Universal Approach to Direct Spatiotemporal Dynamic In Situ Optical Visualization of On-Catalyst Water Splitting Electrochemical Processes

Gaurav Bahuguna, Fernando Patolsky

Research output: Contribution to journalArticlepeer-review

Abstract

Electrochemical reactions are the unrivaled backbone of next-generation energy storage, energy conversion, and healthcare devices. However, the real-time visualization of electrochemical reactions remains the bottleneck for fully exploiting their intrinsic potential. Herein, for the first time, a universal approach to direct spatiotemporal-dynamic in situ optical visualization of pH-based as well as specific byproduct-based electrochemical reactions is performed. As a highly relevant and impactful example, in-operando optical visualization of on-catalyst water splitting processes is performed in neutral water/seawater. HPTS (8-hydroxypyrene-1,3,6-trisulfonicacid), known for its exceptional optical capability of detecting even the tiniest pH changes allows the unprecedented “spatiotemporal” real-time visualization at the electrodes. As a result, it is unprecedentedly revealed that at a critical cathode-to-anode distance, the bulk-electrolyte “self-neutralization” phenomenon can be achieved during the water splitting process, leading to the practical realization of enhanced additive-free neutral water splitting. Furthermore, it is experimentally unveiled that at increasing electrolyte flow rates, a swift and severe inhibition of the concomitantly forming acidic and basic ‘fronts’, developed at anode and cathode compartments are observed, thus acting as a “buffering” mechanism. To demonstrate the universal applicability of this elegant strategy which is not limited to pH changes, the technique is extended to visualization of hypochlorite/ chlorine at the anode during electrolysis of sea water using N-(4-butanoic acid) dansylsulfonamide (BADS). Thus, a unique experimental tool that allows real-time spatiotemporal visualization and simultaneous mechanistic investigation of complex electrochemical processes is developed that can be universally extended to various fields of research.

Original languageEnglish
JournalAdvanced Science
DOIs
StateAccepted/In press - 2024

Keywords

  • HPTS
  • confocal microscopy
  • in-operando analysis
  • spatiotemporal dynamic analysis
  • visualizing water splitting

All Science Journal Classification (ASJC) codes

  • Medicine (miscellaneous)
  • General Chemical Engineering
  • General Materials Science
  • Biochemistry, Genetics and Molecular Biology (miscellaneous)
  • General Engineering
  • General Physics and Astronomy

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