Investigation of Electrochemical Solid-Liquid Interfaces Using In Situ Liquid Time-of-flight Secondary Ion Mass Spectrometry
Electrochemical interfaces are the core of various important fields,such as energy conversion and storage,biochemistry,sensors,and corrosion.The investiga-tions of the structure-performance relationship of electrochemical solid-liquid interfaces have become a hot topic yet extremely challenging due to the fact that the interfaces are ultrathin,highly dynamic and extremely complex.Mass spectrometric techniques cou-pled with electrochemistry are powerful and have been widely applied in investigations of mechanisms of electrochemical reactions.However,traditional mass spectrometry(MS)is difficult to characterize the electrode-electrolyte interfaces in an in situ manner due to inherent limitations existing in their ionization processes.In recent years,the state-of-the-art in situ liquid time-of-flight secondary ion MS(ToF-SIMS)based on high-vacuum compatible microfluidic devices has been developed to tackle with this challenge.This review mainly reviewed the principle,characteristics and rapid develop-ment of in situ liquid ToF-SIMS in real-time and in situ investigations of electrochemical solid-liquid interfaces during the past decade.In situ liquid ToF-SIMS possesses shallow information depth(nm),high temporal resolution(μs)and high detection sensitivity(10-6-10-9).Besides,it ionizes the electrochemical interfaces in a truly in situ manner and provides direct molecular evidences of chemical evolution of both electrode/electro-catalyst surfaces and reactants/intermediates/products in electrolytes at the interfaces simultaneously.Being attributed to its uniqueness,in situ liquid ToF-SIMS has become a powerful and versatile molecular"eye"in in situ and real-time tracking dynamic elec-trochemical solid-liquid interfaces,such as capturing electrochemical reaction intermedi-ates,identification of electrocatalytic active sites,probing fine structures of electro-chemical double layers,and unraveling the formation chemistry of solid-electrolyte interphases in batteries.Further innovations of microfluidic electrochemical devices and ToF-SIMS instruments are desired to promote the enhanced performance and wider applications of in situ liquid ToF-SIMS in the electrochemical field,and in situ liquid ToF-SIMS will make significant contributions to the understanding of the structure-performance relationship of interfaces in complex electrochemical assays and guide the engineering of better electrochemical interfaces in important fields,such as electrocatal-ysis and batteries.
electrochemical solid-liquid interfacesin situ liquid time-of-flight secondary ion mass spectrometryin situ analysisreal-time analysis
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