Hydrogen spillover effect has recently garnered a lot of attention in the field of electrocatalytic hydrogen evolution reactions.A new avenue for understanding the dynamic behavior of atomic migration in which hydroge...Hydrogen spillover effect has recently garnered a lot of attention in the field of electrocatalytic hydrogen evolution reactions.A new avenue for understanding the dynamic behavior of atomic migration in which hydrogen atoms moving on a catalyst surface was opened up by the setup of the word"hydrogen spillover."However,there is currently a dearth of thorough knowledge regarding the hydrogen spillover effect.Currently,the advancement of sophisticated characterization procedures offers progressively useful information to enhance our grasp of the hydrogen spillover effect.The understanding of material fabrication for hydrogen spillover effect has erupted.Considering these factors,we made an effort to review most of the articles published on the hydrogen spillover effect and carefully analyzed the aspect of material fabrication.All of our attention has been directed toward the molecular pathway that leads to improve hydrogen evolution reactions performance.In addition,we have attempted to elucidate the spillover paths through the utilization of DFT calculations.Furthermore,we provide some preliminary research suggestions and highlight the opportunities and obstacles that are still to be confronted in this study area.展开更多
Based on the microscopic phase-field model, ordered domain interfaces formed between D022 （Ni3V） phases along [001] direction in Ni75AlxV25-x alloys were simulated, and the effects of atomic structure on the migrati...Based on the microscopic phase-field model, ordered domain interfaces formed between D022 （Ni3V） phases along [001] direction in Ni75AlxV25-x alloys were simulated, and the effects of atomic structure on the migration characteristic and solute segregation of interfaces were studied. It is found that the migration ability is related to the atomic structure of interfaces, and three kinds of interfaces can migrate except the interface （001）//（002） which has the characteristic of L12 （Ni3Al） structure. V atoms jump to the nearest neighbor site and substitute for Ni, and vice versa. Because of the site selectivity behaviors of jumping atoms, the number of jumping atoms during the migration is the least and the jumping distance of atoms is the shortest among all possible modes, and the atomic structures of interfaces are unchanged before and after the migration. The preferences and degree of segregation or depletion of alloy elements are also related to the atomic structure of interface.展开更多
The electromigration reliability on Sn–10Bi solder joints is investigated and the performance is tried to be improved with trace Zn addition in solder by depressing the growth of interfacial intermetallic compounds(I...The electromigration reliability on Sn–10Bi solder joints is investigated and the performance is tried to be improved with trace Zn addition in solder by depressing the growth of interfacial intermetallic compounds(IMCs)under electromigration.The electromigration test was realized on Cu/solder/Cu linear specimens at a current density of 1.0×10^(4) A/cm^(2) with different stressing time.It was found that Bi atoms in Cu/Sn-10Bi/Cu solder joint were driven towards anode side under current driving force and then accumulated at anode interface with current stressing time increasing.The thickness and growth rate of Cu_(6)Sn_(5) IMCs at anode interface were obviously larger than those at cathode side due to polarity effect.The addition of 0.2 wt.%Zn inhibited the migration of Bi atoms during the electromigration process,and the composition of interfacial IMCs was transformed into Cu_(6)(Sn,Zn)_(5),which played as a diffusion barrier to effectively reduce the asymmetric growth of IMCs and the consumption of Cu substrate during electromigation.展开更多
The void defect in intermetallic compounds(IMCs)layer at the joints caused by inhomogeneous atomic diffusion is one of the most important factors limiting the further development of Sn-based solders.In this work,the t...The void defect in intermetallic compounds(IMCs)layer at the joints caused by inhomogeneous atomic diffusion is one of the most important factors limiting the further development of Sn-based solders.In this work,the thermodynamic stability of IMCs(high-temperatureη-Cu_(6)Sn_(5)and o-Cu_(3)Sn phases)was improved by adding small amounts of indium(In),and the IMCs layers with moderate thickness,low defect concentrations and stable interface bonding were successfully obtained.The formation order of compounds and the interfacial orientation relationships in IMCs layers,the atomic diffusion mechanism,and the growth tuning mechanism of In onη-Cu_(6)Sn_(5)and Cu_(3)Sn,after In adding,were discussed com-prehensively by combining calculations and experiments.It is the first time that the classic heteroge-neous nucleation theory and CALPHAD data were used to obtain the critical nucleus radius ofη-Cu_(6)Sn_(5)and Cu_(3)Sn,and to explain in detail the main factors affecting the formation order and location of IMCs at joints during the welding process.A novel and systematic growth model about IMCs layers in the case of doping with alloying elements was proposed.The growth tuning mechanism of In doping onη-Cu_(6)Sn_(5)and Cu_(3)Sn was further clarified based on the proposed model using first-principles calculations.The growth model used in this study can provide insights into the development and design of multiele-ment Sn-based solders.展开更多
Elucidating the fundamental mechanisms underlying Cu reconstruction is paramount for the rational design of catalysts that meet the stringent activity,selectivity,and durability requirements for industrial-scale CO_(2...Elucidating the fundamental mechanisms underlying Cu reconstruction is paramount for the rational design of catalysts that meet the stringent activity,selectivity,and durability requirements for industrial-scale CO_(2)/CO electroreduction(CO_(2)RR/CORR).While both dissolution-redeposition and atomic migration pathways have been proposed,the operational conditions dictating their relative dominance remain poorly understood.Through quasi in situ Cu^(+)detection and in situ atomic force microscopy(AFM),we reveal a striking mechanistic dichotomy:Cu reconstruction during CO_(2)RR occurs strictly in the presence of Cu^(+),whereas CORR-induced reconstruction proceeds independently of Cu^(+)species.These findings suggest that Cu reconstruction in CO_(2)RR follows a dissolution-redeposition mechanism induced by oxidative radicals,while atomic migration emerges as the dominant pathway in CORR.Density functional theory calculations further demonstrate that adsorbed*CO intermediates reduce Cu-Cu bond strength,creating metastable surface configurations that promote Cu atomic migration.These insights provide a foundation for leveraging reconstruction to design high-performance Cu-based catalysts.展开更多
Top-down strategy has been generally adopted for preparation of metal single atom catalysts(SACs)due to the simplified synthetic process,metal economics,and scalability characteristics.Herein,we propose a general top-...Top-down strategy has been generally adopted for preparation of metal single atom catalysts(SACs)due to the simplified synthetic process,metal economics,and scalability characteristics.Herein,we propose a general top-down route to convert metal nanoparticles into uniformly dispersed metal single atoms in mild electrochemical environment via a facile cathodic corrosion process.Within the synthetic process,Pt nanoparticles precursors are transformed into migrating Pt single atoms(Pt1)driven by a high negative potential;and subsequently these mobile Pt atoms are trapped and stabilized by N coordination sites of N-doped carbon paper(NCP).The as-prepared Pt1/NCP electrodes exhibit a superior catalytic activity toward hydrogen evolution reaction(HER)with a low overpotential of 0.022 V at 10 mA/cm^(2)and a low Tafel slope of 28.5 mV/dec as well as a long-term durability.Notably,the proposed electrochemical atomic migration strategy shows a promising generality for fabricating other metal single atoms(e.g.,Pd,Ir,Cu),which may open a new avenue for metallic SACs preparation.展开更多
Rationally designed heterostructures provide attractive prospects for energy storage electrodes by combining different active materials with distinct electrochemical properties.Herein,through a phase separation strate...Rationally designed heterostructures provide attractive prospects for energy storage electrodes by combining different active materials with distinct electrochemical properties.Herein,through a phase separation strategy,a heterostructure of SnO_(2) encapsulated by amorphous Nb_(2)O_(5) is spontaneously synthesized.Insertion-type anode Nb_(2)O_(5) outer shell,playing as reaction containers and fast ionic pathways,physically inhibits the Sn atoms’migration and enhances the reaction kinetics.Moreover,strong chemical interactions are found at the SnO_(2)/Nb_(2)O_(5) interfaces,which ensure the solid encapsulation of the SnO_(2) cores even after 500 cycles.When used for lithium-ion batteries,this heterostructured anode exhibits high cycling stability with a capacity of 626 mAhg^(-1) after 1000 cycles at 2Ag^(-1)(85% capacity retention)and good rate performance with the capacity of 340 mAhg^(-1) at 8Ag^(-1).展开更多
基金supported by Brain Pool program funded by the Ministry of Science and ICT through the National Research Foundation of Korea(Grant Nos.RS-2023-00284361 and 2021R1A2C2091497)supported by the Nano&Materials Technology Development Program through the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(RS-2024-00436563)
文摘Hydrogen spillover effect has recently garnered a lot of attention in the field of electrocatalytic hydrogen evolution reactions.A new avenue for understanding the dynamic behavior of atomic migration in which hydrogen atoms moving on a catalyst surface was opened up by the setup of the word"hydrogen spillover."However,there is currently a dearth of thorough knowledge regarding the hydrogen spillover effect.Currently,the advancement of sophisticated characterization procedures offers progressively useful information to enhance our grasp of the hydrogen spillover effect.The understanding of material fabrication for hydrogen spillover effect has erupted.Considering these factors,we made an effort to review most of the articles published on the hydrogen spillover effect and carefully analyzed the aspect of material fabrication.All of our attention has been directed toward the molecular pathway that leads to improve hydrogen evolution reactions performance.In addition,we have attempted to elucidate the spillover paths through the utilization of DFT calculations.Furthermore,we provide some preliminary research suggestions and highlight the opportunities and obstacles that are still to be confronted in this study area.
基金Projects (50941020, 10902086, 50875217, 20903075) supported by the National Natural Science Foundation of ChinaProjects (SJ08-ZT05, SJ08-B14) supported by the Natural Science Foundation of Shaanxi Province, ChinaProject (CX200905) supported by the Doctorate Foundation of Northwestern Polytechnical University, China
文摘Based on the microscopic phase-field model, ordered domain interfaces formed between D022 （Ni3V） phases along [001] direction in Ni75AlxV25-x alloys were simulated, and the effects of atomic structure on the migration characteristic and solute segregation of interfaces were studied. It is found that the migration ability is related to the atomic structure of interfaces, and three kinds of interfaces can migrate except the interface （001）//（002） which has the characteristic of L12 （Ni3Al） structure. V atoms jump to the nearest neighbor site and substitute for Ni, and vice versa. Because of the site selectivity behaviors of jumping atoms, the number of jumping atoms during the migration is the least and the jumping distance of atoms is the shortest among all possible modes, and the atomic structures of interfaces are unchanged before and after the migration. The preferences and degree of segregation or depletion of alloy elements are also related to the atomic structure of interface.
基金funded by the National Natural Science Foundation of China(Grant No.51875269)Postgraduate Research&Practice Innovation Program of Jiangsu Province(Grant No.SJCX23_2178).
文摘The electromigration reliability on Sn–10Bi solder joints is investigated and the performance is tried to be improved with trace Zn addition in solder by depressing the growth of interfacial intermetallic compounds(IMCs)under electromigration.The electromigration test was realized on Cu/solder/Cu linear specimens at a current density of 1.0×10^(4) A/cm^(2) with different stressing time.It was found that Bi atoms in Cu/Sn-10Bi/Cu solder joint were driven towards anode side under current driving force and then accumulated at anode interface with current stressing time increasing.The thickness and growth rate of Cu_(6)Sn_(5) IMCs at anode interface were obviously larger than those at cathode side due to polarity effect.The addition of 0.2 wt.%Zn inhibited the migration of Bi atoms during the electromigration process,and the composition of interfacial IMCs was transformed into Cu_(6)(Sn,Zn)_(5),which played as a diffusion barrier to effectively reduce the asymmetric growth of IMCs and the consumption of Cu substrate during electromigation.
基金supported by the Innovation Team Cultivation Project of Yunnan Province(No.202005AE160016)Key Research&Development Program of Yunnan Province(No.202103AA080017)Yunnan Ten Thousand Talents Plan Young&Elite Talents Project(No.YNWR-QNBJ-2018-044).
文摘The void defect in intermetallic compounds(IMCs)layer at the joints caused by inhomogeneous atomic diffusion is one of the most important factors limiting the further development of Sn-based solders.In this work,the thermodynamic stability of IMCs(high-temperatureη-Cu_(6)Sn_(5)and o-Cu_(3)Sn phases)was improved by adding small amounts of indium(In),and the IMCs layers with moderate thickness,low defect concentrations and stable interface bonding were successfully obtained.The formation order of compounds and the interfacial orientation relationships in IMCs layers,the atomic diffusion mechanism,and the growth tuning mechanism of In onη-Cu_(6)Sn_(5)and Cu_(3)Sn,after In adding,were discussed com-prehensively by combining calculations and experiments.It is the first time that the classic heteroge-neous nucleation theory and CALPHAD data were used to obtain the critical nucleus radius ofη-Cu_(6)Sn_(5)and Cu_(3)Sn,and to explain in detail the main factors affecting the formation order and location of IMCs at joints during the welding process.A novel and systematic growth model about IMCs layers in the case of doping with alloying elements was proposed.The growth tuning mechanism of In doping onη-Cu_(6)Sn_(5)and Cu_(3)Sn was further clarified based on the proposed model using first-principles calculations.The growth model used in this study can provide insights into the development and design of multiele-ment Sn-based solders.
基金supported by the National Natural Science Foundation of China(52471235 and 51972223)the National Industry-Education Platform for Energy Storage(Tianjin University)the Fundamental Research Funds for the Central Universities,and the Haihe Laboratory of Sustainable Chemical.
文摘Elucidating the fundamental mechanisms underlying Cu reconstruction is paramount for the rational design of catalysts that meet the stringent activity,selectivity,and durability requirements for industrial-scale CO_(2)/CO electroreduction(CO_(2)RR/CORR).While both dissolution-redeposition and atomic migration pathways have been proposed,the operational conditions dictating their relative dominance remain poorly understood.Through quasi in situ Cu^(+)detection and in situ atomic force microscopy(AFM),we reveal a striking mechanistic dichotomy:Cu reconstruction during CO_(2)RR occurs strictly in the presence of Cu^(+),whereas CORR-induced reconstruction proceeds independently of Cu^(+)species.These findings suggest that Cu reconstruction in CO_(2)RR follows a dissolution-redeposition mechanism induced by oxidative radicals,while atomic migration emerges as the dominant pathway in CORR.Density functional theory calculations further demonstrate that adsorbed*CO intermediates reduce Cu-Cu bond strength,creating metastable surface configurations that promote Cu atomic migration.These insights provide a foundation for leveraging reconstruction to design high-performance Cu-based catalysts.
基金Foundation from Institute of Materials CAEP(Nos.TP03201703,TP03201802,and CX2019018)the National Natural Science Foundation of China(Nos.51701192 and 21706246).
文摘Top-down strategy has been generally adopted for preparation of metal single atom catalysts(SACs)due to the simplified synthetic process,metal economics,and scalability characteristics.Herein,we propose a general top-down route to convert metal nanoparticles into uniformly dispersed metal single atoms in mild electrochemical environment via a facile cathodic corrosion process.Within the synthetic process,Pt nanoparticles precursors are transformed into migrating Pt single atoms(Pt1)driven by a high negative potential;and subsequently these mobile Pt atoms are trapped and stabilized by N coordination sites of N-doped carbon paper(NCP).The as-prepared Pt1/NCP electrodes exhibit a superior catalytic activity toward hydrogen evolution reaction(HER)with a low overpotential of 0.022 V at 10 mA/cm^(2)and a low Tafel slope of 28.5 mV/dec as well as a long-term durability.Notably,the proposed electrochemical atomic migration strategy shows a promising generality for fabricating other metal single atoms(e.g.,Pd,Ir,Cu),which may open a new avenue for metallic SACs preparation.
基金supported by China Postdoctoral Science Foundation(2020M671242 and 2021T140688)the Special Research Assistant program of CASthe Super Postdoctoral Fellow Program of Shanghai。
文摘Rationally designed heterostructures provide attractive prospects for energy storage electrodes by combining different active materials with distinct electrochemical properties.Herein,through a phase separation strategy,a heterostructure of SnO_(2) encapsulated by amorphous Nb_(2)O_(5) is spontaneously synthesized.Insertion-type anode Nb_(2)O_(5) outer shell,playing as reaction containers and fast ionic pathways,physically inhibits the Sn atoms’migration and enhances the reaction kinetics.Moreover,strong chemical interactions are found at the SnO_(2)/Nb_(2)O_(5) interfaces,which ensure the solid encapsulation of the SnO_(2) cores even after 500 cycles.When used for lithium-ion batteries,this heterostructured anode exhibits high cycling stability with a capacity of 626 mAhg^(-1) after 1000 cycles at 2Ag^(-1)(85% capacity retention)and good rate performance with the capacity of 340 mAhg^(-1) at 8Ag^(-1).
