechanisms.展开更多
Microstructure of shale formation is the key to understanding its petrophysical and chemical properties.Optical microscopy, scanning electron microscopy and micro-computed tomography(μ-CT) have been combined for char...Microstructure of shale formation is the key to understanding its petrophysical and chemical properties.Optical microscopy, scanning electron microscopy and micro-computed tomography(μ-CT) have been combined for characterization of microstructure of Longmaxi(LMX)shale from Shizhu area, Sichan Basin. The results indicate that laminated LMX shale consists of mineral matrix-rich layers and organic matter(OM)-rich layers at micrometer scale in two and three dimensions. Mineral matrix layers,mainly consisting of interparticle pores and intraplatelet pores, are approximately parallel to the bedding plane.Pyrite-rich layer, mainly containing intercrystalline pores,shows a strong preferred orientation parallel to the bedding plane. OM-rich layer, mainly containing OM pores, seems to be discontinuous. In addition, intercrystalline pores are enriched in some layers, while OM pores are distributed irregularly in matrix layers. This vertical heterogeneity of pore microscopic structures in LMX shale is of great importance to understand its petrophysical and chemical properties.展开更多
Although various and unique properties of bulk nanobubbles have drawn researchers'attention over the last few years,their formation and stabilization mechanism has remained unsolved.In this paper,we use ultrasonic...Although various and unique properties of bulk nanobubbles have drawn researchers'attention over the last few years,their formation and stabilization mechanism has remained unsolved.In this paper,we use ultrasonic methods to produce bulk nanobubbles in the pure water and give a comprehensive study on the bulk nanobubbles properties and generation.The ultrasonic wave gives rise to constant oscillation in water where positive and negative pressure appears alternately.With the induced cavitation and presence of dissolved air,the bulk nanobubbles formed."Nanosight"(which is a special instrument that combines dynamic light scattering with nanoparticle tracking analysis)was used to analyze the track and concentration of nanobubbles.Our results show that in our experiment,sufficient bulk nanobubbles were generated and we have proven they are not contaminations.We also found nanobubbles in the ultrasonic water change in both size and concentration with ultrasonic time.展开更多
The corrosion behavior of 316H stainless steel(SS)in the impure and purified Na Cl–KCl–Mg Cl_(2) salt was investigated at700°C.Results indicate that the main deleterious impurity induced corrosion in the impure...The corrosion behavior of 316H stainless steel(SS)in the impure and purified Na Cl–KCl–Mg Cl_(2) salt was investigated at700°C.Results indicate that the main deleterious impurity induced corrosion in the impure salt was the absorbed moisture,present in the form of Mg Cl_(2)·6H_(2)O.316H SS occurred severe intergranular corrosion with a corrosion depth of 130μm for1000 h in the impure Na Cl–KCl–Mg Cl_(2) salt.In contrast,the purification treatment of molten chloride salt by the dissolved Mg metal can remove the absorbed moisture,and the corresponding reactions were also discussed.As a result,the corrosiveness of Na Cl–KCl–Mg Cl_(2) salt is reduced significantly.316H SS occurred slight uniform corrosion with a depth of less than 5μm for 3000 h in the purified Na Cl–KCl–Mg Cl_(2) salt.展开更多
The contents and distributions of metal elements in the brain are closely related to neurodegenerative diseases.In this study, we examined Fe, Cu and Zn contents in the brain section associated with Parkinson‘s disea...The contents and distributions of metal elements in the brain are closely related to neurodegenerative diseases.In this study, we examined Fe, Cu and Zn contents in the brain section associated with Parkinson‘s disease(PD)using synchrotron radiation X-ray fluorescence(SRXRF). PD mouse model induced by 1-methyl-4-phenyl-1,2,3,6-terahydropyridine(MPTP) was used for the elemental analysis(e.g., Fe, Cu and Zn) in the substantia nigra pars compacta(SNpc) region of mice brain tissue samples. We found that mice in the MPTP group had higher contents of Fe, Cu and Zn in the SNpc than the control group. After treating the PD mice with rapamycin, the contents of Fe, Cu and Zn were reduced, the dopamine neurons and motor function were rescued correspondingly. The results prompted that the SRXRF provided an ideal method for tracing and analyzing the metal elements in the brain section to assess the pathological changes of PD model and the therapeutic effect of drugs.展开更多
Effective electrocatalysis is crucial for enhancing the efficiency of water splitting to obtain clean fuels.Herein,we report a system of interesting and high-performance Sr-doped perovskite electrocatalysts with porou...Effective electrocatalysis is crucial for enhancing the efficiency of water splitting to obtain clean fuels.Herein,we report a system of interesting and high-performance Sr-doped perovskite electrocatalysts with porous structures,obtained via a facile molten salt method and applied in the oxygen evolution reaction(OER).With increasing the Sr content,the valence states of Co and Fe ions do not clearly increase,according to the Co-L2,3 and Fe-L2,3 as well as the Co-K and the Fe-K X-ray absorption spectroscopy,whereas doped holes are clearly observed in the 0-K edge.High-resolution transmission electron microscopy indicates the appearance of an amorphous layer after the electrochemical reaction.We conclude that the formation of the amorphous layer at the surface,induced by Sr doping,is crucial for achieving high OER activity,and we offer insights into the self-reconstruction of the OER catalyst.展开更多
Perovskite-type mixed protonic-electronic conducting membranes have attracted attention because of their ability to separate and purify hydrogen from a mixture of gases generated by industrial-scale steam reforming ba...Perovskite-type mixed protonic-electronic conducting membranes have attracted attention because of their ability to separate and purify hydrogen from a mixture of gases generated by industrial-scale steam reforming based on an ion diffusion mechanism.Exploring cost-effective membrane materials that can achieve both high H_(2) permeability and strong CO_(2)-tolerant chemical stability has been a major challenge for industrial applications.Herein,we constructed a triple phase(ceramic-metal-ceramic)membrane composed of a perovskite ceramic phase BaZr_(0.1)Ce_(0.7)Y_(0.1)Yb_(0.1)O_(3-δ)(BZCYYb),Ni metal phase and a fluorite ceramic phase CeO_(2).Under H_(2) atmosphere,Ni metal in-situ exsolved from the oxide grains,and decorated the grain surface and boundary,thus the electronic conductivity and hydrogen separation performance can be promoted.The BZCYYbNi-CeO_(2)hybrid membrane achieved an exceptional hydrogen separation performance of 0.53 mL min^(-1)cm^(-2) at 800℃ under a 10 vol% H_(2) atmosphere,surpassing all other perovskite membranes reported to date.Furthermore,the CeO_(2) phase incorporated into the BZCYYb-Ni effectively improved the CO_(2)-tolerant chemical stability.The BZCYYbNi-CeO_(2) membrane exhibited outstanding long-term stability for at least 80 h at 700℃ under 10 vol%CO_(2)-10 vol%H_(2).The success of hybrid membrane construction creates a new direction for simultaneously improving their hydrogen separation performance and CO_(2) resistance stability.展开更多
Sr-substituted ABO_3 perovskite oxides such as La_(0.6) Sr_(0.4 )Mn_(O3-δ)(LSM) and La_(0.6) Sr_(0.4) FeO_(3-δ)(LSF) are widely used as oxygen electrode materials in solid oxide cells. The substituted Sr is not adeq...Sr-substituted ABO_3 perovskite oxides such as La_(0.6) Sr_(0.4 )Mn_(O3-δ)(LSM) and La_(0.6) Sr_(0.4) FeO_(3-δ)(LSF) are widely used as oxygen electrode materials in solid oxide cells. The substituted Sr is not adequately stable under the operating conditions, because of the surface segregation of Sr. Herein, we focused on investigating the relationship between the local geometric structure due to Sr substitution and stability of LSM and LSF. We characterized the local geometric structure of Sr atoms via X-ray absorption spectroscopy. A greater Debye-Waller factor and a longer bond length of both the second and third Sr-O shells were observed in LSF, which demonstrates that LSF has a higher local structural disorder and that Sr in LSF requires less energy to segregate. After 20 h of heat treatment in the presence of a Fe-Cr alloy interconnect, the Sr/La molar ratio on LSF was observed to be much larger than that on LSM. This result unequivocally suggests that Sr in LSF is not as stable as in LSM, and the reaction between Sr and Cr accelerates the Sr surface segregation in LSF.展开更多
Water molecules could form a liquid droplet on the water monolayer on a specific solid surface, which has been referred to as ‘‘ordered water monolayer that does not completely wet water'' at room temperatur...Water molecules could form a liquid droplet on the water monolayer on a specific solid surface, which has been referred to as ‘‘ordered water monolayer that does not completely wet water'' at room temperature. In contrast to the water molecules, the family of alcohol molecules has the same OH polar head and various lengths of their hydrophobic nonpolar tail; the length of the hydrophobic tail can affect the hydrophobic effect. In this study, using molecular dynamics simulations, we investigated the wetting behaviors of methanol, ethanol, and propanol molecules adsorbed on a SiO_2 surface. The results showed that the methanol, ethanol, and propanol molecules could form an ordered monolayer on the SiO_2 surface and a droplet on top of this monolayer, with different contact angles. The differences in the contact angles were attributed to the differences in the interactions between the alcohol monolayer and droplet.展开更多
Anesthetics are extremely important in modem surgery to greatly reduce the patient,s pain. The understanding of anesthesia at molecular level is the preliminary step for the application of anesthetics in clinic safely...Anesthetics are extremely important in modem surgery to greatly reduce the patient,s pain. The understanding of anesthesia at molecular level is the preliminary step for the application of anesthetics in clinic safely and effectively. Inert gases, with low chemical activity, have been found to cause anesthesia for centuries, but the mechanism is unclear yet. In this review, we first summarize the progress of theories about general anesthesia, especially for inert gas narcosis, and then propose a new hypothesis that the aggregated rather than the dispersed inert gas molecules are the key to trigger the narcosis to explain the steep dose-response relationship of anesthesia.展开更多
Understanding the dynamic evolution of active sites of supported metal catalysts during catalysis is fundamentally important for improving its performance,which attracts tremendous research interests in the past decad...Understanding the dynamic evolution of active sites of supported metal catalysts during catalysis is fundamentally important for improving its performance,which attracts tremendous research interests in the past decades.There are two main surficial structures for metal catalysts:terrace sites and step sites,which exhibit catalytic activity discrepancy during catalysis.Herein,by using in situ transmission electron microscopy and in situ Fourier transform infrared spectroscopy(FTIR),the transformation between surface terrace and step sites of Pt-TiO_(2) catalysts was studied under CO and O_(2) environments.We found that the{111}step sites tend to form at{111}terrace under O_(2) environment,while these step sites prefer to transform into terrace under CO environment at elevated temperature.Meanwhile,quantitative ratios of terrace/step sites were obtained by in situ FTIR.It was found that this transformation between terrace sites and step sites was reversible during gas treatment cycling of CO and O_(2).The selective adsorption of O_(2) and CO species at different sites,which stabilized the step/terrace sites,was found to serve as the driving force for active sites transition by density functional theory calculations.Inspired by the in situ results,an enhanced catalytic activity of Pt-TiO_(2) catalysts was successfully achieved through tuning surface-active sites by gas treatments.展开更多
Terahertz biotechnology has been increasingly applied in various biomedical fields and has especially shown great potential for application in brain sciences.In this article,we review the development of terahertz biot...Terahertz biotechnology has been increasingly applied in various biomedical fields and has especially shown great potential for application in brain sciences.In this article,we review the development of terahertz biotechnology and its applications in the field of neuropsychiatry.Available evidence indicates promising prospects for the use of terahertz spectroscopy and terahertz imaging techniques in the diagnosis of amyloid disease,cerebrovascular disease,glioma,psychiatric disease,traumatic brain injury,and myelin deficit.In vitro and animal experiments have also demonstrated the potential therapeutic value of terahertz technology in some neuropsychiatric diseases.Although the precise underlying mechanism of the interactions between terahertz electromagnetic waves and the biosystem is not yet fully understood,the research progress in this field shows great potential for biomedical noninvasive diagnostic and therapeutic applications.However,the biosafety of terahertz radiation requires further exploration regarding its two-sided efficacy in practical applications.This review demonstrates that terahertz biotechnology has the potential to be a promising method in the field of neuropsychiatry based on its unique advantages.展开更多
Aluminium is widely used as an antimicrobial coagulant,food additive,and cookware.However,many reports indicate that aluminium may be a critical factor in many amyloid diseases,such as Alzheimer’s disease and Parkin...Aluminium is widely used as an antimicrobial coagulant,food additive,and cookware.However,many reports indicate that aluminium may be a critical factor in many amyloid diseases,such as Alzheimer’s disease and Parkinson’s disease.Unfortunately,the underlying mechanism is still poorly understood,which limits efforts to prevent and treat these diseases.In this paper,using an ab initio method,we studied the interaction of Al-backbone ring structure with theπ-electron-rich sidechains of His,Phe,Trp,and Tyr.We found that in the absence of water,the Al-backbone ring can stably bind with those sidechains.In the presence of water,the Al-backbone ring can bind to the His sidechain and cannot bind to the other sidechains.As revealed by further investigations,this could be attributed to the fact that there was a coordinate bond of the Al-backbone ring with the His sidechain,while there were theπ-πstacking and cation-π-like interactions with the other sidechains.These findings potentially provide a molecular understanding of Al-related toxicity,and may be helpful in designing drugs for those aforementioned aluminum-linked diseases and encourage treatment of Al-polluted water.展开更多
Using molecular dynamics simulations, we investigate the influence of Na and Cl ions on the evaporation of nanoscale water on graphene oxide surfaces. As the concentration of NaCl increases from 0 to 1.5 M, the evapor...Using molecular dynamics simulations, we investigate the influence of Na and Cl ions on the evaporation of nanoscale water on graphene oxide surfaces. As the concentration of NaCl increases from 0 to 1.5 M, the evaporation rate shows a higher decrease on patterned graphene oxide than that on homogeneous graphene oxide.The analysis shows an obvious decrease in the evaporation rate from unoxidized regions, which can be attributed to the increased amount of Na^+ ions near the contact lines.The proximity of Na^+ significantly extends the H-bond lifetime of the outermost water molecules, which reduces the number of water molecules diffusing from the oxidized to unoxidized regions. Moreover, the effect of the ions on water evaporation is less significant when the oxidation degree varies in a certain range. Our findings advance the understanding of the evaporation process in the presence of ions and highlight the potential application of graphene oxide in achieving controllable evaporation of liquids.展开更多
Electronic structures and optical properties of single-layer In1-xGaxN are studied by employing Heyd-Scuseria-Ernzerh（HSE） method based on the first-principles. The band structure and density of states（DOS） of sin...Electronic structures and optical properties of single-layer In1-xGaxN are studied by employing Heyd-Scuseria-Ernzerh（HSE） method based on the first-principles. The band structure and density of states（DOS） of single-layer In1-xGaxN are calculated, and the band gap ranges from 1.8 eV to 3.8 eV as the ratio x changes, illustrating the potential for the tunability of band gap values via Ga doped. We also have investigated optical properties of single-layer In1-xGaxN such as dielectric function, refractive index and absorption coefficient, the main peak of dielectric function spectrum and the absorption edge are found to have a remarkable blue-shift as the concentration of Ga increases. Furthermore, the optical properties of single-layer In1-xGaxN are analyzed based on the band structures and DOS analysis. Such unique optical properties have profound application in nanoelectronics and optical devices.展开更多
The arrangement of DNA-based nanostructures into the desired large-scale periodic pattern with the highest possible accuracy and control is essential for the DNA application in functional biomaterials;however, formati...The arrangement of DNA-based nanostructures into the desired large-scale periodic pattern with the highest possible accuracy and control is essential for the DNA application in functional biomaterials;however, formation of a DNA nanostructure pattern without utilizing the molecular interactions in nanotechnology field remains difficult. In this article, we use the optimal concentration and adsorption time of origami to induce DNA origami in the form of a large-scale 2D pattern on mica without changing the origami itself. DNA origami structures can form a pattern by close packing of symmetric and electrostatic interactions between ions, which was confirmed by the atomic force microscopy images. Furthermore, we identified favorable conditions for the concentration of enable pattern formation with DNA origami. This work provides an insight to understand the adsorption of DNA on mica and guides researches on regular DNA nanostructure pattern, which can serve as templates for pattern formation of proteins or other biomolecules.展开更多
As a robust platform for genome editing,CRISPR/Cas9 is currently being explored for engineering biology or therapeutics,yet means for quantitative detection of Cas9 proteins remain to be fully realized.Here,we express...As a robust platform for genome editing,CRISPR/Cas9 is currently being explored for engineering biology or therapeutics,yet means for quantitative detection of Cas9 proteins remain to be fully realized.Here,we expressed Cas9 proteins and developed a novel detection method that traced Cas9 based on radiolabeled iodine.Through optimizing the reaction conditions of reaction time,temperature and cycles,we obtained ^(125)I-Cas9 of high labeling yield.The prepared ^(125)I-Cas9 was stable in various media and preserved excellent genome editing efficiency.Thus,our strategy provides a convenient and efficient tool for further tracing biological behaviors of Cas9 proteins in living systems.展开更多
Ni nanocatalysts produced through exsolution have shown strong resistance to particle sintering and carbon coking in a beneficial dry reforming of methane(DRM)reaction utilizing greenhouse gases such as CH_(4)and CO_(...Ni nanocatalysts produced through exsolution have shown strong resistance to particle sintering and carbon coking in a beneficial dry reforming of methane(DRM)reaction utilizing greenhouse gases such as CH_(4)and CO_(2).However,most of the existing oxide supports for exsolution have been limited to perovskite oxide,while studies on fluorite support have been rarely conducted due to the limited solubility despite its excellent redox stability.Here we demonstrate that 3 mol%Ni can be successfully dissolved into the yttria-stabilized zirconia(YSZ)lattice and be further exsolved to the surface in a reducing atmosphere.The YSZ decorated with exsolved Ni nanoparticles shows enhanced catalytic activity for DRM reaction compared to the conventional cermet type of bulk Ni-YSZ.Moreover,the catalytic activity is extremely stable for about 300 h without significant degradation.Overall results suggest that the YSZ-based fluorite structure can be utilized as one of the support oxides for exsolution.展开更多
X-ray scattering is widely used in material structural characterizations.The weak scattering nature,however,makes it susceptible to background noise and can consequently render the final results unreliable.In this pap...X-ray scattering is widely used in material structural characterizations.The weak scattering nature,however,makes it susceptible to background noise and can consequently render the final results unreliable.In this paper,we report an iterative method to determine X-ray scattering background and demonstrate its feasibility by small angle X-ray scattering on gold nanoparticles.This method solely relies on the correct structural modeling of the sample to separate scattering signal from background in data fitting processes,which allows them to be immune from experimental uncertainties.The importance of accurate determination of the scaling factor for background subtraction is also illustrated.展开更多
The first principles density-functional theoretical calculations of U adatom adsorption and diffusion on a planar graphene and quasi-one-dimensional graphene nanoribbons（GNRs） are performed. An energetic preference ...The first principles density-functional theoretical calculations of U adatom adsorption and diffusion on a planar graphene and quasi-one-dimensional graphene nanoribbons（GNRs） are performed. An energetic preference is found for U adatom diffusing to the hollow sites of both graphene and GNRs surface. A number of U distinctive diffusion paths either perpendicular or parallel to the ribbon growth direction are examined. The edge effects are evidenced by the calculated energy barriers of U adatom diffusion on armchair and zigzag nanoribbons surfaces. The calculation results indicate that the diffusion of U adatom from the inner site toward the edge site is a feasible process, particularly in zigzagGNR. It is viable to control the initial morphology of nuclear carbon material to retard the diffusion and concentration of nuclides.展开更多
基金financially supported by the National Natural Science Foundation of China(No.22173104)。
文摘We present a comprehensive study of the CO_(2)-CO interaction potential using a 9-dimensional(9D)potential energy surface(PES)constructed with the fundamental invariant-neural networks(FINN)method.The PES was generated from 65330 CCSD(T)-F12a/aug-cc-pVTZ ab initio data points,with counterpoise correction,applied to eliminate basis set superposition error(BSSE).We performed quasi-classical trajectory simulations using this PES to investigate the rotational energy transfer dynamics.Our results reveal complex energy transfer mechanisms,with significant rotational excitation and relaxation dependent on collision energy and initial rotational states.The 9D PES provides a more accurate representation of the CO_(2)-CO system,offering new insights into molecular dynamics and interaction mechanisms.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB1002010)the Major Program for the Fundamental Research of Shanghai Committee of Science and Technology(No.12JC1410400)the National Natural Science Foundation of China for Distinguished Young Scholars(No.41325016)
文摘Microstructure of shale formation is the key to understanding its petrophysical and chemical properties.Optical microscopy, scanning electron microscopy and micro-computed tomography(μ-CT) have been combined for characterization of microstructure of Longmaxi(LMX)shale from Shizhu area, Sichan Basin. The results indicate that laminated LMX shale consists of mineral matrix-rich layers and organic matter(OM)-rich layers at micrometer scale in two and three dimensions. Mineral matrix layers,mainly consisting of interparticle pores and intraplatelet pores, are approximately parallel to the bedding plane.Pyrite-rich layer, mainly containing intercrystalline pores,shows a strong preferred orientation parallel to the bedding plane. OM-rich layer, mainly containing OM pores, seems to be discontinuous. In addition, intercrystalline pores are enriched in some layers, while OM pores are distributed irregularly in matrix layers. This vertical heterogeneity of pore microscopic structures in LMX shale is of great importance to understand its petrophysical and chemical properties.
文摘Although various and unique properties of bulk nanobubbles have drawn researchers'attention over the last few years,their formation and stabilization mechanism has remained unsolved.In this paper,we use ultrasonic methods to produce bulk nanobubbles in the pure water and give a comprehensive study on the bulk nanobubbles properties and generation.The ultrasonic wave gives rise to constant oscillation in water where positive and negative pressure appears alternately.With the induced cavitation and presence of dissolved air,the bulk nanobubbles formed."Nanosight"(which is a special instrument that combines dynamic light scattering with nanoparticle tracking analysis)was used to analyze the track and concentration of nanobubbles.Our results show that in our experiment,sufficient bulk nanobubbles were generated and we have proven they are not contaminations.We also found nanobubbles in the ultrasonic water change in both size and concentration with ultrasonic time.
基金supported by the National Science Foundation of Shanghai(No.22ZR1474600)the National Natural Science Foundation of China(No.12175302)+1 种基金the“Thorium Molten Salt Reactor Nuclear Energy System”Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA 02040000)the“Transformational Technologies for Clean Energy and Demonstration,”Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA 21000000)。
文摘The corrosion behavior of 316H stainless steel(SS)in the impure and purified Na Cl–KCl–Mg Cl_(2) salt was investigated at700°C.Results indicate that the main deleterious impurity induced corrosion in the impure salt was the absorbed moisture,present in the form of Mg Cl_(2)·6H_(2)O.316H SS occurred severe intergranular corrosion with a corrosion depth of 130μm for1000 h in the impure Na Cl–KCl–Mg Cl_(2) salt.In contrast,the purification treatment of molten chloride salt by the dissolved Mg metal can remove the absorbed moisture,and the corresponding reactions were also discussed.As a result,the corrosiveness of Na Cl–KCl–Mg Cl_(2) salt is reduced significantly.316H SS occurred slight uniform corrosion with a depth of less than 5μm for 3000 h in the purified Na Cl–KCl–Mg Cl_(2) salt.
基金Supported by the Ministry of Science and Technology of China(Nos.2012CB825805 and 2012CB932600)National Natural Science Foundation of China(Nos.11179004,21390414,U1232113,U1232114,U1332119 and U1432116)Youth Innovation Promotion Association of CAS
文摘The contents and distributions of metal elements in the brain are closely related to neurodegenerative diseases.In this study, we examined Fe, Cu and Zn contents in the brain section associated with Parkinson‘s disease(PD)using synchrotron radiation X-ray fluorescence(SRXRF). PD mouse model induced by 1-methyl-4-phenyl-1,2,3,6-terahydropyridine(MPTP) was used for the elemental analysis(e.g., Fe, Cu and Zn) in the substantia nigra pars compacta(SNpc) region of mice brain tissue samples. We found that mice in the MPTP group had higher contents of Fe, Cu and Zn in the SNpc than the control group. After treating the PD mice with rapamycin, the contents of Fe, Cu and Zn were reduced, the dopamine neurons and motor function were rescued correspondingly. The results prompted that the SRXRF provided an ideal method for tracing and analyzing the metal elements in the brain section to assess the pathological changes of PD model and the therapeutic effect of drugs.
基金supported by the “Transformational Technologies for clean Energy and Demonstration”,Strategic Priority Research Program of the Chinese Academy of Sciences(XDA2100000)the Youth Innovation Promotion Association,Chinese Academy of Sciences(2014237)+1 种基金the National Natural Science Foundation of China(21876183)the Scientific Instrument Developing Project of the Chinese Academy of Sciences(YJKYYQ20180066)~~
文摘Effective electrocatalysis is crucial for enhancing the efficiency of water splitting to obtain clean fuels.Herein,we report a system of interesting and high-performance Sr-doped perovskite electrocatalysts with porous structures,obtained via a facile molten salt method and applied in the oxygen evolution reaction(OER).With increasing the Sr content,the valence states of Co and Fe ions do not clearly increase,according to the Co-L2,3 and Fe-L2,3 as well as the Co-K and the Fe-K X-ray absorption spectroscopy,whereas doped holes are clearly observed in the 0-K edge.High-resolution transmission electron microscopy indicates the appearance of an amorphous layer after the electrochemical reaction.We conclude that the formation of the amorphous layer at the surface,induced by Sr doping,is crucial for achieving high OER activity,and we offer insights into the self-reconstruction of the OER catalyst.
基金financially supported by the National Key R&D Program of China(2021YFA1502400)the"Transformational Technologies for Clean Energy and Demonstration"+3 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA2100000)the National Natural Science Foundation of China(52172005,21905295,22179141)the DNL Cooperation Fund,CAS(DNL202008)the Photon Science Center for Carbon Neutrality and the Major Scientific and Technological Innovation Project of Shandong Province(2020CXGC010402)。
文摘Perovskite-type mixed protonic-electronic conducting membranes have attracted attention because of their ability to separate and purify hydrogen from a mixture of gases generated by industrial-scale steam reforming based on an ion diffusion mechanism.Exploring cost-effective membrane materials that can achieve both high H_(2) permeability and strong CO_(2)-tolerant chemical stability has been a major challenge for industrial applications.Herein,we constructed a triple phase(ceramic-metal-ceramic)membrane composed of a perovskite ceramic phase BaZr_(0.1)Ce_(0.7)Y_(0.1)Yb_(0.1)O_(3-δ)(BZCYYb),Ni metal phase and a fluorite ceramic phase CeO_(2).Under H_(2) atmosphere,Ni metal in-situ exsolved from the oxide grains,and decorated the grain surface and boundary,thus the electronic conductivity and hydrogen separation performance can be promoted.The BZCYYbNi-CeO_(2)hybrid membrane achieved an exceptional hydrogen separation performance of 0.53 mL min^(-1)cm^(-2) at 800℃ under a 10 vol% H_(2) atmosphere,surpassing all other perovskite membranes reported to date.Furthermore,the CeO_(2) phase incorporated into the BZCYYb-Ni effectively improved the CO_(2)-tolerant chemical stability.The BZCYYbNi-CeO_(2) membrane exhibited outstanding long-term stability for at least 80 h at 700℃ under 10 vol%CO_(2)-10 vol%H_(2).The success of hybrid membrane construction creates a new direction for simultaneously improving their hydrogen separation performance and CO_(2) resistance stability.
基金supported by the ‘‘The Strategic Priority Research Program’’ of the Chinese Academy of Sciences(No.XDA02040601)the Key Project of Science and Technology of Shanghai(No.15DZ1200100)
文摘Sr-substituted ABO_3 perovskite oxides such as La_(0.6) Sr_(0.4 )Mn_(O3-δ)(LSM) and La_(0.6) Sr_(0.4) FeO_(3-δ)(LSF) are widely used as oxygen electrode materials in solid oxide cells. The substituted Sr is not adequately stable under the operating conditions, because of the surface segregation of Sr. Herein, we focused on investigating the relationship between the local geometric structure due to Sr substitution and stability of LSM and LSF. We characterized the local geometric structure of Sr atoms via X-ray absorption spectroscopy. A greater Debye-Waller factor and a longer bond length of both the second and third Sr-O shells were observed in LSF, which demonstrates that LSF has a higher local structural disorder and that Sr in LSF requires less energy to segregate. After 20 h of heat treatment in the presence of a Fe-Cr alloy interconnect, the Sr/La molar ratio on LSF was observed to be much larger than that on LSM. This result unequivocally suggests that Sr in LSF is not as stable as in LSM, and the reaction between Sr and Cr accelerates the Sr surface segregation in LSF.
基金supported by the National Natural Science Foundation of China(Nos.U1532260,11674345,and 11504032)Key Research Program of Chinese Academy of Sciences(Nos.KJZD-EW-M03 and QYZDJ-SSW-SLH019)+3 种基金Youth Innovation Promotion Association CAS(Grant Number 2014233)Shanghai Supercomputer Center of ChinaComputer Network Information Center of Chinese Academy of SciencesSpecial Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund
文摘Water molecules could form a liquid droplet on the water monolayer on a specific solid surface, which has been referred to as ‘‘ordered water monolayer that does not completely wet water'' at room temperature. In contrast to the water molecules, the family of alcohol molecules has the same OH polar head and various lengths of their hydrophobic nonpolar tail; the length of the hydrophobic tail can affect the hydrophobic effect. In this study, using molecular dynamics simulations, we investigated the wetting behaviors of methanol, ethanol, and propanol molecules adsorbed on a SiO_2 surface. The results showed that the methanol, ethanol, and propanol molecules could form an ordered monolayer on the SiO_2 surface and a droplet on top of this monolayer, with different contact angles. The differences in the contact angles were attributed to the differences in the interactions between the alcohol monolayer and droplet.
基金supported by the Supercomputing Center of Chinese Academy of Sciences in Beijing,Chinathe Shanghai Supercomputer Center,China+3 种基金the National Natural Science Foundation of China(Grant Nos.21273268,11290164,and 11175230)the Startup Funding from Shanghai Institute of Applied Physics,Chinese Academy of Sciences(Grant No.Y290011011)"Hundred People Project"from Chinese Academy of Sciences"Pu-jiang Rencai Project"from Science and Technology Commission of Shanghai Municipality,China(Grant No.13PJ1410400)
文摘Anesthetics are extremely important in modem surgery to greatly reduce the patient,s pain. The understanding of anesthesia at molecular level is the preliminary step for the application of anesthetics in clinic safely and effectively. Inert gases, with low chemical activity, have been found to cause anesthesia for centuries, but the mechanism is unclear yet. In this review, we first summarize the progress of theories about general anesthesia, especially for inert gas narcosis, and then propose a new hypothesis that the aggregated rather than the dispersed inert gas molecules are the key to trigger the narcosis to explain the steep dose-response relationship of anesthesia.
文摘Understanding the dynamic evolution of active sites of supported metal catalysts during catalysis is fundamentally important for improving its performance,which attracts tremendous research interests in the past decades.There are two main surficial structures for metal catalysts:terrace sites and step sites,which exhibit catalytic activity discrepancy during catalysis.Herein,by using in situ transmission electron microscopy and in situ Fourier transform infrared spectroscopy(FTIR),the transformation between surface terrace and step sites of Pt-TiO_(2) catalysts was studied under CO and O_(2) environments.We found that the{111}step sites tend to form at{111}terrace under O_(2) environment,while these step sites prefer to transform into terrace under CO environment at elevated temperature.Meanwhile,quantitative ratios of terrace/step sites were obtained by in situ FTIR.It was found that this transformation between terrace sites and step sites was reversible during gas treatment cycling of CO and O_(2).The selective adsorption of O_(2) and CO species at different sites,which stabilized the step/terrace sites,was found to serve as the driving force for active sites transition by density functional theory calculations.Inspired by the in situ results,an enhanced catalytic activity of Pt-TiO_(2) catalysts was successfully achieved through tuning surface-active sites by gas treatments.
基金supported by grants from the National Key R&D Program of China,No.2017YFC0909200(to DC)the National Natural Science Foundation of China,No.62075225(to HZ)+1 种基金Zhejiang Provincial Medical Health Science and Technology Project,No.2023XY053(to ZP)Zhejiang Provincial Traditional Chinese Medical Science and Technology Project,No.2023ZL703(to ZP).
文摘Terahertz biotechnology has been increasingly applied in various biomedical fields and has especially shown great potential for application in brain sciences.In this article,we review the development of terahertz biotechnology and its applications in the field of neuropsychiatry.Available evidence indicates promising prospects for the use of terahertz spectroscopy and terahertz imaging techniques in the diagnosis of amyloid disease,cerebrovascular disease,glioma,psychiatric disease,traumatic brain injury,and myelin deficit.In vitro and animal experiments have also demonstrated the potential therapeutic value of terahertz technology in some neuropsychiatric diseases.Although the precise underlying mechanism of the interactions between terahertz electromagnetic waves and the biosystem is not yet fully understood,the research progress in this field shows great potential for biomedical noninvasive diagnostic and therapeutic applications.However,the biosafety of terahertz radiation requires further exploration regarding its two-sided efficacy in practical applications.This review demonstrates that terahertz biotechnology has the potential to be a promising method in the field of neuropsychiatry based on its unique advantages.
基金Supported by National Natural Science Foundation of China(Nos.11174310 and 11290164)the Key Research Program of Chinese Academy of Sciences(No.KJZD-EW-M03)
文摘Aluminium is widely used as an antimicrobial coagulant,food additive,and cookware.However,many reports indicate that aluminium may be a critical factor in many amyloid diseases,such as Alzheimer’s disease and Parkinson’s disease.Unfortunately,the underlying mechanism is still poorly understood,which limits efforts to prevent and treat these diseases.In this paper,using an ab initio method,we studied the interaction of Al-backbone ring structure with theπ-electron-rich sidechains of His,Phe,Trp,and Tyr.We found that in the absence of water,the Al-backbone ring can stably bind with those sidechains.In the presence of water,the Al-backbone ring can bind to the His sidechain and cannot bind to the other sidechains.As revealed by further investigations,this could be attributed to the fact that there was a coordinate bond of the Al-backbone ring with the His sidechain,while there were theπ-πstacking and cation-π-like interactions with the other sidechains.These findings potentially provide a molecular understanding of Al-related toxicity,and may be helpful in designing drugs for those aforementioned aluminum-linked diseases and encourage treatment of Al-polluted water.
基金supported by the National Natural Science Foundation of China(Nos.U1832170 and 11474299)Computer Network Information Center of Chinese Academy of Sciences
文摘Using molecular dynamics simulations, we investigate the influence of Na and Cl ions on the evaporation of nanoscale water on graphene oxide surfaces. As the concentration of NaCl increases from 0 to 1.5 M, the evaporation rate shows a higher decrease on patterned graphene oxide than that on homogeneous graphene oxide.The analysis shows an obvious decrease in the evaporation rate from unoxidized regions, which can be attributed to the increased amount of Na^+ ions near the contact lines.The proximity of Na^+ significantly extends the H-bond lifetime of the outermost water molecules, which reduces the number of water molecules diffusing from the oxidized to unoxidized regions. Moreover, the effect of the ions on water evaporation is less significant when the oxidation degree varies in a certain range. Our findings advance the understanding of the evaporation process in the presence of ions and highlight the potential application of graphene oxide in achieving controllable evaporation of liquids.
基金supported by the National Natural Science Foundation of China (No.11404230)Foundation of Science and Technology Bureau of Sichuan Province (No.2013JY0085)
文摘Electronic structures and optical properties of single-layer In1-xGaxN are studied by employing Heyd-Scuseria-Ernzerh（HSE） method based on the first-principles. The band structure and density of states（DOS） of single-layer In1-xGaxN are calculated, and the band gap ranges from 1.8 eV to 3.8 eV as the ratio x changes, illustrating the potential for the tunability of band gap values via Ga doped. We also have investigated optical properties of single-layer In1-xGaxN such as dielectric function, refractive index and absorption coefficient, the main peak of dielectric function spectrum and the absorption edge are found to have a remarkable blue-shift as the concentration of Ga increases. Furthermore, the optical properties of single-layer In1-xGaxN are analyzed based on the band structures and DOS analysis. Such unique optical properties have profound application in nanoelectronics and optical devices.
基金supported by the National Natural Science Foundation of China(No.31670871)the Open Large Infrastructure Research of Chinese Academy of Sciences+1 种基金the Chinese Academy of Sciences Knowledge Innovation Project(No.QYZDJ-SSW-SLH019)the LU JIAXI International team program supported by the K.C.Wong Education Foundation and CAS
文摘The arrangement of DNA-based nanostructures into the desired large-scale periodic pattern with the highest possible accuracy and control is essential for the DNA application in functional biomaterials;however, formation of a DNA nanostructure pattern without utilizing the molecular interactions in nanotechnology field remains difficult. In this article, we use the optimal concentration and adsorption time of origami to induce DNA origami in the form of a large-scale 2D pattern on mica without changing the origami itself. DNA origami structures can form a pattern by close packing of symmetric and electrostatic interactions between ions, which was confirmed by the atomic force microscopy images. Furthermore, we identified favorable conditions for the concentration of enable pattern formation with DNA origami. This work provides an insight to understand the adsorption of DNA on mica and guides researches on regular DNA nanostructure pattern, which can serve as templates for pattern formation of proteins or other biomolecules.
基金supported by the National Key Research and Development Program(No.2016YFA0400902)the Ministry of Science and Technology of China(Nos.2012CB825805,2012CB932600)+3 种基金the National Natural Science Foundation of China(Nos.11675251 and 11275251)Shanghai Rising-Star Program(No.14QA1404400)Distinguished Scientist Fellowship Program of King Saud Universitythe Youth Innovation Promotion Association of CAS(No.2016236)
文摘As a robust platform for genome editing,CRISPR/Cas9 is currently being explored for engineering biology or therapeutics,yet means for quantitative detection of Cas9 proteins remain to be fully realized.Here,we expressed Cas9 proteins and developed a novel detection method that traced Cas9 based on radiolabeled iodine.Through optimizing the reaction conditions of reaction time,temperature and cycles,we obtained ^(125)I-Cas9 of high labeling yield.The prepared ^(125)I-Cas9 was stable in various media and preserved excellent genome editing efficiency.Thus,our strategy provides a convenient and efficient tool for further tracing biological behaviors of Cas9 proteins in living systems.
基金This work was supported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)and the Ministry of Trade,Industry&Energy(MOTIE)of the Republic of Korea(No.20173020032120)This work also was supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(NRF-2019R1C1C1005801)Partial support from“CO2 utilization battery for hydrogen production based on fault-tolerance deep learning”(1.200097.01)is also acknowledged.
文摘Ni nanocatalysts produced through exsolution have shown strong resistance to particle sintering and carbon coking in a beneficial dry reforming of methane(DRM)reaction utilizing greenhouse gases such as CH_(4)and CO_(2).However,most of the existing oxide supports for exsolution have been limited to perovskite oxide,while studies on fluorite support have been rarely conducted due to the limited solubility despite its excellent redox stability.Here we demonstrate that 3 mol%Ni can be successfully dissolved into the yttria-stabilized zirconia(YSZ)lattice and be further exsolved to the surface in a reducing atmosphere.The YSZ decorated with exsolved Ni nanoparticles shows enhanced catalytic activity for DRM reaction compared to the conventional cermet type of bulk Ni-YSZ.Moreover,the catalytic activity is extremely stable for about 300 h without significant degradation.Overall results suggest that the YSZ-based fluorite structure can be utilized as one of the support oxides for exsolution.
基金supported by the National Natural Science Foundation of China(No.11375256)the Science and Technology Commission of Shanghai Municipality(No.14JC1493300)
文摘X-ray scattering is widely used in material structural characterizations.The weak scattering nature,however,makes it susceptible to background noise and can consequently render the final results unreliable.In this paper,we report an iterative method to determine X-ray scattering background and demonstrate its feasibility by small angle X-ray scattering on gold nanoparticles.This method solely relies on the correct structural modeling of the sample to separate scattering signal from background in data fitting processes,which allows them to be immune from experimental uncertainties.The importance of accurate determination of the scaling factor for background subtraction is also illustrated.
基金supported by the International S&T Cooperation Program of China(Grant No.2014DFG60230)the National Natural Science Foundation of China(Grant Nos.91326105,21306220,and 21501189)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA02040104)
文摘The first principles density-functional theoretical calculations of U adatom adsorption and diffusion on a planar graphene and quasi-one-dimensional graphene nanoribbons（GNRs） are performed. An energetic preference is found for U adatom diffusing to the hollow sites of both graphene and GNRs surface. A number of U distinctive diffusion paths either perpendicular or parallel to the ribbon growth direction are examined. The edge effects are evidenced by the calculated energy barriers of U adatom diffusion on armchair and zigzag nanoribbons surfaces. The calculation results indicate that the diffusion of U adatom from the inner site toward the edge site is a feasible process, particularly in zigzagGNR. It is viable to control the initial morphology of nuclear carbon material to retard the diffusion and concentration of nuclides.
