Development of a Sub-ppb Resolution Methane Sensor Using a GaSb-Based DFB Diode Laser near 3270 nm for Fugitive Emission Measurement.

A challenge for mobile measurement of fugitive methane emissions is the availability of portable sensors that feature high sensitivity and fast response times, simultaneously. A methane gas sensor to measure fugitive emissions was developed using a continuous-wave, thermoelectrically cooled, GaSb-based distributed feedback diode laser emitting at a wavelength of 3.27 µm to probe methane in its strong ν3 vibrational band. Direct absorption spectra (DAS) as well as wavelength-modulated spectra (WMS) of pressure-broadened R(3) manifold lines of methane were recorded through a custom-developed open-path multipass cell with an effective optical path length of 6.8 m. A novel metrological approach was taken to characterize the sensor response in terms of the linearity of different WMS metrics, namely, the peak-to-peak amplitude of the X2f component and the peak and/or the integrated area of the background-subtracted quadrature signal (i.e., Q(2f - 2f0)) and the background-subtracted 1f-normalized quadrature signal (i.e., Q(2f/1f - 2f0/1f0)). Comparison with calibration gas concentrations spanning 1.5 to 40 ppmv indicated that the latter WMS metric showed the most linear response, while fitting DAS provides a traceable reference. In the WMS mode, a sensitivity better than 1 ppbv was achieved at a 1 s integration time. The sensitivity and response time are well-suited to measure enhancements in ambient methane levels caused by fugitive emissions.

Systematic experimental comparison of particle filtration efficiency test methods for commercial respirators and face masks.

Respirators, medical masks, and barrier face coverings all filter airborne particles using similar physical principles. However, they are tested for certification using a variety of standardized test methods, creating challenges for the comparison of differently certified products. We have performed systematic experiments to quantify and understand the differences between standardized test methods for N95 respirators (NIOSH TEB-APR-STP-0059 under US 42 CFR 84), medical face masks (ASTM F2299/F2100), and COVID-19-related barrier face coverings (ASTM F3502-21). Our experiments demonstrate the role of face velocity, particle properties (mean size, size variability, electric charge, density, and shape), measurement techniques, and environmental preconditioning. The measured filtration efficiency was most sensitive to changes in face velocity and particle charge. Relative to the NIOSH method, users of the ASTM F2299/F2100 method have commonly used non-neutralized (highly charged) aerosols as well as smaller face velocities, each of which may result in approximately 10% higher measured filtration efficiencies. In the NIOSH method, environmental conditioning at elevated humidity increased filtration efficiency in some commercial samples while decreasing it in others, indicating that measurement should be performed both with and without conditioning. More generally, our results provide an experimental basis for the comparison of respirators certified under various international methods, including FFP2, KN95, P2, Korea 1st Class, and DS2.

Ash-Decorated and Ash-Painted Soot from Residual and Distillate-Fuel Combustion in Four Marine Engines and One Aviation Engine.

Soot is typically the dominant component of the nonvolatile particles emitted from internal combustion engines. Although soot is primarily composed of carbon, its chemistry, toxicity, and oxidation rates may be strongly influenced by internally mixed inorganic metal compounds (ash). Here, we describe the detailed microstructure of ash internally mixed with soot from four marine engines and one aviation engine. The engines were operated on different fuels and lubrication oils; the fuels included four residual fuels and five distillate fuels such as diesel, natural gas, and Jet A-1. Using annular-dark-field scanning transmission electron microscopy (ADF-STEM), we observed that ash may occur either as distinct nodules on the soot particle (decorated) or as continuous streaks (painted). Both structures may exist within a single particle. Decorated soot was observed for both distillate and residual fuels and contained elements associated with either the fuel (V, Ni, Fe, S) or with the lubrication oil (Zn, Ca, P). Painted soot was observed only for residual-fuel soot, and only contained elements associated with the fuel. Additional composition measurements by inductively coupled plasma mass spectrometry (ICP-MS) of filter samples indicated that the internal mixing trends of ash with soot were consistent with the overall ash-to-carbon ratio of the sampled combustion aerosols. Painted soot may form when molten ash coagulates with or condenses onto soot within engines.

Sequential signal detection for high dynamic range time-resolved laser-induced incandescence.

A new method for collecting time-resolved laser-induced incandescence (TiRe-LII) signals with high dynamic range is presented. Gated photomultiplier tubes (PMT) are used to detect temporal sections of the LII signal. This helps to overcome the limitations of PMTs caused by restricted maximum signal current at the strong initial signal and poor signal-to-noise ratios when the signal intensity approaches the noise level. We present a simple method for increasing the accuracy of two-color pyrometry at later decay times and two advanced strategies for getting high accuracy over the complete temperature trace or even achieve single-shot capability with high dynamic range. Validation measurements in a standardized flame show that the method is sensitive enough to even resolve the local increase in gas temperature as a consequence of heating the soot particles with a laser pulse.

Evaluation and comparison of portable emissions measurement systems and federal reference methods for emissions from a back-up generator and a diesel truck operated on a chassis dynamometer.

There is considerable interest in portable emissions measurement systems (PEMS) for emission inventory and regulatory applications. For this study, four commercial PEMS were compared with a Federal Reference Method (FRM) for measuring emissions from a back-up generator (BUG) over steady-state loads and a diesel truck on transient and steady-state chassis dynamometer tests. The agreement between the PEMS and the FRM varied depending on the pollutant and the particular PEMS tested for both the BUG and chassis dynamometer testing. The best performing PEMS for both the BUG and chassis testing was within approximately 12% for NOx of the FRM. For the BUG testing, several PEMS showed agreement with the FRM within approximately 5% for CO2. For the chassis dynamometer testing, the best PEMS showed agreement typically within approximately 5% for CO2. PM measurements for the BUG testing were low compared to the FRM, with the best measurements approximately 20% lower. For the chassis testing, two PM PEMS showed a good correlation but a high bias, while the correlation was worse for the other two PEMS. For each emissions component, some PEMS under different test conditions showed considerably larger deviations than those for the best performing PEMS.

Deconvolution of axisymmetric flame properties using Tikhonov regularization.

We present a method based on Tikhonov regularization for solving one-dimensional inverse tomography problems that arise in combustion applications. In this technique, Tikhonov regularization transforms the ill-conditioned set of equations generated by onion-peeling deconvolution into a well-conditioned set that is less susceptible to measurement errors that arise in experimental settings. The performance of this method is compared to that of onion-peeling and Abel three-point deconvolution by solving for a known field variable distribution from projected data contaminated with an artificially generated error. The results show that Tikhonov deconvolution provides a more accurate field distribution than onion-peeling and Abel three-point deconvolution and is more stable than the other two methods as the distance between projected data points decreases.