Soft X-ray detectors play a vital role in materials science,high-energy physics and medical imaging.Cs_(2)AgBiBr_(6),a lead-free double perovskite,has gained attention for its excellent optoelectronic properties,stabi...Soft X-ray detectors play a vital role in materials science,high-energy physics and medical imaging.Cs_(2)AgBiBr_(6),a lead-free double perovskite,has gained attention for its excellent optoelectronic properties,stability,and nontoxicity.However,its fast crystallization and requirement for high-temperature annealing(>250℃)often lead to inferior film quality,limiting its application in flexible devices.This study introduces an alloying strategy that significantly improves the quality of Cs_(2)AgBiBr_(6)thin films annealed at a reduced temperature of 150℃.Devices based on the alloyed thin films exhibit an ultra-low dark current of 0.32 nA·cm^(-2)and a quantum efficiency of 725%.Furthermore,the first successful integration of Cs_(2)AgBiBr_(6)with a thinfilm transistor backplane demonstrates its superior imaging performance,indicating that Cs_(2)AgBiBr_(6)is a promising material for next-generation soft X-ray sensors.展开更多
Objective The present study aimed to estimate the association between susceptibility to migraine and the 12nucleotide insertion/deletion （indel） polymorphism in promoter region ofα 2B -adrenergic receptor gene （AD...Objective The present study aimed to estimate the association between susceptibility to migraine and the 12nucleotide insertion/deletion （indel） polymorphism in promoter region ofα 2B -adrenergic receptor gene （ADRA2B）.Methods A case-control study was carried out in Chinese Han population,including 368 cases of migraine and 517 controls.Genomic DNA was extracted from blood samples,and DNA fragments containing the site of polymorphism were amplified by PCR.Data were adjusted for sex,age,migraine history and family history,and analyzed using a logistic regression model.Results There was no association between indel polymorphism and migraine,at either the allele or the genotype level.Conclusion These findings do not support a functional significance of ADRA2B indel polymorphism at position-4825 relative to the start codon in the far upstream region of the promoter in the present migraine subjects.展开更多
Electrochemical insertion/extraction of Li on cathode materials of spinel type LiMn2O4 and ordered rock-salt type LiCo0.5 Ni0.5O2 was measured on samples of which structures were well characterized. On the basis of ex...Electrochemical insertion/extraction of Li on cathode materials of spinel type LiMn2O4 and ordered rock-salt type LiCo0.5 Ni0.5O2 was measured on samples of which structures were well characterized. On the basis of experimental results on structure, morphology and charge-discharge characteristics, the effect of crystallinity of the cathode materiaIs on electrochemical Li insertion/extraction performance was discussed. These two transition metal oxides belong to onegroup that the crystallinity of these oxides affects to the performance.展开更多
Electrochemical insertion/extraction of Li on cathode materials of anatase type TiO_2, quasilayered structure V_2O_5 and layered structure MoO_3 was measured on samples of which structures were well characterized and...Electrochemical insertion/extraction of Li on cathode materials of anatase type TiO_2, quasilayered structure V_2O_5 and layered structure MoO_3 was measured on samples of which structures were well characterized and showed a wide range of crystallinity. On the basis of experimental results on structure, morphology and charge-discharge characteristics, the effect of crystallinity of the cathode materials on electrochemical Li insertion/extraction pedermance was discussed. These three transition metal oxides were classified as one group on the basis of whether the crystallinity of these oxides affects to the performance or not; LiMn_2O_4 and LiCo_(0.5)O_2 belongs to the former group and TiO_2, V_2O_5 and MoO_3 to the latter.展开更多
Sixteen two-photon absorption (TPA) transition line strengths were calculated for the Pr 3+ ion in the cubic host Cs_2NaPrCl_6. In the calculation, two kinds of intermediate virtual excited (4f5d) states were utilized...Sixteen two-photon absorption (TPA) transition line strengths were calculated for the Pr 3+ ion in the cubic host Cs_2NaPrCl_6. In the calculation, two kinds of intermediate virtual excited (4f5d) states were utilized, one was the direct product of 4f1 core and 5d1 electronic states, and the other was 4f5d coupled states obtained by using the Reid f2 and fd programs. It was found that the calculated trends in intensities are fairly similar and the interaction between the 5d electron and the (4f)1 core in the 4f5d configuration does not provide dominant contributions to the two-photon absorption transition intensity of the Pr 3+ ion. In addition, the main channels of the strongest two-photon transition 3H_4Γ_1→3P_2Γ_5 were also obtained.展开更多
Theoretical investigations on the insertion reaction mechanisms of three- membered-ring silylenoid H2 Si Li F with GeH 3R（R = F, OH, NH2） have been systematically carried out by combined density functional theory（...Theoretical investigations on the insertion reaction mechanisms of three- membered-ring silylenoid H2 Si Li F with GeH 3R（R = F, OH, NH2） have been systematically carried out by combined density functional theory（DFT） and ab initio quantum chemical calculations. The geometries of all stationary points for these reactions were optimized using the B3 LYP method and then the QCISD method was used to calculate the single-point energies. The calculated results indicate that, there are one precursor complex（Q）, one transition state（TS）, and one intermediate（IM） which connect the reactants and the products along the potential energy surface. The insertion reactions of three-membered-ring silylenoid with Ge H3 R proceed in a concerted manner, forming H2RSi-Ge H3 and Li F. The calculated potential energy barriers of the three reactions are 29.17, 30.90, and 54.07 k J/mol, and the reaction energies for the three reactions are –127.05, –116.91, and –103.31 k J/mol, respectively. The insertion reactions in solvents are similar to those in vacuum. Under the same situation, the insertion reactions should occur easily in the following order： GeH 3-F GeH 3-OH GeH 3-NH2. The elucidations of the mechanism of these insertion reactions provided a new mode of silicon-germanium bond formation.展开更多
Developing efficient photocatalysts for CO_(2)conversion under full-spectrum irradiation remains a key challenge for solar-to-chemical energy conversion.In this study,a novel S-scheme heterojunction composed of reduct...Developing efficient photocatalysts for CO_(2)conversion under full-spectrum irradiation remains a key challenge for solar-to-chemical energy conversion.In this study,a novel S-scheme heterojunction composed of reduction Cs_(0.32)WO_(3)(CWO)nanosheets with hexagonal structure and oxidation WO_(3)·2H_(2)O(WO)nanorods with monoclinic structure photocatalyst was successfully constructed via an ultrasound strategy.Under full-spectrum irradiation for 4 h,the optimized 2D/1D of heterostructure CWO/WO-0.8 exhibited superior photocatalytic performance,achieving CO and CH_(3)OH yields of 29.74 and 63.71μmol·g^(-1),respectively.The enhanced activity is primarily ascribed to the formation of an S-scheme charge transfer pathway,which facilitates efficient separation and directional migration of photogenerated charge carriers through the internal electric field at the CWO/WO interface.This process facilitates the electron enrichment on the CWO surface and significantly enhances its CO_(2)reduction ability.Besides,the results of various characterizations show that CWO/WO-0.8 possesses enhanced optical response capability.The results of density functional theory calculations and CO_(2)-temperature programmed desorption analysis confirmed that the CWO/WO heterojunction exhibits stronger CO_(2)adsorption and activation abilities compared to the pristine CWO and WO.The reaction pathway for CH_(3)OH production was elucidated by in-situ diffused reflectance Fourier transformed infrared tests.This work provides new insights into the rational design of S-scheme photocatalysts for efficient and selective CO_(2)conversion.展开更多
In this study,a batch of φ12 mm Cs_(2)LiYCl_(6):Ce crystals codoped with different contents of Cu^(+)and Sc^(3+)was successfully grown using the Multi-ampule Bridgeman method.A new emission peaking at 418 nm is found...In this study,a batch of φ12 mm Cs_(2)LiYCl_(6):Ce crystals codoped with different contents of Cu^(+)and Sc^(3+)was successfully grown using the Multi-ampule Bridgeman method.A new emission peaking at 418 nm is found in the photoluminescence spectra of CLYC:Ce codoped with Cu^(+)ion.Codoping Cu^(+)or Sc^(3+)both increases the proportion of intrinsic self-trapped exciton(STE)luminescence,and extends the excitation band of Ce^(3+),especially in Cu^(+)codoped samples,where a new absorption peak at 248 nm can be identified.The light yield of Cu^(+)codoped samples remains largely unchanged,but the energy resolution shows a slight deterioration.Both light yield and energy resolution degrade after Sc^(3+)codoping,and the effect is much severe than that of Cu^(+)codoped samples.X-ray induced afterglow can be suppressed after Cu^(+)codoping and low content of Sc^(3+)codoping.The scintillation decay variation also depends on the codoping ions and their contents.展开更多
Neutron well logging,using instruments equipped with neutron source and detectors(e.g.,^(3)He-tubes,Nal,BGO),plays a key role in lithological differentiation,porosity determination,and fluid property evaluation in the...Neutron well logging,using instruments equipped with neutron source and detectors(e.g.,^(3)He-tubes,Nal,BGO),plays a key role in lithological differentiation,porosity determination,and fluid property evaluation in the petroleum industry.The growing trend of multifu nctional neutron well logging,which enables simultaneous extraction of multiple reservoir characteristics,requiring high-performance detectors capable of withstanding high-temperature downhole conditions,limited space,and instrument vibrations,while also detecting multiple particle types.The Cs_(2)LiYCl_(6):Ce^(3+)(CLYC)elpasolite scintillator demonstrates excellent temperature resistance and detection efficiency,making it become a promising candidate for leading the development of the novel neutron-based double-particle logging technology.This study employed Monte Carlo simulations to generate equivalent gamma spectra and proposed a pulse shape discrimination simulation method based on theoretical analysis and probabilistic iteration.The performance of CLYC was compared to that of common detectors in terms of physical properties and detection efficiency.A double-particle pulsed neutron detection system for porosity determination was established,based on the count ratio of equivalent gamma rays from the range of 2.95-3.42 MeVee energy bins.Results showed that CLYC can effectively replace ^(3)He-tubes for porosity measurement,providing consistent responses.This study offers numerical simulation support for the design of future neutron well logging tools and the application of double-particle detectors in logging systems.展开更多
In this manuscript,Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites was fabricated via an ultrasonic-assisted process.The activity of the as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites for photocatalytic CO_(2) ...In this manuscript,Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites was fabricated via an ultrasonic-assisted process.The activity of the as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites for photocatalytic CO_(2) reduction was studied under visible light.The as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites show a superior activity for photocatalytic CO_(2) reduction to produce CH4 and CO,with an optimum activity achieved over 0.5 Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6).The obvious superior activity observed over Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites as compared with bare Cs_(2)AgBiBr_(6) and bare Bi_(2)WO_(6) as well as a mechanical mixture of Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6) can be owe to the fabrication of an efficient S-scheme heterojunction,which accelerates the separation of the photogenerated charge carriers in Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6) without sacrificing the high redox capability of Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6).This work demonstrates that the coupling of two photocatalytic materials with staggered band alignment to form an S-scheme heterojunction is an effective strategy to develop efficient photocatalytic systems and also highlights the promising role of using lead free perovskites in photocatalysis.展开更多
Lead halide perovskite (LHP) nanocrystals have been intensely studied as photocatalysts for artificial photosynthesis in recent years.However,the toxicity of lead in LHP seriously limits their potential for widespread...Lead halide perovskite (LHP) nanocrystals have been intensely studied as photocatalysts for artificial photosynthesis in recent years.However,the toxicity of lead in LHP seriously limits their potential for widespread applications.Herein,we first present the synthesis of 2D lead-free halide perovskite (Cs_(3)Bi_(2)I_(9)) nanosheets with self-template-oriented method,in which BiOI/Bi_(2)O_(2) nanosheets were used as the template and Bi ion source simultaneously.Through facile electrostatic self-assembly strategy,a Z-scheme heterojunction composed of Cs_(3)Bi_(2)I_(9)nanosheets and CeO_(2) nanosheets (Cs_(3)Bi_(2)I_(9)/CeO_(2)-3:1) was constructed as photocatalyst for the photo-reduction of CO_(2) coupled with the oxidation of H_(2)O.Due to the matching energy levels and the close interfacial contact between Cs_(3)Bi_(2)I_(9)and CeO_(2) nanosheets,the separation efficiency of the photogenerated carriers in Cs_(3)Bi_(2)I_(9)/CeO_(2)-3:1 composite was significantly improved.Consequently,the environment-friendly halide perovskite heterojunction Cs_(3)Bi_(2)I_(9)/CeO_(2)-3:1presents impressive photocatalytic activity for the reduction of CO_(2)to CH_(4)and CO with an electron consumption yield of 877.04μmol g^(-1),which is over 7 and 15 times higher than those of pristine Cs_(3)Bi_(2)I_(9)and CeO_(2)nanosheets,exceeding the yield of other reported bismuth-based perovskite for photocatalytic CO_(2)reduction.展开更多
Background: Intensive care units (ICUs) have an increased risk of Central line associated bloodstream infection (CLABSI) due to the prevalence of invasive procedures, devices, immunosuppression, comorbidity, frailty, ...Background: Intensive care units (ICUs) have an increased risk of Central line associated bloodstream infection (CLABSI) due to the prevalence of invasive procedures, devices, immunosuppression, comorbidity, frailty, and elderly patients. We have seen a successful reduction in Central line associated bloodstream infection related the past decade. In spite of this, Intensive care unit-Catheter related bloodstream infections remain high. The emergence of new pathogens further complicates treatment and threatens patient outcomes in this context. In addition, the SARS-CoV-2 (COVID-19) pandemic served as a reminder that an emerging pathogen poses a challenge for adjusting prevention measures regarding both the risk of exposure to caregivers and maintaining a high level of care. ICU nurses play an important role in the prevention and management of CLABSI as they are involved in basic hygienic care, quality improvement initiatives, microbiological sampling, and aspects of antimicrobial stewardship. Microbiological techniques that are more sensitive and our increased knowledge of the interactions between critically ill patients and their microbiota are forcing us to rethink how we define CLABSIs and how we can diagnose, treat, and prevent them in the ICU. The objective of this multidisciplinary expert review, focused on the ICU setting, is to summarize the recently observed occurrence of CLABSI in ICU, to consider the role of modern microbiological techniques in their diagnosis, to examine clinical and epidemiological definitions, and to redefine several controversial preventive measures including antimicrobial-impregnated catheters, chlorhexidine-gluconate impregnated sponge, and catheter dressings.展开更多
Multicomponent polymerizations(MCPs)are powerful tools to synthesize functional polymers with great structural diversity,low cost and high efficiency,which usually generate single polymer product.Herein,a robust one-p...Multicomponent polymerizations(MCPs)are powerful tools to synthesize functional polymers with great structural diversity,low cost and high efficiency,which usually generate single polymer product.Herein,a robust one-pot diamines,CS_(2)and monoisocyanide-participated catalyst-free polymerization was developed at room temperature to produce polythiourea and thioformamide simultaneously in equal equivalent,which was featured with cheap monomers,simple operation and mild condition,affording various polythioureas with high Mws of up to 4.75×10^(4)g/mol in high yields of up to 98%.Polythioureas with varied chain composition and sequence-controlled structure could be synthesized in 62 g-scale from copolymerization or multicomponent tandem polymerization,enabling facile tuning of thermal property,crystallinity,mechanical property,and fluorescence.The abundant irregular hydrogen bonds endowed the polythioureas excellent glassy state self-healing property at room temperature or below 0℃.This polymerization provided an efficient and economic approach to access functional polythioureas.展开更多
Multifunctional lead-free double perovskites demonstrate remarkable potential towards applications in various fields.Herein,an environmentally-friendly,low-cost,high-throughput Cs_(2)NaFeCl_(6) single crystal with exc...Multifunctional lead-free double perovskites demonstrate remarkable potential towards applications in various fields.Herein,an environmentally-friendly,low-cost,high-throughput Cs_(2)NaFeCl_(6) single crystal with exceedingly high thermal stability is designed and grown.It obtains a cubic lattice system in the temperature range of 80-500 K,accompanied by a completely reversible chromatic variation ranging from yellow to black.Importantly,the intriguing thermochromism is proved to own extremely high reproducibility(over 1000 cycles)without a hysteretic effect,originating from its structural flexibility that including(i)the noteworthy distortion/deformation of[NaCl_(6)]5−and[FeCl_(6)]3−octahedra;(ii)order-disorder arrangement transition of[NaCl_(6)]5−and[FeCl6]3−octahedra as the function of temperature.This study paves the way towards a new class of smart windows and camouflage coatings with an unprecedented colour range based on a Cs_(2)NaFeCl_(6) perovskite.展开更多
Rechargeable aqueous zinc ion batteries(AZIBs)were considered as one of the most promising candidates for large-scale energy storage due to the merits of high safety and inexpensiveness.As AZIBs cathode material,Mn O_...Rechargeable aqueous zinc ion batteries(AZIBs)were considered as one of the most promising candidates for large-scale energy storage due to the merits of high safety and inexpensiveness.As AZIBs cathode material,Mn O_(2)possesses great merits but was greatly hindered due to the sluggish diffusion kinetic of Zn^(2+) during electrochemical operations.Herein,deep Zn^(2+) ions intercalatedδ-Mn O_(2)(Zn-Mn O_(2))was achieved by the in situ electrochemical deposition route,which significantly enhanced the diffusion ability of Zn^(2+) due to the synergistic effects of Zn^(2+) pillars and structural H;O.The resultant Zn-Mn O_(2)based AZIBs delivers a record capacity of 696 m Ah/g(0.5 m Ah/cm^(2))based on the initial mass loading,which is approaching the theoretical capacity of Mn O_(2)with a two-electrons reaction.In-situ Raman studies reveal highly reversible Zn^(2+)ions insertion/extraction behaviors and here the Zn-Mn O_(2)plays the role of a container during the charge–discharge process.Further charge storage mechanism investigations point out the insertion/extraction of Zn^(2+) and H^(+) coincides,and such process is significantly facilitated results from superior interlayered configurations of Zn-Mn O_(2)The excellent electrochemical performance of Zn-Mn O_(2)achieved in this work suggests the deep ions pre-intercalation strategy may aid in the future development of advanced cathodes for AZIBs.展开更多
An inverse spinel-type metal oxide, magnesium-manganese-titanium oxide （Mg2Mn0.5Ti0.5O4）, were prepared using the coprecipitation/thermal crystallization method. The extraction/insertion reaction with this material ...An inverse spinel-type metal oxide, magnesium-manganese-titanium oxide （Mg2Mn0.5Ti0.5O4）, were prepared using the coprecipitation/thermal crystallization method. The extraction/insertion reaction with this material was investigated by X-ray, saturation capacity of exchange, pH titration, and distribution coefficient （Kd） measurement. The acid treatments of Mg2Mn0.5Ti0.5O4 caused Mg^2＋ extractions of more than 81%, whereas the dissolutions of Mn^4＋ and Ti^4＋ were less than 10%. The experimental results proved that the acid-treated sample has a capacity of exchange 56 mg·g^-1 for Li^＋ in the solution. The chemical analysis showed that the Li^＋ extraction/insertion progressed mainly by ion-exchange mechanism and surface adsorption.展开更多
Converting hydrocarbons into aldehydes in a green and environmentally benign way is of great signif-icance in fine chemistry.In this work,all-inorganic Cs_(3)Bi_(2)B_(9) perovskite nanoparticles were uniformly loaded ...Converting hydrocarbons into aldehydes in a green and environmentally benign way is of great signif-icance in fine chemistry.In this work,all-inorganic Cs_(3)Bi_(2)B_(9) perovskite nanoparticles were uniformly loaded on BiOBr nanosheets via an in-situ growth method,which can selectivity photoactivate aromatic C(sp^(3))-H bond of toluene to generate benzaldehyde.According to the in-situ X-ray photoelectron spec-troscopy characterization,the photogenerated electrons of BiOBr transfer to Cs_(3)Bi_(2)B_(9) enforced by the in-ternal electric field under light irradiation,resulting in S-scheme heterojunction.Furthermore,theoretical calculations indicate that toluene molecules are inclined to adsorb on the BiOBr surface,subsequently in-volving the oxidation reaction to generate benzyl radical(PhCH_(2)·)by using the energetic holes of BiOBr,while the remaining photoinduced electrons in the conduction band(CB)of Cs_(3)Bi_(2)B_(9) with powerful reduction ability reduce O2 into·O_(2)^(-),which is the vital oxidative active species working on toluene selective oxidation process.Such an unexceptionable charge carrier utilization mode and tendentious ad-sorption behavior of reactants contribute to the optimized Cs_(3)Bi_(2)B_(9)/BiOBr heterojunction with excellent photocatalytic performance,achieving a maximum of 22.5%toluene conversion and 96.2%selectivity to-wards benzaldehyde formation.This work provides a rational photocatalyst heterojunction construction protocol for the selective oxidation of saturated aromatic C-H bonds.展开更多
基金supported by the NSFC under Grant No.62474169the National Key Research and Development Program of China under Grant No.2024YFB3212200the funding from USTC under Grant Nos.WK2100000025,KY2190000003,and KY2190000006。
文摘Soft X-ray detectors play a vital role in materials science,high-energy physics and medical imaging.Cs_(2)AgBiBr_(6),a lead-free double perovskite,has gained attention for its excellent optoelectronic properties,stability,and nontoxicity.However,its fast crystallization and requirement for high-temperature annealing(>250℃)often lead to inferior film quality,limiting its application in flexible devices.This study introduces an alloying strategy that significantly improves the quality of Cs_(2)AgBiBr_(6)thin films annealed at a reduced temperature of 150℃.Devices based on the alloyed thin films exhibit an ultra-low dark current of 0.32 nA·cm^(-2)and a quantum efficiency of 725%.Furthermore,the first successful integration of Cs_(2)AgBiBr_(6)with a thinfilm transistor backplane demonstrates its superior imaging performance,indicating that Cs_(2)AgBiBr_(6)is a promising material for next-generation soft X-ray sensors.
基金supported by the National Natural Science Foundation of China(No.30800621)China Postdoctoral Science Foundation(No.20080431121,200902530)
文摘Objective The present study aimed to estimate the association between susceptibility to migraine and the 12nucleotide insertion/deletion （indel） polymorphism in promoter region ofα 2B -adrenergic receptor gene （ADRA2B）.Methods A case-control study was carried out in Chinese Han population,including 368 cases of migraine and 517 controls.Genomic DNA was extracted from blood samples,and DNA fragments containing the site of polymorphism were amplified by PCR.Data were adjusted for sex,age,migraine history and family history,and analyzed using a logistic regression model.Results There was no association between indel polymorphism and migraine,at either the allele or the genotype level.Conclusion These findings do not support a functional significance of ADRA2B indel polymorphism at position-4825 relative to the start codon in the far upstream region of the promoter in the present migraine subjects.
文摘Electrochemical insertion/extraction of Li on cathode materials of spinel type LiMn2O4 and ordered rock-salt type LiCo0.5 Ni0.5O2 was measured on samples of which structures were well characterized. On the basis of experimental results on structure, morphology and charge-discharge characteristics, the effect of crystallinity of the cathode materiaIs on electrochemical Li insertion/extraction performance was discussed. These two transition metal oxides belong to onegroup that the crystallinity of these oxides affects to the performance.
文摘Electrochemical insertion/extraction of Li on cathode materials of anatase type TiO_2, quasilayered structure V_2O_5 and layered structure MoO_3 was measured on samples of which structures were well characterized and showed a wide range of crystallinity. On the basis of experimental results on structure, morphology and charge-discharge characteristics, the effect of crystallinity of the cathode materials on electrochemical Li insertion/extraction pedermance was discussed. These three transition metal oxides were classified as one group on the basis of whether the crystallinity of these oxides affects to the performance or not; LiMn_2O_4 and LiCo_(0.5)O_2 belongs to the former group and TiO_2, V_2O_5 and MoO_3 to the latter.
文摘Sixteen two-photon absorption (TPA) transition line strengths were calculated for the Pr 3+ ion in the cubic host Cs_2NaPrCl_6. In the calculation, two kinds of intermediate virtual excited (4f5d) states were utilized, one was the direct product of 4f1 core and 5d1 electronic states, and the other was 4f5d coupled states obtained by using the Reid f2 and fd programs. It was found that the calculated trends in intensities are fairly similar and the interaction between the 5d electron and the (4f)1 core in the 4f5d configuration does not provide dominant contributions to the two-photon absorption transition intensity of the Pr 3+ ion. In addition, the main channels of the strongest two-photon transition 3H_4Γ_1→3P_2Γ_5 were also obtained.
基金supported by the National Natural Science Foundation Committee of China(No.21103145)the Natural Science Foundation of Shandong Province(No.ZR2009BQ006)+3 种基金the Fund for Doctor of Yantai University(No.HY05B30)the Special Foundation of Youth Academic Backbone of Yantai Universitysupport by the Open fund(sklssm201418)of the State Key Laboratory of Supramolecular Structure and Materials,Jilin Universitythe Graduate Innovation Foundation of Yantai University,GIFYTU
文摘Theoretical investigations on the insertion reaction mechanisms of three- membered-ring silylenoid H2 Si Li F with GeH 3R（R = F, OH, NH2） have been systematically carried out by combined density functional theory（DFT） and ab initio quantum chemical calculations. The geometries of all stationary points for these reactions were optimized using the B3 LYP method and then the QCISD method was used to calculate the single-point energies. The calculated results indicate that, there are one precursor complex（Q）, one transition state（TS）, and one intermediate（IM） which connect the reactants and the products along the potential energy surface. The insertion reactions of three-membered-ring silylenoid with Ge H3 R proceed in a concerted manner, forming H2RSi-Ge H3 and Li F. The calculated potential energy barriers of the three reactions are 29.17, 30.90, and 54.07 k J/mol, and the reaction energies for the three reactions are –127.05, –116.91, and –103.31 k J/mol, respectively. The insertion reactions in solvents are similar to those in vacuum. Under the same situation, the insertion reactions should occur easily in the following order： GeH 3-F GeH 3-OH GeH 3-NH2. The elucidations of the mechanism of these insertion reactions provided a new mode of silicon-germanium bond formation.
文摘Developing efficient photocatalysts for CO_(2)conversion under full-spectrum irradiation remains a key challenge for solar-to-chemical energy conversion.In this study,a novel S-scheme heterojunction composed of reduction Cs_(0.32)WO_(3)(CWO)nanosheets with hexagonal structure and oxidation WO_(3)·2H_(2)O(WO)nanorods with monoclinic structure photocatalyst was successfully constructed via an ultrasound strategy.Under full-spectrum irradiation for 4 h,the optimized 2D/1D of heterostructure CWO/WO-0.8 exhibited superior photocatalytic performance,achieving CO and CH_(3)OH yields of 29.74 and 63.71μmol·g^(-1),respectively.The enhanced activity is primarily ascribed to the formation of an S-scheme charge transfer pathway,which facilitates efficient separation and directional migration of photogenerated charge carriers through the internal electric field at the CWO/WO interface.This process facilitates the electron enrichment on the CWO surface and significantly enhances its CO_(2)reduction ability.Besides,the results of various characterizations show that CWO/WO-0.8 possesses enhanced optical response capability.The results of density functional theory calculations and CO_(2)-temperature programmed desorption analysis confirmed that the CWO/WO heterojunction exhibits stronger CO_(2)adsorption and activation abilities compared to the pristine CWO and WO.The reaction pathway for CH_(3)OH production was elucidated by in-situ diffused reflectance Fourier transformed infrared tests.This work provides new insights into the rational design of S-scheme photocatalysts for efficient and selective CO_(2)conversion.
基金Project supported by the National Key Research and Development Program,China(2022YFB3503600)Manned Space Station Engineering Space Science and Applications Program(MSAP)(ZDBS-ZRKJZTLC011)+3 种基金National Natural Science Foundation of China,China(11975303,12211530561,12305211)Shanghai Municipal Natural Science Foundation,China(21TS1400100)CAS Cooperative Research Project(121631KYSB20210017)CAS Project for Young Scientist in Basic Research(YSBR-024)。
文摘In this study,a batch of φ12 mm Cs_(2)LiYCl_(6):Ce crystals codoped with different contents of Cu^(+)and Sc^(3+)was successfully grown using the Multi-ampule Bridgeman method.A new emission peaking at 418 nm is found in the photoluminescence spectra of CLYC:Ce codoped with Cu^(+)ion.Codoping Cu^(+)or Sc^(3+)both increases the proportion of intrinsic self-trapped exciton(STE)luminescence,and extends the excitation band of Ce^(3+),especially in Cu^(+)codoped samples,where a new absorption peak at 248 nm can be identified.The light yield of Cu^(+)codoped samples remains largely unchanged,but the energy resolution shows a slight deterioration.Both light yield and energy resolution degrade after Sc^(3+)codoping,and the effect is much severe than that of Cu^(+)codoped samples.X-ray induced afterglow can be suppressed after Cu^(+)codoping and low content of Sc^(3+)codoping.The scintillation decay variation also depends on the codoping ions and their contents.
基金the support of the National Natural Science Foundation of China(42174147,42474155)the Scientific and Technological Innovation Projects of Laoshan Laboratory(LSKJ20220347)。
文摘Neutron well logging,using instruments equipped with neutron source and detectors(e.g.,^(3)He-tubes,Nal,BGO),plays a key role in lithological differentiation,porosity determination,and fluid property evaluation in the petroleum industry.The growing trend of multifu nctional neutron well logging,which enables simultaneous extraction of multiple reservoir characteristics,requiring high-performance detectors capable of withstanding high-temperature downhole conditions,limited space,and instrument vibrations,while also detecting multiple particle types.The Cs_(2)LiYCl_(6):Ce^(3+)(CLYC)elpasolite scintillator demonstrates excellent temperature resistance and detection efficiency,making it become a promising candidate for leading the development of the novel neutron-based double-particle logging technology.This study employed Monte Carlo simulations to generate equivalent gamma spectra and proposed a pulse shape discrimination simulation method based on theoretical analysis and probabilistic iteration.The performance of CLYC was compared to that of common detectors in terms of physical properties and detection efficiency.A double-particle pulsed neutron detection system for porosity determination was established,based on the count ratio of equivalent gamma rays from the range of 2.95-3.42 MeVee energy bins.Results showed that CLYC can effectively replace ^(3)He-tubes for porosity measurement,providing consistent responses.This study offers numerical simulation support for the design of future neutron well logging tools and the application of double-particle detectors in logging systems.
文摘In this manuscript,Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites was fabricated via an ultrasonic-assisted process.The activity of the as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites for photocatalytic CO_(2) reduction was studied under visible light.The as-obtained Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites show a superior activity for photocatalytic CO_(2) reduction to produce CH4 and CO,with an optimum activity achieved over 0.5 Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6).The obvious superior activity observed over Cs_(2)AgBiBr_(6)/Bi_(2)WO_(6) nanocomposites as compared with bare Cs_(2)AgBiBr_(6) and bare Bi_(2)WO_(6) as well as a mechanical mixture of Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6) can be owe to the fabrication of an efficient S-scheme heterojunction,which accelerates the separation of the photogenerated charge carriers in Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6) without sacrificing the high redox capability of Cs_(2)AgBiBr_(6) and Bi_(2)WO_(6).This work demonstrates that the coupling of two photocatalytic materials with staggered band alignment to form an S-scheme heterojunction is an effective strategy to develop efficient photocatalytic systems and also highlights the promising role of using lead free perovskites in photocatalysis.
基金financially supported by the Natural Science Foundation of Tianjin City (17JCJQJC43800, 19JCQNJC05500)the National Key R&D Program of China (2017YFA0700104)+1 种基金NSFC (21931007)the 111 Project of China (D17003)。
文摘Lead halide perovskite (LHP) nanocrystals have been intensely studied as photocatalysts for artificial photosynthesis in recent years.However,the toxicity of lead in LHP seriously limits their potential for widespread applications.Herein,we first present the synthesis of 2D lead-free halide perovskite (Cs_(3)Bi_(2)I_(9)) nanosheets with self-template-oriented method,in which BiOI/Bi_(2)O_(2) nanosheets were used as the template and Bi ion source simultaneously.Through facile electrostatic self-assembly strategy,a Z-scheme heterojunction composed of Cs_(3)Bi_(2)I_(9)nanosheets and CeO_(2) nanosheets (Cs_(3)Bi_(2)I_(9)/CeO_(2)-3:1) was constructed as photocatalyst for the photo-reduction of CO_(2) coupled with the oxidation of H_(2)O.Due to the matching energy levels and the close interfacial contact between Cs_(3)Bi_(2)I_(9)and CeO_(2) nanosheets,the separation efficiency of the photogenerated carriers in Cs_(3)Bi_(2)I_(9)/CeO_(2)-3:1 composite was significantly improved.Consequently,the environment-friendly halide perovskite heterojunction Cs_(3)Bi_(2)I_(9)/CeO_(2)-3:1presents impressive photocatalytic activity for the reduction of CO_(2)to CH_(4)and CO with an electron consumption yield of 877.04μmol g^(-1),which is over 7 and 15 times higher than those of pristine Cs_(3)Bi_(2)I_(9)and CeO_(2)nanosheets,exceeding the yield of other reported bismuth-based perovskite for photocatalytic CO_(2)reduction.
文摘Background: Intensive care units (ICUs) have an increased risk of Central line associated bloodstream infection (CLABSI) due to the prevalence of invasive procedures, devices, immunosuppression, comorbidity, frailty, and elderly patients. We have seen a successful reduction in Central line associated bloodstream infection related the past decade. In spite of this, Intensive care unit-Catheter related bloodstream infections remain high. The emergence of new pathogens further complicates treatment and threatens patient outcomes in this context. In addition, the SARS-CoV-2 (COVID-19) pandemic served as a reminder that an emerging pathogen poses a challenge for adjusting prevention measures regarding both the risk of exposure to caregivers and maintaining a high level of care. ICU nurses play an important role in the prevention and management of CLABSI as they are involved in basic hygienic care, quality improvement initiatives, microbiological sampling, and aspects of antimicrobial stewardship. Microbiological techniques that are more sensitive and our increased knowledge of the interactions between critically ill patients and their microbiota are forcing us to rethink how we define CLABSIs and how we can diagnose, treat, and prevent them in the ICU. The objective of this multidisciplinary expert review, focused on the ICU setting, is to summarize the recently observed occurrence of CLABSI in ICU, to consider the role of modern microbiological techniques in their diagnosis, to examine clinical and epidemiological definitions, and to redefine several controversial preventive measures including antimicrobial-impregnated catheters, chlorhexidine-gluconate impregnated sponge, and catheter dressings.
基金supported by the National Natural Science Foundation of China(Nos.52173005,21788102 and 21822102)the Ministry of Science and Technology of China(No.2021YFA1501600)+1 种基金the Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates(No.2019B030301003)the Fundamental Research Funds for the Central Universities.
文摘Multicomponent polymerizations(MCPs)are powerful tools to synthesize functional polymers with great structural diversity,low cost and high efficiency,which usually generate single polymer product.Herein,a robust one-pot diamines,CS_(2)and monoisocyanide-participated catalyst-free polymerization was developed at room temperature to produce polythiourea and thioformamide simultaneously in equal equivalent,which was featured with cheap monomers,simple operation and mild condition,affording various polythioureas with high Mws of up to 4.75×10^(4)g/mol in high yields of up to 98%.Polythioureas with varied chain composition and sequence-controlled structure could be synthesized in 62 g-scale from copolymerization or multicomponent tandem polymerization,enabling facile tuning of thermal property,crystallinity,mechanical property,and fluorescence.The abundant irregular hydrogen bonds endowed the polythioureas excellent glassy state self-healing property at room temperature or below 0℃.This polymerization provided an efficient and economic approach to access functional polythioureas.
基金The research was funded by the National Natural Science Foundation of China(No.51802120,51872126,22075103,51672111)Guangdong Basic and Applied Basic Research Foundation for Distinguished Young Scholar(No.2019B151502030)+7 种基金Natural Science Foundation of Guangdong Province(No.2018030310181)the Science and Technology Plan Project of Guangzhou(No.202002030159)Guangdong Basic and Applied Basic Research Foundation for Young Scholar(No.2020A1515111057)‘100 Talents Program of Hebei Province’(No.E2014100008)the Fundamental Research Funds for the Central Universities(No.21619406)X.Y.thanks for the Special Funds for the Cultivation of Guangdong College Students'Scientific and Technological Innovation("Climbing Program"Special Funds)(No.pdjh2019a0055)J.Fan also thanks for the project support for"Young Top talents"in the Pearl River Talent Project of Guangdong Province(2017GC010424)the Guangdong Provincial Innovation and Entrepreneurship Project(grant 2016ZT06D081).
文摘Multifunctional lead-free double perovskites demonstrate remarkable potential towards applications in various fields.Herein,an environmentally-friendly,low-cost,high-throughput Cs_(2)NaFeCl_(6) single crystal with exceedingly high thermal stability is designed and grown.It obtains a cubic lattice system in the temperature range of 80-500 K,accompanied by a completely reversible chromatic variation ranging from yellow to black.Importantly,the intriguing thermochromism is proved to own extremely high reproducibility(over 1000 cycles)without a hysteretic effect,originating from its structural flexibility that including(i)the noteworthy distortion/deformation of[NaCl_(6)]5−and[FeCl_(6)]3−octahedra;(ii)order-disorder arrangement transition of[NaCl_(6)]5−and[FeCl6]3−octahedra as the function of temperature.This study paves the way towards a new class of smart windows and camouflage coatings with an unprecedented colour range based on a Cs_(2)NaFeCl_(6) perovskite.
基金financially supported by the National Natural Science Foundation of China(Nos.51772138,51572118,and 51601082)the Fundamental Research Funds for the Central Universities(No.lzujbky-2020-59)。
文摘Rechargeable aqueous zinc ion batteries(AZIBs)were considered as one of the most promising candidates for large-scale energy storage due to the merits of high safety and inexpensiveness.As AZIBs cathode material,Mn O_(2)possesses great merits but was greatly hindered due to the sluggish diffusion kinetic of Zn^(2+) during electrochemical operations.Herein,deep Zn^(2+) ions intercalatedδ-Mn O_(2)(Zn-Mn O_(2))was achieved by the in situ electrochemical deposition route,which significantly enhanced the diffusion ability of Zn^(2+) due to the synergistic effects of Zn^(2+) pillars and structural H;O.The resultant Zn-Mn O_(2)based AZIBs delivers a record capacity of 696 m Ah/g(0.5 m Ah/cm^(2))based on the initial mass loading,which is approaching the theoretical capacity of Mn O_(2)with a two-electrons reaction.In-situ Raman studies reveal highly reversible Zn^(2+)ions insertion/extraction behaviors and here the Zn-Mn O_(2)plays the role of a container during the charge–discharge process.Further charge storage mechanism investigations point out the insertion/extraction of Zn^(2+) and H^(+) coincides,and such process is significantly facilitated results from superior interlayered configurations of Zn-Mn O_(2)The excellent electrochemical performance of Zn-Mn O_(2)achieved in this work suggests the deep ions pre-intercalation strategy may aid in the future development of advanced cathodes for AZIBs.
文摘An inverse spinel-type metal oxide, magnesium-manganese-titanium oxide （Mg2Mn0.5Ti0.5O4）, were prepared using the coprecipitation/thermal crystallization method. The extraction/insertion reaction with this material was investigated by X-ray, saturation capacity of exchange, pH titration, and distribution coefficient （Kd） measurement. The acid treatments of Mg2Mn0.5Ti0.5O4 caused Mg^2＋ extractions of more than 81%, whereas the dissolutions of Mn^4＋ and Ti^4＋ were less than 10%. The experimental results proved that the acid-treated sample has a capacity of exchange 56 mg·g^-1 for Li^＋ in the solution. The chemical analysis showed that the Li^＋ extraction/insertion progressed mainly by ion-exchange mechanism and surface adsorption.
基金National Natural Science Foundation of China(Nos.21905209,52171145,and 51973078)Natural Science Foundation of Xinjiang Uygur Autonomous Region(No.2020D01B25).
文摘Converting hydrocarbons into aldehydes in a green and environmentally benign way is of great signif-icance in fine chemistry.In this work,all-inorganic Cs_(3)Bi_(2)B_(9) perovskite nanoparticles were uniformly loaded on BiOBr nanosheets via an in-situ growth method,which can selectivity photoactivate aromatic C(sp^(3))-H bond of toluene to generate benzaldehyde.According to the in-situ X-ray photoelectron spec-troscopy characterization,the photogenerated electrons of BiOBr transfer to Cs_(3)Bi_(2)B_(9) enforced by the in-ternal electric field under light irradiation,resulting in S-scheme heterojunction.Furthermore,theoretical calculations indicate that toluene molecules are inclined to adsorb on the BiOBr surface,subsequently in-volving the oxidation reaction to generate benzyl radical(PhCH_(2)·)by using the energetic holes of BiOBr,while the remaining photoinduced electrons in the conduction band(CB)of Cs_(3)Bi_(2)B_(9) with powerful reduction ability reduce O2 into·O_(2)^(-),which is the vital oxidative active species working on toluene selective oxidation process.Such an unexceptionable charge carrier utilization mode and tendentious ad-sorption behavior of reactants contribute to the optimized Cs_(3)Bi_(2)B_(9)/BiOBr heterojunction with excellent photocatalytic performance,achieving a maximum of 22.5%toluene conversion and 96.2%selectivity to-wards benzaldehyde formation.This work provides a rational photocatalyst heterojunction construction protocol for the selective oxidation of saturated aromatic C-H bonds.
