Electrochemical Mapping Reveals Direct Correlation between Heterogeneous Electron‐Transfer Kinetics and Local Density of States in Diamond Electrodes

Patten, Hollie V.; Meadows, Katherine E.; Hutton, Laura A.; Iacobini, James G.; Battistel, Dario; McKelvey, Kim; Colburn, Alexander W.; Newton, Mark E.; Macpherson, Julie V.; Unwin, Patrick R.

doi:10.1002/ange.201203057

Cited by 31 publications

(57 citation statements)

References 65 publications

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“…(61). SECCM has also been employed, as part of a multimicroscopy approach, to perform localized capacitance measurements on various pBDD facets to link electrochemical reaction rates with the local boron concentration (74). In this study, Because of its ability to confine electrochemical measurements on complex substrates, SECCM has been used to study the electrochemical activity of vertically aligned (SWNT) forests (79).…”

Section: Point Measurements: From Voltammetry To Local Capacitancementioning

confidence: 99%

Scanning Electrochemical Cell Microscopy: A Versatile Technique for Nanoscale Electrochemistry and Functional Imaging

Ebejer

Güell²,

Lai³

et al. 2013

Annual Rev. Anal. Chem.

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274

369

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■ Abstract Scanning electrochemical cell microscopy (SECCM) is a new pipette-based imaging techniquepurposely designed to allow simultaneous electrochemical, conductance, and topographical visualization of surfaces and interfaces. SECCM uses a tiny meniscus or droplet, confined between the probe and the surface, for high-resolution functional imaging and nanoscale electrochemical measurements. Here we introduce this technique and provide an overview of its principles, instrumentation, and theory. We discuss the power of SECCM in resolving complex structure-activity problems and provide considerable new information on electrode processes by referring to key example systems, including graphene, graphite, carbon nanotubes, nanoparticles, and conducting diamond. The many longstanding questions that SECCM has been able to answer during its short existence demonstrate its potential to become a major technique in electrochemistry and interfacial science.

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Section: Point Measurements: From Voltammetry To Local Capacitancementioning

confidence: 99%

Scanning Electrochemical Cell Microscopy: A Versatile Technique for Nanoscale Electrochemistry and Functional Imaging

Ebejer

Güell²,

Lai³

et al. 2013

Annual Rev. Anal. Chem.

Self Cite

274

369

View full text Add to dashboard Cite

show abstract

“…This is a key finding that is very clear now. However, several details of the electron-transfer process to/from the tubes are still unclear and the topic is still debated today [40] because "questions remain regarding the fundamental electrochemical properties of CNTs, that need to be resolved for the field to advance in a rational manner" [41].…”

Section: Introductionmentioning

confidence: 99%

“…However, we will see that thin layer effects explain peak shifts occurring on hydrogen peroxide while do not support peaks shift on etoposide and ferrocyanide on MWCNT. Moreover, "heterogeneous electrochemical processes are further complicated by the fact that the vast majority of electrode/electrolyte systems involve solid electrodes that have spatially non uniform properties which may impact significantly on the local activity" [40] while more complex electrochemical systems are usually involved in biosensing with the integration of very large biomolecules such as enzymes that provide direct electron transfer.…”

Section: Introductionmentioning

confidence: 99%

Do Carbon Nanotubes contribute to Electrochemical Biosensing?

Carrara

Baj-Rossi

Boero

et al. 2014

Electrochimica Acta

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a b s t r a c tCarbon nanotubes have been attracting a lot of interest as electron transfer mediators to enhance electrochemical biosensing. The main reason behind this is usually recognized in terms of augmented electrochemical active surface area. The aim of this paper is to review other phenomena that occur at the electrochemical interface. Three distinct features of these phenomena mainly appear in electrochemical biosensing. We introduce the Cottrell, Randle-Sevčick, and Nernst effects to address these features. By using these features, several electrochemical biosensing systems are investigated. Differences among the proposed systems are presented and analyzed in light of these effects. We finally have demonstrated that carbon nanotubes may induce completely opposite effects when dealing with different biosensing systems. This paper also shows that even seemingly small differences (e.g., changing metabolite as detected by the same enzyme) might result in opposite effects on the same carbon nanotube based sensor. Nevertheless, it is shown that carbon nanotubes, in some cases, confirm their exceptional nature in enhancing the sensor performance by orders of magnitude. The sensitivity increases from 87 ± 62 to 3718 ± 73 nA/M ×cm 2 and detection limit decreases from 7.5 ± 5.3 mM to 84 ± 2 M in case of cyclophosphamide detected by the cytochromes P450 3A4.

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“…However, a drawback is that LiFePO 4 suffers from low electronic conductivity 31 , requiring that it is blended with a conductive material such as acetylene black (AB). This results in a complex composite material for which the local structure-function properties are largely unknown, and hence is considered as an ideal system to demonstrate the capabilities of SECCM imaging and multi-microscopy 32 .…”

mentioning

confidence: 99%

Nanoscale visualization of redox activity at lithium-ion battery cathodes

et al. 2014

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Intercalation and deintercalation of lithium ions at electrode surfaces are central to the operation of lithium-ion batteries. Yet, on the most important composite cathode surfaces, this is a rather complex process involving spatially heterogeneous reactions that have proved difficult to resolve with existing techniques. Here we report a scanning electrochemical cell microscope based approach to define a mobile electrochemical cell that is used to quantitatively visualize electrochemical phenomena at the battery cathode material LiFePO 4 , with resolution of B100 nm. The technique measures electrode topography and different electrochemical properties simultaneously, and the information can be combined with complementary microscopic techniques to reveal new perspectives on structure and activity. These electrodes exhibit highly spatially heterogeneous electrochemistry at the nanoscale, both within secondary particles and at individual primary nanoparticles, which is highly dependent on the local structure and composition.

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Electrochemical Mapping Reveals Direct Correlation between Heterogeneous Electron‐Transfer Kinetics and Local Density of States in Diamond Electrodes

Cited by 31 publications

References 65 publications

Scanning Electrochemical Cell Microscopy: A Versatile Technique for Nanoscale Electrochemistry and Functional Imaging

Scanning Electrochemical Cell Microscopy: A Versatile Technique for Nanoscale Electrochemistry and Functional Imaging

Do Carbon Nanotubes contribute to Electrochemical Biosensing?

Nanoscale visualization of redox activity at lithium-ion battery cathodes

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