Abstract

Ammonia (NH₃) is regarded as an important nitrogen oxides (NOx) precursor and also as an effective reductant for NOx removal in energy utilization through combustion, and it has recently become an attractive non-carbon alternative fuel. To have a better understanding of thermochemical properties of NH₃, accurate in situ detection of NH₃ in high temperature environments is desirable. Ultraviolet (UV) absorption spectroscopy is a feasible technique. To achieve quantitative measurements, spectrally resolved UV absorption cross-sections of NH₃ in hot gas environments at different temperatures from 295 K to 590 K were experimentally measured for the first time. Based on the experimental results, vibrational constants of NH₃ were determined and used for the calculation of the absorption cross-section of NH₃ at high temperatures above 590 K using the PGOPHER software. The investigated UV spectra covered the range of wavelengths from 190 nm to 230 nm, where spectral structures of the A∼ ¹A″₂X∼ ¹A'₁ transition of NH₃ in the umbrella bending mode, v₂, were recognized. The absorption cross-section was found to decrease at higher temperatures. For example, the absorption cross-section peak of the (6, 0) vibrational band of NH₃ decreases from ∼2 × 10⁻¹⁷ to ∼0.5 × 10⁻¹⁷ cm²/molecule with the increase of temperature from 295 K to 1570 K. Using the obtained absorption cross-section, in situ nonintrusive quantification of NH₃ in different hot gas environments was achieved with a detection limit varying from below 10 parts per million (ppm) to around 200 ppm as temperature increased from 295 K to 1570 K. The quantitative measurement was applied to an experimental investigation of NH₃ combustion process. The concentrations of NH₃ and nitric oxide (NO) in the post flame zone of NH₃–methane (CH₄)–air premixed flames at different equivalence ratios were measured.

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