The effects of Zr on crystallization kinetics of Pr Fe B amorphous alloys have been investigated by DTA and XRD methods. It was found that for Pr 8Fe 86- x Zr x B 6 ( x =0, 1, 2) amorphous alloys, the final crystalliz...The effects of Zr on crystallization kinetics of Pr Fe B amorphous alloys have been investigated by DTA and XRD methods. It was found that for Pr 8Fe 86- x Zr x B 6 ( x =0, 1, 2) amorphous alloys, the final crystallized mixture is α Fe and Pr 2Fe 14 B, and the metastable Pr 2Fe 23 B 3 phase occurs during crystallization of Pr 8Fe 86 B 6 amorphous alloy, not during crystallization of Pr 8Fe 86- x Zr x B 6( x =1, 2) amorphous alloys. By analyzing the activation energy of crystallization, the formation of an α Fe/Pr 2Fe 14 B composite microstructure with a coarse grain size in annealed Pr 8Fe 86 B 6 alloy, is attributed to a difficult nucleation and an easy growth for both the α Fe and Pr 2Fe 14 B in the alloy. The addition of Zr can be used to change the crystallization behavior of the α Fe phase in Pr Fe B amorphous alloy, which is helpful to reduce the grain size for the α Fe phase.展开更多
In general,the rapid growth of α-Fe clusters is a challenge in high Fe-content Fe-based amorphous alloys,negatively affecting their physical properties.Herein,we introduce an efficient and rapid post-treatment techni...In general,the rapid growth of α-Fe clusters is a challenge in high Fe-content Fe-based amorphous alloys,negatively affecting their physical properties.Herein,we introduce an efficient and rapid post-treatment technique known as ultrasonic vibration rapid processing(UVRP),which enables the formation of high-density strong magnetic α-Fe clusters,thereby enhancing the soft magnetic properties of Fe_(78)Si(13)B_(9) amorphous alloy ribbon.展开更多
The effects of deep cryogenic-cycling treatment(DCT)on the mechanical properties,soft magnetic properties,and atomic scale structure of the Fe_(73.5)Si_(13.5)B_(9)Nb_(3)Cu_(1)amorphous nanocrystalline alloy were inves...The effects of deep cryogenic-cycling treatment(DCT)on the mechanical properties,soft magnetic properties,and atomic scale structure of the Fe_(73.5)Si_(13.5)B_(9)Nb_(3)Cu_(1)amorphous nanocrystalline alloy were investigated.The DCT samples were obtained by subjecting the as-annealed samples to a thermal cycling process between the temperature of the supercooled liquid zone and the temperature of liquid nitrogen.Through flat plate bending testing,hardness measurements,and nanoindentation experiment,it is found that the bending toughness of the DCT samples is improved and the soft magnetic properties are also slightly enhanced.These are attributed to the rejuvenation behavior of the DCT samples,which demonstrate a higher enthalpy of relaxation.Therefore,DCT is an effective method to enhance the bending toughness of Fe-based amorphous nanocrystalline alloys without degrading the soft magnetic properties.展开更多
Developing an industrially relevant electrode with high catalytic activity,stability,and tunable composition/size for large-scale water electrolysis is a significant challenge.We have created an integrated elec-trode(...Developing an industrially relevant electrode with high catalytic activity,stability,and tunable composition/size for large-scale water electrolysis is a significant challenge.We have created an integrated elec-trode(NFM30-N)for the oxygen evolution reaction(OER)using a facile top-down approach that combines arc melting with dealloying-oxidation.Due to the dealloying-oxidation effect,the asderived porous amorphous M-O,M-OH,and M-OOH(M=Ni,Fe)nanocones cover the basic NiFeMn alloy.This integrated design enables NFM30-N to exhibit outstanding OER performance at high current densities,requiring low overpotentials of only 282 and 323 mV to achieve large current densities of 100 and 500 mA cm^(-2),respectively.It also displays a small Tafel slope of 44.1 mV dec^(-1) and remarkable stability for over 100 h at 100 and 500 mA cm^(-2).When used as an anode,a two-electrode electrolyzer cell with NFM30-N at 500 mA cm^(-2) only requires a cell voltage of 1.619 V and exhibits excellent stability,with almost no performance degradation after continuous chronopotentiometry test for each 100 h at 500 and 100 mA cm^(-2).This exceptional OER electrocatalytic performance is attributed to the integrated structure providing high electrical conductivity and stability,the presence of numerous active sites due to dealloying and the amorphous structure,and the promotion of the OER process by M-O,M-OH,and M-OOH species.This work offers a novel idea for fabricating integrated,industrially relevant electrocatalytic electrodes through traditional metallurgy combined with dealloying-oxidation.展开更多
Ruthenium dioxide(RuO_(2))is one of the most promising acidic oxygen evolution reaction(OER)catalysts to replace the expensive and prevalent iridium(Ir)-based materials.However,the lattice oxygen oxidation induced Ru ...Ruthenium dioxide(RuO_(2))is one of the most promising acidic oxygen evolution reaction(OER)catalysts to replace the expensive and prevalent iridium(Ir)-based materials.However,the lattice oxygen oxidation induced Ru dissolution during OER compromises the activity and stability.Amorphous materials have been identified as a viable strategy to promote the stability of RuO_(2)in acidic OER applications.This study reported a nanoporous amorphous-rich RuMnO_(x)(A-RuMnO_(x))aerogel for efficient and stable acidic OER.Compared with highly crystalline RuMnO_(x),the weakened Ru–O covalency of A-RuMnO_(x)by forming amorphous structure is favorable to inhibiting the oxidation of lattice oxygen.Meanwhile,this also optimizes the electronic structure of Ru sites from overoxidation and reduces the reaction energy barrier of the rate-determining step.As a result,A-RuMnO_(x)aerogel exhibits an ultra-low overpotential of 145 mV at 10 mA cm^(-2)and durability exceeding 100 h,as well as high mass activity up to 153 mA mg^(-1)_(Ru)at 1.5 V vs.reversible hydrogen electrode(RHE).This work provides valuable guidance for preparing highly active and stable Ru-based catalysts for acidic OER.展开更多
A suction casting experiment was conducted on Zr_(55)Cu_(30)Al_(10)Ni_(5)(at%)amorphous alloy.Using ProCAST software,numerical simulations were performed to analyze the filling and solidification processes.The velocit...A suction casting experiment was conducted on Zr_(55)Cu_(30)Al_(10)Ni_(5)(at%)amorphous alloy.Using ProCAST software,numerical simulations were performed to analyze the filling and solidification processes.The velocity field during the filling process and the temperature field during the solidification process of the alloy melt under different process parameters were obtained.Based on the simulation results,a Zr-based amorphous alloy micro-gear was prepared via casting.The results indicate that increasing the suction casting temperature enhances the fluidity of alloy melt but induces unstable flow rate during filling,which is detrimental to complete filling.Zr-based amorphous micro-gears with a module of 0.6 mm,a tooth top diameter of 8 mm,and 10 teeth were prepared through the suction casting.X-ray diffraction and differential scanning calorimetry analyses confirm that the fabricated micro-gear exhibits characteristic amorphous structural features,demonstrating well-defined geometrical contours and satisfactory forming completeness.展开更多
The inverse relationship between the saturation magnetic flux density(Bs)and coercivity(Hc)of Febased amorphous alloys is a very active research topic that has been extensively debated.In this work,we conducted a deta...The inverse relationship between the saturation magnetic flux density(Bs)and coercivity(Hc)of Febased amorphous alloys is a very active research topic that has been extensively debated.In this work,we conducted a detailed investigation on the magnetic softness of Fe_(83.2-x)Co_(x)B_(10)C_(6)Cu_(0.8)(x=0 and 6 at.%)amorphous alloys based on analysis of the surface morphology,microstructure,magnetic anisotropy,and magnetic domain structure.Enhanced magnetic softness-magnetization synergy was realized in the present alloys by magnetic field annealing(MFA)during the de-stressing process.A dramatic 84%reduction of Hc to 2.2 A/m was achieved for the Co-doped alloy under MFA,exhibiting excellent magnetic performance with a superb Bs of 1.86 T.The consistency between the experimental results and theoretical analysis revealed that the MFA process can mitigate the trade-off between stress-induced anisotropy and induced uniaxial anisotropy owing to the homogenized structure formed by field annealing.Thus,the process favored a low Hc due to the significant continuous decline in the total magnetic anisotropy,which coincided well with the results of Magneto-optical Kerr microscopy.The study elucidates a mechanism for tuning Hc in Co-doped alloy systems and affords a possible pathway for softening amorphous alloys with high Bs.展开更多
Establishing the structure-property relationship in amorphous materials has been a long-term grand challenge due to the lack of a unified description of the degree of disorder.In this work,we develop SPRamNet,a neural...Establishing the structure-property relationship in amorphous materials has been a long-term grand challenge due to the lack of a unified description of the degree of disorder.In this work,we develop SPRamNet,a neural network based machine-learning pipeline that effectively predicts structure-property relationship of amorphous material via global descriptors.Applying SPRamNet on the recently discovered amorphous monolayer carbon,we successfully predict the thermal and electronic properties.More importantly,we reveal that a short range of pair correlation function can readily encode sufficiently rich information of the structure of amorphous material.Utilizing powerful machine learning architectures,the encoded information can be decoded to reconstruct macroscopic properties involving many-body and long-range interactions.Establishing this hidden relationship offers a unified description of the degree of disorder and eliminates the heavy burden of measuring atomic structure,opening a new avenue in studying amorphous materials.展开更多
The hydrazine oxidation reaction(HzOR)has garnered significant attention as a feasible approach to replace sluggish anodic reactions to save energy.Nevertheless,there are still difficulties in developing highly effici...The hydrazine oxidation reaction(HzOR)has garnered significant attention as a feasible approach to replace sluggish anodic reactions to save energy.Nevertheless,there are still difficulties in developing highly efficient catalysts for the HzOR.Herein,we report amorphous ruthenium nanosheets(a-Ru NSs)with a thickness of approximately 9.6 nm.As a superior bifunctional electrocatalyst,a-Ru NSs exhibited enhanced electrocatalytic performance toward both the HzOR and hydrogen evolution reaction(HER),outperforming benchmark Pt/C catalysts,where the a-Ru NSs achieved a work-ing potential of merely-76 mV and a low overpotential of only 17 mV to attain a current density of 10 mA·cm^(-2) for the HzOR and HER,respectively.Furthermore,a-Ru NSs displayed a low cell voltage of 28 mV at 10 mA·cm^(-2) for overall hy-drazine splitting in a two-electrode electrolyzer.In situ Raman spectra revealed that the a-Ru NSs can efficiently promote N‒N bond cleavage,thereby producing more*NH_(2)and accelerating the progress of the reaction.展开更多
[Background and purposes]Proton exchange membrane fuel cells(PEMFCs),which convert hydrogen energy directly into electrical energy and water,have received overwhelming attention,owing to their potential to significant...[Background and purposes]Proton exchange membrane fuel cells(PEMFCs),which convert hydrogen energy directly into electrical energy and water,have received overwhelming attention,owing to their potential to significantly reduce energy consumption,pollution emissions and reliance on fossil fuels.Bipolar plates are the major part and key component of PEMFCs stack,which provide mechanical strength,collect and conduct current segregate oxidants and reduce agents.They contribute 70-80%weight and 20-30%cost of a whole stack,while significantly affecting the power density.There are three types plates,including metal bipolar plate,graphite bipolar plate and composite bipolar plate.Stainless steel bipolar plates,as one of metal bipolar plate,exhibit promising manufacturability,competitive cost and durability among various metal materials.However,stainless steel would be corroded in the harsh acid(pH 2-5)and humid PEMFCs environment,whereas the leached ions will contaminate the membrane.In addition,the passivated film formed on the surface will increase the interfacial contact resistance(ICR).In order to improve the corrosion resistance and electrical conductivity of steel bipolar plates,surface coatings are essential.Metal nitride coatings,metal carbide coatings,polymer coatings and carbon-based coatings have been introduced in recent years.Carbon-based coatings,mainly including a-C(amorphous Carbon),Ta-C(Tetrahedral amorphous carbon)and DLC(diamond-like carbon),have attracted considerable attention from both academia and industry,owing to their superior performance,such as chemical inertness,mechanical hardness and electrical conductivity.However,Ta-C films as protective coating of PEMFCs have been rarely reported,due to the difficulty in production for industrial application.In this paper,multi-layer Ta-C composite films were produced by using customized industrial-scale vacuum equipment to address those issues.[Methods]Multiple layered Ta-C coatings were prepared by using PIS624 equipment,which assembled filtered cathodic arc evaporation,ion beam and magnetron sputtering into one equipment,while SS304 and silicon specimens were used as substrate for testing and analysis.Adhesion layer and intermediate layer were deposited by using magnetron sputtering at deposition temperature of 150℃and pressure of 3×10^(−1) Pa,while the sputtering current was set to be 5 A and bias power to be 300 V.The Ta-C layer was coated at arc current of 80-100 A,bias voltage of 1500 V and gas flow of 75 sccm.A scanning electron microscope(CIQTEK SEM3200)was used to characterize surface morphology,coating structure and cross-section profile of the coatings.Raman spectrometer(LabRam HR Evolution,HORIBA JOBIN YVON)was used to identify the bonding valence states.Electrochemical tests were performed by using an electrochemical work station(CHI760,Shanghai Chenhua Instrument Co.,Ltd.),with the traditional three electrode system,where saturated Ag/AgCl and platinum mesh were used as the reference electrode and counter electrode,respectively.All samples were mounted in plastic tube and sealed with epoxy resin,with an exposure area of 2.25 cm^(2),serving as the working electrode.Electrochemical measurements were carried out in simulated PEMFCs cathode environment in 0.5 mol·L^(−1) H_(2)SO_(4)+5 ppm F−solution,at operating temperature of 70℃.As the cathode environment was harsher than the anode environment,all the samples are stabilized at the open-circuit potential(OCP)for approximately 30 min before the EIS measurements.ICR between bipolar plates and GDL was a key parameter affecting performance of the PEMFCs stack.The test sample sandwiched between 2 pieces of carbon paper(simulate gas diffusion layer,GDL)was placed between 2 gold-plated copper electrodes at a compaction pressure of 1.4 MPa,which was considered to be the conventional compaction pressure in the PEMFCs.Under the same conditions,the resistance of a single carbon paper was measured as well.The ICR was calculated according to the formula ICR=1/2(R2−R1)×S,where S was the contact area between GDL and coated stainless steel BPPs.All data of ICR were measured three times for averaging.[Results]The coatings deposited by filtered cathodic arc technology were compact and smooth,which reduced coating porosity and favorable to corrosion resistance.The coating thickness of adhesion and intermediate layers were 180 nm,while the protective Ta-C coating thickness was about 300 nm,forming multiple coating to provide stronger protection for metal bipolar plates.Cr,Ti,Nb and Ta coatings were selected as adhesion layers for comparison.According to electrochemical test,Ta and Nb coatings have higher corrosion resistance.However,Ta and Nb materials would be costly when they are used for mass production.Relatively,Cr and Ti materials were cost effective.Hence,a comprehensive assessment was indispensable to decide the materials to be selected as adhesion layer.Ta-TiN and Ti-TiN combined adhesion and intermediate layer exhibited stronger corrosion resistance,with the corrosion current to be less than 10^(−6) A·cm^(−2).Ta-C protective coating deposited by using filtered cathodic arc technology indicated displayed higher corrosion resistance,with the average corrosion density to be about 1.26×10^(−7) A·cm^(−2).Ta-C coating also shown larger contact angle,with the highest hydrophobicity,which was one of the important advantages for Ta-C,in terms of corrosion resistance.According to Raman spectroscopy,the I(D)/I(G)=549.8/1126.7=0.487,with the estimated fraction of sp^(3) bonding to be in the range of 5154%.The intermediate layer TiN has higher conductivity than the CrN layer.Considering cost,corrosion performance and ICR result,the Ti-TiN layer combination is recommended for industrial scale application.[Conclusions]Multiple layer coating structure of Ta-C film had stronger corrosion resistance;with more than 50%sp^(3) content,while it also had larger water contact angle and higher corrosion resistance than DLC film.The filtered arcing deposition technology was able to make the film to be more consistent and stable than normal arcing technology in terms of the preparation of Ta-C.The coating displayed corrosion density of 1.26×10^(−7) A·cm^(−2) and ICR of less than 5 mΩ·cm^(2),far beyond technical target of 2025 DOE(US Department of Energy).This indicated that the mass-production scale coating technology for PEMFC bipolar plates is highly possible.展开更多
Noble metal-based intermetallic compounds(IMCs)with ordered atomic arrangements exhibit remarkable electrocatalytic activity owing to their unique crystal and electronic structures.During the past years,great advance ...Noble metal-based intermetallic compounds(IMCs)with ordered atomic arrangements exhibit remarkable electrocatalytic activity owing to their unique crystal and electronic structures.During the past years,great advance has been made in the development of noble metal-based IMCs.Recently,Lu and coworkers reported ultrathin“amorphous/intermetallic”(A/IMC)heterophase PtPbBi nanosheets(NSs)with a thickness of 2.5±0.3 nm.The oxidative etching effect caused by the coexistence of O_(2)and Br^(-)ions plays a crucial role in the formation of the IMC and unique two-dimensional structure with irregular shapes and curled edges.This study shows that fabricating an A/IMC heterophase structure with a multimetallic composition can effectively enhance the catalytic performances of noble metal-based electrocatalysts.展开更多
The unique long-range disordered atomic arrangement inherent in amorphous materials endows them with a range of superior properties,rendering them highly promising for applications in catalysis,medicine,and battery te...The unique long-range disordered atomic arrangement inherent in amorphous materials endows them with a range of superior properties,rendering them highly promising for applications in catalysis,medicine,and battery technology,among other fields.Since not all materials can be synthesized into an amorphous structure,the composition design of amorphous materials holds significant importance.Machine learning offers a valuable alternative to traditional“trial-anderror”methods by predicting properties through experimental data,thus providing efficient guidance in material design.In this study,we develop a machine learning workflow to predict the critical casting diameter,glass transition temperature,and Young's modulus for 45 ternary reported amorphous alloy systems.The predicted results have been organized into a database,enabling direct retrieval of predicted values based on compositional information.Furthermore,the applications of high glass forming ability region screening for specified system,multi-property target system screening and high glass forming ability region search through iteration are also demonstrated.By utilizing machine learning predictions,researchers can effectively narrow the experimental scope and expedite the exploration of compositions.展开更多
Carbon nanotubes(CNTs)reinforced copper(CNTs/Cu)is one of the most promising and extensively researched materials for replacing traditional Cu-based materials in high-load and high-current applications,particularly wi...Carbon nanotubes(CNTs)reinforced copper(CNTs/Cu)is one of the most promising and extensively researched materials for replacing traditional Cu-based materials in high-load and high-current applications,particularly within the aerospace industry.Amorphous carbon nanotubes(aCNTs)are a type of carbon nanotubes characterized by the presence of mesopores distributed across their amorphous sidewalls,facilitating connectivity between the hollow core and the external environment.Therefore,we propose utilizing aCNTs as a reinforcing agent for Cu.The mesoporous structure of aCNTs facilitates the interpenetration of Cu into the aCNTs,thereby maintaining the continuity of the matrix properties.Experimental results demonstrate that Cu effectively penetrates the mesoporous sidewalls of aCNTs.Both pure Cu and aCNTs-reinforced Cu exhibit comparable electrical conductivity,while the hardness of the aCNTs/Cu composite is significantly enhanced.Additionally,both the density and porosity of aCNTs/Cu are lower than those of pure Cu,and the introduction of aCNTs helps to reduce the sintering temperature.展开更多
Polyanionic materials are considered one of the most promising cathode materials for sodium-ion batteries because of the stable structure framework and high working voltage.However,most polyanionic materials possess l...Polyanionic materials are considered one of the most promising cathode materials for sodium-ion batteries because of the stable structure framework and high working voltage.However,most polyanionic materials possess limited sodium storage sites and have to undergo complex local structure evolution during charge/discharge.Herein,we conducted a systematic investigation into the impact of structural forms of NaVOPO_(4)on the electrochemical properties.Amorphous and crystalline NaVOPO_(4)are synthesized through a controlled reflux reduction method,and the amorphous NaVOPO_(4)(a-NVOP)demonstrates much better electrochemical performance compared to the crystalline counterpart.Specifically,the a-NVOP electrode delivers high reversible capacity(142 mAh g^(-1)at 14.5 mA g^(-1),close to the theoretical capacity of 145 mAh g^(-1)),high energy density(497 Wh kg^(-1)based on cathode material)and remarkable cyclability with capacity retention of 80%after 500 cycles.In situ and ex situ experimental analyses and theoretical calculations reveal that the superior performance is primarily due to the maintaining of the amorphous state during the charge/discharge process to endow high stability and accelerated intercalation/deintercalation of large-sized Na^(+)without lattice constraints.Furthermore,the amorphous cathode materials show promising electrochemical properties in lithium-,potassium-and zinc-ion batteries,highlighting their broad adaptability and potential across various battery systems.展开更多
Mg_(x)(Ni_(0.8)La_(0.2))_(100-x),where x=60,70,80,exhibiting a nanocrystalline microstructure,were prepared through the crystallization of amorphous alloys.The investigation encompassed the phase constitution,grain si...Mg_(x)(Ni_(0.8)La_(0.2))_(100-x),where x=60,70,80,exhibiting a nanocrystalline microstructure,were prepared through the crystallization of amorphous alloys.The investigation encompassed the phase constitution,grain size,microstructural stability,and hydrogen storage properties.Crystallization kinetics,along with in-situ high-energy XRD characterization,revealed a concentrated and synchronous crystallization of Mg_(2)Ni and RE-Mg-Ni ternary phases with the increase in La and Ni content.The attributed synchronous crystallization process was found to be a result of the close local affinity of Mg_(2)Ni and RE-Mg-Ni ternary phases,as assessed by the thermodynamic Miedema model.Significant secondary phase pinning effect,arising from the high likelihood of well-matching phase structures between Mg_(2)Ni,LaMg_(2)Ni,and LaMgNi_(4),was validated through both the edge-to-edge matching model prediction and experimental observation.Thefine and homogeneous microstructure was shown to be a consequence of fast crystallization kinetics and the secondary phase pinning effect.Improved activation performance and cycling stability were observed,stemming from grain refinement and excellent microstructural stability.Our study provides insights into mechanism of grain refinement of nanocrystalline microstructure tailored by phase constitution and crystallization kinetics in the amorphous-crystallization route.We also demonstrate the potential of material design guided by phase equilibria and crystallographic predictions to improve nanocrystalline with excellent microstructural stability.展开更多
At present,the most common preparation method of amorphous boron powder is magnesium thermal reduction method,but the amorphous boron powder obtained by this method mostly contains impurities such as magnesium and oxy...At present,the most common preparation method of amorphous boron powder is magnesium thermal reduction method,but the amorphous boron powder obtained by this method mostly contains impurities such as magnesium and oxygen which are difficult to remove,and these impurities will seriously affect the application of amorphous boron powder and need to be strictly removed.In this research,the acid-insoluble impurities were modified through sintering and quenching,while the magnesium impurities were optimized via ultrasonic acid leaching.We observed that the quenching temperature played a crucial role in determining the efficiency of magnesium impurity removal.The results show that the magnesium content in amorphous boron powder can be reduced from 5.67%to 2.40%by quenching the amorphous boron powder at 800°C and using ultrasonic assisted acid leaching.Furthermore,the oxidation reaction of boron is influenced by the powder's particle size and specific surface area,with the effective activation energy being intimately tied to both these factors.Post-quenching and acid leaching,we observed an increase in the specific surface area of the boron powder samples,leading to enhanced activity.In conclusion,our study presents an effective strategy to mitigate magnesium impurities and elevate the performance of amorphous boron powder,offering promising avenues for advancing its utilization across diverse industries.展开更多
Achieving a delicate synergy between mechanical robustness and antifouling attributes in coatings remains a formidable challenge for marine applications. Inspired by the assembly of nacre, we present a novel approach ...Achieving a delicate synergy between mechanical robustness and antifouling attributes in coatings remains a formidable challenge for marine applications. Inspired by the assembly of nacre, we present a novel approach to fabricate a nacre-like metallic coating. This coating comprises an amorphous matrix with excellent anti-corrosion and anti-wear properties, as well as Cu-rich 3D interconnected channels for antifouling function. The coating is produced by high velocity oxygen fuel (HVOF) thermal spraying of surface-modified Fe-based amorphous powders with a Cu-layer. The resulting coating exhibits exceptional mechanical robustness, including high resistance to erosion, abrasion, and impact, surpassing conventional polymer antifouling coatings. Furthermore, the controlled Cu+ leaching capability of the in-situ constructed 3D interconnected diffusion channels, facilitated by the Cu-rich intersplats, contributes to the remarkable antifouling performance. This includes nearly 100 % resistance to bacterial adhesion after 1 day of immersion and over 98 % resistance to algal attachment after 7 d of immersion, resulting in a prolonged service lifetime. Notably, even after 200 cycles of wear damage, the Cu-modified amorphous coating still maintains its excellent antifouling properties. The Cu-rich intersplats play a critical role in transporting and sustainably leaching Cu ions, thereby accounting for the outstanding antifouling performance. Ultimately, we aim to advance the design of high-performance coatings suited for diverse marine applications, where both the mechanical robustness and antifouling properties are essential.展开更多
Lithium-ion batteries with LiCoO_(2)(LCO)cathodes are widely used in various electronic devices,resulting in a large amount of spent LCO(SLCO).Therefore,there is an urgent need for an efficient technique for recycling...Lithium-ion batteries with LiCoO_(2)(LCO)cathodes are widely used in various electronic devices,resulting in a large amount of spent LCO(SLCO).Therefore,there is an urgent need for an efficient technique for recycling SLCO.However,due to the presence of cobalt oxide with a spinel phase on the surface of highly-degraded LCO,the strong electrostatic repulsion from the transition metal octahedron poses a high Li replenishment barrier,making the regeneration of highly-degraded LCO a challenge.Herein,we propose a structural transformation strategy for reconstructing Li replenishment channels to aid the direct regeneration of highly-degraded LCO.In this approach,ball milling is employed to disrupt the inherent structure of highly-degraded LCO,thereby releasing the internal stress and converting the surface spinel phase into a homogeneous amorphous structure,which promotes Li insertion and regeneration.The regenerated LCO(RLCO)exhibits an outstanding discharge capacity of 179.10 mAh·g^(−1) in the voltage range of 3.0–4.5 V at 0.5 C.The proposed strategy is an effective regeneration approach for highly-degraded LCO,thereby facilitating the efficient recycling of spent lithium-ion battery cathode materials.展开更多
In this work,a series of Ce-Ti composite oxides with different Ti/Ce molar ratios was prepared by coprecipitation method,and investigated for the catalytic degradation of toluene and selective catalytic reduction of N...In this work,a series of Ce-Ti composite oxides with different Ti/Ce molar ratios was prepared by coprecipitation method,and investigated for the catalytic degradation of toluene and selective catalytic reduction of NO.The phase transition process between Ce species and Ti species is limited by modulating the interaction between Ce4+and Ti4+,while a completely amorphous composite is generated with an appropriate molar ratio of Ti/Ce(1.5/1).The catalyst CeTi1.5Oxexhibits the best catalytic performance,where the values of T90and T50for deep degradation of toluene are 297 and 330℃respectively at high weight hours space velocity(WHSV=120000 mL/(g·h)).Compared with CeO_(2),T90and T50decrease by48 and 34℃respectively while declining by 67 and 70℃compared to TiO_(2).For the SCR reaction,CeTi1.5Oxreaches 100%NO conversion at 250℃with WHSV=60000 mL/(g·h),reduced by 50℃compared to pure CeO_(2).The amorphous nanostructure with highly dispersed Ce and Ti species was confirmed by transmission electron microscopy(TEM)and X-ray diffraction(XRD)characterizations.The X-ray photoelectron spectroscopy(XPS)and Raman analyses show that a large number of active Ce-O-Ti species and surface oxygen vacancies are generated due to the strong interaction between Ti^(4+)and Ce^(4+)in CeTi_(1.5)O_(x).Additionally,H_(2)-TPR and O_(2)-TPD further confirm that the interaction promotes the low-temperature reducibility and mobility of surface-active oxygen species.Meanwhile,in-situ DRIFTS study reveals that CeTi1.5Oxwith amorphous nanostructure can dramatically enhance the dissociative and complete oxidation capacity for toluene.展开更多
Recent advancements in electrocatalysis have highlighted the exceptional application value of amorphous electrocatalysts. Withtheir unique atomic configurations, these electrocatalysts exhibit superior catalytic perfo...Recent advancements in electrocatalysis have highlighted the exceptional application value of amorphous electrocatalysts. Withtheir unique atomic configurations, these electrocatalysts exhibit superior catalytic performance compared to that of their crystalline coun-terparts. Transition metal(TM) amorphous ribbon-shaped electrocatalysts have recently emerged as a new frontier in the catalysis field.Dealloying is widely considered a fascinating method for enhancing the electrocatalyst performance. In this review, we comprehensivelyexamine the principles of water electrolysis, discuss the prevalent methods for fabricating ribbon-configured electrocatalysts, and providean overview of amorphous alloys. Furthermore, we discuss binary, ternary, and high-entropy amorphous TM-based electrocatalysts,which satisfy the requirements necessary for effective water electrolysis. We also propose strategies to enhance the activity of amorphousTM-based ribbons, including morphology control, defect engineering, composition optimization, and heterostructure creation in differentelectrolytes. Our focus extends to the latest developments in the design of heterogeneous micro/nanostructures, management of prepara-tion techniques, and synthesis of different compositions. Finally, we address the ongoing challenges and provide a perspective on the fu-ture development of broadly applicable, self-supporting TM ribbon-shaped electrocatalysts.展开更多
文摘The effects of Zr on crystallization kinetics of Pr Fe B amorphous alloys have been investigated by DTA and XRD methods. It was found that for Pr 8Fe 86- x Zr x B 6 ( x =0, 1, 2) amorphous alloys, the final crystallized mixture is α Fe and Pr 2Fe 14 B, and the metastable Pr 2Fe 23 B 3 phase occurs during crystallization of Pr 8Fe 86 B 6 amorphous alloy, not during crystallization of Pr 8Fe 86- x Zr x B 6( x =1, 2) amorphous alloys. By analyzing the activation energy of crystallization, the formation of an α Fe/Pr 2Fe 14 B composite microstructure with a coarse grain size in annealed Pr 8Fe 86 B 6 alloy, is attributed to a difficult nucleation and an easy growth for both the α Fe and Pr 2Fe 14 B in the alloy. The addition of Zr can be used to change the crystallization behavior of the α Fe phase in Pr Fe B amorphous alloy, which is helpful to reduce the grain size for the α Fe phase.
基金supported by the Major Science and Technology Project of Zhongshan City(No.2022AJ004)the Key Basic and Applied Research Program of Guangdong Province(Nos.2019B030302010 and 2022B1515120082)Guangdong Science and Technology Innovation Project(No.2021TX06C111).
文摘In general,the rapid growth of α-Fe clusters is a challenge in high Fe-content Fe-based amorphous alloys,negatively affecting their physical properties.Herein,we introduce an efficient and rapid post-treatment technique known as ultrasonic vibration rapid processing(UVRP),which enables the formation of high-density strong magnetic α-Fe clusters,thereby enhancing the soft magnetic properties of Fe_(78)Si(13)B_(9) amorphous alloy ribbon.
基金supported by Liaoning Joint Fund of NSFC(No.U1908219)。
文摘The effects of deep cryogenic-cycling treatment(DCT)on the mechanical properties,soft magnetic properties,and atomic scale structure of the Fe_(73.5)Si_(13.5)B_(9)Nb_(3)Cu_(1)amorphous nanocrystalline alloy were investigated.The DCT samples were obtained by subjecting the as-annealed samples to a thermal cycling process between the temperature of the supercooled liquid zone and the temperature of liquid nitrogen.Through flat plate bending testing,hardness measurements,and nanoindentation experiment,it is found that the bending toughness of the DCT samples is improved and the soft magnetic properties are also slightly enhanced.These are attributed to the rejuvenation behavior of the DCT samples,which demonstrate a higher enthalpy of relaxation.Therefore,DCT is an effective method to enhance the bending toughness of Fe-based amorphous nanocrystalline alloys without degrading the soft magnetic properties.
基金the National Natural Science Foundation of China(Nos.52174365,52004155,52334009 and 52130204)the National Key R&D Program of China(Nos.2023YFB3506701 and 2022YFB3706801)the Science and Technology Commission of Shanghai Municipality(No.21DZ1208900).
文摘Developing an industrially relevant electrode with high catalytic activity,stability,and tunable composition/size for large-scale water electrolysis is a significant challenge.We have created an integrated elec-trode(NFM30-N)for the oxygen evolution reaction(OER)using a facile top-down approach that combines arc melting with dealloying-oxidation.Due to the dealloying-oxidation effect,the asderived porous amorphous M-O,M-OH,and M-OOH(M=Ni,Fe)nanocones cover the basic NiFeMn alloy.This integrated design enables NFM30-N to exhibit outstanding OER performance at high current densities,requiring low overpotentials of only 282 and 323 mV to achieve large current densities of 100 and 500 mA cm^(-2),respectively.It also displays a small Tafel slope of 44.1 mV dec^(-1) and remarkable stability for over 100 h at 100 and 500 mA cm^(-2).When used as an anode,a two-electrode electrolyzer cell with NFM30-N at 500 mA cm^(-2) only requires a cell voltage of 1.619 V and exhibits excellent stability,with almost no performance degradation after continuous chronopotentiometry test for each 100 h at 500 and 100 mA cm^(-2).This exceptional OER electrocatalytic performance is attributed to the integrated structure providing high electrical conductivity and stability,the presence of numerous active sites due to dealloying and the amorphous structure,and the promotion of the OER process by M-O,M-OH,and M-OOH species.This work offers a novel idea for fabricating integrated,industrially relevant electrocatalytic electrodes through traditional metallurgy combined with dealloying-oxidation.
基金financial support from the National Natural Science Foundation of China(22478278,22308246)the Central Government Guides the Local Science and Technology Development Special Fund(YDZJSX20231A015)the Fundamental Research Program of Shanxi Province(202203021212266)。
文摘Ruthenium dioxide(RuO_(2))is one of the most promising acidic oxygen evolution reaction(OER)catalysts to replace the expensive and prevalent iridium(Ir)-based materials.However,the lattice oxygen oxidation induced Ru dissolution during OER compromises the activity and stability.Amorphous materials have been identified as a viable strategy to promote the stability of RuO_(2)in acidic OER applications.This study reported a nanoporous amorphous-rich RuMnO_(x)(A-RuMnO_(x))aerogel for efficient and stable acidic OER.Compared with highly crystalline RuMnO_(x),the weakened Ru–O covalency of A-RuMnO_(x)by forming amorphous structure is favorable to inhibiting the oxidation of lattice oxygen.Meanwhile,this also optimizes the electronic structure of Ru sites from overoxidation and reduces the reaction energy barrier of the rate-determining step.As a result,A-RuMnO_(x)aerogel exhibits an ultra-low overpotential of 145 mV at 10 mA cm^(-2)and durability exceeding 100 h,as well as high mass activity up to 153 mA mg^(-1)_(Ru)at 1.5 V vs.reversible hydrogen electrode(RHE).This work provides valuable guidance for preparing highly active and stable Ru-based catalysts for acidic OER.
基金National Natural Science Foundation of China(51971103)Key Research and Development Program in Gansu Province(20YF8GA052)。
文摘A suction casting experiment was conducted on Zr_(55)Cu_(30)Al_(10)Ni_(5)(at%)amorphous alloy.Using ProCAST software,numerical simulations were performed to analyze the filling and solidification processes.The velocity field during the filling process and the temperature field during the solidification process of the alloy melt under different process parameters were obtained.Based on the simulation results,a Zr-based amorphous alloy micro-gear was prepared via casting.The results indicate that increasing the suction casting temperature enhances the fluidity of alloy melt but induces unstable flow rate during filling,which is detrimental to complete filling.Zr-based amorphous micro-gears with a module of 0.6 mm,a tooth top diameter of 8 mm,and 10 teeth were prepared through the suction casting.X-ray diffraction and differential scanning calorimetry analyses confirm that the fabricated micro-gear exhibits characteristic amorphous structural features,demonstrating well-defined geometrical contours and satisfactory forming completeness.
基金supported by the Anhui Provincial Natural Science Foundation(No.2208085QE121)the Key Research&Development plan of Anhui Province(No.2022a05020016)+2 种基金the University Natural Science Research Project of Anhui Province(No.2023AH051084)the National Natural Science Foundation of China(No.52071078)the“Zhishan”Scholars Programs of Southeast University(No.2242021R41158).
文摘The inverse relationship between the saturation magnetic flux density(Bs)and coercivity(Hc)of Febased amorphous alloys is a very active research topic that has been extensively debated.In this work,we conducted a detailed investigation on the magnetic softness of Fe_(83.2-x)Co_(x)B_(10)C_(6)Cu_(0.8)(x=0 and 6 at.%)amorphous alloys based on analysis of the surface morphology,microstructure,magnetic anisotropy,and magnetic domain structure.Enhanced magnetic softness-magnetization synergy was realized in the present alloys by magnetic field annealing(MFA)during the de-stressing process.A dramatic 84%reduction of Hc to 2.2 A/m was achieved for the Co-doped alloy under MFA,exhibiting excellent magnetic performance with a superb Bs of 1.86 T.The consistency between the experimental results and theoretical analysis revealed that the MFA process can mitigate the trade-off between stress-induced anisotropy and induced uniaxial anisotropy owing to the homogenized structure formed by field annealing.Thus,the process favored a low Hc due to the significant continuous decline in the total magnetic anisotropy,which coincided well with the results of Magneto-optical Kerr microscopy.The study elucidates a mechanism for tuning Hc in Co-doped alloy systems and affords a possible pathway for softening amorphous alloys with high Bs.
基金supported by the National Key R&D Program of China under Grant No.2021YFA1400500the Strategic Priority Research Program of the Chinese Academy of Sciences under Grant No.XDB33000000+1 种基金the National Natural Science Foundation of China under Grant No.12334003the Beijing Municipal Natural Science Foundation under Grant Nos.JQ22001 and QY23014。
文摘Establishing the structure-property relationship in amorphous materials has been a long-term grand challenge due to the lack of a unified description of the degree of disorder.In this work,we develop SPRamNet,a neural network based machine-learning pipeline that effectively predicts structure-property relationship of amorphous material via global descriptors.Applying SPRamNet on the recently discovered amorphous monolayer carbon,we successfully predict the thermal and electronic properties.More importantly,we reveal that a short range of pair correlation function can readily encode sufficiently rich information of the structure of amorphous material.Utilizing powerful machine learning architectures,the encoded information can be decoded to reconstruct macroscopic properties involving many-body and long-range interactions.Establishing this hidden relationship offers a unified description of the degree of disorder and eliminates the heavy burden of measuring atomic structure,opening a new avenue in studying amorphous materials.
基金supported by the National Key R&D Program of China(2018YFA0702001)National Natural Science Foundation of China(22371268,22301287)+3 种基金Fundamental Research Funds for the Central Universities(WK2060000016)Anhui Provincial Natural Science Foundation(2208085J09,2208085QB33)Collaborative Innovation Program of Hefei Science Center,CAS(2022HSC-CIP020)Youth Innovation Promotion Association of the Chinese Academy of Science(2018494)and USTC Tang Scholar.
文摘The hydrazine oxidation reaction(HzOR)has garnered significant attention as a feasible approach to replace sluggish anodic reactions to save energy.Nevertheless,there are still difficulties in developing highly efficient catalysts for the HzOR.Herein,we report amorphous ruthenium nanosheets(a-Ru NSs)with a thickness of approximately 9.6 nm.As a superior bifunctional electrocatalyst,a-Ru NSs exhibited enhanced electrocatalytic performance toward both the HzOR and hydrogen evolution reaction(HER),outperforming benchmark Pt/C catalysts,where the a-Ru NSs achieved a work-ing potential of merely-76 mV and a low overpotential of only 17 mV to attain a current density of 10 mA·cm^(-2) for the HzOR and HER,respectively.Furthermore,a-Ru NSs displayed a low cell voltage of 28 mV at 10 mA·cm^(-2) for overall hy-drazine splitting in a two-electrode electrolyzer.In situ Raman spectra revealed that the a-Ru NSs can efficiently promote N‒N bond cleavage,thereby producing more*NH_(2)and accelerating the progress of the reaction.
基金Major Science and technology projects of Anhui Province (202103a05020003)。
文摘[Background and purposes]Proton exchange membrane fuel cells(PEMFCs),which convert hydrogen energy directly into electrical energy and water,have received overwhelming attention,owing to their potential to significantly reduce energy consumption,pollution emissions and reliance on fossil fuels.Bipolar plates are the major part and key component of PEMFCs stack,which provide mechanical strength,collect and conduct current segregate oxidants and reduce agents.They contribute 70-80%weight and 20-30%cost of a whole stack,while significantly affecting the power density.There are three types plates,including metal bipolar plate,graphite bipolar plate and composite bipolar plate.Stainless steel bipolar plates,as one of metal bipolar plate,exhibit promising manufacturability,competitive cost and durability among various metal materials.However,stainless steel would be corroded in the harsh acid(pH 2-5)and humid PEMFCs environment,whereas the leached ions will contaminate the membrane.In addition,the passivated film formed on the surface will increase the interfacial contact resistance(ICR).In order to improve the corrosion resistance and electrical conductivity of steel bipolar plates,surface coatings are essential.Metal nitride coatings,metal carbide coatings,polymer coatings and carbon-based coatings have been introduced in recent years.Carbon-based coatings,mainly including a-C(amorphous Carbon),Ta-C(Tetrahedral amorphous carbon)and DLC(diamond-like carbon),have attracted considerable attention from both academia and industry,owing to their superior performance,such as chemical inertness,mechanical hardness and electrical conductivity.However,Ta-C films as protective coating of PEMFCs have been rarely reported,due to the difficulty in production for industrial application.In this paper,multi-layer Ta-C composite films were produced by using customized industrial-scale vacuum equipment to address those issues.[Methods]Multiple layered Ta-C coatings were prepared by using PIS624 equipment,which assembled filtered cathodic arc evaporation,ion beam and magnetron sputtering into one equipment,while SS304 and silicon specimens were used as substrate for testing and analysis.Adhesion layer and intermediate layer were deposited by using magnetron sputtering at deposition temperature of 150℃and pressure of 3×10^(−1) Pa,while the sputtering current was set to be 5 A and bias power to be 300 V.The Ta-C layer was coated at arc current of 80-100 A,bias voltage of 1500 V and gas flow of 75 sccm.A scanning electron microscope(CIQTEK SEM3200)was used to characterize surface morphology,coating structure and cross-section profile of the coatings.Raman spectrometer(LabRam HR Evolution,HORIBA JOBIN YVON)was used to identify the bonding valence states.Electrochemical tests were performed by using an electrochemical work station(CHI760,Shanghai Chenhua Instrument Co.,Ltd.),with the traditional three electrode system,where saturated Ag/AgCl and platinum mesh were used as the reference electrode and counter electrode,respectively.All samples were mounted in plastic tube and sealed with epoxy resin,with an exposure area of 2.25 cm^(2),serving as the working electrode.Electrochemical measurements were carried out in simulated PEMFCs cathode environment in 0.5 mol·L^(−1) H_(2)SO_(4)+5 ppm F−solution,at operating temperature of 70℃.As the cathode environment was harsher than the anode environment,all the samples are stabilized at the open-circuit potential(OCP)for approximately 30 min before the EIS measurements.ICR between bipolar plates and GDL was a key parameter affecting performance of the PEMFCs stack.The test sample sandwiched between 2 pieces of carbon paper(simulate gas diffusion layer,GDL)was placed between 2 gold-plated copper electrodes at a compaction pressure of 1.4 MPa,which was considered to be the conventional compaction pressure in the PEMFCs.Under the same conditions,the resistance of a single carbon paper was measured as well.The ICR was calculated according to the formula ICR=1/2(R2−R1)×S,where S was the contact area between GDL and coated stainless steel BPPs.All data of ICR were measured three times for averaging.[Results]The coatings deposited by filtered cathodic arc technology were compact and smooth,which reduced coating porosity and favorable to corrosion resistance.The coating thickness of adhesion and intermediate layers were 180 nm,while the protective Ta-C coating thickness was about 300 nm,forming multiple coating to provide stronger protection for metal bipolar plates.Cr,Ti,Nb and Ta coatings were selected as adhesion layers for comparison.According to electrochemical test,Ta and Nb coatings have higher corrosion resistance.However,Ta and Nb materials would be costly when they are used for mass production.Relatively,Cr and Ti materials were cost effective.Hence,a comprehensive assessment was indispensable to decide the materials to be selected as adhesion layer.Ta-TiN and Ti-TiN combined adhesion and intermediate layer exhibited stronger corrosion resistance,with the corrosion current to be less than 10^(−6) A·cm^(−2).Ta-C protective coating deposited by using filtered cathodic arc technology indicated displayed higher corrosion resistance,with the average corrosion density to be about 1.26×10^(−7) A·cm^(−2).Ta-C coating also shown larger contact angle,with the highest hydrophobicity,which was one of the important advantages for Ta-C,in terms of corrosion resistance.According to Raman spectroscopy,the I(D)/I(G)=549.8/1126.7=0.487,with the estimated fraction of sp^(3) bonding to be in the range of 5154%.The intermediate layer TiN has higher conductivity than the CrN layer.Considering cost,corrosion performance and ICR result,the Ti-TiN layer combination is recommended for industrial scale application.[Conclusions]Multiple layer coating structure of Ta-C film had stronger corrosion resistance;with more than 50%sp^(3) content,while it also had larger water contact angle and higher corrosion resistance than DLC film.The filtered arcing deposition technology was able to make the film to be more consistent and stable than normal arcing technology in terms of the preparation of Ta-C.The coating displayed corrosion density of 1.26×10^(−7) A·cm^(−2) and ICR of less than 5 mΩ·cm^(2),far beyond technical target of 2025 DOE(US Department of Energy).This indicated that the mass-production scale coating technology for PEMFC bipolar plates is highly possible.
文摘Noble metal-based intermetallic compounds(IMCs)with ordered atomic arrangements exhibit remarkable electrocatalytic activity owing to their unique crystal and electronic structures.During the past years,great advance has been made in the development of noble metal-based IMCs.Recently,Lu and coworkers reported ultrathin“amorphous/intermetallic”(A/IMC)heterophase PtPbBi nanosheets(NSs)with a thickness of 2.5±0.3 nm.The oxidative etching effect caused by the coexistence of O_(2)and Br^(-)ions plays a crucial role in the formation of the IMC and unique two-dimensional structure with irregular shapes and curled edges.This study shows that fabricating an A/IMC heterophase structure with a multimetallic composition can effectively enhance the catalytic performances of noble metal-based electrocatalysts.
基金Project supported by funding from the National Natural Science Foundation of China(Grant Nos.52172258,52473227 and 52171150)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB0500200)。
文摘The unique long-range disordered atomic arrangement inherent in amorphous materials endows them with a range of superior properties,rendering them highly promising for applications in catalysis,medicine,and battery technology,among other fields.Since not all materials can be synthesized into an amorphous structure,the composition design of amorphous materials holds significant importance.Machine learning offers a valuable alternative to traditional“trial-anderror”methods by predicting properties through experimental data,thus providing efficient guidance in material design.In this study,we develop a machine learning workflow to predict the critical casting diameter,glass transition temperature,and Young's modulus for 45 ternary reported amorphous alloy systems.The predicted results have been organized into a database,enabling direct retrieval of predicted values based on compositional information.Furthermore,the applications of high glass forming ability region screening for specified system,multi-property target system screening and high glass forming ability region search through iteration are also demonstrated.By utilizing machine learning predictions,researchers can effectively narrow the experimental scope and expedite the exploration of compositions.
文摘Carbon nanotubes(CNTs)reinforced copper(CNTs/Cu)is one of the most promising and extensively researched materials for replacing traditional Cu-based materials in high-load and high-current applications,particularly within the aerospace industry.Amorphous carbon nanotubes(aCNTs)are a type of carbon nanotubes characterized by the presence of mesopores distributed across their amorphous sidewalls,facilitating connectivity between the hollow core and the external environment.Therefore,we propose utilizing aCNTs as a reinforcing agent for Cu.The mesoporous structure of aCNTs facilitates the interpenetration of Cu into the aCNTs,thereby maintaining the continuity of the matrix properties.Experimental results demonstrate that Cu effectively penetrates the mesoporous sidewalls of aCNTs.Both pure Cu and aCNTs-reinforced Cu exhibit comparable electrical conductivity,while the hardness of the aCNTs/Cu composite is significantly enhanced.Additionally,both the density and porosity of aCNTs/Cu are lower than those of pure Cu,and the introduction of aCNTs helps to reduce the sintering temperature.
基金financially supported by the National Nature Science Foundation of China(Nos.22209125,22479118,and 22479117)the National Key Research and Development Program of China(No.2021YFB3800300)
文摘Polyanionic materials are considered one of the most promising cathode materials for sodium-ion batteries because of the stable structure framework and high working voltage.However,most polyanionic materials possess limited sodium storage sites and have to undergo complex local structure evolution during charge/discharge.Herein,we conducted a systematic investigation into the impact of structural forms of NaVOPO_(4)on the electrochemical properties.Amorphous and crystalline NaVOPO_(4)are synthesized through a controlled reflux reduction method,and the amorphous NaVOPO_(4)(a-NVOP)demonstrates much better electrochemical performance compared to the crystalline counterpart.Specifically,the a-NVOP electrode delivers high reversible capacity(142 mAh g^(-1)at 14.5 mA g^(-1),close to the theoretical capacity of 145 mAh g^(-1)),high energy density(497 Wh kg^(-1)based on cathode material)and remarkable cyclability with capacity retention of 80%after 500 cycles.In situ and ex situ experimental analyses and theoretical calculations reveal that the superior performance is primarily due to the maintaining of the amorphous state during the charge/discharge process to endow high stability and accelerated intercalation/deintercalation of large-sized Na^(+)without lattice constraints.Furthermore,the amorphous cathode materials show promising electrochemical properties in lithium-,potassium-and zinc-ion batteries,highlighting their broad adaptability and potential across various battery systems.
基金supported by National Natural Science Foundation of China(51761034,51961032,51962028 and 52261041)Innovation Foundation of Inner Mongolia University of Science and Technology(2019YQL03)+2 种基金Major Science and Technology Project of Inner Mongolia(2021ZD0029)Program for Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(NJYT23005,NJYT23007)Program for Innovative Research Team in Universities of Inner Mongolia Autonomous Region(NMGIRT2401).
文摘Mg_(x)(Ni_(0.8)La_(0.2))_(100-x),where x=60,70,80,exhibiting a nanocrystalline microstructure,were prepared through the crystallization of amorphous alloys.The investigation encompassed the phase constitution,grain size,microstructural stability,and hydrogen storage properties.Crystallization kinetics,along with in-situ high-energy XRD characterization,revealed a concentrated and synchronous crystallization of Mg_(2)Ni and RE-Mg-Ni ternary phases with the increase in La and Ni content.The attributed synchronous crystallization process was found to be a result of the close local affinity of Mg_(2)Ni and RE-Mg-Ni ternary phases,as assessed by the thermodynamic Miedema model.Significant secondary phase pinning effect,arising from the high likelihood of well-matching phase structures between Mg_(2)Ni,LaMg_(2)Ni,and LaMgNi_(4),was validated through both the edge-to-edge matching model prediction and experimental observation.Thefine and homogeneous microstructure was shown to be a consequence of fast crystallization kinetics and the secondary phase pinning effect.Improved activation performance and cycling stability were observed,stemming from grain refinement and excellent microstructural stability.Our study provides insights into mechanism of grain refinement of nanocrystalline microstructure tailored by phase constitution and crystallization kinetics in the amorphous-crystallization route.We also demonstrate the potential of material design guided by phase equilibria and crystallographic predictions to improve nanocrystalline with excellent microstructural stability.
基金support on this research from the Talent Training Program of Yunnan of China(Grant Nos.202005AC160041 and KKXY202252002)the"Xingdian Talent"Industry Innovation Talent Program in Yunnan Province(Grant No.XDYC-CYCX-2022-0042)。
文摘At present,the most common preparation method of amorphous boron powder is magnesium thermal reduction method,but the amorphous boron powder obtained by this method mostly contains impurities such as magnesium and oxygen which are difficult to remove,and these impurities will seriously affect the application of amorphous boron powder and need to be strictly removed.In this research,the acid-insoluble impurities were modified through sintering and quenching,while the magnesium impurities were optimized via ultrasonic acid leaching.We observed that the quenching temperature played a crucial role in determining the efficiency of magnesium impurity removal.The results show that the magnesium content in amorphous boron powder can be reduced from 5.67%to 2.40%by quenching the amorphous boron powder at 800°C and using ultrasonic assisted acid leaching.Furthermore,the oxidation reaction of boron is influenced by the powder's particle size and specific surface area,with the effective activation energy being intimately tied to both these factors.Post-quenching and acid leaching,we observed an increase in the specific surface area of the boron powder samples,leading to enhanced activity.In conclusion,our study presents an effective strategy to mitigate magnesium impurities and elevate the performance of amorphous boron powder,offering promising avenues for advancing its utilization across diverse industries.
基金supported by the National Key R&D Program of China(No.2021YFE0100600)the National Natural Science Foundation of China(Nos.92166103,U23A20621,and 92066202)+1 种基金the Top-Notch Young Talents Program of Hubei.Yasir is grateful for financial support from the Pakistan Science Foundation(Project Reference:PSF/CRP-18th Protocol(05))the State Key Laboratory of Materials Processing and Die&Mould Technology(Project Reference:2021-008).
文摘Achieving a delicate synergy between mechanical robustness and antifouling attributes in coatings remains a formidable challenge for marine applications. Inspired by the assembly of nacre, we present a novel approach to fabricate a nacre-like metallic coating. This coating comprises an amorphous matrix with excellent anti-corrosion and anti-wear properties, as well as Cu-rich 3D interconnected channels for antifouling function. The coating is produced by high velocity oxygen fuel (HVOF) thermal spraying of surface-modified Fe-based amorphous powders with a Cu-layer. The resulting coating exhibits exceptional mechanical robustness, including high resistance to erosion, abrasion, and impact, surpassing conventional polymer antifouling coatings. Furthermore, the controlled Cu+ leaching capability of the in-situ constructed 3D interconnected diffusion channels, facilitated by the Cu-rich intersplats, contributes to the remarkable antifouling performance. This includes nearly 100 % resistance to bacterial adhesion after 1 day of immersion and over 98 % resistance to algal attachment after 7 d of immersion, resulting in a prolonged service lifetime. Notably, even after 200 cycles of wear damage, the Cu-modified amorphous coating still maintains its excellent antifouling properties. The Cu-rich intersplats play a critical role in transporting and sustainably leaching Cu ions, thereby accounting for the outstanding antifouling performance. Ultimately, we aim to advance the design of high-performance coatings suited for diverse marine applications, where both the mechanical robustness and antifouling properties are essential.
基金supported by a project of the Tsinghua Shenzhen International Graduate School-Shenzhen Pengrui Young Faculty Program of Shenzhen Pengrui Foundation(Grant No.SZPR2023007)Natural Science Foundation of Sichuan Province(Grant No.2025ZNSFSC0449)Shenzhen Science and Technology Program(Grant No.RCBS20231211090637065).
文摘Lithium-ion batteries with LiCoO_(2)(LCO)cathodes are widely used in various electronic devices,resulting in a large amount of spent LCO(SLCO).Therefore,there is an urgent need for an efficient technique for recycling SLCO.However,due to the presence of cobalt oxide with a spinel phase on the surface of highly-degraded LCO,the strong electrostatic repulsion from the transition metal octahedron poses a high Li replenishment barrier,making the regeneration of highly-degraded LCO a challenge.Herein,we propose a structural transformation strategy for reconstructing Li replenishment channels to aid the direct regeneration of highly-degraded LCO.In this approach,ball milling is employed to disrupt the inherent structure of highly-degraded LCO,thereby releasing the internal stress and converting the surface spinel phase into a homogeneous amorphous structure,which promotes Li insertion and regeneration.The regenerated LCO(RLCO)exhibits an outstanding discharge capacity of 179.10 mAh·g^(−1) in the voltage range of 3.0–4.5 V at 0.5 C.The proposed strategy is an effective regeneration approach for highly-degraded LCO,thereby facilitating the efficient recycling of spent lithium-ion battery cathode materials.
基金Project supported by the National Natural Science Foundation of China(22072096,22108184)。
文摘In this work,a series of Ce-Ti composite oxides with different Ti/Ce molar ratios was prepared by coprecipitation method,and investigated for the catalytic degradation of toluene and selective catalytic reduction of NO.The phase transition process between Ce species and Ti species is limited by modulating the interaction between Ce4+and Ti4+,while a completely amorphous composite is generated with an appropriate molar ratio of Ti/Ce(1.5/1).The catalyst CeTi1.5Oxexhibits the best catalytic performance,where the values of T90and T50for deep degradation of toluene are 297 and 330℃respectively at high weight hours space velocity(WHSV=120000 mL/(g·h)).Compared with CeO_(2),T90and T50decrease by48 and 34℃respectively while declining by 67 and 70℃compared to TiO_(2).For the SCR reaction,CeTi1.5Oxreaches 100%NO conversion at 250℃with WHSV=60000 mL/(g·h),reduced by 50℃compared to pure CeO_(2).The amorphous nanostructure with highly dispersed Ce and Ti species was confirmed by transmission electron microscopy(TEM)and X-ray diffraction(XRD)characterizations.The X-ray photoelectron spectroscopy(XPS)and Raman analyses show that a large number of active Ce-O-Ti species and surface oxygen vacancies are generated due to the strong interaction between Ti^(4+)and Ce^(4+)in CeTi_(1.5)O_(x).Additionally,H_(2)-TPR and O_(2)-TPD further confirm that the interaction promotes the low-temperature reducibility and mobility of surface-active oxygen species.Meanwhile,in-situ DRIFTS study reveals that CeTi1.5Oxwith amorphous nanostructure can dramatically enhance the dissociative and complete oxidation capacity for toluene.
基金financially supported by the Yancheng Polytechnic College School-Level Scientific Research, China (No. ygy1903)the National Natural Science Foundation of China (Nos. 52001163, 52075237, and 52371157)+2 种基金the Open Project of Taihu Laboratory of Deep-Sea Technology Science, Key Research and Development Plan of Jiangsu Province, China (No. BE2019119)supported by the Priority Academic Program Development of Jiangsu Higher Education Institution (PAPD), Chinathe research funding for the Jiangsu Specially-Appointed Professor Program, China。
文摘Recent advancements in electrocatalysis have highlighted the exceptional application value of amorphous electrocatalysts. Withtheir unique atomic configurations, these electrocatalysts exhibit superior catalytic performance compared to that of their crystalline coun-terparts. Transition metal(TM) amorphous ribbon-shaped electrocatalysts have recently emerged as a new frontier in the catalysis field.Dealloying is widely considered a fascinating method for enhancing the electrocatalyst performance. In this review, we comprehensivelyexamine the principles of water electrolysis, discuss the prevalent methods for fabricating ribbon-configured electrocatalysts, and providean overview of amorphous alloys. Furthermore, we discuss binary, ternary, and high-entropy amorphous TM-based electrocatalysts,which satisfy the requirements necessary for effective water electrolysis. We also propose strategies to enhance the activity of amorphousTM-based ribbons, including morphology control, defect engineering, composition optimization, and heterostructure creation in differentelectrolytes. Our focus extends to the latest developments in the design of heterogeneous micro/nanostructures, management of prepara-tion techniques, and synthesis of different compositions. Finally, we address the ongoing challenges and provide a perspective on the fu-ture development of broadly applicable, self-supporting TM ribbon-shaped electrocatalysts.
