Hydrogen energy is expected to be an“ideal fuel”in the era of decarbonization.The discovery,de-velopment,and modification of high-performance hydrogen storage materials are the keys to the fu-ture development of sol...Hydrogen energy is expected to be an“ideal fuel”in the era of decarbonization.The discovery,de-velopment,and modification of high-performance hydrogen storage materials are the keys to the fu-ture development of solid-state hydrogen storage and hydrogen energy utilization.Magnesium hydride(MgH_(2)),with its high hydrogen storage capacity,abundant natural reserves,and environmental friend-liness,has been extensively researched.Herein,we briefly summarize the typical structure and hy-drogenation/dehydrogenation reaction mechanism of MgH_(2)and provide a comprehensive overview of strategies to effectively tune the thermodynamics and kinetics of Mg-based materials,such as alloy-ing,nanosizing,the introduction of additives,and composite modification.With substantial efforts,great achievements have been achieved,such as lower absorption/desorption temperatures and better cy-cling stability.Nonetheless,some pivotal issues remain to be addressed,such as unfavorable hydro-genation/dehydrogenation factors,harsh conditions,slow kinetics,incomplete dehydrogenation,low hy-drogen purity,expensive catalysts,and a lack of valid exploration of mechanisms in the hydrogena-tion/dehydrogenation process.Lastly,some future development prospects of MgH_(2)in energy-efficient conversion and storage have been presented,including advanced manufacturing ways,stabilization of nanostructures,the introduction of additives combined with structural modification,and utilization of advanced characterization techniques.展开更多
Bulk Mg-based hydrogen storage materials have the potential to provide a low-cost solution to diversify energy storage and transportation.Compared to nano powders which require handling and processing under hydrogen o...Bulk Mg-based hydrogen storage materials have the potential to provide a low-cost solution to diversify energy storage and transportation.Compared to nano powders which require handling and processing under hydrogen or an inert gas atmosphere,bulk Mg-based alloys are safer and are more oxidation re-sistant.Conventional methods and existing infrastructures can be used to process and handle these ma-terials.However,bulk Mg alloys have smaller specific surface areas,resulting in slower hydrogen sorp-tion kinetics,higher equilibrium temperatures,and enthalpies of hydride formation.This work reviews the effects of the additions of a list of alloying elements and the use of innovative processing meth-ods,e.g.,rapid solidification and severe plastic deformation processes,to overcome these drawbacks.The challenges,advantages,and weaknesses of each method and future perspectives for the development of Mg-based hydrogen storage materials are discussed.展开更多
The flame propagation processes of MgH_(2)dust clouds with four different particle sizes were recorded by a high-speed camera.The dynamic flame temperature distributions of MgH_(2)dust clouds were reconstructed by the...The flame propagation processes of MgH_(2)dust clouds with four different particle sizes were recorded by a high-speed camera.The dynamic flame temperature distributions of MgH_(2)dust clouds were reconstructed by the two-color pyrometer technique,and the chemical composition of solid combustion residues were analyzed.The experimental results showed that the average flame propagation velocities of 23μm,40μm,60μm and 103μm MgH_(2)dust clouds in the stable propagation stage were 3.7 m/s,2.8 m/s,2.1 m/s and 0.9 m/s,respectively.The dust clouds with smaller particle sizes had faster flame propagation velocity and stronger oscillation intensity,and their flame temperature distributions were more even and the temperature gradients were smaller.The flame structures of MgH_(2)dust clouds were significantly affected by the particle sinking velocity,and the combustion processes were accompanied by micro-explosion of particles.The falling velocities of 23μm and 40μm MgH_(2)particles were 2.24 cm/s and 6.71 cm/s,respectively.While the falling velocities of 60μm and 103μm MgH_(2)particles were as high as 15.07 cm/s and 44.42 cm/s,respectively,leading to a more rapid downward development and irregular shape of the flame.Furthermore,the dehydrogenation reaction had a significant effect on the combustion performance of MgH_(2)dust.The combustion of H_(2)enhanced the ignition and combustion characteristics of MgH_(2)dust,resulting in a much higher explosion power than the pure Mg dust.The micro-structure characteristics and combustion residues composition analysis of MgH_(2)dust indicated that the combustion control mechanism of MgH_(2)dust flame was mainly the heterogeneous reaction,which was affected by the dehydrogenation reaction.展开更多
The application of Mg-based electrochemical energy storage materials in high performance supercapacitors is an essential step to promote the exploitation and utilization of magnesium resources in the field of energy s...The application of Mg-based electrochemical energy storage materials in high performance supercapacitors is an essential step to promote the exploitation and utilization of magnesium resources in the field of energy storage.Unfortunately,the inherent chemical properties of magnesium lead to poor cycling stability and electrochemical reactivity,which seriously limit the application of Mg-based materials in supercapacitors.Herein,in this review,more than 70 research papers published in recent 10 years were collected and analyzed.Some representative research works were selected,and the results of various regulative strategies to improve the electrochemical performance of Mg-based materials were discussed.The effects of various regulative strategies(such as constructing nanostructures,synthesizing composites,defect engineering,and binder-free synthesis,etc.)on the electrochemical performance and their mechanism are demonstrated using spinelstructured MgX_(2)O_(4) and layered structured Mg-X-LDHs as examples.In addition,the application of magnesium oxide and magnesium hydroxide in electrode materials,MXene's solid spacers and hard templates are introduced.Finally,the challenges and outlooks of Mg-based electrochemical energy storage materials in high performance supercapacitors are also discussed.展开更多
Following the recent report by Dasenbrock-Gammon et al.[Nature 615,244–250(2023)]of near-ambient superconductivity in nitrogendoped lutetium trihydride(LuH_(3-δ)N_(ε)),significant debate has emerged surrounding the...Following the recent report by Dasenbrock-Gammon et al.[Nature 615,244–250(2023)]of near-ambient superconductivity in nitrogendoped lutetium trihydride(LuH_(3-δ)N_(ε)),significant debate has emerged surrounding the composition and interpretation of the observed sharp resistance drop.Here,we meticulously revisit these claims through comprehensive characterization and investigations.We definitively identify the reported material as lutetium dihydride(LuH_(2)),resolving the ambiguity surrounding its composition.Under similar conditions(270–295 K and 1–2 GPa),we replicate the reported sharp decrease in electrical resistance with a 30%success rate,aligning with the observations by Dasenbrock-Gammon et al.However,our extensive investigations reveal this phenomenon to be a novel pressure-induced metal-to-metal transition intrinsic to LuH_(2),distinct from superconductivity.Intriguingly,nitrogen doping exerts minimal impact on this transition.Our work not only elucidates the fundamental properties of LuH_(2)andLuH_(3),but also critically challenges the notion of superconductivity in these lutetium hydride systems.These findings pave the way for future research on lutetium hydride systems,while emphasizing the crucial importance of rigorous verification in claims of ambient-temperature superconductivity.展开更多
Mg-based amorphous alloys exhibit efficient catalytic performance and excellent biocompatibility with a promising application probability,specifically in the field of azo dye wastewater degradation.However,the problem...Mg-based amorphous alloys exhibit efficient catalytic performance and excellent biocompatibility with a promising application probability,specifically in the field of azo dye wastewater degradation.However,the problems like difficulty in preparation and poor cycling stability need to be solved.At present,Mg-based amorphous alloys applied in wastewater degradation are available in powder and ribbon.The amorphous alloy powder fabricated by ball milling has a high specific surface area,and its reactivity is thousands of times better than that of gas atomized alloy powder.But the development is limited due to the high energy consumption,difficult and costly process of powder recycling.The single roller melt-spinning method is a new manufacturing process of amorphous alloy ribbon.Compared to amorphous powder,the specific surface area of amorphous ribbon is relatively lower,therefore,it is necessary to carry out surface modification to enhance it.Dealloying is a way that can form a pore structure on the surface of the amorphous alloys,increasing the specific surface area and providing more reactive sites,which all contribute to the catalytic performance.Exploring the optimal conditions for Mg-based amorphous alloys in wastewater degradation by adjusting amorphous alloy composition,choosing suitable method to preparation and surface modification,reducing cost,expanding the pH range will advance the steps to put Mg-based amorphous alloys in industrial environments into practice.展开更多
Hydride precipitation in zirconium cladding materials can damage their integrity and durability.Service temperature and material defects have a significant effect on the dynamic growth of hydrides.In this study,we hav...Hydride precipitation in zirconium cladding materials can damage their integrity and durability.Service temperature and material defects have a significant effect on the dynamic growth of hydrides.In this study,we have developed a phasefield model based on the assumption of elastic behaviour within a specific temperature range(613 K-653 K).This model allows us to study the influence of temperature and interfacial effects on the morphology,stress,and average growth rate of zirconium hydride.The results suggest that changes in temperature and interfacial energy influence the length-to-thickness ratio and average growth rate of the hydride morphology.The ultimate determinant of hydride orientation is the loss of interfacial coherency,primarily induced by interfacial dislocation defects and quantifiable by the mismatch degree q.An escalation in interfacial coherency loss leads to a transition of hydride growth from horizontal to vertical,accompanied by the onset of redirection behaviour.Interestingly,redirection occurs at a critical mismatch level,denoted as qc,and remains unaffected by variations in temperature and interfacial energy.However,this redirection leads to an increase in the maximum stress,which may influence the direction of hydride crack propagation.This research highlights the importance of interfacial coherency and provides valuable insights into the morphology and growth kinetics of hydrides in zirconium alloys.展开更多
This study explores how the chemical interaction between magnesium hydride(MgH_(2))and the additive CrO_(3) influences the hydrogen/lithium storage characteristics of MgH_(2).We have observed that a 5 wt.%CrO_(3) addi...This study explores how the chemical interaction between magnesium hydride(MgH_(2))and the additive CrO_(3) influences the hydrogen/lithium storage characteristics of MgH_(2).We have observed that a 5 wt.%CrO_(3) additive reduces the dehydrogenation activation energy of MgH_(2) by 68 kJ/mol and lowers the required dehydrogenation temperature by 80℃.CrO_(3) added MgH_(2) was also tested as an anode in an Li ion battery,and it is possible to deliver over 90%of the total theoretical capacity(2038 mAh/g).Evidence for improved reversibility in the battery reaction is found only after the incorporation of additives with MgH_(2).In depth characterization study by X-ray diffraction(XRD)technique provides convincing evidence that the CrO_(3) additive interacts with MgH_(2) and produces Cr/MgO byproducts.Gibbs free energy analyses confirm the thermodynamic feasibility of conversion from MgH_(2)/CrO_(3) to MgO/Cr,which is well supported by the identification of Cr(0)in the powder by X ray photoelectron spectroscopy(XPS)technique.Through high resolution transmission electron microscopy(HRTEM)and energy dispersive spectroscopy(EDS)we found evidence for the presence of 5 nm size Cr nanocrystals on the surface of MgO rock salt nanoparticles.There is also convincing ground to consider that MgO rock salt accommodates Cr in the lattice.These observations support the argument that creation of active metal–metal dissolved rock salt oxide interface may be vital for improving the reactivity of MgH_(2),both for the improved storage of hydrogen and lithium.展开更多
Magnesium(Mg)is a widely used and attractive metal,known for its unique physical and chemical properties,and it has been employed in the manufacture of many practical materials.Layered Double Hydroxides(LDHs),particul...Magnesium(Mg)is a widely used and attractive metal,known for its unique physical and chemical properties,and it has been employed in the manufacture of many practical materials.Layered Double Hydroxides(LDHs),particularly Mg-based LDHs,rank among the most prevalent two-dimensional materials utilized in separation processes,which include adsorption,extraction,and membrane technology.The high popularity of Mg-based LDHs in separation applications can be attributed to their properties,such as excellent hydrophilicity,high surface area,ion exchangeability,and adjustable interlayer space.Currently,polymer membranes play a pivotal role in semi-industrial and industrial separation processes.Consequently,the development of polymer membranes and the mitigation of their limitations have emerged as compelling topics for researchers.Several methods exist to enhance the separation performance and anti-fouling properties of polymer membranes.Among these,incorporating additives into the membrane polymer matrix stands out as a cost-effective,straightforward,readily available,and efficient approach.The use of Mg-based LDHs,either in combination with other materials or as a standalone additive in the polymer membrane matrix,represents a promising strategy to bolster the separation and anti-fouling efficacy of flat sheet mixed matrix polymer membranes.This review highlights Mg-based LDHs as high-potential additives designed to refine flat sheet mixed matrix polymer membranes for applications in wastewater treatment and brackish water desalination.展开更多
Zirconium hydride(ZrH_(2)) is an ideal neutron moderator material. However, radiation effect significantly changes its properties, which affect its behavior and the lifespan of the reactor. The threshold energy of dis...Zirconium hydride(ZrH_(2)) is an ideal neutron moderator material. However, radiation effect significantly changes its properties, which affect its behavior and the lifespan of the reactor. The threshold energy of displacement is an important quantity of the number of radiation defects produced, which helps us to predict the evolution of radiation defects in ZrH_(2).Molecular dynamics(MD) and ab initio molecular dynamics(AIMD) are two main methods of calculating the threshold energy of displacement. The MD simulations with empirical potentials often cannot accurately depict the transitional states that lattice atoms must surpass to reach an interstitial state. Additionally, the AIMD method is unable to perform largescale calculation, which poses a computational challenge beyond the simulation range of density functional theory. Machine learning potentials are renowned for their high accuracy and efficiency, making them an increasingly preferred choice for molecular dynamics simulations. In this work, we develop an accurate potential energy model for the ZrH_(2) system by using the deep-potential(DP) method. The DP model has a high degree of agreement with first-principles calculations for the typical defect energy and mechanical properties of the ZrH_(2) system, including the basic bulk properties, formation energy of point defects, as well as diffusion behavior of hydrogen and zirconium. By integrating the DP model with Ziegler–Biersack–Littmark(ZBL) potential, we can predict the threshold energy of displacement of zirconium and hydrogen in ε-ZrH_(2).展开更多
Although Mg-based hydrides are extensively considered as a prospective material for solid-state hydrogen storage and clean energy carriers,their high operating temperature and slow kinetics are the main challenges for...Although Mg-based hydrides are extensively considered as a prospective material for solid-state hydrogen storage and clean energy carriers,their high operating temperature and slow kinetics are the main challenges for practical application.Here,a Mg-Ni based hydride,Mg_(2)NiH_(4) nanoparticles(~100 nm),with dual modification strategies of nanosizing and alloying is successfully prepared via a gas-solid preparation process.It is demonstrated that Mg_(2)NiH_(4) nanoparticles form a unique chain-like structure by oriented stacking and exhibit impressive hydrogen storage performance:it starts to release H2 at~170℃ and completes below 230℃ with a saturated capacity of 3.32 wt%and desorbs 3.14 wt% H_(2) within 1800 s at 200℃.The systematic characterizations of Mg_(2)NiH_(4) nanoparticles at different states reveal the dehydrogenation behavior and demonstrate the excellent structural and hydrogen storage stabilities during the de/hydrogenated process.This research is believed to provide new insights for optimizing the kinetic performance of metal hydrides and novel perspectives for designing highly active and stable hydrogen storage alloys.展开更多
Hydrogen energy has emerged as a pivotal solution to address the global energy crisis and pave the way for a cleaner,low-carbon,secure,and efficient modern energy system.A key imperative in the utilization of hydrogen...Hydrogen energy has emerged as a pivotal solution to address the global energy crisis and pave the way for a cleaner,low-carbon,secure,and efficient modern energy system.A key imperative in the utilization of hydrogen energy lies in the development of high-performance hydrogen storage materials.Magnesium-based hydrogen storage materials exhibit remarkable advantages,including high hydrogen storage density,cost-effectiveness,and abundant magnesium resources,making them highly promising for the hydrogen energy sector.Nonetheless,practical applications of magnesium hydride for hydrogen storage face significant challenges,primarily due to their slow kinetics and stable thermodynamic properties.Herein,we briefly summarize the thermodynamic and kinetic properties of MgH2,encompassing strategies such as alloying,nanoscaling,catalyst doping,and composite system construction to enhance its hydrogen storage performance.Notably,nanoscaling and catalyst doping have emerged as more effective modification strategies.The discussion focuses on the thermodynamic changes induced by nanoscaling and the kinetic enhancements resulting from catalyst doping.Particular emphasis lies in the synergistic improvement strategy of incorporating nanocatalysts with confinement materials,and we revisit typical works on the multi-strategy optimization of MgH2.In conclusion,we conduct an analysis of outstanding challenges and issues,followed by presenting future research and development prospects for MgH2 as hydrogen storage materials.展开更多
We report experimental discovery of tantalum polyhydride superconductor.It was synthesized under highpressure and high-temperature conditions using diamond anvil cell combined with in situ high-pressure laser heating ...We report experimental discovery of tantalum polyhydride superconductor.It was synthesized under highpressure and high-temperature conditions using diamond anvil cell combined with in situ high-pressure laser heating techniques.The superconductivity was investigated via resistance measurements at pressures.The highest superconducting transition temperature T_(c)was found to be~30 K at 197 GPa in the sample that was synthesized at the same pressure with~2000 K heating.The transitions are shifted to low temperature upon applying magnetic fields that support the superconductivity nature.The upper critical field at zero temperatureμ_0H_(c2)(0)of the superconducting phase is estimated to be~20 T that corresponds to Ginzburg-Landau coherent length~40 A.Our results suggest that the superconductivity may arise from 143d phase of TaH_(3).It is,for the first time to our best knowledge,experimental realization of superconducting hydrides for the VB group of transition metals.展开更多
With the depletion of fossil fuels and global warming,there is an urgent demand to seek green,low-cost,and high-efficiency energy resources.Hydrogen has been considered as a potential candidate to replace fossil fuels...With the depletion of fossil fuels and global warming,there is an urgent demand to seek green,low-cost,and high-efficiency energy resources.Hydrogen has been considered as a potential candidate to replace fossil fuels,due to its high gravimetric energy density(142 MJ kg^(-1)),high abundance(H_(2)O),and environmentalfriendliness.However,due to its low volume density,effective and safe hydrogen storage techniques are now becoming the bottleneck for the"hydrogen economy".Under such a circumstance,Mg-based hydrogen storage materials garnered tremendous interests due to their high hydrogen storage capacity(~7.6 wt%for MgH_(2)),low cost,and excellent reversibility.However,the high thermodynamic stability(ΔH=-74.7 kJ mol^(-1)H_(2))and sluggish kinetics result in a relatively high desorption temperature(>300℃),which severely restricts widespread applications of MgH_(2).Nano-structuring has been proven to be an effective strategy that can simultaneously enhance the ab/de-sorption thermodynamic and kinetic properties of MgH_(2),possibly meeting the demand for rapid hydrogen desorption,economic viability,and effective thermal management in practical applications.Herein,the fundamental theories,recent advances,and practical applications of the nanostructured Mg-based hydrogen storage materials are discussed.The synthetic strategies are classified into four categories:free-standing nano-sized Mg/MgH_(2)through electrochemical/vapor-transport/ultrasonic methods,nanostructured Mg-based composites via mechanical milling methods,construction of core-shell nano-structured Mg-based composites by chemical reduction approaches,and multi-dimensional nano-sized Mg-based heterostructure by nanoconfinement strategy.Through applying these strategies,near room temperature ab/de-sorption(<100℃)with considerable high capacity(>6 wt%)has been achieved in nano Mg/MgH_(2)systems.Some perspectives on the future research and development of nanostructured hydrogen storage materials are also provided.展开更多
The lutetium dihydride LuH2is stable at ambient conditions.Here we show that its color undergoes sequential changes from dark blue at ambient pressure to pink at ~2.2 GPa and then to bright red at ~4 GPa upon compress...The lutetium dihydride LuH2is stable at ambient conditions.Here we show that its color undergoes sequential changes from dark blue at ambient pressure to pink at ~2.2 GPa and then to bright red at ~4 GPa upon compression in a diamond anvil cell.Such a pressure-induced color change in LuH2is reversible and it is very similar to that recently reported in the N-doped lutetium hydride [Nature 615,244(2023)].However,our preliminary resistance measurements on LuH2under pressures up to ~7 GPa evidenced no superconductivity down to 1.5 K.展开更多
Aiming to elucidate the hydrogen absorption/desorption cycling properties of Mg-based alloys with in-situ formed Mg_(2)Ni and LaH_(x)(x=2,3)nanocrystallines,the hydrogen storage cycle stability,hydriding/dehydriding c...Aiming to elucidate the hydrogen absorption/desorption cycling properties of Mg-based alloys with in-situ formed Mg_(2)Ni and LaH_(x)(x=2,3)nanocrystallines,the hydrogen storage cycle stability,hydriding/dehydriding cycling kinetics and thermodynamic stability of the experimental alloys have been investigated in detail.The results show that the Mg-Ni-La alloys exhibit improved hydrogen storage cycling properties and can remain storage hydrogen above 5.5 wt%after 200 cycles.With the increase of cycling numbers,the dehydrogenation rates of the experimental samples increase firstly and then gradually decrease,and eventually maintain relative stable state.Microstructure observation reveals that powders sintering and hydrogen decrepitation both exist during hydrogen absorption/desorption cycles due to repeated volume expansion and contraction.Meanwhile,the in-situ formed LaH_(x)(x=2,3)and Mg_(2)Ni nanocrystallines stabilize the microstructures of the particles and hinder the powders sintering.After 200 cycles,the average particle size of the experimental samples decreases and the specific surface area apparently increases,which leads to the decomposition temperatures of MgH_(2)and Mg_(2)NiH_(4)slightly shift to lower temperatures.Moreover,Mg_(2)Ni and LaH_(x)(x=2,3)have been proven to be stable catalysts during long-term cycling,which can still uniformly distribute within the powders after 200 cycles.展开更多
Biodegradable magnesium(Mg) and its alloy show huge potential as temporary bone substitute due to the favorable biocompatibility and mechanical compatibility. However, one issue deserves attention is the too fast degr...Biodegradable magnesium(Mg) and its alloy show huge potential as temporary bone substitute due to the favorable biocompatibility and mechanical compatibility. However, one issue deserves attention is the too fast degradation. In this work, mesoporous bioglass(MBG)with high pore volume(0.59 cc/g) and huge specific surface area(110.78 m^(2)/g) was synthesized using improved sol-gel method, and introduced into Mg-based composite via laser additive manufacturing. Immersion tests showed that the incorporated MBG served as powerful adsorption sites, which promoted the in-situ deposition of apatite by successively adsorbing Ca2+and HPO42-. Such dense apatite film acted as an efficient protection layer and enhanced the corrosion resistance of Mg matrix, which was proved by the electrochemical impedance spectroscopy measurements. Thereby, Mg based composite showed a significantly decreased degradation rate of 0.31 mm/year. Furthermore,MBG also improved the mechanical properties as well as cell behavior. This work highlighted the advantages of MBG in the fabrication of Mg-based implant with enhanced overall performance for orthopedic application.展开更多
The catalytic effect of FeCoNiCrMo high entropy alloy nanosheets on the hydrogen storage performance of magnesium hydride(MgH_(2))was investigated for the first time in this paper.Experimental results demonstrated tha...The catalytic effect of FeCoNiCrMo high entropy alloy nanosheets on the hydrogen storage performance of magnesium hydride(MgH_(2))was investigated for the first time in this paper.Experimental results demonstrated that 9wt%FeCoNiCrMo doped MgH_(2)started to dehydrogenate at 200℃and discharged up to 5.89wt%hydrogen within 60 min at 325℃.The fully dehydrogenated composite could absorb3.23wt%hydrogen in 50 min at a temperature as low as 100℃.The calculated de/hydrogenation activation energy values decreased by44.21%/55.22%compared with MgH_(2),respectively.Moreover,the composite’s hydrogen capacity dropped only 0.28wt%after 20 cycles,demonstrating remarkable cycling stability.The microstructure analysis verified that the five elements,Fe,Co,Ni,Cr,and Mo,remained stable in the form of high entropy alloy during the cycling process,and synergistically serving as a catalytic union to boost the de/hydrogenation reactions of MgH_(2).Besides,the FeCoNiCrMo nanosheets had close contact with MgH_(2),providing numerous non-homogeneous activation sites and diffusion channels for the rapid transfer of hydrogen,thus obtaining a superior catalytic effect.展开更多
Mg-based materials are one of the most promising hydrogen storage candidates due to their high hydrogen storage capacity,environmental benignity,and high Clarke number characteristics.However,the limited thermodynamic...Mg-based materials are one of the most promising hydrogen storage candidates due to their high hydrogen storage capacity,environmental benignity,and high Clarke number characteristics.However,the limited thermodynamics and kinetic properties pose major challenges for their engineering applications.Herein,we review the recent progress in improving their thermodynamics and kinetics,with an emphasis on the models and the influence of various parameters in the calculated models.Subsequently,the impact of alloying,composite,and nanocrystallization on both thermodynamics and dynamics are discussed in detail.In particular,the correlation between various modification strategies and the hydrogen capacity,dehydrogenation enthalpy and temperature,hydriding/dehydriding rates are summarized.In addition,the mechanism of hydrogen storage processes of Mg-based materials is discussed from the aspect of classical kinetic theories and microscope hydrogen transferring behavior.This review concludes with an outlook on the remaining challenge issues and prospects.展开更多
Recently,near-ambient superconductivity was claimed in nitrogen-doped lutetium hydride(LuH_(3-δ)N_(ε)).Unfortunately,all follow-up research still cannot find superconductivity signs in successfully synthesized lutet...Recently,near-ambient superconductivity was claimed in nitrogen-doped lutetium hydride(LuH_(3-δ)N_(ε)).Unfortunately,all follow-up research still cannot find superconductivity signs in successfully synthesized lutetium dihydride(LuH_(2)) and N-doped LuH_(2±x)N_(y).However,a similar intriguing observation was the pressure-induced color changes(from blue to pink and subsequent red).The physical understanding of its origin and the correlation between the color,crystal structure,and chemical composition of Lu–H–N is still lacking.In this work,we systematically investigated the optical properties of LuH_(2) and LuH_(3),and the effects of hydrogen vacancies and nitrogen doping using the first-principles calculations by considering both interband and intraband contributions.Our results demonstrate that the evolution of reflectivity peaks near blue and red light,which is driven by changes in the band gap and Fermi velocity of free electrons,resulting in the blue-to-red color change under pressure.In contrast,LuH_(3) exhibits gray and no color change up to 50 GPa.Furthermore,we investigated the effects of hydrogen vacancies and nitrogen doping on its optical properties.Hydrogen vacancies can significantly decrease the pressure of blue-to-red color change in LuH_(2) but do not have a noticeable effect on the color of LuH_(3).The N-doped LuH_(2) with the substitution of a hydrogen atom at the tetrahedral position maintains the color change when the N-doping concentration is low.As the doping level increases,this trend becomes less obvious,while other N-doped structures do not show a blue-to-red color change.Our results can clarify the origin of the experimental observed blue-to-red color change in lutetium hydride and also provide a further understanding of the potential N-doped lutetium dihydride.展开更多
基金supported by the National Natu-ral Science Foundation of China(Nos.U20A20237,51863005,52271205,51871065,51971068,and 52101245)the Scientific Research and Technology Development Program of Guangxi(Nos.AA19182014,AD17195073,AA17202030-1,AB21220027,and 2021AB17045)+2 种基金National Natural Science Foundation of Guangxi Province(Nos.2021GXNSFBA075057,2018GXNSFDA281051,2014GXNSFAA118401,and 2013GXNSFBA019244)the Scientific Research and Technology Development Program of Guilin(Nos.20210102-4 and 20210216-1)Guangxi Bagui Scholar Founda-tion,Guilin Lijiang Scholar Foundation,Guangxi Collaborative Innovation centre of Structure and Property for New Energy and Materials,Guangxi Advanced Functional Materials Foundation and Application Talents Small Highlands,Chinesisch-Deutsche Kooperationsgruppe(No.GZ1528).
文摘Hydrogen energy is expected to be an“ideal fuel”in the era of decarbonization.The discovery,de-velopment,and modification of high-performance hydrogen storage materials are the keys to the fu-ture development of solid-state hydrogen storage and hydrogen energy utilization.Magnesium hydride(MgH_(2)),with its high hydrogen storage capacity,abundant natural reserves,and environmental friend-liness,has been extensively researched.Herein,we briefly summarize the typical structure and hy-drogenation/dehydrogenation reaction mechanism of MgH_(2)and provide a comprehensive overview of strategies to effectively tune the thermodynamics and kinetics of Mg-based materials,such as alloy-ing,nanosizing,the introduction of additives,and composite modification.With substantial efforts,great achievements have been achieved,such as lower absorption/desorption temperatures and better cy-cling stability.Nonetheless,some pivotal issues remain to be addressed,such as unfavorable hydro-genation/dehydrogenation factors,harsh conditions,slow kinetics,incomplete dehydrogenation,low hy-drogen purity,expensive catalysts,and a lack of valid exploration of mechanisms in the hydrogena-tion/dehydrogenation process.Lastly,some future development prospects of MgH_(2)in energy-efficient conversion and storage have been presented,including advanced manufacturing ways,stabilization of nanostructures,the introduction of additives combined with structural modification,and utilization of advanced characterization techniques.
基金supported by the Australian Research Council (No.LP160100690)a Japan Society for the Promotion of Science (JSPS)Postdoctoral Fellowship for Research in Japan (Standard) (No.P22739)supported by an Aus-tralian Government Research Training Program (RTP)Scholarship.
文摘Bulk Mg-based hydrogen storage materials have the potential to provide a low-cost solution to diversify energy storage and transportation.Compared to nano powders which require handling and processing under hydrogen or an inert gas atmosphere,bulk Mg-based alloys are safer and are more oxidation re-sistant.Conventional methods and existing infrastructures can be used to process and handle these ma-terials.However,bulk Mg alloys have smaller specific surface areas,resulting in slower hydrogen sorp-tion kinetics,higher equilibrium temperatures,and enthalpies of hydride formation.This work reviews the effects of the additions of a list of alloying elements and the use of innovative processing meth-ods,e.g.,rapid solidification and severe plastic deformation processes,to overcome these drawbacks.The challenges,advantages,and weaknesses of each method and future perspectives for the development of Mg-based hydrogen storage materials are discussed.
基金supported by the National Natural Science Foundation of China(Grant Nos.12272001,11972046)the Outstanding Youth Project of Natural Science Foundation of Anhui Province(Grant No.2108085Y02)the Major Project of Anhui University Natural Science Foundation(Grant No.KJ2020ZD30)。
文摘The flame propagation processes of MgH_(2)dust clouds with four different particle sizes were recorded by a high-speed camera.The dynamic flame temperature distributions of MgH_(2)dust clouds were reconstructed by the two-color pyrometer technique,and the chemical composition of solid combustion residues were analyzed.The experimental results showed that the average flame propagation velocities of 23μm,40μm,60μm and 103μm MgH_(2)dust clouds in the stable propagation stage were 3.7 m/s,2.8 m/s,2.1 m/s and 0.9 m/s,respectively.The dust clouds with smaller particle sizes had faster flame propagation velocity and stronger oscillation intensity,and their flame temperature distributions were more even and the temperature gradients were smaller.The flame structures of MgH_(2)dust clouds were significantly affected by the particle sinking velocity,and the combustion processes were accompanied by micro-explosion of particles.The falling velocities of 23μm and 40μm MgH_(2)particles were 2.24 cm/s and 6.71 cm/s,respectively.While the falling velocities of 60μm and 103μm MgH_(2)particles were as high as 15.07 cm/s and 44.42 cm/s,respectively,leading to a more rapid downward development and irregular shape of the flame.Furthermore,the dehydrogenation reaction had a significant effect on the combustion performance of MgH_(2)dust.The combustion of H_(2)enhanced the ignition and combustion characteristics of MgH_(2)dust,resulting in a much higher explosion power than the pure Mg dust.The micro-structure characteristics and combustion residues composition analysis of MgH_(2)dust indicated that the combustion control mechanism of MgH_(2)dust flame was mainly the heterogeneous reaction,which was affected by the dehydrogenation reaction.
基金financial support provided by Projects(no.2020CDJXZ001)the Fundamental Research Funds for the Central Universities+1 种基金the Technology Innovation and Application Development Special Project of Chongqing(Z20211350 and Z20211351)Scientific Research Project of Chongqing Ecological Environment Bureau(no.CQEE2022-STHBZZ118)。
文摘The application of Mg-based electrochemical energy storage materials in high performance supercapacitors is an essential step to promote the exploitation and utilization of magnesium resources in the field of energy storage.Unfortunately,the inherent chemical properties of magnesium lead to poor cycling stability and electrochemical reactivity,which seriously limit the application of Mg-based materials in supercapacitors.Herein,in this review,more than 70 research papers published in recent 10 years were collected and analyzed.Some representative research works were selected,and the results of various regulative strategies to improve the electrochemical performance of Mg-based materials were discussed.The effects of various regulative strategies(such as constructing nanostructures,synthesizing composites,defect engineering,and binder-free synthesis,etc.)on the electrochemical performance and their mechanism are demonstrated using spinelstructured MgX_(2)O_(4) and layered structured Mg-X-LDHs as examples.In addition,the application of magnesium oxide and magnesium hydroxide in electrode materials,MXene's solid spacers and hard templates are introduced.Finally,the challenges and outlooks of Mg-based electrochemical energy storage materials in high performance supercapacitors are also discussed.
基金the National Key Research and Development Program of China(Grant Nos.2022YFA1402301 and 2018YFA0305703)the National Natural Science Foundation of China(Grant No.U2230401)+2 种基金the National Key R&D Program of China(Grant No.2021YFA1400200),the National Natural Science Foundation of China(Grant Nos.12025408 and 11921004)the Strategic Priority Research Program of CAS(Grant No.XDB33000000).
文摘Following the recent report by Dasenbrock-Gammon et al.[Nature 615,244–250(2023)]of near-ambient superconductivity in nitrogendoped lutetium trihydride(LuH_(3-δ)N_(ε)),significant debate has emerged surrounding the composition and interpretation of the observed sharp resistance drop.Here,we meticulously revisit these claims through comprehensive characterization and investigations.We definitively identify the reported material as lutetium dihydride(LuH_(2)),resolving the ambiguity surrounding its composition.Under similar conditions(270–295 K and 1–2 GPa),we replicate the reported sharp decrease in electrical resistance with a 30%success rate,aligning with the observations by Dasenbrock-Gammon et al.However,our extensive investigations reveal this phenomenon to be a novel pressure-induced metal-to-metal transition intrinsic to LuH_(2),distinct from superconductivity.Intriguingly,nitrogen doping exerts minimal impact on this transition.Our work not only elucidates the fundamental properties of LuH_(2)andLuH_(3),but also critically challenges the notion of superconductivity in these lutetium hydride systems.These findings pave the way for future research on lutetium hydride systems,while emphasizing the crucial importance of rigorous verification in claims of ambient-temperature superconductivity.
基金supported by the National Natural Science Foundation of China(Grant No.52071276)the Natural Science Foundation of Chongqing,China(Grant No.CSTB2022NSCQ-MSX0440)the Fundamental Research Funds for the Central Universities(Grant No.SWUXDJH202313,SWU-KQ22083).
文摘Mg-based amorphous alloys exhibit efficient catalytic performance and excellent biocompatibility with a promising application probability,specifically in the field of azo dye wastewater degradation.However,the problems like difficulty in preparation and poor cycling stability need to be solved.At present,Mg-based amorphous alloys applied in wastewater degradation are available in powder and ribbon.The amorphous alloy powder fabricated by ball milling has a high specific surface area,and its reactivity is thousands of times better than that of gas atomized alloy powder.But the development is limited due to the high energy consumption,difficult and costly process of powder recycling.The single roller melt-spinning method is a new manufacturing process of amorphous alloy ribbon.Compared to amorphous powder,the specific surface area of amorphous ribbon is relatively lower,therefore,it is necessary to carry out surface modification to enhance it.Dealloying is a way that can form a pore structure on the surface of the amorphous alloys,increasing the specific surface area and providing more reactive sites,which all contribute to the catalytic performance.Exploring the optimal conditions for Mg-based amorphous alloys in wastewater degradation by adjusting amorphous alloy composition,choosing suitable method to preparation and surface modification,reducing cost,expanding the pH range will advance the steps to put Mg-based amorphous alloys in industrial environments into practice.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.U2230401,U1930401,and 12004048)the National Key Research and Development Program of China (Grant No.2021YFB3501503)+1 种基金the Science Challenge Project (Grant No.TZ2018002)the Foundation of LCP。
文摘Hydride precipitation in zirconium cladding materials can damage their integrity and durability.Service temperature and material defects have a significant effect on the dynamic growth of hydrides.In this study,we have developed a phasefield model based on the assumption of elastic behaviour within a specific temperature range(613 K-653 K).This model allows us to study the influence of temperature and interfacial effects on the morphology,stress,and average growth rate of zirconium hydride.The results suggest that changes in temperature and interfacial energy influence the length-to-thickness ratio and average growth rate of the hydride morphology.The ultimate determinant of hydride orientation is the loss of interfacial coherency,primarily induced by interfacial dislocation defects and quantifiable by the mismatch degree q.An escalation in interfacial coherency loss leads to a transition of hydride growth from horizontal to vertical,accompanied by the onset of redirection behaviour.Interestingly,redirection occurs at a critical mismatch level,denoted as qc,and remains unaffected by variations in temperature and interfacial energy.However,this redirection leads to an increase in the maximum stress,which may influence the direction of hydride crack propagation.This research highlights the importance of interfacial coherency and provides valuable insights into the morphology and growth kinetics of hydrides in zirconium alloys.
基金supported by the projects UIDB/00481/2020 and UIDP/00481/2020-Fundação para a Ciência e a Tecnologia,DOI 10.54499/UIDB/00481/2020(https://doi.org/10.54499/UIDB/00481/2020)and DOI 10.54499/UIDP/00481/2020(https://doi.org/10.54499/UIDP/00481/2020)supported by CENTRO-01-0145-FEDER-022083-Centro Portugal Regional Operational Programme(Centro 2020),under the PORTUGAL 2020 Partnership Agreement,through the European Regional Development Fund(ERDF).This article is a result of the Innovation Pact“NGS-New Generation Storage”(C644936001-00000045)+3 种基金by“NGS”Consortium,co-financed by NextGeneration EU,through the Incentive System“Agendas para a Inovação Empresarial”(“Agendas for Business Innovation”)within the Recovery and Resilience Plan(PRR).D.P acknowledges FCT,Portugal for the financial support with reference CEECIND/04158/2017(https://doi.org/10.54499/CEECIND/04158/2017/CP1459/CT0029)funding from the SMART-ER project,funded by the European Union’s Horizon 2020 research and innovation programme under Grant Agreement#101016888.support granted by the Recovery and Resilience Plan(PRR)and by the Next Generation EU European Funds to Universidade de Aveiro,through the Agenda for Business Innovation“NGS-Next Generation Storage”(Project no 02/C05-i01.01/2022 with the application C644936001-00000045).
文摘This study explores how the chemical interaction between magnesium hydride(MgH_(2))and the additive CrO_(3) influences the hydrogen/lithium storage characteristics of MgH_(2).We have observed that a 5 wt.%CrO_(3) additive reduces the dehydrogenation activation energy of MgH_(2) by 68 kJ/mol and lowers the required dehydrogenation temperature by 80℃.CrO_(3) added MgH_(2) was also tested as an anode in an Li ion battery,and it is possible to deliver over 90%of the total theoretical capacity(2038 mAh/g).Evidence for improved reversibility in the battery reaction is found only after the incorporation of additives with MgH_(2).In depth characterization study by X-ray diffraction(XRD)technique provides convincing evidence that the CrO_(3) additive interacts with MgH_(2) and produces Cr/MgO byproducts.Gibbs free energy analyses confirm the thermodynamic feasibility of conversion from MgH_(2)/CrO_(3) to MgO/Cr,which is well supported by the identification of Cr(0)in the powder by X ray photoelectron spectroscopy(XPS)technique.Through high resolution transmission electron microscopy(HRTEM)and energy dispersive spectroscopy(EDS)we found evidence for the presence of 5 nm size Cr nanocrystals on the surface of MgO rock salt nanoparticles.There is also convincing ground to consider that MgO rock salt accommodates Cr in the lattice.These observations support the argument that creation of active metal–metal dissolved rock salt oxide interface may be vital for improving the reactivity of MgH_(2),both for the improved storage of hydrogen and lithium.
文摘Magnesium(Mg)is a widely used and attractive metal,known for its unique physical and chemical properties,and it has been employed in the manufacture of many practical materials.Layered Double Hydroxides(LDHs),particularly Mg-based LDHs,rank among the most prevalent two-dimensional materials utilized in separation processes,which include adsorption,extraction,and membrane technology.The high popularity of Mg-based LDHs in separation applications can be attributed to their properties,such as excellent hydrophilicity,high surface area,ion exchangeability,and adjustable interlayer space.Currently,polymer membranes play a pivotal role in semi-industrial and industrial separation processes.Consequently,the development of polymer membranes and the mitigation of their limitations have emerged as compelling topics for researchers.Several methods exist to enhance the separation performance and anti-fouling properties of polymer membranes.Among these,incorporating additives into the membrane polymer matrix stands out as a cost-effective,straightforward,readily available,and efficient approach.The use of Mg-based LDHs,either in combination with other materials or as a standalone additive in the polymer membrane matrix,represents a promising strategy to bolster the separation and anti-fouling efficacy of flat sheet mixed matrix polymer membranes.This review highlights Mg-based LDHs as high-potential additives designed to refine flat sheet mixed matrix polymer membranes for applications in wastewater treatment and brackish water desalination.
基金Project supported by the Joint Fund of the National Natural Science Foundation of China–“Ye Qisun”Science Fund(Grant No.U2341251)。
文摘Zirconium hydride(ZrH_(2)) is an ideal neutron moderator material. However, radiation effect significantly changes its properties, which affect its behavior and the lifespan of the reactor. The threshold energy of displacement is an important quantity of the number of radiation defects produced, which helps us to predict the evolution of radiation defects in ZrH_(2).Molecular dynamics(MD) and ab initio molecular dynamics(AIMD) are two main methods of calculating the threshold energy of displacement. The MD simulations with empirical potentials often cannot accurately depict the transitional states that lattice atoms must surpass to reach an interstitial state. Additionally, the AIMD method is unable to perform largescale calculation, which poses a computational challenge beyond the simulation range of density functional theory. Machine learning potentials are renowned for their high accuracy and efficiency, making them an increasingly preferred choice for molecular dynamics simulations. In this work, we develop an accurate potential energy model for the ZrH_(2) system by using the deep-potential(DP) method. The DP model has a high degree of agreement with first-principles calculations for the typical defect energy and mechanical properties of the ZrH_(2) system, including the basic bulk properties, formation energy of point defects, as well as diffusion behavior of hydrogen and zirconium. By integrating the DP model with Ziegler–Biersack–Littmark(ZBL) potential, we can predict the threshold energy of displacement of zirconium and hydrogen in ε-ZrH_(2).
基金supported by the National Key R&D Program of China(No.2022YFB3803801)National Natural Science Foundation of China(52071177,21975125 and 52171214)the Priority Academic Program Development(PAPD)of Jiangsu Higher Education Institutions.
文摘Although Mg-based hydrides are extensively considered as a prospective material for solid-state hydrogen storage and clean energy carriers,their high operating temperature and slow kinetics are the main challenges for practical application.Here,a Mg-Ni based hydride,Mg_(2)NiH_(4) nanoparticles(~100 nm),with dual modification strategies of nanosizing and alloying is successfully prepared via a gas-solid preparation process.It is demonstrated that Mg_(2)NiH_(4) nanoparticles form a unique chain-like structure by oriented stacking and exhibit impressive hydrogen storage performance:it starts to release H2 at~170℃ and completes below 230℃ with a saturated capacity of 3.32 wt%and desorbs 3.14 wt% H_(2) within 1800 s at 200℃.The systematic characterizations of Mg_(2)NiH_(4) nanoparticles at different states reveal the dehydrogenation behavior and demonstrate the excellent structural and hydrogen storage stabilities during the de/hydrogenated process.This research is believed to provide new insights for optimizing the kinetic performance of metal hydrides and novel perspectives for designing highly active and stable hydrogen storage alloys.
基金supported by National Key Research and Development Program of China(2021YFB4000604)National Natural Science Foundation of China(52271220)111 Project(B12015)and the Fundamental Research Funds for the Central Universities.
文摘Hydrogen energy has emerged as a pivotal solution to address the global energy crisis and pave the way for a cleaner,low-carbon,secure,and efficient modern energy system.A key imperative in the utilization of hydrogen energy lies in the development of high-performance hydrogen storage materials.Magnesium-based hydrogen storage materials exhibit remarkable advantages,including high hydrogen storage density,cost-effectiveness,and abundant magnesium resources,making them highly promising for the hydrogen energy sector.Nonetheless,practical applications of magnesium hydride for hydrogen storage face significant challenges,primarily due to their slow kinetics and stable thermodynamic properties.Herein,we briefly summarize the thermodynamic and kinetic properties of MgH2,encompassing strategies such as alloying,nanoscaling,catalyst doping,and composite system construction to enhance its hydrogen storage performance.Notably,nanoscaling and catalyst doping have emerged as more effective modification strategies.The discussion focuses on the thermodynamic changes induced by nanoscaling and the kinetic enhancements resulting from catalyst doping.Particular emphasis lies in the synergistic improvement strategy of incorporating nanocatalysts with confinement materials,and we revisit typical works on the multi-strategy optimization of MgH2.In conclusion,we conduct an analysis of outstanding challenges and issues,followed by presenting future research and development prospects for MgH2 as hydrogen storage materials.
基金the National Natural Science Foundation of China(Grant No.11921004)the National Key R&D Program of China(Grant Nos.2021YFA1401800 and 2022YFA1402301)+2 种基金Chinese Academy of Sciences(Grant No.XDB33010200)supported by the National Science Foundation Earth Sciences(EAR 1634415)used resources of the Advanced Photon Source,a U.S.Department of Energy(DOE)Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory(Grant No.DEAC02-06CH11357)。
文摘We report experimental discovery of tantalum polyhydride superconductor.It was synthesized under highpressure and high-temperature conditions using diamond anvil cell combined with in situ high-pressure laser heating techniques.The superconductivity was investigated via resistance measurements at pressures.The highest superconducting transition temperature T_(c)was found to be~30 K at 197 GPa in the sample that was synthesized at the same pressure with~2000 K heating.The transitions are shifted to low temperature upon applying magnetic fields that support the superconductivity nature.The upper critical field at zero temperatureμ_0H_(c2)(0)of the superconducting phase is estimated to be~20 T that corresponds to Ginzburg-Landau coherent length~40 A.Our results suggest that the superconductivity may arise from 143d phase of TaH_(3).It is,for the first time to our best knowledge,experimental realization of superconducting hydrides for the VB group of transition metals.
基金support from the National Key Research&Development Program(2022YFB3803700)of ChinaNational Natural Science Foundation(No.52171186)financial support from the Center of Hydrogen Science,Shanghai Jiao Tong University。
文摘With the depletion of fossil fuels and global warming,there is an urgent demand to seek green,low-cost,and high-efficiency energy resources.Hydrogen has been considered as a potential candidate to replace fossil fuels,due to its high gravimetric energy density(142 MJ kg^(-1)),high abundance(H_(2)O),and environmentalfriendliness.However,due to its low volume density,effective and safe hydrogen storage techniques are now becoming the bottleneck for the"hydrogen economy".Under such a circumstance,Mg-based hydrogen storage materials garnered tremendous interests due to their high hydrogen storage capacity(~7.6 wt%for MgH_(2)),low cost,and excellent reversibility.However,the high thermodynamic stability(ΔH=-74.7 kJ mol^(-1)H_(2))and sluggish kinetics result in a relatively high desorption temperature(>300℃),which severely restricts widespread applications of MgH_(2).Nano-structuring has been proven to be an effective strategy that can simultaneously enhance the ab/de-sorption thermodynamic and kinetic properties of MgH_(2),possibly meeting the demand for rapid hydrogen desorption,economic viability,and effective thermal management in practical applications.Herein,the fundamental theories,recent advances,and practical applications of the nanostructured Mg-based hydrogen storage materials are discussed.The synthetic strategies are classified into four categories:free-standing nano-sized Mg/MgH_(2)through electrochemical/vapor-transport/ultrasonic methods,nanostructured Mg-based composites via mechanical milling methods,construction of core-shell nano-structured Mg-based composites by chemical reduction approaches,and multi-dimensional nano-sized Mg-based heterostructure by nanoconfinement strategy.Through applying these strategies,near room temperature ab/de-sorption(<100℃)with considerable high capacity(>6 wt%)has been achieved in nano Mg/MgH_(2)systems.Some perspectives on the future research and development of nanostructured hydrogen storage materials are also provided.
基金supported by the National Natural Science Foundation of China (Grant Nos.12025408,11921004,11888101,and 11974029)the Beijing Natural Science Foundation (Grant No.Z190008)+2 种基金the National Key R&D Program of China (Grant Nos.2018YFA0305700 and 2021YFA1400200)the Strategic Priority Research Program of CAS (Grant No.XDB33000000)the CAS Interdisciplinary Innovation Team (Grant No.JCTD-2019-01)。
文摘The lutetium dihydride LuH2is stable at ambient conditions.Here we show that its color undergoes sequential changes from dark blue at ambient pressure to pink at ~2.2 GPa and then to bright red at ~4 GPa upon compression in a diamond anvil cell.Such a pressure-induced color change in LuH2is reversible and it is very similar to that recently reported in the N-doped lutetium hydride [Nature 615,244(2023)].However,our preliminary resistance measurements on LuH2under pressures up to ~7 GPa evidenced no superconductivity down to 1.5 K.
基金supported by Natural Science Foundation of Shaanxi Province,China(2017JM5079)The 111 project(No.B08040)is also acknowledged.
文摘Aiming to elucidate the hydrogen absorption/desorption cycling properties of Mg-based alloys with in-situ formed Mg_(2)Ni and LaH_(x)(x=2,3)nanocrystallines,the hydrogen storage cycle stability,hydriding/dehydriding cycling kinetics and thermodynamic stability of the experimental alloys have been investigated in detail.The results show that the Mg-Ni-La alloys exhibit improved hydrogen storage cycling properties and can remain storage hydrogen above 5.5 wt%after 200 cycles.With the increase of cycling numbers,the dehydrogenation rates of the experimental samples increase firstly and then gradually decrease,and eventually maintain relative stable state.Microstructure observation reveals that powders sintering and hydrogen decrepitation both exist during hydrogen absorption/desorption cycles due to repeated volume expansion and contraction.Meanwhile,the in-situ formed LaH_(x)(x=2,3)and Mg_(2)Ni nanocrystallines stabilize the microstructures of the particles and hinder the powders sintering.After 200 cycles,the average particle size of the experimental samples decreases and the specific surface area apparently increases,which leads to the decomposition temperatures of MgH_(2)and Mg_(2)NiH_(4)slightly shift to lower temperatures.Moreover,Mg_(2)Ni and LaH_(x)(x=2,3)have been proven to be stable catalysts during long-term cycling,which can still uniformly distribute within the powders after 200 cycles.
基金National Natural Science Foundation of China (51935014,52165043, 82072084, 81871498)Jiang Xi Provincial Natural Science Foundation of China (20192ACB20005,2020ACB214004)+6 种基金The Provincial Key R&D Projects of Jiangxi (20201BBE51012)Guangdong Province Higher Vocational Colleges&Schools Pearl River Scholar Funded Scheme (2018)Shenzhen Science and Technology Plan Project (JCYJ20170817112445033)Innovation Team Project on University of Guangdong Province(2018GKCXTD001)Technology Innovation Platform Project of Shenzhen Institute of Information Technology 2020(PT2020E002)China Postdoctoral Science Foundation(2020M682114)Open Research Fund of Jiangsu Key Laboratory of Precision and Micro-Manufacturing Technology。
文摘Biodegradable magnesium(Mg) and its alloy show huge potential as temporary bone substitute due to the favorable biocompatibility and mechanical compatibility. However, one issue deserves attention is the too fast degradation. In this work, mesoporous bioglass(MBG)with high pore volume(0.59 cc/g) and huge specific surface area(110.78 m^(2)/g) was synthesized using improved sol-gel method, and introduced into Mg-based composite via laser additive manufacturing. Immersion tests showed that the incorporated MBG served as powerful adsorption sites, which promoted the in-situ deposition of apatite by successively adsorbing Ca2+and HPO42-. Such dense apatite film acted as an efficient protection layer and enhanced the corrosion resistance of Mg matrix, which was proved by the electrochemical impedance spectroscopy measurements. Thereby, Mg based composite showed a significantly decreased degradation rate of 0.31 mm/year. Furthermore,MBG also improved the mechanical properties as well as cell behavior. This work highlighted the advantages of MBG in the fabrication of Mg-based implant with enhanced overall performance for orthopedic application.
基金National Natural Science Foundation of China(No.51801078)。
文摘The catalytic effect of FeCoNiCrMo high entropy alloy nanosheets on the hydrogen storage performance of magnesium hydride(MgH_(2))was investigated for the first time in this paper.Experimental results demonstrated that 9wt%FeCoNiCrMo doped MgH_(2)started to dehydrogenate at 200℃and discharged up to 5.89wt%hydrogen within 60 min at 325℃.The fully dehydrogenated composite could absorb3.23wt%hydrogen in 50 min at a temperature as low as 100℃.The calculated de/hydrogenation activation energy values decreased by44.21%/55.22%compared with MgH_(2),respectively.Moreover,the composite’s hydrogen capacity dropped only 0.28wt%after 20 cycles,demonstrating remarkable cycling stability.The microstructure analysis verified that the five elements,Fe,Co,Ni,Cr,and Mo,remained stable in the form of high entropy alloy during the cycling process,and synergistically serving as a catalytic union to boost the de/hydrogenation reactions of MgH_(2).Besides,the FeCoNiCrMo nanosheets had close contact with MgH_(2),providing numerous non-homogeneous activation sites and diffusion channels for the rapid transfer of hydrogen,thus obtaining a superior catalytic effect.
基金supported by the Chongqing Special Key Project of Technology Innovation and Application Development,China(cstc2019jscx-dxwt B0029)the National Natural Science Foundation of China(51871143)+5 种基金the Science and Technology Committee of Shanghai(19010500400)the Shanghai Rising-Star Program(21QA1403200)Chongqing Research Program of Basic Research and Frontier Technology(No.cstc2019jcyj-msxm X0306)the Start-up Funds of Chongqing University(02110011044171)the Senior Talent Start-up Funds of Jiangsu University(4111310024)the Independent Research Project of State Key Laboratory of Mechanical Transmissions(SKLMT-ZZKT-2021M11)
文摘Mg-based materials are one of the most promising hydrogen storage candidates due to their high hydrogen storage capacity,environmental benignity,and high Clarke number characteristics.However,the limited thermodynamics and kinetic properties pose major challenges for their engineering applications.Herein,we review the recent progress in improving their thermodynamics and kinetics,with an emphasis on the models and the influence of various parameters in the calculated models.Subsequently,the impact of alloying,composite,and nanocrystallization on both thermodynamics and dynamics are discussed in detail.In particular,the correlation between various modification strategies and the hydrogen capacity,dehydrogenation enthalpy and temperature,hydriding/dehydriding rates are summarized.In addition,the mechanism of hydrogen storage processes of Mg-based materials is discussed from the aspect of classical kinetic theories and microscope hydrogen transferring behavior.This review concludes with an outlook on the remaining challenge issues and prospects.
基金supported by the National Key Research and Development Program of China(Grant Nos.2022YFA1403203 and 2021YFA1600200)the National Natural Science Foundation of China(Grant Nos.U2032215 and 12241405)。
文摘Recently,near-ambient superconductivity was claimed in nitrogen-doped lutetium hydride(LuH_(3-δ)N_(ε)).Unfortunately,all follow-up research still cannot find superconductivity signs in successfully synthesized lutetium dihydride(LuH_(2)) and N-doped LuH_(2±x)N_(y).However,a similar intriguing observation was the pressure-induced color changes(from blue to pink and subsequent red).The physical understanding of its origin and the correlation between the color,crystal structure,and chemical composition of Lu–H–N is still lacking.In this work,we systematically investigated the optical properties of LuH_(2) and LuH_(3),and the effects of hydrogen vacancies and nitrogen doping using the first-principles calculations by considering both interband and intraband contributions.Our results demonstrate that the evolution of reflectivity peaks near blue and red light,which is driven by changes in the band gap and Fermi velocity of free electrons,resulting in the blue-to-red color change under pressure.In contrast,LuH_(3) exhibits gray and no color change up to 50 GPa.Furthermore,we investigated the effects of hydrogen vacancies and nitrogen doping on its optical properties.Hydrogen vacancies can significantly decrease the pressure of blue-to-red color change in LuH_(2) but do not have a noticeable effect on the color of LuH_(3).The N-doped LuH_(2) with the substitution of a hydrogen atom at the tetrahedral position maintains the color change when the N-doping concentration is low.As the doping level increases,this trend becomes less obvious,while other N-doped structures do not show a blue-to-red color change.Our results can clarify the origin of the experimental observed blue-to-red color change in lutetium hydride and also provide a further understanding of the potential N-doped lutetium dihydride.