Interfacial Electrochemistry in Liquids Probed with Photoemission Electron Microscopy

Nemšák, Slavomír; Strelcov, Evgheni; Duchoň, Tomáš; Guo, Hongxuan; Hackl, Johanna; Yulaev, Alexander; Vlassiouk, Ivan; Mueller, David N.; Schneider, Claus M.; Kolmakov, Andrei

doi:10.1021/jacs.7b07365

Cited by 30 publications

(10 citation statements)

References 31 publications

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“…Copyright 2018 American Chemical Society using higher-quality graphene with fewer defects would reduce the number of sites for preferential attack, but this is practically limited by the quality of graphene that can be reliably obtained by CVD. Stacking multiple graphene layers may also be beneficial, as the probability of two defects overlapping will correspond to the square of the defect density of SLG, and this approach has indeed been used in several reports to improve stability [98,99,108,133], although it comes at the expense of reduced photoelectron transmission, as discussed earlier. Instead of this, other 2D materials could be employed which are more resistant to oxidative attack such as h-BN [134], however its insulating behaviour is likely to result in undesirable charging during measurement.…”

Section: Chemical Stabilitymentioning

confidence: 99%

“…This has included X-ray absorption measurements of the O K-edge of liquid water acquired in partial electron yield (PEY) mode [98], as well as similar Auger electron spectroscopy (AES) measurements [108]. This approach has also been applied to detect Cu ions in aqueous solutions of CuSO 4 and H 2 SO 4 during electrochemical cycling [133]. Measuring the Cu L 3 -edge at different potentials reveals differences in the ratio of Cu + to Cu 2+ ions as the graphene membranes is biased relative to a Pt counter electrode, consistent with copper(II) ion reduction on the graphene electrode.…”

Section: Solid-liquid Interfacesmentioning

confidence: 99%

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2D Material Membranes for Operando Atmospheric Pressure Photoelectron Spectroscopy

Weatherup

2018

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Probing the chemistry that occurs at catalyst interfaces under realistic process conditions is key to the rational design of better materials for industrial catalytic reactions. Ambient pressure X-ray photoelectron spectroscopy, has until recently been limited to pressures two orders of magnitude below atmosphere. However, the development of photoelectron transparent membranes based on two-dimensional materials that can maintain large pressure differences and yet have thicknesses approaching or even falling below the inelastic mean free path of photoelectrons, now allows the atmospheric pressure regime and above to be accessed. We introduce here the fundamental principles underlying this membrane-based approach to atmospheric pressure photoelectron spectroscopy, and in this context highlight some of the key design concepts and challenges in performing experiments with this technique. We discuss a number of recent proof-of-concept studies, and highlight the potential of the membrane-based approach for operando characterisation of catalyst interfaces under reaction conditions, as well as some current challenges and limitations in this area.

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Section: Chemical Stabilitymentioning

confidence: 99%

Section: Solid-liquid Interfacesmentioning

confidence: 99%

2D Material Membranes for Operando Atmospheric Pressure Photoelectron Spectroscopy

Weatherup

2018

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“…The third approach is to reduce the thickness of the solid. Graphene-capped microchannels 4 , 5 or an electrochemical in-situ cell with graphene windows 6 − 8 used exactly that strategy to enable soft X-ray spectroscopy of a solid–liquid interface. In the latter case, it is assured that the liquid phase has bulk properties, but the fragile, atomically thin windows pose a high risk to the experimental setup (see Table 1 ).…”

Section: Introductionmentioning

confidence: 99%

Graphene-Capped Liquid Thin Films for Electrochemical Operando X-ray Spectroscopy and Scanning Electron Microscopy

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Diaz

et al. 2020

ACS Appl. Mater. Interfaces

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Electrochemistry is a promising building block for the global transition to a sustainable energy market. Particularly the electroreduction of CO 2 and the electrolysis of water might be strategic elements for chemical energy conversion. The reactions of interest are inner-sphere reactions, which occur on the surface of the electrode, and the biased interface between the electrode surface and the electrolyte is of central importance to the reactivity of an electrode. However, a potential-dependent observation of this buried interface is challenging, which slows the development of catalyst materials. Here we describe a sample architecture using a graphene blanket that allows surface sensitive studies of biased electrochemical interfaces. At the examples of near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) and environmental scanning electron microscopy (ESEM), we show that the combination of a graphene blanket and a permeable membrane leads to the formation of a liquid thin film between them. This liquid thin film is stable against a water partial pressure below 1 mbar. These properties of the sample assembly extend the study of solid–liquid interfaces to highly surface sensitive techniques, such as electron spectroscopy/microscopy. In fact, photoelectrons with an effective attenuation length of only 10 Å can be detected, which is close to the absolute minimum possible in aqueous solutions. The in-situ cells and the sample preparation necessary to employ our method are comparatively simple. Transferring this approach to other surface sensitive measurement techniques should therefore be straightforward. We see our approach as a starting point for more studies on electrochemical interfaces and surface processes under applied potential. Such studies would be of high value for the rational design of electrocatalysts.

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“…Using this MCA platform, we studied the pure water and electrochemical reaction in aqueous electrolytes, such as CuSO4 with different electron imaging and spectroscopy techniques. [4][5][6] In this study, we found that secondary electron (SE) yield from graphene membrane on the top of electrolyte sensitively depends on the MCA cell polarization potential. The SE depends on the electron density of states in the graphene and within EDL as well as the local potential inside the electron escape depth region.…”

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confidence: 84%

Polarization of the Graphene-Liquid Electrolyte Interface Probed by SEM

et al. 2018

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Interfacial Electrochemistry in Liquids Probed with Photoemission Electron Microscopy

Cited by 30 publications

References 31 publications

2D Material Membranes for Operando Atmospheric Pressure Photoelectron Spectroscopy

2D Material Membranes for Operando Atmospheric Pressure Photoelectron Spectroscopy

Graphene-Capped Liquid Thin Films for Electrochemical Operando X-ray Spectroscopy and Scanning Electron Microscopy

Polarization of the Graphene-Liquid Electrolyte Interface Probed by SEM

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