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Area of Science:

  • Analytical Chemistry
  • Environmental Science
  • Materials Science

Background:

  • Ammonia is a critical impurity in hydrogen fuel, irreversibly poisoning proton exchange membrane fuel cells.
  • International standards (ISO 14687) mandate stringent ammonia thresholds (100 nmol/mol) for hydrogen fuel purity.
  • Ammonia's role as a hydrogen carrier necessitates accurate quantification, but trace humidity complicates measurements.

Purpose of the Study:

  • To enable accurate trace ammonia quantification for hydrogen purity assessments.
  • To investigate the methodological challenges posed by trace humidity in ammonia measurements.
  • To understand the fundamental interactions between trace ammonia and water in gas sensing systems.

Main Methods:

  • Utilized ultra-long-path Optical-Feedback Cavity-Enhanced Absorption Spectroscopy (OF-CEAS) with an effective optical path length of ~6.17 km.
  • Studied ammonia concentrations of (38.2 ± 0.8), (74.8 ± 0.7), and (112.1 ± 1.2) nmol/mol.
  • Investigated ammonia at trace humidity levels ranging from 0.8 to 8.5 ppmV.

Main Results:

  • Observed a systematic, nonlinear, humidity-dependent positive bias of up to + (1.0 ± 0.2) nmol/mol at 8.5 ppmV humidity.
  • Attributed the bias to water-induced ammonia accumulation in the optical cavity, not spectral interference.
  • Identified distinct hydration states of surface-bound ammonia and enhanced surface adhesion via intermolecular clustering under dry conditions.

Conclusions:

  • Provided deeper insights into trace-level ammonia-water interactions relevant to gas sensing.
  • Established a framework for optimizing methodologies for ultra-long-path optical gas measurement systems.
  • Highlighted the critical impact of trace humidity on the accuracy of ammonia quantification in hydrogen.