Trends in Electrocatalysis: The Microenvironment Moves to Center Stage

Schreier, Marcel; Kenis, Paul; Che, Fanglin; Hall, Anthony Shoji

doi:10.1021/acsenergylett.3c01623

Cited by 27 publications

(18 citation statements)

References 59 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The applied potential is a crucial handle for tuning electrocatalytic reactions, as changes in electrochemical reaction rates result from the modification of the reaction microenvironment via the potential-induced rearrangement of charged compounds. − By listening to the variation in pitch as the potential changed (Video S1), we gained intuitive insight into the potential regions where significant changes in EDL behavior occurred for a polycrystalline Pt electrode immersed in 7 mM KClO 4 .…”

Section: Resultsmentioning

confidence: 99%

Electrochemical Synthesis of Sound: Hearing the Electrochemical Double Layer

Kelly,

Yan,

Lucky

et al. 2024

ACS Cent. Sci.

Self Cite

View full text Add to dashboard Cite

Electrochemical double layers (EDLs) govern the operation of batteries, fuel cells, electrochemical sensors, and electrolyzers. However, their invisible nature makes their properties and function difficult to conceptualize, creating an impediment to the broader understanding of double-layer function required for future technologies in energy storage and chemical synthesis. To render the behavior of electrochemical interfaces more intuitive, we made the rearrangement of interfacial components audible by employing the EDL as a variable element in a relaxation oscillator circuit. Connecting the circuit to a speaker generated an audible output corresponding to the change in potential resulting from EDL rearrangement. Variations in the applied voltage, electrolyte concentration and identity, as well as in the electrode material, yielded audible frequency variations that provide an intuitive understanding of EDL behavior. We expect that hearing the trends in behavior will provide a helpful and alternative method for understanding molecular movement at the electrochemical interface.

show abstract

Section: Resultsmentioning

confidence: 99%

Electrochemical Synthesis of Sound: Hearing the Electrochemical Double Layer

Kelly,

Yan,

Lucky

et al. 2024

ACS Cent. Sci.

Self Cite

View full text Add to dashboard Cite

show abstract

“…The electric field resulting from equilibration or an externally applied potential interacts with the ions and the dipole of solvent molecules to drive their rearrangement at the interface. This rearrangement leads to interfacial ordering, where solvent molecules and ions are recruited to or excluded from the electrode in a potential-dependent manner to form the electrochemical double layer . While limited in scope, the Gouy–Chapman–Stern model is commonly used to describe the electrochemical double layer as a compact layer of ions near the electrode surface, followed by a diffuse layer where ions of the opposite charge of that of the electrode are present at levels above their bulk concentration.…”

Section: Impact Of the Potential On The Electrode Charge And Interfac...mentioning

confidence: 99%

“…Solvated ions in the compact layer then accumulate at their distance of closest approach in the outer Helmholtz plane (OHP) and in the diffuse layer beyond that (Figure ). The number and nature of the ions recruited depends on the properties of the electrolyte, which also determines the charge on the electrode at a given applied potential …”

Section: Impact Of the Potential On The Electrode Charge And Interfac...mentioning

confidence: 99%

“…Consequently, adsorption and reactivity trends result from both the direct interaction of the electrode with the substrate as well as the indirect effects of complex interactions between all species present at the interface (Figure ). In the following, we summarize the thermodynamic models used to describe adsorption at electrochemical interfaces, show how these models relate to electrocatalyst material properties, and discuss the manifestation of adsorption phenomena in two reactions of contemporary importance in electrocatalysis: CO 2 reduction and the transformation of hydrocarbons. Through this discussion, we aim to provide an overview of the phenomena steering electrochemical adsorption and how these factors should be considered in electrocatalysis research.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Mind the Interface: The Role of Adsorption in Electrocatalysis

Lucky,

Schreier

2024

ACS Nano

Self Cite

View full text Add to dashboard Cite

In the field of electrocatalysis, significant emphasis has been placed on developing electrode materials to enable critical energy storage reactions and sustainable chemical synthesis. However, the electrode is just one part of a complex interfacial environment that controls substrate adsorption and reactivity. In the presence of a liquid electrolyte and an electrochemical interface, adsorption processes behave substantially differently than those in the gas phase. Understanding these adsorption processes, which play an important role in all electrocatalytic reactions, is critical for the design of effective electrocatalysts. In this Perspective, we discuss the current understanding of electrochemical adsorption and its implications for catalyst design.

show abstract

“…Modulating the aqueous microenvironment at electrochemical interfaces is vitally important for improving the performance of energy storage materials and electrocatalysts . The electrochemical window of aqueous batteries can be extended by adding chemical species to the electrolyte that form strong hydrogen bonds with water molecules, − while weakening the H-bonds of water may increase the activity for HER .…”

Section: Introductionmentioning

confidence: 99%

Tuning the Microenvironment of Water Confined in Ti₃C₂T_x MXene by Cation Intercalation

Lounasvuori,

Zhang,

Gogotsi

et al. 2024

J. Phys. Chem. C

View full text Add to dashboard Cite

The local microenvironment has recently been found to play a major role in the electrocatalytic activity of nanomaterials. Modulating the microenvironment by adding alkali metal cations into the electrolyte can be used to either suppress hydrogen or oxygen evolution, thereby extending the electrochemical window of energy storage systems, or to tune the selectivity of electrocatalysts. MXenes are a large family of twodimensional transition metal carbides, nitrides, and carbonitrides that have shown potential for use in electrochemical energy storage applications. Due to their negatively charged surfaces, MXenes can accommodate cations and water molecules between the layers. Nevertheless, the nature of the aqueous microenvironment in the MXene interlayer space is poorly understood. Here, we apply Fourier transform infrared spectroscopy (FTIR) to probe the hydrogen bonding of intercalated water in Ti 3 C 2 T x as a function of intercalated cation and relative humidity. Substantial changes in the FTIR spectra after cation exchange demonstrate that the hydrogen bonding of water molecules confined between the MXene layers is strongly cation-dependent. Furthermore, the IR absorbance of the confined water correlates with resistivity estimated by 4-point probe measurements and interlayer distance calculated from XRD patterns. This work demonstrates that cation intercalation strongly modulates the confined microenvironment, which can be used to tune the activity or selectivity of electrochemical reactions in the interlayer space of MXenes in the future.

show abstract

Trends in Electrocatalysis: The Microenvironment Moves to Center Stage

Cited by 27 publications

References 59 publications

Electrochemical Synthesis of Sound: Hearing the Electrochemical Double Layer

Electrochemical Synthesis of Sound: Hearing the Electrochemical Double Layer

Mind the Interface: The Role of Adsorption in Electrocatalysis

Tuning the Microenvironment of Water Confined in Ti₃C₂T_x MXene by Cation Intercalation

Contact Info

Product

Resources

About

Trends in Electrocatalysis: The Microenvironment Moves to Center Stage

Cited by 27 publications

References 59 publications

Electrochemical Synthesis of Sound: Hearing the Electrochemical Double Layer

Electrochemical Synthesis of Sound: Hearing the Electrochemical Double Layer

Mind the Interface: The Role of Adsorption in Electrocatalysis

Tuning the Microenvironment of Water Confined in Ti3C2Tx MXene by Cation Intercalation

Contact Info

Product

Resources

About

Tuning the Microenvironment of Water Confined in Ti₃C₂T_x MXene by Cation Intercalation