Abstract

The development of novel in situ/operando spectroscopic tools has provided the opportunity for a molecular level understanding of solid/liquid interfaces. Ambient pressure photoelectron spectroscopy using hard X-rays is an excellent interface characterization tool, due to its ability to interrogate simultaneously the chemical composition and built-in electrical potentials, in situ. In this work, we briefly describe the “dip and pull” method, which is currently used as a way to investigate in situ solid/liquid interfaces. By simulating photoelectron intensities from a functionalized TiO2 surface buried by a nanometric-thin layer of water, we obtain the optimal photon energy range that provides the greatest sensitivity to the interface. We also study the evolution of the functionalized TiO2 surface chemical composition and correlated band-bending with a change in the electrolyte pH from 7 to 14. Our results provide general information about the optimal experimental conditions for characterizing the solid/liquid interface using the “dip and pull” method, and the unique possibilities offered by this technique.

Highlights

  • Molecular-level processes occurring at solid/liquid interfaces are intriguing from a fundamental physical-chemical perspective, and from a practical perspective since they are an essential part ofelectrochemical systems, which are key to future renewable energy storage technologies

  • We briefly describe the so-called “dip and pull” method that can be used as a way to investigate the solid/liquid interface in situ by coupling it with ambient pressure hard X-ray photoelectron spectroscopy (AP-HAXPES) using X-ray energies between 2.0 and 10.0 keV [21]

  • Our results provide general information about the experimental conditions that allow for an optimal characterization of the solid/liquid interface using the “dip and pull” method and AP-HAXPES, showing at the same time the capabilities offered by this technique to address fundamental questions in energy materials and conversion research

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Summary

Introduction

Molecular-level processes occurring at solid/liquid interfaces are intriguing from a fundamental physical-chemical perspective, and from a practical perspective since they are an essential part of (photo)electrochemical systems, which are key to future renewable energy storage technologies. This provides a powerful driving force for the development of novel in situ/operando characterization tools that can directly probe the interface [1,2,3,4,5,6,7]. To characterize the true interfacial properties, one should use an experimental probe that limits the Surfaces 2019, 2, 78–99; doi:10.3390/surfaces2010008 www.mdpi.com/journal/surfaces

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