Electrocatalysis is key to improving energy efficiency,reducing carbon emissions,and providing a sustainable way of meeting global energy needs.Therefore,elucidating electrochemical reaction mechanisms at the electrol...Electrocatalysis is key to improving energy efficiency,reducing carbon emissions,and providing a sustainable way of meeting global energy needs.Therefore,elucidating electrochemical reaction mechanisms at the electrolyte/electrode interfaces is essential for developing advanced renewable energy technologies.However,the direct probing of real-time interfacial changes,i.e.,the surface intermediates,chemical environment,and electronic structure,under operating conditions is challenging and necessitates the use of in situ methods.Herein,we present a new lab-based instrument commissioned to perform in situ chemical analysis at liquid/solid interfaces using ambient pressure X-ray photoelectron spectroscopy(APXPS).This setup takes advantage of a chromium source of tender X-rays and is designed to study liquid/solid interfaces by the“dip and pull”method.Each of the main components was carefully described,and the results of performance tests are presented.Using a three-electrode setup,the system can probe the intermediate species and potential shifts across the liquid electrolyte/solid electrode interface.In addition,we demonstrate how this system allows the study of interfacial changes at gas/solid interfaces using a case study:a sodium–oxygen model battery.However,the use of APXPS in electrochemical studies is still in the early stages,so we summarize the current challenges and some developmental frontiers.Despite the challenges,we expect that joint efforts to improve instruments and the electrochemical setup will enable us to obtain a better understanding of the composition–reactivity relationship at electrochemical interfaces under realistic reaction conditions.展开更多
The liquid/solid(L/S)interface of dissimilar metals is critical to the microstructure,mechanical strength,and structural integrity of interconnects in many important applications such as electronics,automotive,aeronau...The liquid/solid(L/S)interface of dissimilar metals is critical to the microstructure,mechanical strength,and structural integrity of interconnects in many important applications such as electronics,automotive,aeronautics,and astronautics,and therefore has drawn increasing research interests.To design preferential microstructure and optimize mechanical properties of the interconnects,it is crucial to understand the formation and growth mechanisms of diversified structures at the L/S interface during interconnecting.In situ synchrotron radiation or tube-generated X-ray radiography and tomography technologies make it possible to observe the evolution of the L/S interface directly and therefore have greatly propelled the research in this field.Here,we review the recent progress in understanding the L/S interface behaviors using advanced in situ X-ray imaging techniques with a particular focus on the following two issues:(1)interface behaviors in the solder joints for microelectronic packaging including the intermetallic compounds(IMCs)during refl ow,Sn dendrites,and IMCs during solidification and refl ow porosities and(2)growth characteristics and morphological transition of IMCs in the interconnect of dissimilar metals at high temperature.Furthermore,the main achievements and future research perspectives in terms of metallurgical bonding mechanisms under complex conditions with improved X-ray sources and detectors are remarked and discussed.展开更多
The detailed understanding of various underlying processes at liquid/solid interfaces requires the development of interface-sensitive and high-resolution experimental techniques with atomic precision.In this perspecti...The detailed understanding of various underlying processes at liquid/solid interfaces requires the development of interface-sensitive and high-resolution experimental techniques with atomic precision.In this perspective,we review the recent advances in studying the liquid/solid interfaces at atomic level by electrochemical scanning tunneling microscope(EC-STM),non-contact atomic force microscopy(NC-AFM),and surface-sensitive vibrational spectroscopies.Different from the ultrahigh vacuum and cryogenic experiments,these techniques are all operated in situ under ambient condition,making the measurements close to the native state of the liquid/solid interface.In the end,we present some perspectives on emerging techniques,which can defeat the limitation of existing imaging and spectroscopic methods in the characterization of liquid/solid interfaces.展开更多
Silicon is considered one of the most promising candidates for incorporation into carbon-based anodes in lithium-ion batteries(LIBs)due to its high specific capacity.However,the significant volume changes during charg...Silicon is considered one of the most promising candidates for incorporation into carbon-based anodes in lithium-ion batteries(LIBs)due to its high specific capacity.However,the significant volume changes during charge and discharge cycles lead to repeated reconstruction of the solid electrolyte interface(SEI)film and continuous loss of active lithium.Pre-lithiation method is regarded as a highly attractive approach for effectively compensating for active lithium loss during the charge and discharge cycles of LIBs.Constructing a stable SEI film is particularly crucial in the pre-lithiation process.In this study,we developed a direct contact pre-lithiation(DC-Pr)method to create a temperature-tailored robust SEI film interface on silicon-carbon(Si@C)electrodes.By investigating the morphology,structure,and composition of the SEI formed on Si@C electrodes at different pre-lithiation temperatures(50,25,0,and-25℃),we demonstrated that controlling the lithiation temperature to regulate the migration rate of lithium ions within the Si@C electrode yields a lithiated Si@C anode(25-Pr-Si@C)at 25℃ with a continuous,uniform SEI film(~3.65 nm)enriched with Li_(2)O-LiF,which exhibits synergistic effects.Importantly,the initial Coulombic efficiency(ICE)of 25-Pr-Si@C significantly improved from 85.4% in the unlithiated Si@C electrode(Blank-Si@C)to 106.1%.Additionally,the full cell configuration using a high areal loading of lithiated Si@C(~5.5 mA h cm^(-2))as the anode and NCM811 as the cathode(NCM811||25-Pr-Si@C)demonstrated superior cycling performance,maintaining 69.4% of capacity retention and achieving a Coulombic efficiency of over 99.7% after 150 cycles(0.5 C).Therefore,this simple and efficient experimental design provides a high-performance,controllable,and scalable pre-lithiation method for LIBs,paving the way for the commercialization of LIBs utilizing pre-lithiation techniques.展开更多
Aqueous zinc metal batteries(ZMBs)are promising for grid-scale energy storage,but their practical application is hindered by limited cycling life and inferior low-temperature performance,primarily due to Zn dendrite g...Aqueous zinc metal batteries(ZMBs)are promising for grid-scale energy storage,but their practical application is hindered by limited cycling life and inferior low-temperature performance,primarily due to Zn dendrite growth and parasitic reactions at the electrolyte-electrode interface.To address these challenges,we develop a new and cheap hydrated eutectic electrolyte(HEE)composed of ZnCl_(2),choline chloride(ChCl),and H_(2)O,which can fundamentally tune desirable interface chemistries for dendrite-free and low-temperature ZMBs.The optimized HEE with a solvation structure of ZnCl_(3)(ChCl)(H_(2)O)_(2) shows a high co nductivity of 15.98 mS cm^(-1)and excellent freeze resistance below-40℃.It has been found that hydrogen bonding between ChCl and H_(2)O effectively reduces water activity,while preferential adsorption of ChCl molecules at the inner Helmholtz plane promotes the formation of a protective solid electrolyte interphase(SEI)on Zn metal anodes,which greatly suppresses the dendrites and side reactions.Therefore,the HEE endows the as-fabricated Zn//Zn symmetric cells and Zn//polyaniline full batteries with superior electrochemical performance at-40℃,such as a long cycling life of 870 h at 1 mA cm^(-2)and 1 mAh cm^(-2)and a high capacity of 75 mAh g^(-1)at 0.3 A g^(-1).The HEE reported here may pave a new way to construct high-performance ZMBs for specific low-temperature application scenarios.展开更多
We study the effects of gas adsorption on the dynamics and stability of nanobubbles at the solid–liquid interface. The phase diagram and dynamic evolution of surface nanobubbles were analyzed under varying equilibriu...We study the effects of gas adsorption on the dynamics and stability of nanobubbles at the solid–liquid interface. The phase diagram and dynamic evolution of surface nanobubbles were analyzed under varying equilibrium adsorption constant.Four distinct dynamic behaviors appear in the phase diagram: shrinking to dissolution, expanding to bursting, shrinking to stability, and expanding to stability. Special boundary states are identified in phase diagram, where the continuous growth of nanobubbles can take place even under very weak gas–surface interaction or with very small initial bubble size. Surface adsorption plays a critical role in the stability, lifetime, radius, and contact angle of nanobubbles, thereby demonstrating that pinning is not a prerequisite for stabilization. Furthermore, stable equilibrium nanobubbles exhibit a characteristic range of footprint radius, a limited height, and a small contact angle, consistent with experimental observations.展开更多
Lithium-ion batteries are at the forefront of modern energy storage technology.However,the accumulation of by-products such as ethylene and carbon dioxide during charging and discharging cycles reduces battery effecti...Lithium-ion batteries are at the forefront of modern energy storage technology.However,the accumulation of by-products such as ethylene and carbon dioxide during charging and discharging cycles reduces battery effective capacity and threatens large-scale safe performance.With significant advantages over ethylene carbonate(EC)electrolytes,fluorinated electrolytes can more effectively suppress internal gas evolution,thereby improving battery safety and cycling stability.To reveal the mechanism behind gas formation in lithium-ion batteries,our study investigated the transport behavior and interfacial products of fluorinated electrolytes under various operation conditions,including electrode material and electrolyte composition.Innovatively,we applied the reaction network integrator ReacNetGenerator to the analysis of the solid electrolyte interface(SEI)in lithium batteries,providing more molecular fingerprint information from the perspective of specific products.Using reactive molecular dynamics(MD)simulations with the ReaxFF force field and EChemDID,complemented by density functional theory(DFT)calculations,our results demonstrate that fluorinated electrolytes can effectively suppress the decomposition of LiPF_(6) to produce toxic gases PFs and PF_3.DFT analysis further reveals that highly fluorinated solvents(e.g.,FEMC)enhance the anti-reduction stability of PF_(6)~-through synergistic regulation of molecular orbital energy levels,thermodynamic electron affinity,charge transfer,and electrostatic potential distribution,thereby mitigating LiPF_(6) decomposition.Additionally,fluorinated electrolytes generate significantly more LiF components than non-fluorinated ones to promote the formation of a stable and durable solid electrolyte interface(SEI).Experimental validations via XPS and GC-MS confirm reduced CO_(2) generation and LiF-enriched SEI formation,aligning with simulation and DFT data.The findings provide valuable insights for the design of advanced electrolytes aimed at ensuring large-scale,safe energy storage solutions.展开更多
Nonlinear reflection of SV shear wave at the isotropic solid-solid interfaces is experimentally studied. The reflected second harmonic SV shear wave is measured for glass-air,glass-iron, copper and aluminum interfaces...Nonlinear reflection of SV shear wave at the isotropic solid-solid interfaces is experimentally studied. The reflected second harmonic SV shear wave is measured for glass-air,glass-iron, copper and aluminum interfaces. The relation of nonlinear reflective coefficient with the incident angle and linear as well as nonlinear characteristics of the materials is thoroughly investigated. Comparison of the experiment with the theory gives qualitatively agreement.展开更多
Due to its high theoretical capacity(820 mAh g^(−1)),low standard electrode potential(−0.76 V vs.SHE),excellent stability in aqueous solutions,low cost,environmental friendliness and intrinsically high safety,zinc(Zn)...Due to its high theoretical capacity(820 mAh g^(−1)),low standard electrode potential(−0.76 V vs.SHE),excellent stability in aqueous solutions,low cost,environmental friendliness and intrinsically high safety,zinc(Zn)-based batteries have attracted much attention in developing new energy storage devices.In Zn battery system,the battery performance is significantly affected by the solid electrolyte interface(SEI),which is controlled by electrode and electrolyte,and attracts dendrite growth,electrochemical stability window range,metallic Zn anode corrosion and passivation,and electrolyte mutations.Therefore,the design of SEI is decisive for the overall performance of Zn battery systems.This paper summarizes the formation mechanism,the types and characteristics,and the characterization techniques associated with SEI.Meanwhile,we analyze the influence of SEI on battery performance,and put forward the design strategies of SEI.Finally,the future research of SEI in Zn battery system is prospected to seize the nature of SEI,improve the battery performance and promote the large-scale application.展开更多
Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this ...Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this paper,homotype heterojunctions are designed on HC to induce the generation of stable solid electrolyte interfaces,which can effectively increase the ICE of HC from 64.7%to 81.1%.The results show that using a simple surface engineering strategy to construct a homotypic amorphous Al_(2)O_(3) layer on the HC could shield the active sites,and further inhibit electrolyte decomposition and side effects occurrence.Particularly,due to the suppression of continuous decomposition of NaPF 6 in ester-based electrolytes,the accumulation of NaF could be reduced,leading to the formation of thinner and denser solid electrolyte interface films and a decrease in the interface resistance.The HC anode can not only improve the ICE but elevate its sodium storage performance based on this homotype heterojunction composed of HC and Al_(2)O_(3).The optimized HC anode exhibits an outstanding reversible capacity of 321.5mAhg^(−1) at 50mAg^(−1).The cycling stability is also improved effectively,and the capacity retention rate is 86.9%after 2000 cycles at 1Ag^(−1) while that of the untreated HC is only 52.6%.More importantly,the improved sodium storage behaviors are explained by electrochemical kinetic analysis.展开更多
The (100) texture of solidified fcc metals, caused by the preferential (100) dendrite growth, could be closeIy related to solid/melt interfaces which behave differently along different crystallographic orientation. Th...The (100) texture of solidified fcc metals, caused by the preferential (100) dendrite growth, could be closeIy related to solid/melt interfaces which behave differently along different crystallographic orientation. The stability and roughness of {111} and {100} solid/melt interfaces of fcc metals were investigated using a modified Temkin multi-layer model. It is demonstrated that {100}crystal/melt interface is more unstable and rougher than {111} interface. The effect of the stability of crystal/melt interface on the (100) texture formation in solidified fcc metals has been analysed and discussed.展开更多
The effect of the pulsed magnetic field on the grain refinement of superalloy K4169 has been studied in directional solidification.In the presence of the solid-liquid interface condition,the distributions of the elect...The effect of the pulsed magnetic field on the grain refinement of superalloy K4169 has been studied in directional solidification.In the presence of the solid-liquid interface condition,the distributions of the electromagnetic force,flow field,temperature field,and Joule heat in front of the solid-liquid interface in directional solidification with the pulsed magnetic field are simulated.The calculation results show that the largest electromagnetic force in the melt appears near the solid-liquid interface,and the electromagnetic force is distributed in a gradient.There are intensive electromagnetic vibrations in front of the solid-liquid interface.The forced melt convection is mainly concentrated in front of the solid-liquid interface,accompanied by a larger flow velocity.The simulation results indicate that the grain refinement is attributed to that the electromagnetic vibration and forced convection increase the nucleation rate and the probability of dendrite fragments survival,for making dendrite easily fragmented,homogenizing the melt temperature,and increasing the undercooling in front of the solid-liquid interface.展开更多
Transition metal selenides have been widely studied as anode materials of sodium ion batteries(SIBs),however,the investigation of solid-electrolyte-interface(SEI)on these materials,which is critical to the electrochem...Transition metal selenides have been widely studied as anode materials of sodium ion batteries(SIBs),however,the investigation of solid-electrolyte-interface(SEI)on these materials,which is critical to the electrochemical performance of SIBs,remains at its infancy.Here in this paper,ZnSe@C nanoparticles were prepared from ZIF-8 and the SEI layers on these electrodes with and without reduced graphene oxide(rGO)layers were examined in details by X-ray photoelectron spectroscopies at varied charged/discharged states.It is observed that fast and complicated electrolyte decomposition reactions on ZnSe@C leads to quite thick SEI film and intercalation of solvated sodium ions through such thick SEI film results in slow ion diffusion kinetics and unstable electrode structure.However,the presence of rGO could efficiently suppress the decomposition of electrolyte,thus thin and stable SEI film was formed.ZnSe@C electrodes wrapped by rGO demonstrates enhanced interfacial charge transfer kinetics and high electrochemical performance,a capacity retention of 96.4%,after 1000 cycles at 5 A/g.This study might offer a simple avenue for the designing high performance anode materials through manipulation of SEI film.展开更多
Owing to its low potential, crustal abundances and environmental friendliness, calcium metal anode(CMA) is emerging as a powerful contender in post-lithium era. However, the passivation of CMA fatally hinders its deve...Owing to its low potential, crustal abundances and environmental friendliness, calcium metal anode(CMA) is emerging as a powerful contender in post-lithium era. However, the passivation of CMA fatally hinders its development. Recently, several feasible electrolytes have been developed. Nevertheless, as a pivotal part, the solid electrolyte interface(SEI) formed on CMA has not been paid enough attention to. In this review, based on the passivation mechanism of CMA, the favorable composition of SEI is emphasized with the corresponding electrolytes. It is considered that boron-containing and organic–inorganic hybrid SEI might be preferred. By comparing electrolytes and SEI on CMA with lithium and magnesium metal anodes, the root causes of CMA passivation are further elaborated, enlightening rational design rules of suitable SEI. Furthermore, some noteworthy details when assembling secondary calcium metal batteries(CMBs) are put forward. It is expected that deeper understanding of SEI on CMA will promote the development of CMBs.展开更多
The solid/liquid interface of a directionally solidified Ni-base superalloy with different phosphorus contents was quantitatively described by means of fractat method.When the solidification rate was fixed,the relatio...The solid/liquid interface of a directionally solidified Ni-base superalloy with different phosphorus contents was quantitatively described by means of fractat method.When the solidification rate was fixed,the relationship between the fractal dimensionality of the solid/liquid interface and the phos- phorus content of the test alloy was given.Combined the thermodynamics and fractal theory,the ef- fect mechanism of phosphorus content on fractal dimensionality of the solid/liquid interface was discussed.展开更多
Thermal rectification refers to the phenomenon by which the magnitude of the heat flux in one direction is much larger than that in the opposite direction.In this study,we propose to implement the thermal rectificatio...Thermal rectification refers to the phenomenon by which the magnitude of the heat flux in one direction is much larger than that in the opposite direction.In this study,we propose to implement the thermal rectification phenomenon in an asymmetric solid–liquid–solid sandwiched system with a nano-structured interface.By using the non-equilibrium molecular dynamics simulations,the thermal transport through the solid–liquid–solid system is examined,and the thermal rectification phenomenon can be observed.It is revealed that the thermal rectification effect can be attributed to the significant difference in the interfacial thermal resistance between Cassie and Wenzel states when reversing the temperature bias.In addition,effects of the liquid density,solid–liquid bonding strength and nanostructure size on the thermal rectification are examined.The findings may provide a new way for designs of certain thermal devices.展开更多
We propose a scheme to implement quantum state transfer between two distant quantum nodes via a hybrid solid–optomechanical interface. The quantum state is encoded on the native superconducting qubit, and transferred...We propose a scheme to implement quantum state transfer between two distant quantum nodes via a hybrid solid–optomechanical interface. The quantum state is encoded on the native superconducting qubit, and transferred to the microwave photon, then the optical photon successively, which afterwards is transmitted to the remote node by cavity leaking,and finally the quantum state is transferred to the remote superconducting qubit. The high efficiency of the state transfer is achieved by controllable Gaussian pulses sequence and numerically demonstrated with theoretically feasible parameters.Our scheme has the potential to implement unified quantum computing–communication–computing, and high fidelity of the microwave–optics–microwave transfer process of the quantum state.展开更多
The reversibility and stability of aqueous Zn metal batteries(AZMBs)are largely limited by Zn dendrites and interfacial parasitic reactions.Herein,we propose a parallel modulation strategy to boost the reversibility o...The reversibility and stability of aqueous Zn metal batteries(AZMBs)are largely limited by Zn dendrites and interfacial parasitic reactions.Herein,we propose a parallel modulation strategy to boost the reversibility of the Zn anode by introducing N,N,N',N'-tetramethylchloroformamidinium hexafluorophosphate(TCFH)as an additive in the electrolyte.TCFH is composed of PF6-and TN+with opposite charges.PF6-can spontaneously induce the in-situ generation of ZnF_(2)solid electrolyte interface(SEI)on the anode,which can improve the transport kinetics of Zn^(2+)at the interface,thus promoting the rapid and uniform deposition of Zn as well as inhibiting the growth of dendrites.In addition,TN+is enriched at the anode surface during Zn deposition through the anchoring effect,which brings a reconfiguration of the ion/molecule distribution.The anchored-TN+reduces the concentrations of H_(2)O and SO_(4)^(2-),sufficiently restraining the parasitic reaction.Thanks to the dual-phase interface engineering constructed of PF6-and TN+in parallel,the symmetric cell with the proposed electrolyte survives long cycling stability over750 h at 20 mA cm^(-2),10 mAh cm^(-2).This study offers a distinct viewpoint to the multidimensional optimization of Zn anodes for high-performance AZMBs.展开更多
Considering the growing pre-lithiation demand for high-performance Si-based anodes and consequent additional costs caused by the strict pre-lithiation environment,developing effective and environmentally stable pre-li...Considering the growing pre-lithiation demand for high-performance Si-based anodes and consequent additional costs caused by the strict pre-lithiation environment,developing effective and environmentally stable pre-lithiation additives is a challenging research hotspot.Herein,interfacial engineered multifunctional Li_(13)Si_(4)@perfluoropolyether(PFPE)/LiF micro/nanoparticles are proposed as anode pre-lithiation additives,successfully constructed with the hybrid interface on the surface of Li_(13)Si_(4)through PFPE-induced nucleophilic substitution.The synthesized multifunctional Li_(13)Si_(4)@PFPE/LiF realizes the integration of active Li compensation,long-term chemical structural stability in air,and solid electrolyte interface(SEI)optimization.In particular,the Li_(13)Si_(4)@PFPE/LiF with a high pre-lithiation capacity(1102.4 mAh g^(-1))is employed in the pre-lithiation Si-based anode,which exhibits a superior initial Coulombic efficiency of 102.6%.Additionally,in situ X-ray diffraction/Raman,density functional theory calculation,and finite element analysis jointly illustrate that PFPE-predominant hybrid interface with modulated abundant highly electronegative F atoms distribution reduces the water adsorption energy and oxidation kinetics of Li_(13)Si_(4)@PFPE/LiF,which delivers a high pre-lithiation capacity retention of 84.39%after exposure to extremely moist air(60%relative humidity).Intriguingly,a LiF-rich mechanically stable bilayer SEI is constructed on anodes through a pre-lithiation-driven regulation for the behavior of electrolyte decomposition.Benefitting from pre-lithiation via multifunctional Li_(13)Si_(4)@PFPE/LiF,the full cell and pouch cell assembled with pre-lithiated anodes operate with long-time stability of 86.5%capacity retention over 200 cycles and superior energy density of 549.9 Wh kg^(-1),respectively.The universal multifunctional pre-lithiation additives provide enlightenment on promoting large-scale applications of pre-lithiation on commercial high-energy-density and long-cycle-life lithium-ion batteries.展开更多
Metal-carbon dioxide(CO_(2))batteries hold great promise for reducing greenhouse gas emissions and are regarded as one of the most promising energy storage techniques due to their efficiency advantages in CO_(2)recove...Metal-carbon dioxide(CO_(2))batteries hold great promise for reducing greenhouse gas emissions and are regarded as one of the most promising energy storage techniques due to their efficiency advantages in CO_(2)recovery and conversion.Moreover,rechargeable nonaqueous metal-CO_(2)batteries have attracted much attention due to their high theoretical energy density.However,the stability issues of the electrode-electrolyte interfaces of nonaqueous metal-CO_(2)(lithium(Li)/sodium(Na)/potassium(K)-CO_(2))batteries have been troubling its development,and a large number of related research in the field of electrolytes have conducted in recent years.This review retraces the short but rapid research history of nonaqueous metal-CO_(2)batteries with a detailed electrochemical mechanism analysis.Then it focuses on the basic characteristics and design principles of electrolytes,summarizes the latest achievements of various types of electrolytes in a timely manner and deeply analyzes the construction strategies of stable electrode-electrolyte interfaces for metal-CO_(2)batteries.Finally,the key issues related to electrolytes and interface engineering are fully discussed and several potential directions for future research are proposed.This review enriches a comprehensive understanding of electrolytes and interface engineering toward the practical applications of next-generation metal-CO_(2)batteries.展开更多
文摘Electrocatalysis is key to improving energy efficiency,reducing carbon emissions,and providing a sustainable way of meeting global energy needs.Therefore,elucidating electrochemical reaction mechanisms at the electrolyte/electrode interfaces is essential for developing advanced renewable energy technologies.However,the direct probing of real-time interfacial changes,i.e.,the surface intermediates,chemical environment,and electronic structure,under operating conditions is challenging and necessitates the use of in situ methods.Herein,we present a new lab-based instrument commissioned to perform in situ chemical analysis at liquid/solid interfaces using ambient pressure X-ray photoelectron spectroscopy(APXPS).This setup takes advantage of a chromium source of tender X-rays and is designed to study liquid/solid interfaces by the“dip and pull”method.Each of the main components was carefully described,and the results of performance tests are presented.Using a three-electrode setup,the system can probe the intermediate species and potential shifts across the liquid electrolyte/solid electrode interface.In addition,we demonstrate how this system allows the study of interfacial changes at gas/solid interfaces using a case study:a sodium–oxygen model battery.However,the use of APXPS in electrochemical studies is still in the early stages,so we summarize the current challenges and some developmental frontiers.Despite the challenges,we expect that joint efforts to improve instruments and the electrochemical setup will enable us to obtain a better understanding of the composition–reactivity relationship at electrochemical interfaces under realistic reaction conditions.
基金supported by the National Key Research and Development Program(Nos.2017YFA0403800 and 2017YFB0305301)the National Natural Science Foundation of ChinaExcellent Young Scholars(No.51922068)+1 种基金the National Natural Science Foundation of China(Nos.51727802,51821001 and 51904187)funded by China Postdoctoral Science Foundation(No.2019M661500)。
文摘The liquid/solid(L/S)interface of dissimilar metals is critical to the microstructure,mechanical strength,and structural integrity of interconnects in many important applications such as electronics,automotive,aeronautics,and astronautics,and therefore has drawn increasing research interests.To design preferential microstructure and optimize mechanical properties of the interconnects,it is crucial to understand the formation and growth mechanisms of diversified structures at the L/S interface during interconnecting.In situ synchrotron radiation or tube-generated X-ray radiography and tomography technologies make it possible to observe the evolution of the L/S interface directly and therefore have greatly propelled the research in this field.Here,we review the recent progress in understanding the L/S interface behaviors using advanced in situ X-ray imaging techniques with a particular focus on the following two issues:(1)interface behaviors in the solder joints for microelectronic packaging including the intermetallic compounds(IMCs)during refl ow,Sn dendrites,and IMCs during solidification and refl ow porosities and(2)growth characteristics and morphological transition of IMCs in the interconnect of dissimilar metals at high temperature.Furthermore,the main achievements and future research perspectives in terms of metallurgical bonding mechanisms under complex conditions with improved X-ray sources and detectors are remarked and discussed.
文摘The detailed understanding of various underlying processes at liquid/solid interfaces requires the development of interface-sensitive and high-resolution experimental techniques with atomic precision.In this perspective,we review the recent advances in studying the liquid/solid interfaces at atomic level by electrochemical scanning tunneling microscope(EC-STM),non-contact atomic force microscopy(NC-AFM),and surface-sensitive vibrational spectroscopies.Different from the ultrahigh vacuum and cryogenic experiments,these techniques are all operated in situ under ambient condition,making the measurements close to the native state of the liquid/solid interface.In the end,we present some perspectives on emerging techniques,which can defeat the limitation of existing imaging and spectroscopic methods in the characterization of liquid/solid interfaces.
基金the financial support from the Shanghai Oriental Talent Program(QNDS2024007)On-Campus Scene Verification Project of Tongji University(kh0170020242359)+4 种基金Shanghai Research Institute of China Shenhua Coal-to-Liquids Chemical Co.,Ltd.the National Natural Science Foundation of China(52307249)National Science Foundation of Shanghai Province(23ZR1465900)Fundamental Research Funds for the Central Universities at Tongji University(PA2022000668,22120220426)Nanchang Automotive Institute of Intelligence&New Energy of Tongji University(TPDTC202211-02)。
文摘Silicon is considered one of the most promising candidates for incorporation into carbon-based anodes in lithium-ion batteries(LIBs)due to its high specific capacity.However,the significant volume changes during charge and discharge cycles lead to repeated reconstruction of the solid electrolyte interface(SEI)film and continuous loss of active lithium.Pre-lithiation method is regarded as a highly attractive approach for effectively compensating for active lithium loss during the charge and discharge cycles of LIBs.Constructing a stable SEI film is particularly crucial in the pre-lithiation process.In this study,we developed a direct contact pre-lithiation(DC-Pr)method to create a temperature-tailored robust SEI film interface on silicon-carbon(Si@C)electrodes.By investigating the morphology,structure,and composition of the SEI formed on Si@C electrodes at different pre-lithiation temperatures(50,25,0,and-25℃),we demonstrated that controlling the lithiation temperature to regulate the migration rate of lithium ions within the Si@C electrode yields a lithiated Si@C anode(25-Pr-Si@C)at 25℃ with a continuous,uniform SEI film(~3.65 nm)enriched with Li_(2)O-LiF,which exhibits synergistic effects.Importantly,the initial Coulombic efficiency(ICE)of 25-Pr-Si@C significantly improved from 85.4% in the unlithiated Si@C electrode(Blank-Si@C)to 106.1%.Additionally,the full cell configuration using a high areal loading of lithiated Si@C(~5.5 mA h cm^(-2))as the anode and NCM811 as the cathode(NCM811||25-Pr-Si@C)demonstrated superior cycling performance,maintaining 69.4% of capacity retention and achieving a Coulombic efficiency of over 99.7% after 150 cycles(0.5 C).Therefore,this simple and efficient experimental design provides a high-performance,controllable,and scalable pre-lithiation method for LIBs,paving the way for the commercialization of LIBs utilizing pre-lithiation techniques.
基金supported by the National Natural Science Foundation of China(22479022,52174276)the Central Guidance for Local Science and Technology Development Foundation(Youth Science Program Type A of Liaoning Province,2025JH6/101100007)+1 种基金the Liaoning Revitalization Talents Program(XLYC2007129)the Fundamental Research Funds for the Central Universities(N25QNR011)。
文摘Aqueous zinc metal batteries(ZMBs)are promising for grid-scale energy storage,but their practical application is hindered by limited cycling life and inferior low-temperature performance,primarily due to Zn dendrite growth and parasitic reactions at the electrolyte-electrode interface.To address these challenges,we develop a new and cheap hydrated eutectic electrolyte(HEE)composed of ZnCl_(2),choline chloride(ChCl),and H_(2)O,which can fundamentally tune desirable interface chemistries for dendrite-free and low-temperature ZMBs.The optimized HEE with a solvation structure of ZnCl_(3)(ChCl)(H_(2)O)_(2) shows a high co nductivity of 15.98 mS cm^(-1)and excellent freeze resistance below-40℃.It has been found that hydrogen bonding between ChCl and H_(2)O effectively reduces water activity,while preferential adsorption of ChCl molecules at the inner Helmholtz plane promotes the formation of a protective solid electrolyte interphase(SEI)on Zn metal anodes,which greatly suppresses the dendrites and side reactions.Therefore,the HEE endows the as-fabricated Zn//Zn symmetric cells and Zn//polyaniline full batteries with superior electrochemical performance at-40℃,such as a long cycling life of 870 h at 1 mA cm^(-2)and 1 mAh cm^(-2)and a high capacity of 75 mAh g^(-1)at 0.3 A g^(-1).The HEE reported here may pave a new way to construct high-performance ZMBs for specific low-temperature application scenarios.
基金Project supported by the Natural Science Foundation of Guangxi Zhuang Autonomous Region, China (Grant No. 2022GXNSFAA035487)the National Natural Science Foundation of China (Grant Nos. 12272100, 11474285, and 12074382)+2 种基金the Graduate Education Innovation Project of Guangxi Zhuang Autonomous Region, China (Grant No. XJCY2022012)the Guangxi Normal University Ideological and Political Demonstration Course Construction Project (Grant Nos. 2022kcsz15 and 2023kcsz29)the Innovation Project of Graduate Education of Guangxi Zhuang Autonomous Region, China (Grant No. YCBZ2024087)。
文摘We study the effects of gas adsorption on the dynamics and stability of nanobubbles at the solid–liquid interface. The phase diagram and dynamic evolution of surface nanobubbles were analyzed under varying equilibrium adsorption constant.Four distinct dynamic behaviors appear in the phase diagram: shrinking to dissolution, expanding to bursting, shrinking to stability, and expanding to stability. Special boundary states are identified in phase diagram, where the continuous growth of nanobubbles can take place even under very weak gas–surface interaction or with very small initial bubble size. Surface adsorption plays a critical role in the stability, lifetime, radius, and contact angle of nanobubbles, thereby demonstrating that pinning is not a prerequisite for stabilization. Furthermore, stable equilibrium nanobubbles exhibit a characteristic range of footprint radius, a limited height, and a small contact angle, consistent with experimental observations.
基金funding support from the National Natural Science Foundation of China(Grant No.52302302)the National Key R&D Program of China(Grant No.2022YFE0208000)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Special Funds of Tongji University for“Sino-German Cooperation 2.0 Strategy”。
文摘Lithium-ion batteries are at the forefront of modern energy storage technology.However,the accumulation of by-products such as ethylene and carbon dioxide during charging and discharging cycles reduces battery effective capacity and threatens large-scale safe performance.With significant advantages over ethylene carbonate(EC)electrolytes,fluorinated electrolytes can more effectively suppress internal gas evolution,thereby improving battery safety and cycling stability.To reveal the mechanism behind gas formation in lithium-ion batteries,our study investigated the transport behavior and interfacial products of fluorinated electrolytes under various operation conditions,including electrode material and electrolyte composition.Innovatively,we applied the reaction network integrator ReacNetGenerator to the analysis of the solid electrolyte interface(SEI)in lithium batteries,providing more molecular fingerprint information from the perspective of specific products.Using reactive molecular dynamics(MD)simulations with the ReaxFF force field and EChemDID,complemented by density functional theory(DFT)calculations,our results demonstrate that fluorinated electrolytes can effectively suppress the decomposition of LiPF_(6) to produce toxic gases PFs and PF_3.DFT analysis further reveals that highly fluorinated solvents(e.g.,FEMC)enhance the anti-reduction stability of PF_(6)~-through synergistic regulation of molecular orbital energy levels,thermodynamic electron affinity,charge transfer,and electrostatic potential distribution,thereby mitigating LiPF_(6) decomposition.Additionally,fluorinated electrolytes generate significantly more LiF components than non-fluorinated ones to promote the formation of a stable and durable solid electrolyte interface(SEI).Experimental validations via XPS and GC-MS confirm reduced CO_(2) generation and LiF-enriched SEI formation,aligning with simulation and DFT data.The findings provide valuable insights for the design of advanced electrolytes aimed at ensuring large-scale,safe energy storage solutions.
文摘Nonlinear reflection of SV shear wave at the isotropic solid-solid interfaces is experimentally studied. The reflected second harmonic SV shear wave is measured for glass-air,glass-iron, copper and aluminum interfaces. The relation of nonlinear reflective coefficient with the incident angle and linear as well as nonlinear characteristics of the materials is thoroughly investigated. Comparison of the experiment with the theory gives qualitatively agreement.
基金This research was supported by the Fundamental Research Funds for the Central Universities(0515022GH0202253 and 0515022SH0201253).
文摘Due to its high theoretical capacity(820 mAh g^(−1)),low standard electrode potential(−0.76 V vs.SHE),excellent stability in aqueous solutions,low cost,environmental friendliness and intrinsically high safety,zinc(Zn)-based batteries have attracted much attention in developing new energy storage devices.In Zn battery system,the battery performance is significantly affected by the solid electrolyte interface(SEI),which is controlled by electrode and electrolyte,and attracts dendrite growth,electrochemical stability window range,metallic Zn anode corrosion and passivation,and electrolyte mutations.Therefore,the design of SEI is decisive for the overall performance of Zn battery systems.This paper summarizes the formation mechanism,the types and characteristics,and the characterization techniques associated with SEI.Meanwhile,we analyze the influence of SEI on battery performance,and put forward the design strategies of SEI.Finally,the future research of SEI in Zn battery system is prospected to seize the nature of SEI,improve the battery performance and promote the large-scale application.
基金supported by the National Natural Science Foundation of China(grant nos.21975026 and 22005033)the National Postdoctoral Program of China(no.BX20180037)+1 种基金China Postdoctoral Science Foundation(no.2018M640077)the Beijing Institute of Technology Research Fund Program for Young Scholars(no.XSQD-202108005).
文摘Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this paper,homotype heterojunctions are designed on HC to induce the generation of stable solid electrolyte interfaces,which can effectively increase the ICE of HC from 64.7%to 81.1%.The results show that using a simple surface engineering strategy to construct a homotypic amorphous Al_(2)O_(3) layer on the HC could shield the active sites,and further inhibit electrolyte decomposition and side effects occurrence.Particularly,due to the suppression of continuous decomposition of NaPF 6 in ester-based electrolytes,the accumulation of NaF could be reduced,leading to the formation of thinner and denser solid electrolyte interface films and a decrease in the interface resistance.The HC anode can not only improve the ICE but elevate its sodium storage performance based on this homotype heterojunction composed of HC and Al_(2)O_(3).The optimized HC anode exhibits an outstanding reversible capacity of 321.5mAhg^(−1) at 50mAg^(−1).The cycling stability is also improved effectively,and the capacity retention rate is 86.9%after 2000 cycles at 1Ag^(−1) while that of the untreated HC is only 52.6%.More importantly,the improved sodium storage behaviors are explained by electrochemical kinetic analysis.
文摘The (100) texture of solidified fcc metals, caused by the preferential (100) dendrite growth, could be closeIy related to solid/melt interfaces which behave differently along different crystallographic orientation. The stability and roughness of {111} and {100} solid/melt interfaces of fcc metals were investigated using a modified Temkin multi-layer model. It is demonstrated that {100}crystal/melt interface is more unstable and rougher than {111} interface. The effect of the stability of crystal/melt interface on the (100) texture formation in solidified fcc metals has been analysed and discussed.
基金financially supported by the National Natural Science Foundation of China (No. 51674236)the Key Research and Development Program of Liaoning Province (No.2019JH2/10100009)+1 种基金the National Science and Technology Major Project (No.2017-Ⅵ-0003-0073)the National Key Research and Development Program (No.2018Y-FA0702900)。
文摘The effect of the pulsed magnetic field on the grain refinement of superalloy K4169 has been studied in directional solidification.In the presence of the solid-liquid interface condition,the distributions of the electromagnetic force,flow field,temperature field,and Joule heat in front of the solid-liquid interface in directional solidification with the pulsed magnetic field are simulated.The calculation results show that the largest electromagnetic force in the melt appears near the solid-liquid interface,and the electromagnetic force is distributed in a gradient.There are intensive electromagnetic vibrations in front of the solid-liquid interface.The forced melt convection is mainly concentrated in front of the solid-liquid interface,accompanied by a larger flow velocity.The simulation results indicate that the grain refinement is attributed to that the electromagnetic vibration and forced convection increase the nucleation rate and the probability of dendrite fragments survival,for making dendrite easily fragmented,homogenizing the melt temperature,and increasing the undercooling in front of the solid-liquid interface.
基金supported by the Fundamental Research Funds for Central Universities(SCUT Grant No.2019ZD22)the Guangdong Innovative and Entrepreneurial Research Team Program(No.2016ZT06N569)。
文摘Transition metal selenides have been widely studied as anode materials of sodium ion batteries(SIBs),however,the investigation of solid-electrolyte-interface(SEI)on these materials,which is critical to the electrochemical performance of SIBs,remains at its infancy.Here in this paper,ZnSe@C nanoparticles were prepared from ZIF-8 and the SEI layers on these electrodes with and without reduced graphene oxide(rGO)layers were examined in details by X-ray photoelectron spectroscopies at varied charged/discharged states.It is observed that fast and complicated electrolyte decomposition reactions on ZnSe@C leads to quite thick SEI film and intercalation of solvated sodium ions through such thick SEI film results in slow ion diffusion kinetics and unstable electrode structure.However,the presence of rGO could efficiently suppress the decomposition of electrolyte,thus thin and stable SEI film was formed.ZnSe@C electrodes wrapped by rGO demonstrates enhanced interfacial charge transfer kinetics and high electrochemical performance,a capacity retention of 96.4%,after 1000 cycles at 5 A/g.This study might offer a simple avenue for the designing high performance anode materials through manipulation of SEI film.
基金supported by the National Natural Science Foundation of China(51872196)the Natural Science Foundation of Tianjin,China(17JCJQJC44100)。
文摘Owing to its low potential, crustal abundances and environmental friendliness, calcium metal anode(CMA) is emerging as a powerful contender in post-lithium era. However, the passivation of CMA fatally hinders its development. Recently, several feasible electrolytes have been developed. Nevertheless, as a pivotal part, the solid electrolyte interface(SEI) formed on CMA has not been paid enough attention to. In this review, based on the passivation mechanism of CMA, the favorable composition of SEI is emphasized with the corresponding electrolytes. It is considered that boron-containing and organic–inorganic hybrid SEI might be preferred. By comparing electrolytes and SEI on CMA with lithium and magnesium metal anodes, the root causes of CMA passivation are further elaborated, enlightening rational design rules of suitable SEI. Furthermore, some noteworthy details when assembling secondary calcium metal batteries(CMBs) are put forward. It is expected that deeper understanding of SEI on CMA will promote the development of CMBs.
文摘The solid/liquid interface of a directionally solidified Ni-base superalloy with different phosphorus contents was quantitatively described by means of fractat method.When the solidification rate was fixed,the relationship between the fractal dimensionality of the solid/liquid interface and the phos- phorus content of the test alloy was given.Combined the thermodynamics and fractal theory,the ef- fect mechanism of phosphorus content on fractal dimensionality of the solid/liquid interface was discussed.
基金the National Natural Science Foundation of China(Grant No.51976002)the Beijing Nova Program of Science and Technology(Grant No.Z191100001119033)。
文摘Thermal rectification refers to the phenomenon by which the magnitude of the heat flux in one direction is much larger than that in the opposite direction.In this study,we propose to implement the thermal rectification phenomenon in an asymmetric solid–liquid–solid sandwiched system with a nano-structured interface.By using the non-equilibrium molecular dynamics simulations,the thermal transport through the solid–liquid–solid system is examined,and the thermal rectification phenomenon can be observed.It is revealed that the thermal rectification effect can be attributed to the significant difference in the interfacial thermal resistance between Cassie and Wenzel states when reversing the temperature bias.In addition,effects of the liquid density,solid–liquid bonding strength and nanostructure size on the thermal rectification are examined.The findings may provide a new way for designs of certain thermal devices.
基金Project supported by the National Natural Science Foundation of China(Grant No.11305021)the Fundamental Research Funds for the Central Universities of China(Grants Nos.3132017072 and 3132015149)
文摘We propose a scheme to implement quantum state transfer between two distant quantum nodes via a hybrid solid–optomechanical interface. The quantum state is encoded on the native superconducting qubit, and transferred to the microwave photon, then the optical photon successively, which afterwards is transmitted to the remote node by cavity leaking,and finally the quantum state is transferred to the remote superconducting qubit. The high efficiency of the state transfer is achieved by controllable Gaussian pulses sequence and numerically demonstrated with theoretically feasible parameters.Our scheme has the potential to implement unified quantum computing–communication–computing, and high fidelity of the microwave–optics–microwave transfer process of the quantum state.
基金financially supported by the National Natural Science Foundation of China(52172159)the Postdoctoral Fellowship Program of CPSF(GZB20230631).
文摘The reversibility and stability of aqueous Zn metal batteries(AZMBs)are largely limited by Zn dendrites and interfacial parasitic reactions.Herein,we propose a parallel modulation strategy to boost the reversibility of the Zn anode by introducing N,N,N',N'-tetramethylchloroformamidinium hexafluorophosphate(TCFH)as an additive in the electrolyte.TCFH is composed of PF6-and TN+with opposite charges.PF6-can spontaneously induce the in-situ generation of ZnF_(2)solid electrolyte interface(SEI)on the anode,which can improve the transport kinetics of Zn^(2+)at the interface,thus promoting the rapid and uniform deposition of Zn as well as inhibiting the growth of dendrites.In addition,TN+is enriched at the anode surface during Zn deposition through the anchoring effect,which brings a reconfiguration of the ion/molecule distribution.The anchored-TN+reduces the concentrations of H_(2)O and SO_(4)^(2-),sufficiently restraining the parasitic reaction.Thanks to the dual-phase interface engineering constructed of PF6-and TN+in parallel,the symmetric cell with the proposed electrolyte survives long cycling stability over750 h at 20 mA cm^(-2),10 mAh cm^(-2).This study offers a distinct viewpoint to the multidimensional optimization of Zn anodes for high-performance AZMBs.
基金Huaiyu Shao acknowledges the Shenzhen-Hong Kong-Macao Science and Technology Plan Project(Category C)(Grant No.SGDX20220530111004028)the Macao Science and Technology Development Fund(FDCT)for funding(FDCT No.0013/2024/RIB1,FDCT-MOST joint project No.0026/2022/AMJ and No.006/2022/ALC of the Macao Centre for Research and Development in Advanced Materials[2022–2024])+2 种基金the Multi-Year Research Grant(MYRG)from University of Macao(project No.MYRG-GRG2023-00140-IAPME-UMDF and No.MYRG-GRG2024-00206-IAPME)Natural Science Foundation of Guangdong Province(Grant No.2023A1515010765)Science and Technology Program of Guangdong Province of China(Grant No.2023A0505030001)。
文摘Considering the growing pre-lithiation demand for high-performance Si-based anodes and consequent additional costs caused by the strict pre-lithiation environment,developing effective and environmentally stable pre-lithiation additives is a challenging research hotspot.Herein,interfacial engineered multifunctional Li_(13)Si_(4)@perfluoropolyether(PFPE)/LiF micro/nanoparticles are proposed as anode pre-lithiation additives,successfully constructed with the hybrid interface on the surface of Li_(13)Si_(4)through PFPE-induced nucleophilic substitution.The synthesized multifunctional Li_(13)Si_(4)@PFPE/LiF realizes the integration of active Li compensation,long-term chemical structural stability in air,and solid electrolyte interface(SEI)optimization.In particular,the Li_(13)Si_(4)@PFPE/LiF with a high pre-lithiation capacity(1102.4 mAh g^(-1))is employed in the pre-lithiation Si-based anode,which exhibits a superior initial Coulombic efficiency of 102.6%.Additionally,in situ X-ray diffraction/Raman,density functional theory calculation,and finite element analysis jointly illustrate that PFPE-predominant hybrid interface with modulated abundant highly electronegative F atoms distribution reduces the water adsorption energy and oxidation kinetics of Li_(13)Si_(4)@PFPE/LiF,which delivers a high pre-lithiation capacity retention of 84.39%after exposure to extremely moist air(60%relative humidity).Intriguingly,a LiF-rich mechanically stable bilayer SEI is constructed on anodes through a pre-lithiation-driven regulation for the behavior of electrolyte decomposition.Benefitting from pre-lithiation via multifunctional Li_(13)Si_(4)@PFPE/LiF,the full cell and pouch cell assembled with pre-lithiated anodes operate with long-time stability of 86.5%capacity retention over 200 cycles and superior energy density of 549.9 Wh kg^(-1),respectively.The universal multifunctional pre-lithiation additives provide enlightenment on promoting large-scale applications of pre-lithiation on commercial high-energy-density and long-cycle-life lithium-ion batteries.
基金supports from the Beijing Laboratory of New Energy Storage Technology, North China Electric Power Universitythe Program of the National Energy Storage Industry-Education Platformthe Interdisciplinary Innovation Program of North China Electric Power University (No. XM2212315)
文摘Metal-carbon dioxide(CO_(2))batteries hold great promise for reducing greenhouse gas emissions and are regarded as one of the most promising energy storage techniques due to their efficiency advantages in CO_(2)recovery and conversion.Moreover,rechargeable nonaqueous metal-CO_(2)batteries have attracted much attention due to their high theoretical energy density.However,the stability issues of the electrode-electrolyte interfaces of nonaqueous metal-CO_(2)(lithium(Li)/sodium(Na)/potassium(K)-CO_(2))batteries have been troubling its development,and a large number of related research in the field of electrolytes have conducted in recent years.This review retraces the short but rapid research history of nonaqueous metal-CO_(2)batteries with a detailed electrochemical mechanism analysis.Then it focuses on the basic characteristics and design principles of electrolytes,summarizes the latest achievements of various types of electrolytes in a timely manner and deeply analyzes the construction strategies of stable electrode-electrolyte interfaces for metal-CO_(2)batteries.Finally,the key issues related to electrolytes and interface engineering are fully discussed and several potential directions for future research are proposed.This review enriches a comprehensive understanding of electrolytes and interface engineering toward the practical applications of next-generation metal-CO_(2)batteries.
