Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantia...Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantial resources and low cost of sodium.Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)solid electrolyte is attracting considerable interest owing to its excellent thermal and chemical stability and favorable compatibility with Na metal anode and high-voltage cathode.However,two main challenges of poor roomtemperature ionic conductivity and high interfacial resistance limit the application of NZSP electrolyte in SSSBs.So far,intensive efforts have been devoted to developing modification strategies to improve the room-temperature ionic conductivity of NZSP.This review aims to provide a comprehensive summary and discussion of some optimization strategies for enhancing the room-temperature ionic conductivity of the NZSP solid electrolyte.These optimization strategies are categorized into foreignion doping or substitution,sintering behavior modulation,and regulation of chemical composition based on precursors,and their optimization mechanisms are also elaborated.Finally,the prospects of NZSP-based solid electrolytes are presented.This review is expected to offer better guidance for designing and developing high-performance NZSP-based solid electrolytes for accelerating the practical application of SSSBs.展开更多
We report the results of the experiment on synthesizing ^(287,288)Mc isotopes (Z=115) using the fusionevaporation reaction ^(243)Am(^(48)Ca,4n,3n)^(287,288)Mc at the Spectrometer for Heavy Atoms and Nuclear Structure-...We report the results of the experiment on synthesizing ^(287,288)Mc isotopes (Z=115) using the fusionevaporation reaction ^(243)Am(^(48)Ca,4n,3n)^(287,288)Mc at the Spectrometer for Heavy Atoms and Nuclear Structure-2(SHANS2),a gas-filled recoil separator located at the China Accelerator Facility for Superheavy Elements(CAFE2).In total,20 decay chains are attributed to ^(288)Mc and 1 decay chain is assigned to ^(287)Mc.The measured oa-decay properties of ^(287,288)Mc as well as its descendants are consistent with the known data.No additional decay chains originating from the 2n or 5n reaction channels were detected.The excitation function of the ^(243)Am(^(48)Ca,3n)^(288)Mc reaction was measured at the cross-section level of picobarn,which indicates the promising capability for the study of heavy and superheavy nuclei at the facility.展开更多
Fig.3.(a)α-particle energy spectra,and(b)decay-time distributions on a logarithmic scale for the observed 288Mc and its descendant nuclei.In the panel(a),the red histograms show the observed full-energy events,while ...Fig.3.(a)α-particle energy spectra,and(b)decay-time distributions on a logarithmic scale for the observed 288Mc and its descendant nuclei.In the panel(a),the red histograms show the observed full-energy events,while the corresponding blue histograms show the reconstructed events.The red smooth curves in panel(b)are the expected time distributions according to the corresponding half-lives extracted from this work.展开更多
The dissolved hydrogen, rather than gaseous hydrogen, plays a crucial role in the hydrogenation process. A thorough understanding of hydrogen dissolution is essential for optimizing the hydrogenation process. In this ...The dissolved hydrogen, rather than gaseous hydrogen, plays a crucial role in the hydrogenation process. A thorough understanding of hydrogen dissolution is essential for optimizing the hydrogenation process. In this paper, the dynamic pressure step method was modified to reduce the temperature difference between the hydrogen and solution, from which the hydrogen solubility and volumetric liquid-side mass transfer coefficient (k_(L)a) of the vacuum residue were obtained. It was discovered that temperature was the most critical factor in hydrogen dissolution, simultaneously enhancing both the hydrogen solubility and k_(L)a. Pressure played a significant role in promoting hydrogen solubility, but had a relatively small impact on kLa. Stirring speed, although it enhanced k_(L)a, did not affect hydrogen solubility. By normalizing the dissolution parameter, the results showed that the gas-liquid mass transfer rate decreased continuously during hydrogen dissolution and that the SD-tD curves after normalization were almost the same in all experimental conditions.展开更多
Upgrading of abundant cellulosic biomass to isosorbide can reduce the dependence on limited fossil resources and provide a sustainable way to produce isosorbide,utilized for polymers,medicine and health care product s...Upgrading of abundant cellulosic biomass to isosorbide can reduce the dependence on limited fossil resources and provide a sustainable way to produce isosorbide,utilized for polymers,medicine and health care product synth-esis.This review comprehensively examines the key steps and catalytic systems involved in the conversion of cel-lulose to isosorbide.Initially,the reaction pathway from cellulose to isosorbide is elucidated,emphasizing three critical steps:cellulose hydrolysis,glucose hydrogenation,and the two-step dehydration of sorbitol to produce isosorbide.Additionally,the activation energy and acidic sites during cellulose hydrolysis,the impact of metal particle size and catalyst support on hydrogenation,and the effects of catalyst acidity,pore structure,and reaction conditions on sorbitol dehydration have been thoroughly examined.Finally,the progress made in cellulose con-version to isosorbide is summarized,current challenges are highlighted,and future development trends are pro-jected in this review.展开更多
China possesses abundant heavy oil resources,yet faces challenges such as high viscosity,underdeveloped production technologies,and elevated development cost.Although the in-situ catalytic viscosity-reduction technolo...China possesses abundant heavy oil resources,yet faces challenges such as high viscosity,underdeveloped production technologies,and elevated development cost.Although the in-situ catalytic viscosity-reduction technology can address certain technical,environmental,and cost problems during the extraction process,the catalysts often suffer from poor stability and low catalytic efficiency.In this study,a green and simple room-temperature stirring method was employed to synthesize a class of highly efficient and stable 2D MOF catalysts,which possess the capability to conduct in-situ catalytic pyrolysis of heavy oil and reduce the viscosity.Under the condition of 160℃,a catalyst concentration of 0.5 wt%,and a hydrogen donor(tetralin)concentration of 2 wt%,the viscosity-reduction rate of Fe-MOF is as high as 89.09%,and it can decrease the asphaltene content by 8.42%.In addition,through the structural identification and analysis of crude oil asphaltenes,the causes for the high viscosity of heavy oil are explained at the molecular level.Through the analysis of catalytic products and molecular dynamics simulation,the catalytic mechanism is studied.It is discovered that Fe-MOF can interact with heavy oil macromolecules via coordination and pore-channel effects,facilitating their cracking and dispersal.Furthermore,synergistic interactions between Fe-MOF and the hydrogen donor facilitates hydrogenation reactions and enhances the viscosity-reducing effect.This study provides a novel strategy for boosting heavy oil recovery and underscores the potential of 2D MOFs in catalytic pyrolysis applications.展开更多
The influences of reaction temperature,duration,pressure,and catalyst concentration on the molecular transformation of residual slurry phase hydrocracking process were investigated.The molecular composition of the het...The influences of reaction temperature,duration,pressure,and catalyst concentration on the molecular transformation of residual slurry phase hydrocracking process were investigated.The molecular composition of the heteroatom compounds in the residue feedstock and its upgrading products were characterized using high-resolution Orbitrap mass spectrometry coupled with multiple ionization methods.The simultaneous promotion of cracking and hydrogenation reactions was observed with increasing of the reaction temperature and time.Specifically,there was a significant increase in the cracking degree of alkyl side chain,while the removal of low-condensation sulfur compounds such as sulfides and benzothiophenes was enhanced.In particular,the cracking reactions were more significantly facilitated by high temperatures,while an appropriately extended reaction time can result in the complete elimination of the aforementioned sulfur compounds with a lower degree of condensation.Under conditions of low hydrogen pressure and catalyst concentration,the products still exhibit a high relative abundance of easily convertible compounds such as sulfoxides,indicating a significant deficiency in the effectiveness of hydrogenation.The hydrogen pressure exhibits an optimal value,beyond which further increments have no effect on the composition and performance of the liquid product but can increase the yield of the liquid product.At significantly high catalyst concentration,the effect of desulfurization and deoxidation slightly diminishes,while the aromatic saturation of highly condensed compounds was notably enhanced.This hydrogenation saturation effect cannot be attained through manipulation of other operational parameters,thereby potentially benefiting subsequent product processing and utilization.This present study demonstrates a profound comprehension of the molecular-level residue slurry phase hydrocracking process,offering not only specific guide for process design and optimization but also valuable fundamental data for constructing reaction models at the molecular level.展开更多
State-selective single-and double-electron capture processes in collisions of S^(5+)ions with helium at energies ranging from 50.8 keV to 100 keV were investigated using cold target recoil ion momentum spectroscopy(CO...State-selective single-and double-electron capture processes in collisions of S^(5+)ions with helium at energies ranging from 50.8 keV to 100 keV were investigated using cold target recoil ion momentum spectroscopy(COLTRIMS).Q-value spectra and projectile scattering angle distributions were obtained.For single-electron capture,single electron capture into n=3 states of the projectile ion is dominant.As the projectile energy increases,the contribution of single electron capture into n=4 states is observed.Experimental relative cross-sections for single-electron capture into different projectile final states were compared with theoretical predictions based on the molecular orbital close-coupling(MOCC)method.In double-electron capture,two-electron populating into the 3s^(2)3p and 3s3p^(2)states of projectile dominates.The reaction window calculated from the classical molecular Coulombic barrier model can qualitatively explain the experimental results.The scattering angle distribution of the multi-peak structure of the double-electron capture process is observed.The database is openly available in Science Data Bank at https://doi.org/10.57760/sciencedb.j00113.00233.展开更多
We study the fragmentation of NO^(q+)(q=2,3)molecular ions produced by collisions between 96 keV O^(6+)ions and neutral nitric oxide(NO)molecules,using the cold target recoil ion momentum spectrometer(COLTRIMS).The ki...We study the fragmentation of NO^(q+)(q=2,3)molecular ions produced by collisions between 96 keV O^(6+)ions and neutral nitric oxide(NO)molecules,using the cold target recoil ion momentum spectrometer(COLTRIMS).The kinetic energy release(KER)for various dissociation channels is obtained.For the channel NO^(2+)→N^(+)+O^(+),double-electron capture followed by autoionization of the projectile ions is the dominant process,which can be explained by the recapture of loosely bound electrons into highly excited states of the target.For NO3+trication,two dissociation channels,i.e.,(a)N^(+)+O^(2+)and(b)N^(2+)+O^(+),are observed,where channel(b)is the dominant channel.Moreover,for dissociation channels originating from the same parent molecular ion,the dissociation channel with a higher charge for the oxygen ion fragment exhibits a higher most probable KER,which is consistent with studies of CO fragmentation by Rajput et al.Additionally,it is observed that as capture stability increases,the average KER shifts to higher values.展开更多
Lignin contains abundant aromatic ring structures,which can be converted into green sustainable aviation fuelrange arenes through hydrodeoxygenation(HDO).A series of supported FeMoS/NC catalysts were synthesized by a ...Lignin contains abundant aromatic ring structures,which can be converted into green sustainable aviation fuelrange arenes through hydrodeoxygenation(HDO).A series of supported FeMoS/NC catalysts were synthesized by a hydrothermal method.The HDO performance of the catalysts was evaluated using 4-ethylguaiacol as a model compound at 340℃ under 3 MPa H2.The MoS_(2)/NC catalyst exhibited a deoxygenation degree of 83.4%,whereas the Fe-modified catalyst(Fe_(0.3)MoS/NC)attained complete deoxygenation(100%)with an arenes selectivity of 78.6%.Beyond the optimal ratio,the deoxygenation degree is inversely proportional to the Fe/Mo molar ratio.The catalysts were characterized by X-ray diffraction(XRD),transmission electron microscopy(TEM),low-temperature nitrogen adsorption(BET method)and X-ray photoelectron spectroscopy(XPS).The characterization results indicated that the introduction of Fe enhanced the uniform dispersion of MoS_(2)on the NC support surface.This modification further increased the acidity of the catalyst surface and raised the concentration of sulfur vacancies,thereby promoting the adsorption of oxygencontaining compounds.Furthermore,the HDO performance of the Fe_(0.3)MoS/NC catalyst was evaluated using actual lignin as a feedstock under the conditions of 340℃,3 MPa H2 and 12 h.The results showed a green hydrocarbon yield of 65.5%,of which the C_(8)-C_(16)fraction accounted for 54.4%of the total hydrocarbons.Within this fraction,aromatic compounds constituted 63.4%,suggesting its potential use as green aviation fuel-range arenes.This work thus establishes a viable catalytic pathway for efficient conversion of lignin to arenes.展开更多
Aiming at the problems of insufficient activity and selectivity of Cu-based catalysts in CO_(2)hydrogenation to methanol,Al_(2)O_(3),ZrO_(2)and CeO_(2)modified Cu-ZnO catalysts by the co-precipitation method were prep...Aiming at the problems of insufficient activity and selectivity of Cu-based catalysts in CO_(2)hydrogenation to methanol,Al_(2)O_(3),ZrO_(2)and CeO_(2)modified Cu-ZnO catalysts by the co-precipitation method were prepared,and the influence mechanism of additives on the structure-performance relationship of the catalysts was systematically explored.Through a variety of characterization methods such as XRD,N2 physical adsorption-desorption,TEM,H_(2)-TPR,CO_(2)-TPD and XPS,combined with catalytic performance evaluation experiments,the correlation between the microstructure of catalysts and the reaction performance of CO_(2)hydrogenation to methanol was analyzed in depth.The results show that metal additives significantly improve the performance of catalysts.After the introduction of additives,the specific surface area and pore volume of the catalysts increase,the grain size of Cu decreases,and its dispersion improves.The Ce-modified CZC catalyst exhibited the best performance,with the grain size of CuO as small as 11.41 nm,and the surface oxygen vacancy concentration(OⅡ/OⅠ=3.15)was significantly higher than that of other samples.The reaction performance test shows that under the conditions of 2.8 MPa,8000 h−1 and 280℃,the CO_(2)conversion of the CZC catalyst reached 18.83%,the methanol selectivity was 68.40%,and the methanol yield was 12.88%,all of which are superior to other catalysts.Its excellent performance can be attributed to the fact that CeO_(2)enhances the metal-support interaction,increases the surface basicity,promotes the adsorption and activation of CO_(2),and simultaneously inhibits the reverse water-gas shift side reaction.This study clarifies the structure-activity regulation mechanism of additive modification on Cu-ZnO catalysts,providing a theoretical basis and technical reference for the development of efficient catalysts for CO_(2)hydrogenation to methanol.展开更多
Pitch is an excellent precursor for the production of hard carbon,with pre-oxidation crucial process in the fabrication.The structural changes in the different molecular components of pitch during thermochemical treat...Pitch is an excellent precursor for the production of hard carbon,with pre-oxidation crucial process in the fabrication.The structural changes in the different molecular components of pitch during thermochemical treatment are a key factor in determining the sodium-ion storage of pitchbased hard carbon anodes.We investigated the effects of the different molecular structures in the asphaltene precursor,including aromatic rings and aliphatic chains,on the sodiumion storage behavior of the resulting carbon.We found that polar oxygen functional groups limit the steric hindrance caused by the aromatic rings in pitch,and thus facilitate the introduction of cross-linked structures.During high-temperature carbonization,aromatic rings form a rigid carbon framework that prevents the rearrangement of ordered carbon layers,leading to a short-range disordered carbon structure and promotes the production of closed pores.For example,a material prepared from asphaltene,which contains a large number of oxygen-containing functional groups and macromolecular aromatic rings,using pre-oxidation at 300℃ and carbonization at 1200℃ had a reversible capacity of 316.7 mAh g^(−1) when used as the anode for sodium ion batteries.Our research provides a theoretical basis for the selection of raw materials for the development of high-quality pitch-based hard carbons.展开更多
Catalytic decomposition of methane,which produces high-purity hydrogen and high-value-added carbon nanomaterials,has shown considerable potential for development and is expected to yield significant economic benefits ...Catalytic decomposition of methane,which produces high-purity hydrogen and high-value-added carbon nanomaterials,has shown considerable potential for development and is expected to yield significant economic benefits in the future.However,designing catalysts that simultaneously exhibit high activity and long-term stability remains a significant challenge.Tuning the catalyst’s structure and electronic properties is an effective strategy for enhancing the reaction performance.In this work,a series of NixZr/ZSM-5 catalysts were prepared using the incipient wetness impregnation method,and the effect of Zr loadings on catalyst properties and performance was systematically investigated.The calcined and reduced catalysts were characterized by low-temperature N_(2)adsorption-desorption,XRD,SEM,H_(2)-TPR and XPS.The results showed that the addition of Zr significantly increased the specific surface area of the catalyst and reduced the metal particle size.Smaller NiO particles were found to enter the pores of the HZSM-5 support,and electronic interactions between NiO and ZrO_(2)markedly enhanced the metal-support interaction.The catalyst exhibited optimal catalytic performance at a Zr loading of 5%,achieving a maximum methane conversion of 68%at 625℃,maintaining activity for 900 min,and delivering a carbon yield of 1927%.Further increasing the Zr loading yielded only limited improvements in catalytic performance.Characterization of the spent catalysts and carbon products via TEM,Raman spectroscopy,and TGA revealed that the introduction of ZrO_(2)reduced metal sintering and promoted a shift in carbon nanofibers growth mode from tip-growth to base-growth.The mechanism of base-growth enabled the catalyst to maintain reaction activity for an extended period.展开更多
Electrochemical liquid lithium extraction technology has attracted much attention because of its high selectivity,good efficiency,and eco-friendliness.However,the low energy density per unit area and poor stability of...Electrochemical liquid lithium extraction technology has attracted much attention because of its high selectivity,good efficiency,and eco-friendliness.However,the low energy density per unit area and poor stability of traditional thin film electrodes(F-LMO),as well as manganese dissolution loss induced by the Jahn-Teller distortion of LiMn_(2)O_(4),hinder their industrial scalability.Herein,a durable and high-efficiency multistage porous LiMn_(2)O_(4) thick electrode was prepared sustainably by 3D printing technology(3DPLMO)for enhancing lithium recovery from salt lake brine.The multistage porous structure reduced the mass transfer resistance and shortened the ion diffusion path,which was conducive to accelerating the diffusion rate of Li+.Simultaneously,the three-dimensional conductive networks composed of reduced graphene oxide(r GO)and carbon nanotubes(CNT)synergized with the multistage pores effectively weakened the polarization phenomenon of the electrode and improved the stability of 3DP-LMO.The3DP-LMO exhibited a 5.5-fold higher extraction capacity per unit area and the Mn dissolution loss rate was only 1/15 compared with the F-LMO.Notably,the capacity retention rate of 3DP-LMO was 87.6%,significantly better than that of F-LMO(66.3%).Based on the quasi-in situ X-ray Diffraction results,the mechanism of lithium intercalation and deintercalation in 3DP-LMO was elucidated.Furthermore,lithium extraction parameters were optimized using response surface method-center composite design(RSM-CCD),resulting in an increase in lithium extraction capacity to 15.66 mg g^(-1)and a reduction in energy consumption to only 12.33 Wh mol^(-1).The results show that 3DP-LMO has significantly improved lithium extraction performance and stability,and has considerable prospects in practical application.展开更多
Rational design of nanozymes with enhanced catalytic efficiency remains a central challenge in the development of artificial enzymes.Herein,we report the construction of ultrasmall gold nanoclusterbased nanoassemblies...Rational design of nanozymes with enhanced catalytic efficiency remains a central challenge in the development of artificial enzymes.Herein,we report the construction of ultrasmall gold nanoclusterbased nanoassemblies(Dp-Au NCs@Fe^(2+)) through the coordination of Fe^(2+) ions by a dopa-containing peptidomimetic ligand(Dp CDp).This nanoarchitecture simultaneously integrates catalytically active gold cores and redox-active Fe^(2+)centers,bridged by Dp CDp to facilitate directional electron transfer.Comprehensive spectroscopic and kinetic analyses reveal that Dp CDp promotes efficient charge migration from the Au core to surface-bound Fe^(2+),significantly enhancing H_(2)O_(2)-mediated peroxidase-like activity.Compared to bare Dp-Au NCs,Dp-Au NCs@Fe^(2+) display a 4.3-fold improvement in detection sensitivity,a 6.7-fold increase in catalytic efficiency,and markedly stronger hydroxyl radical generation.Mechanistically,this activity stems from a synergistic triad:direct H_(2)O_(2) oxidation at gold surfaces,radical generation at Fe^(2+) sites,and Dp CDp-facilitated electron shuttling.This work presents a robust strategy for nanozyme enhancement via electronic and structural co-engineering,offering valuable insights for the future design of bioinspired catalytic systems.展开更多
Petroleum leakage is a major groundwater contamination source,with chemical composition of water soluble fractions(WSFs)from diverse oil sources significantly impacting groundwater quality and source identification.Th...Petroleum leakage is a major groundwater contamination source,with chemical composition of water soluble fractions(WSFs)from diverse oil sources significantly impacting groundwater quality and source identification.The aim of this study was to assess impact of 15 diverse oils on groundwater quality and environmental forensics based on oil-water equilibrium experiments.Our results indicate that contamination of groundwater by gasoline and naphtha is primarily attributed to volatile hydrocarbons,while pollution from diesel,kerosene,and crude oil is predominantly from non-hydrocarbons.Rapid determination of the extent of non-hydrocarbon pollution in WSFs was achieved through a new quantitative index.Gasoline and naphtha exhibited the highest groundwater contamination potential while kerosene and light crude oils were also likely to cause groundwater contamina-tion.Although volatile hydrocarbons in the WSFs of diesel and jet fuel do not easily exceed current regulatory standards,unregulated non-hydrocarbons may pose a more severe contamination risk to groundwater.Notably,the presence of significant benzene and toluene,hydrogenation and alkylation products(e.g.,C4-C5 alkylben-zenes,alkylindenes,alkyltetralins,and dihydro-indenes),cycloalkanes in WSFs can effectively be utilized for preliminary source identification of light distillates,middle distillates,and crude oils,respectively.展开更多
The advancement of hydrogen-based energy systems necessitates innovative solutions for safe,efficient hydrogen storage and transportation.Liquid organic hydrogen carriers(LOHCs)emerge as a transformative technology by...The advancement of hydrogen-based energy systems necessitates innovative solutions for safe,efficient hydrogen storage and transportation.Liquid organic hydrogen carriers(LOHCs)emerge as a transformative technology by combining high hydrogen capacity,excellent stability,and seamless integration with existing fuel infrastructure,enabling large-scale,long-distance hydrogen logistics.Despite these merits,challenges in dehydrogenation kinetics and catalyst instability impede practical deployment.Herein,we present a comprehensive mechanistic review of dehydrogenation pathways across diverse LOHC platforms,including cyclohexane,methylcyclohexane,decalin,dodecahydro-N-ethylcarbazole,perhydro-dibenzyltoluene/benzyltoluene,bicyclohexyl,and indole-based LOHCs.Compared with previous reviews,this study integrates geometric and electronic effects across multiple LOHC systems to identify cross-cutting structure-activity principles.Building on this framework,it further reveals reactant-dependent rules for active-site regulation,where the molecular architecture of hydrogen carriers critically determines the required catalyst characteristics.This perspective establishes a unified framework that links molecular descriptors to coordination-specific active sites,thereby advancing precision catalyst design for next-generation LOHC technologies.展开更多
The Cooling-Storage-Ring External-target Experiment(CEE)at the Heavy Ion Research Facility in Lanzhou(HIRFL)is designed to study the properties of nuclear matter created in heavy-ion collisions at beam energies from a...The Cooling-Storage-Ring External-target Experiment(CEE)at the Heavy Ion Research Facility in Lanzhou(HIRFL)is designed to study the properties of nuclear matter created in heavy-ion collisions at beam energies from a few hundred MeV/u up to 1 GeV/u.It aims to facilitate research on the quantum chromodynamics(QCD)phase structure in the high-baryondensity region.Collective flow is a fundamental observable in heavy-ion collision experiments,providing information on the bulk properties of the produced matter.Although the standard event plane method has been widely used to measure collective flow,it is still important to validate and optimize this method for the CEE spectrometer.In this paper,we study the experimental procedures for measuring directed flow in^(238)U+^(238)U collisions at 500 MeV/u,using event planes reconstructed by Multi-Wire Drift Chamber and Zero Degree Calorimeter,respectively.Jet AA Microscopic(JAM)transport generator is used to generate events,and the detector response is simulated by the CEE Fast Simulation(CFS)package.Finally,the optimal kinematic region for proton directed flow measurements is discussed for the future CEE experiment.展开更多
A new multi-detector array named HALIMA(Hybrid Array for LIfetime MeAsurement)has been developed at Lanzhou for nuclear structure studies in fission.The array comprises eight BGO-shielded High-Purity Germanium detecto...A new multi-detector array named HALIMA(Hybrid Array for LIfetime MeAsurement)has been developed at Lanzhou for nuclear structure studies in fission.The array comprises eight BGO-shielded High-Purity Germanium detectors and twenty fast Ce-doped Lanthanum Bromide[LaBr_(3)(Ce)]detectors shielded with CsI(Tl).HALIMA is further complemented by two ancillary detector systems:fission fragment(FF)detectors and β detectors.This configuration enables precise sub-nanosecond lifetime measurements using the fourfold FF/β-Ge-LaBr_(3)(Ce)-LaBr_(3)(Ce)coincidence technique.The performance and specifications of the detectors,associated electronics,and the data acquisition system are presented in detail.The advantage of FF selectivity is emphasized,which significantly enhances sensitivity to specific fission channels.Using this approach,the lifetimes of the nuclear excited states populated in the spontaneous fission of^(252)Cf were measured,showing good agreement with the established literature values.展开更多
Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via lo...Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via low-temperature coprecipitation,exhibiting excellent performance for the selective hydrogenation of 5-hydroxymethylfurfural(HMF).A linear correlation is first observed between solvent polarity(E_(T)(30))and product selectivity within both polar aprotic and protic solvent classes,suggesting that solvent properties play a vital role in directing reaction pathways.Among these,1,4-dioxane(aprotic)favors the formation of 2,5-bis(hydroxymethyl)furan(BHMF)with 97.5%selectivity,while isopropanol(iPrOH,protic)promotes 2,5-dimethylfuran production with up to 99.5%selectivity.Mechanistic investigations further reveal that beyond polarity,proton-donating ability is critical in facilitating hydrodeoxygenation.iPrOH enables a hydrogen shuttle mechanism where protons assist in hydroxyl group removal,lowering the activation barrier.In contrast,1,4-dioxane,lacking hydrogen bond donors,stabilizes BHMF and hinders further conversion.Density functional theory calculations confirm a lower activation energy in iPrOH(0.60 eV)compared to 1,4-dioxane(1.07 eV).This work offers mechanistic insights and a practical strategy for solvent-mediated control of product selectivity in biomass hydrogenation,highlighting the decisive role of solvent-catalyst-substrate interactions.展开更多
基金National Natural Science Foundation of China,Grant/Award Number:52272225。
文摘Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantial resources and low cost of sodium.Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)solid electrolyte is attracting considerable interest owing to its excellent thermal and chemical stability and favorable compatibility with Na metal anode and high-voltage cathode.However,two main challenges of poor roomtemperature ionic conductivity and high interfacial resistance limit the application of NZSP electrolyte in SSSBs.So far,intensive efforts have been devoted to developing modification strategies to improve the room-temperature ionic conductivity of NZSP.This review aims to provide a comprehensive summary and discussion of some optimization strategies for enhancing the room-temperature ionic conductivity of the NZSP solid electrolyte.These optimization strategies are categorized into foreignion doping or substitution,sintering behavior modulation,and regulation of chemical composition based on precursors,and their optimization mechanisms are also elaborated.Finally,the prospects of NZSP-based solid electrolytes are presented.This review is expected to offer better guidance for designing and developing high-performance NZSP-based solid electrolytes for accelerating the practical application of SSSBs.
基金supported in part by the National Key R&D Program of China (Contract Nos.2023YFA1606500,2024YFE0109800,and 2024YFE0110400)Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB34010000)+5 种基金the Gansu Key Project of Science and Technology (Grant No.23ZDGA014)the Guangdong Major Project of Basic and Applied Basic Research (Grant No.2021B0301030006)the National Natural Science Foundation of China (Grant Nos.12105328,W2412040,12475126,12422507,12035011,12375118,12435008,and W2412043)the Chinese Academy of Sciences Project for Young Scientists in Basic Research(Grant No.YSBR-002)the Youth Innovation Promotion Association of the Chinese Academy of Sciences (Grant Nos.2020409 and 2023439)the Russian Science Foundation (Grant No.25-42-00003)。
文摘We report the results of the experiment on synthesizing ^(287,288)Mc isotopes (Z=115) using the fusionevaporation reaction ^(243)Am(^(48)Ca,4n,3n)^(287,288)Mc at the Spectrometer for Heavy Atoms and Nuclear Structure-2(SHANS2),a gas-filled recoil separator located at the China Accelerator Facility for Superheavy Elements(CAFE2).In total,20 decay chains are attributed to ^(288)Mc and 1 decay chain is assigned to ^(287)Mc.The measured oa-decay properties of ^(287,288)Mc as well as its descendants are consistent with the known data.No additional decay chains originating from the 2n or 5n reaction channels were detected.The excitation function of the ^(243)Am(^(48)Ca,3n)^(288)Mc reaction was measured at the cross-section level of picobarn,which indicates the promising capability for the study of heavy and superheavy nuclei at the facility.
文摘Fig.3.(a)α-particle energy spectra,and(b)decay-time distributions on a logarithmic scale for the observed 288Mc and its descendant nuclei.In the panel(a),the red histograms show the observed full-energy events,while the corresponding blue histograms show the reconstructed events.The red smooth curves in panel(b)are the expected time distributions according to the corresponding half-lives extracted from this work.
基金supported by the National Key R&D Program of China(No.2022YFB4101300)National Natural Science Foundation of China(NSFC)(No.22278430 and 21878329)Project of R&D Department of CNPC(2020B-2011 and 21-CB-05-05).
文摘The dissolved hydrogen, rather than gaseous hydrogen, plays a crucial role in the hydrogenation process. A thorough understanding of hydrogen dissolution is essential for optimizing the hydrogenation process. In this paper, the dynamic pressure step method was modified to reduce the temperature difference between the hydrogen and solution, from which the hydrogen solubility and volumetric liquid-side mass transfer coefficient (k_(L)a) of the vacuum residue were obtained. It was discovered that temperature was the most critical factor in hydrogen dissolution, simultaneously enhancing both the hydrogen solubility and k_(L)a. Pressure played a significant role in promoting hydrogen solubility, but had a relatively small impact on kLa. Stirring speed, although it enhanced k_(L)a, did not affect hydrogen solubility. By normalizing the dissolution parameter, the results showed that the gas-liquid mass transfer rate decreased continuously during hydrogen dissolution and that the SD-tD curves after normalization were almost the same in all experimental conditions.
文摘Upgrading of abundant cellulosic biomass to isosorbide can reduce the dependence on limited fossil resources and provide a sustainable way to produce isosorbide,utilized for polymers,medicine and health care product synth-esis.This review comprehensively examines the key steps and catalytic systems involved in the conversion of cel-lulose to isosorbide.Initially,the reaction pathway from cellulose to isosorbide is elucidated,emphasizing three critical steps:cellulose hydrolysis,glucose hydrogenation,and the two-step dehydration of sorbitol to produce isosorbide.Additionally,the activation energy and acidic sites during cellulose hydrolysis,the impact of metal particle size and catalyst support on hydrogenation,and the effects of catalyst acidity,pore structure,and reaction conditions on sorbitol dehydration have been thoroughly examined.Finally,the progress made in cellulose con-version to isosorbide is summarized,current challenges are highlighted,and future development trends are pro-jected in this review.
基金supported by the National Natural Science Foundation of China(52174047)Sinopec Project(No.P23138).
文摘China possesses abundant heavy oil resources,yet faces challenges such as high viscosity,underdeveloped production technologies,and elevated development cost.Although the in-situ catalytic viscosity-reduction technology can address certain technical,environmental,and cost problems during the extraction process,the catalysts often suffer from poor stability and low catalytic efficiency.In this study,a green and simple room-temperature stirring method was employed to synthesize a class of highly efficient and stable 2D MOF catalysts,which possess the capability to conduct in-situ catalytic pyrolysis of heavy oil and reduce the viscosity.Under the condition of 160℃,a catalyst concentration of 0.5 wt%,and a hydrogen donor(tetralin)concentration of 2 wt%,the viscosity-reduction rate of Fe-MOF is as high as 89.09%,and it can decrease the asphaltene content by 8.42%.In addition,through the structural identification and analysis of crude oil asphaltenes,the causes for the high viscosity of heavy oil are explained at the molecular level.Through the analysis of catalytic products and molecular dynamics simulation,the catalytic mechanism is studied.It is discovered that Fe-MOF can interact with heavy oil macromolecules via coordination and pore-channel effects,facilitating their cracking and dispersal.Furthermore,synergistic interactions between Fe-MOF and the hydrogen donor facilitates hydrogenation reactions and enhances the viscosity-reducing effect.This study provides a novel strategy for boosting heavy oil recovery and underscores the potential of 2D MOFs in catalytic pyrolysis applications.
基金supported by the National Key R&D Program of China(2021YFA1501200)the National Natural Science Foundation of China(NSFC U23B20169 and 22021004)the Project of R&D Department of CNPC(2020B-2011)。
文摘The influences of reaction temperature,duration,pressure,and catalyst concentration on the molecular transformation of residual slurry phase hydrocracking process were investigated.The molecular composition of the heteroatom compounds in the residue feedstock and its upgrading products were characterized using high-resolution Orbitrap mass spectrometry coupled with multiple ionization methods.The simultaneous promotion of cracking and hydrogenation reactions was observed with increasing of the reaction temperature and time.Specifically,there was a significant increase in the cracking degree of alkyl side chain,while the removal of low-condensation sulfur compounds such as sulfides and benzothiophenes was enhanced.In particular,the cracking reactions were more significantly facilitated by high temperatures,while an appropriately extended reaction time can result in the complete elimination of the aforementioned sulfur compounds with a lower degree of condensation.Under conditions of low hydrogen pressure and catalyst concentration,the products still exhibit a high relative abundance of easily convertible compounds such as sulfoxides,indicating a significant deficiency in the effectiveness of hydrogenation.The hydrogen pressure exhibits an optimal value,beyond which further increments have no effect on the composition and performance of the liquid product but can increase the yield of the liquid product.At significantly high catalyst concentration,the effect of desulfurization and deoxidation slightly diminishes,while the aromatic saturation of highly condensed compounds was notably enhanced.This hydrogenation saturation effect cannot be attained through manipulation of other operational parameters,thereby potentially benefiting subsequent product processing and utilization.This present study demonstrates a profound comprehension of the molecular-level residue slurry phase hydrocracking process,offering not only specific guide for process design and optimization but also valuable fundamental data for constructing reaction models at the molecular level.
基金Project supported by the National Key Research and Development Program of China(Grant No.2022YFA1602500)the National Natural Science Foundation of China(Grant No.11974358)。
文摘State-selective single-and double-electron capture processes in collisions of S^(5+)ions with helium at energies ranging from 50.8 keV to 100 keV were investigated using cold target recoil ion momentum spectroscopy(COLTRIMS).Q-value spectra and projectile scattering angle distributions were obtained.For single-electron capture,single electron capture into n=3 states of the projectile ion is dominant.As the projectile energy increases,the contribution of single electron capture into n=4 states is observed.Experimental relative cross-sections for single-electron capture into different projectile final states were compared with theoretical predictions based on the molecular orbital close-coupling(MOCC)method.In double-electron capture,two-electron populating into the 3s^(2)3p and 3s3p^(2)states of projectile dominates.The reaction window calculated from the classical molecular Coulombic barrier model can qualitatively explain the experimental results.The scattering angle distribution of the multi-peak structure of the double-electron capture process is observed.The database is openly available in Science Data Bank at https://doi.org/10.57760/sciencedb.j00113.00233.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFA1602500)the National Natural Science Foundation of China(Grant Nos.11934004,12064040,and 11974358)Strategic Key Research Program of the Chinese Academy of Sciences(Grant No.XDB34020000).
文摘We study the fragmentation of NO^(q+)(q=2,3)molecular ions produced by collisions between 96 keV O^(6+)ions and neutral nitric oxide(NO)molecules,using the cold target recoil ion momentum spectrometer(COLTRIMS).The kinetic energy release(KER)for various dissociation channels is obtained.For the channel NO^(2+)→N^(+)+O^(+),double-electron capture followed by autoionization of the projectile ions is the dominant process,which can be explained by the recapture of loosely bound electrons into highly excited states of the target.For NO3+trication,two dissociation channels,i.e.,(a)N^(+)+O^(2+)and(b)N^(2+)+O^(+),are observed,where channel(b)is the dominant channel.Moreover,for dissociation channels originating from the same parent molecular ion,the dissociation channel with a higher charge for the oxygen ion fragment exhibits a higher most probable KER,which is consistent with studies of CO fragmentation by Rajput et al.Additionally,it is observed that as capture stability increases,the average KER shifts to higher values.
基金Supported by grants from National Key Research and Development Program of China(2024YFB4205903)the National Natural Science Foundation of China(52274308,U22B20144,22278440 and 22078362)Shandong Provincial Technology Innovation Guidance Plan(YDZX2023060)。
文摘Lignin contains abundant aromatic ring structures,which can be converted into green sustainable aviation fuelrange arenes through hydrodeoxygenation(HDO).A series of supported FeMoS/NC catalysts were synthesized by a hydrothermal method.The HDO performance of the catalysts was evaluated using 4-ethylguaiacol as a model compound at 340℃ under 3 MPa H2.The MoS_(2)/NC catalyst exhibited a deoxygenation degree of 83.4%,whereas the Fe-modified catalyst(Fe_(0.3)MoS/NC)attained complete deoxygenation(100%)with an arenes selectivity of 78.6%.Beyond the optimal ratio,the deoxygenation degree is inversely proportional to the Fe/Mo molar ratio.The catalysts were characterized by X-ray diffraction(XRD),transmission electron microscopy(TEM),low-temperature nitrogen adsorption(BET method)and X-ray photoelectron spectroscopy(XPS).The characterization results indicated that the introduction of Fe enhanced the uniform dispersion of MoS_(2)on the NC support surface.This modification further increased the acidity of the catalyst surface and raised the concentration of sulfur vacancies,thereby promoting the adsorption of oxygencontaining compounds.Furthermore,the HDO performance of the Fe_(0.3)MoS/NC catalyst was evaluated using actual lignin as a feedstock under the conditions of 340℃,3 MPa H2 and 12 h.The results showed a green hydrocarbon yield of 65.5%,of which the C_(8)-C_(16)fraction accounted for 54.4%of the total hydrocarbons.Within this fraction,aromatic compounds constituted 63.4%,suggesting its potential use as green aviation fuel-range arenes.This work thus establishes a viable catalytic pathway for efficient conversion of lignin to arenes.
基金Supported by National Key R&D Program of China(2022YFA1503400)。
文摘Aiming at the problems of insufficient activity and selectivity of Cu-based catalysts in CO_(2)hydrogenation to methanol,Al_(2)O_(3),ZrO_(2)and CeO_(2)modified Cu-ZnO catalysts by the co-precipitation method were prepared,and the influence mechanism of additives on the structure-performance relationship of the catalysts was systematically explored.Through a variety of characterization methods such as XRD,N2 physical adsorption-desorption,TEM,H_(2)-TPR,CO_(2)-TPD and XPS,combined with catalytic performance evaluation experiments,the correlation between the microstructure of catalysts and the reaction performance of CO_(2)hydrogenation to methanol was analyzed in depth.The results show that metal additives significantly improve the performance of catalysts.After the introduction of additives,the specific surface area and pore volume of the catalysts increase,the grain size of Cu decreases,and its dispersion improves.The Ce-modified CZC catalyst exhibited the best performance,with the grain size of CuO as small as 11.41 nm,and the surface oxygen vacancy concentration(OⅡ/OⅠ=3.15)was significantly higher than that of other samples.The reaction performance test shows that under the conditions of 2.8 MPa,8000 h−1 and 280℃,the CO_(2)conversion of the CZC catalyst reached 18.83%,the methanol selectivity was 68.40%,and the methanol yield was 12.88%,all of which are superior to other catalysts.Its excellent performance can be attributed to the fact that CeO_(2)enhances the metal-support interaction,increases the surface basicity,promotes the adsorption and activation of CO_(2),and simultaneously inhibits the reverse water-gas shift side reaction.This study clarifies the structure-activity regulation mechanism of additive modification on Cu-ZnO catalysts,providing a theoretical basis and technical reference for the development of efficient catalysts for CO_(2)hydrogenation to methanol.
文摘Pitch is an excellent precursor for the production of hard carbon,with pre-oxidation crucial process in the fabrication.The structural changes in the different molecular components of pitch during thermochemical treatment are a key factor in determining the sodium-ion storage of pitchbased hard carbon anodes.We investigated the effects of the different molecular structures in the asphaltene precursor,including aromatic rings and aliphatic chains,on the sodiumion storage behavior of the resulting carbon.We found that polar oxygen functional groups limit the steric hindrance caused by the aromatic rings in pitch,and thus facilitate the introduction of cross-linked structures.During high-temperature carbonization,aromatic rings form a rigid carbon framework that prevents the rearrangement of ordered carbon layers,leading to a short-range disordered carbon structure and promotes the production of closed pores.For example,a material prepared from asphaltene,which contains a large number of oxygen-containing functional groups and macromolecular aromatic rings,using pre-oxidation at 300℃ and carbonization at 1200℃ had a reversible capacity of 316.7 mAh g^(−1) when used as the anode for sodium ion batteries.Our research provides a theoretical basis for the selection of raw materials for the development of high-quality pitch-based hard carbons.
基金Supported by Innovative Research Groups of the National Natural Science Foundation of China(22021004)。
文摘Catalytic decomposition of methane,which produces high-purity hydrogen and high-value-added carbon nanomaterials,has shown considerable potential for development and is expected to yield significant economic benefits in the future.However,designing catalysts that simultaneously exhibit high activity and long-term stability remains a significant challenge.Tuning the catalyst’s structure and electronic properties is an effective strategy for enhancing the reaction performance.In this work,a series of NixZr/ZSM-5 catalysts were prepared using the incipient wetness impregnation method,and the effect of Zr loadings on catalyst properties and performance was systematically investigated.The calcined and reduced catalysts were characterized by low-temperature N_(2)adsorption-desorption,XRD,SEM,H_(2)-TPR and XPS.The results showed that the addition of Zr significantly increased the specific surface area of the catalyst and reduced the metal particle size.Smaller NiO particles were found to enter the pores of the HZSM-5 support,and electronic interactions between NiO and ZrO_(2)markedly enhanced the metal-support interaction.The catalyst exhibited optimal catalytic performance at a Zr loading of 5%,achieving a maximum methane conversion of 68%at 625℃,maintaining activity for 900 min,and delivering a carbon yield of 1927%.Further increasing the Zr loading yielded only limited improvements in catalytic performance.Characterization of the spent catalysts and carbon products via TEM,Raman spectroscopy,and TGA revealed that the introduction of ZrO_(2)reduced metal sintering and promoted a shift in carbon nanofibers growth mode from tip-growth to base-growth.The mechanism of base-growth enabled the catalyst to maintain reaction activity for an extended period.
基金supported by the National Key R&D Program of China(No.2022YFE0208300)the National Natural Science Foundation of China(No.22278426)+2 种基金the China National Funds for Distinguished Young Scientists(No.22425808)the China Postdoctoral Science Foundation(No.2025M771155)the Science Foundation of China University of Petroleum,Beijing(Nos.2462024XKBH001,2462022YJRC003,2462022YJRC002,2462025BJRC002)。
文摘Electrochemical liquid lithium extraction technology has attracted much attention because of its high selectivity,good efficiency,and eco-friendliness.However,the low energy density per unit area and poor stability of traditional thin film electrodes(F-LMO),as well as manganese dissolution loss induced by the Jahn-Teller distortion of LiMn_(2)O_(4),hinder their industrial scalability.Herein,a durable and high-efficiency multistage porous LiMn_(2)O_(4) thick electrode was prepared sustainably by 3D printing technology(3DPLMO)for enhancing lithium recovery from salt lake brine.The multistage porous structure reduced the mass transfer resistance and shortened the ion diffusion path,which was conducive to accelerating the diffusion rate of Li+.Simultaneously,the three-dimensional conductive networks composed of reduced graphene oxide(r GO)and carbon nanotubes(CNT)synergized with the multistage pores effectively weakened the polarization phenomenon of the electrode and improved the stability of 3DP-LMO.The3DP-LMO exhibited a 5.5-fold higher extraction capacity per unit area and the Mn dissolution loss rate was only 1/15 compared with the F-LMO.Notably,the capacity retention rate of 3DP-LMO was 87.6%,significantly better than that of F-LMO(66.3%).Based on the quasi-in situ X-ray Diffraction results,the mechanism of lithium intercalation and deintercalation in 3DP-LMO was elucidated.Furthermore,lithium extraction parameters were optimized using response surface method-center composite design(RSM-CCD),resulting in an increase in lithium extraction capacity to 15.66 mg g^(-1)and a reduction in energy consumption to only 12.33 Wh mol^(-1).The results show that 3DP-LMO has significantly improved lithium extraction performance and stability,and has considerable prospects in practical application.
基金supported by the National Natural Science Foundation of China (Nos.22177133,22278438)。
文摘Rational design of nanozymes with enhanced catalytic efficiency remains a central challenge in the development of artificial enzymes.Herein,we report the construction of ultrasmall gold nanoclusterbased nanoassemblies(Dp-Au NCs@Fe^(2+)) through the coordination of Fe^(2+) ions by a dopa-containing peptidomimetic ligand(Dp CDp).This nanoarchitecture simultaneously integrates catalytically active gold cores and redox-active Fe^(2+)centers,bridged by Dp CDp to facilitate directional electron transfer.Comprehensive spectroscopic and kinetic analyses reveal that Dp CDp promotes efficient charge migration from the Au core to surface-bound Fe^(2+),significantly enhancing H_(2)O_(2)-mediated peroxidase-like activity.Compared to bare Dp-Au NCs,Dp-Au NCs@Fe^(2+) display a 4.3-fold improvement in detection sensitivity,a 6.7-fold increase in catalytic efficiency,and markedly stronger hydroxyl radical generation.Mechanistically,this activity stems from a synergistic triad:direct H_(2)O_(2) oxidation at gold surfaces,radical generation at Fe^(2+) sites,and Dp CDp-facilitated electron shuttling.This work presents a robust strategy for nanozyme enhancement via electronic and structural co-engineering,offering valuable insights for the future design of bioinspired catalytic systems.
基金supported by the National Science Foundation of China(Nos.42177042,and 42477051)the National Key R&D Program of China(No.2023YFC3708700)the Science Foundation of China University of Petroleum-Beijing(No.2462022QNXZ006).
文摘Petroleum leakage is a major groundwater contamination source,with chemical composition of water soluble fractions(WSFs)from diverse oil sources significantly impacting groundwater quality and source identification.The aim of this study was to assess impact of 15 diverse oils on groundwater quality and environmental forensics based on oil-water equilibrium experiments.Our results indicate that contamination of groundwater by gasoline and naphtha is primarily attributed to volatile hydrocarbons,while pollution from diesel,kerosene,and crude oil is predominantly from non-hydrocarbons.Rapid determination of the extent of non-hydrocarbon pollution in WSFs was achieved through a new quantitative index.Gasoline and naphtha exhibited the highest groundwater contamination potential while kerosene and light crude oils were also likely to cause groundwater contamina-tion.Although volatile hydrocarbons in the WSFs of diesel and jet fuel do not easily exceed current regulatory standards,unregulated non-hydrocarbons may pose a more severe contamination risk to groundwater.Notably,the presence of significant benzene and toluene,hydrogenation and alkylation products(e.g.,C4-C5 alkylben-zenes,alkylindenes,alkyltetralins,and dihydro-indenes),cycloalkanes in WSFs can effectively be utilized for preliminary source identification of light distillates,middle distillates,and crude oils,respectively.
基金partially supported by the National Natural Science Foundation of China(No.22208374,22578497,22478419)the Excellent Youth Scientist Award Foundation of Shandong Province(No.ZR2024YQ009)+2 种基金the Distinguished Young Scholars of the National Natural Science Foundation of China(No.22322814)CNPC Innovation Found(2022DQ02-0607)Foundation of Hubei Key Laboratory of Processing and Application of Catalytic Materials(No.202441504)。
文摘The advancement of hydrogen-based energy systems necessitates innovative solutions for safe,efficient hydrogen storage and transportation.Liquid organic hydrogen carriers(LOHCs)emerge as a transformative technology by combining high hydrogen capacity,excellent stability,and seamless integration with existing fuel infrastructure,enabling large-scale,long-distance hydrogen logistics.Despite these merits,challenges in dehydrogenation kinetics and catalyst instability impede practical deployment.Herein,we present a comprehensive mechanistic review of dehydrogenation pathways across diverse LOHC platforms,including cyclohexane,methylcyclohexane,decalin,dodecahydro-N-ethylcarbazole,perhydro-dibenzyltoluene/benzyltoluene,bicyclohexyl,and indole-based LOHCs.Compared with previous reviews,this study integrates geometric and electronic effects across multiple LOHC systems to identify cross-cutting structure-activity principles.Building on this framework,it further reveals reactant-dependent rules for active-site regulation,where the molecular architecture of hydrogen carriers critically determines the required catalyst characteristics.This perspective establishes a unified framework that links molecular descriptors to coordination-specific active sites,thereby advancing precision catalyst design for next-generation LOHC technologies.
基金supported in part by the National Key R&D Program of China(No.2024YFA1610700)the National Natural Science Foundation of China(No.12475147)。
文摘The Cooling-Storage-Ring External-target Experiment(CEE)at the Heavy Ion Research Facility in Lanzhou(HIRFL)is designed to study the properties of nuclear matter created in heavy-ion collisions at beam energies from a few hundred MeV/u up to 1 GeV/u.It aims to facilitate research on the quantum chromodynamics(QCD)phase structure in the high-baryondensity region.Collective flow is a fundamental observable in heavy-ion collision experiments,providing information on the bulk properties of the produced matter.Although the standard event plane method has been widely used to measure collective flow,it is still important to validate and optimize this method for the CEE spectrometer.In this paper,we study the experimental procedures for measuring directed flow in^(238)U+^(238)U collisions at 500 MeV/u,using event planes reconstructed by Multi-Wire Drift Chamber and Zero Degree Calorimeter,respectively.Jet AA Microscopic(JAM)transport generator is used to generate events,and the detector response is simulated by the CEE Fast Simulation(CFS)package.Finally,the optimal kinematic region for proton directed flow measurements is discussed for the future CEE experiment.
基金supported by the National Natural Science Foundation of China(Nos.12275321,12121005,12475129,and 12335009)the Natural Science Foundation of Guangdong Province,China(No.2025A1515012112)+6 种基金the International Atomic Energy Agency Coordinated Research Project F41034(No.28649)the computational resources from Sun Yat-sen University the National Supercomputer Center in Guangzhouthe Open Project of Guangxi Key Laboratory of Nuclear Physics and Nuclear Technology(No.NLK2023-08)the Central Government Guidance Funds for Local Scientific and Technological Development,China(No.Guike ZY22096024)the Guangdong Major Project of Basic and Applied Basic Research(No.2021B0301030006)Young Scientists Fund of the National Natural Science Foundation of China(No.12405144)the National Key Research and Development Program(MOST 2022YFA1602304).
文摘A new multi-detector array named HALIMA(Hybrid Array for LIfetime MeAsurement)has been developed at Lanzhou for nuclear structure studies in fission.The array comprises eight BGO-shielded High-Purity Germanium detectors and twenty fast Ce-doped Lanthanum Bromide[LaBr_(3)(Ce)]detectors shielded with CsI(Tl).HALIMA is further complemented by two ancillary detector systems:fission fragment(FF)detectors and β detectors.This configuration enables precise sub-nanosecond lifetime measurements using the fourfold FF/β-Ge-LaBr_(3)(Ce)-LaBr_(3)(Ce)coincidence technique.The performance and specifications of the detectors,associated electronics,and the data acquisition system are presented in detail.The advantage of FF selectivity is emphasized,which significantly enhances sensitivity to specific fission channels.Using this approach,the lifetimes of the nuclear excited states populated in the spontaneous fission of^(252)Cf were measured,showing good agreement with the established literature values.
基金the National Nature Science Foundation of China for Excellent Young Scientists Fund(32222058)Fundamental Research Foundation of CAF(CAFYBB2022QB001).
文摘Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via low-temperature coprecipitation,exhibiting excellent performance for the selective hydrogenation of 5-hydroxymethylfurfural(HMF).A linear correlation is first observed between solvent polarity(E_(T)(30))and product selectivity within both polar aprotic and protic solvent classes,suggesting that solvent properties play a vital role in directing reaction pathways.Among these,1,4-dioxane(aprotic)favors the formation of 2,5-bis(hydroxymethyl)furan(BHMF)with 97.5%selectivity,while isopropanol(iPrOH,protic)promotes 2,5-dimethylfuran production with up to 99.5%selectivity.Mechanistic investigations further reveal that beyond polarity,proton-donating ability is critical in facilitating hydrodeoxygenation.iPrOH enables a hydrogen shuttle mechanism where protons assist in hydroxyl group removal,lowering the activation barrier.In contrast,1,4-dioxane,lacking hydrogen bond donors,stabilizes BHMF and hinders further conversion.Density functional theory calculations confirm a lower activation energy in iPrOH(0.60 eV)compared to 1,4-dioxane(1.07 eV).This work offers mechanistic insights and a practical strategy for solvent-mediated control of product selectivity in biomass hydrogenation,highlighting the decisive role of solvent-catalyst-substrate interactions.
