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The operation of all electrochemical energy-related systems, such as supercapacitors, batteries, fuel cells, etc. depends largely on the processes occurring at electrochemical interfaces at which charge separation and chemical reactions occur. Evolution of structure and composition at the interface between electrodes and electrolytes affects all the device’s functional parameters including power and long-term performance stability. The analytical techniques capable of exploring the interfaces are still very limited, and more often only ex situ studies are performed. This sometimes leads to a loss of important pieces of the puzzle, hindering the development of novel technologies, as in many cases intermediates and electrochemical reaction products cannot be “quenched” for post-process analyses. Moreover, real electrochemical interfaces are buried, so that they are inaccessible directly to the common surface science tools. At the same time the bulk sensitive techniques suffer from a minor contribution of the interface to the signal. There are following approaches, which potentially address the problem: 1. Attempts to implement traditional surface-sensitive tools like photoemission with increased probing depth and/or minimized electrode or electrolyte layer thickness. 2. Application of techniques with intrinsic interface sensitivity (surface X-ray scattering, vibrational sum frequency generation spectroscopy, surface-enhanced Raman spectroscopy). 3. Efforts to enhance the surface sensitivity of traditionally “bulk-sensitive” techniques such as X-ray absorption spectroscopy. This presentation aims at highlighting approaches and developing ideas on the adaptation of photoelectron, X-ray absorption and vibrational spectroscopy in electrochemical studies