Hydrogen Spillover Effect in Electrocatalysis:Delving into the Mysteries of the Atomic Migration

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.

Effect of atomic structure on migration characteristic and solute segregation of ordered domain interfaces formed in Ni_(75)Al_xV_(25-x)

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.

Cathodic corrosion as a facile and universal method for the preparation of supported metal single atoms

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.

Tuning the growth of intermetallic compounds at Sn-0.7Cu solder/Cu substrate interface by adding small amounts of indium

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.

Achieving highly stable Sn-based anode by a stiff encapsulation heterostructure

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).