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PreprintCC BYChemRxiv

Time-Resolved Raman Spectroscopy of Nitrate Electroreduction Reveals Dynamic Interfacial Adsorbate Evolution

  • Gabriel Floriano Costa1
  • Jaxiry Barroso-Martinez1
  • Dídac Armand Fenoll Silvestre2
  • Connor Brennan-Pollak3
  • Max García-Melchor2,4
  • María Escudero-Escribano1,5
5 affiliations
  1. 1Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and Barcelona Institute of Science and Technology, UAB Campus, 08193 Bellaterra, Barcelona, Spain
  2. 2CIC energiGUNE, Parque Tecnológico, C/Albert Einstein, 4801510 Vitoria-Gasteiz, Spain
  3. 3School of Chemistry, Trinity College Dublin, Dublin 2, Ireland
  4. 4IKERBASQUE, Basque Foundation for Science, Plaza de Euskadi 5, 48009 Bilbao, Spain
  5. 5Catalan Institution for Research and Advanced Studies (ICREA), Pg. Lluís Companys 23, 08010 Barcelona, Spain
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Abstract

Nitrate electroreduction offers a pathway for coupling wastewater remediation with sustainable ammonia production, yet its mechanistic details under operating conditions remain poorly understood. In this work, we directly resolve the dynamic evolution of nitrate-derived intermediates at electrified interfaces, addressing a key limitation in understanding dynamic reaction pathways. We employ time-resolved surface-enhanced Raman spectroscopy (TR-SERS) to monitor the interfacial behavior of NO 3 – and NO 2 – during nitrate reduction on roughened silver electrodes and observe potential-dependent vibrational shifts attributed to systematic changes in adsorption modes under increasingly cathodic potentials. Density functional theory calculations further support the vibrational assignments and provide insight into preferred binding motifs across the applied potential range. By tracking the time evolution of adsorbates, this approach provides insights into the sequence of adsorption and transformation steps on silver. The combined experimental and computational analysis contributes to a molecular-level understanding of nitrate electroreduction and provides a framework for probing dynamic reaction intermediates in nitrogen conversion electrocatalysis.

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Cite

BibTeXRIS
BibTeX
@misc{costa2026timeresolved,
  title = {{Time-Resolved Raman Spectroscopy of Nitrate Electroreduction Reveals Dynamic Interfacial Adsorbate Evolution}},
  author = {Gabriel Floriano Costa and Jaxiry Barroso-Martinez and Dídac Armand Fenoll Silvestre and Connor Brennan-Pollak and Max García-Melchor and María Escudero-Escribano},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv-2025-v4rj1/v5},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv-2025-v4rj1/v5},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Time-Resolved Raman Spectroscopy of Nitrate Electroreduction Reveals Dynamic Interfacial Adsorbate Evolution
AU  - Gabriel Floriano Costa
AU  - Jaxiry Barroso-Martinez
AU  - Dídac Armand Fenoll Silvestre
AU  - Connor Brennan-Pollak
AU  - Max García-Melchor
AU  - María Escudero-Escribano
PY  - 2026
DA  - 2026/09/29
PB  - ChemRxiv
DO  - 10.26434/chemrxiv-2025-v4rj1/v5
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv-2025-v4rj1/v5
AB  - Nitrate electroreduction offers a pathway for coupling wastewater remediation with sustainable ammonia production, yet its mechanistic details under operating conditions remain poorly understood. In this work, we directly resolve the dynamic evolution of nitrate-derived intermediates at electrified interfaces, addressing a key limitation in understanding dynamic reaction pathways. We employ time-resolved surface-enhanced Raman spectroscopy (TR-SERS) to monitor the interfacial behavior of NO 3 – and NO 2 – during nitrate reduction on roughened silver electrodes and observe potential-dependent vibrational shifts attributed to systematic changes in adsorption modes under increasingly cathodic potentials. Density functional theory calculations further support the vibrational assignments and provide insight into preferred binding motifs across the applied potential range. By tracking the time evolution of adsorbates, this approach provides insights into the sequence of adsorption and transformation steps on silver. The combined experimental and computational analysis contributes to a molecular-level understanding of nitrate electroreduction and provides a framework for probing dynamic reaction intermediates in nitrogen conversion electrocatalysis.
ER  -