Bryan Rainwater

Methane emissions from end-use installations in residential natural gas systems remain poorly quantified, despite their importance to both safety and climate policies worldwide. While distribution networks and appliances have received research attention, interior piping between the meter and appliances represents a critical knowledge gap. To address this gap, a systematic survey of 473 residential systems in Saarlouis, Germany was conducted using standardized pressure-decay tests (DVGW G 600). Measurements were performed during the installation of gas regulators necessitated by a grid pressure increase from 23 mbar to 55 mbar above ambient. This provided a unique opportunity to assess whole-system leakage under controlled conditions without installation modifications. Leak rates were standardized to reference pressure and converted to methane emissions using measured gas composition. A total of 411 (86.9%) installations showed no detectable leak rate (LDL: 0.2 l h-1). However, seven systems (1.5%) exceeded 1 l h-1, and one surpassed the unacceptable threshold of 5 l h-1. Mean emissions across all systems were 0.067 [0.041, 0.098] g h-1, with smaller installations showing higher volume-normalized rates. Critically, fewer than 1.48% of systems contributed more than 46% of total emissions, demonstrating a strongly skewed, heavy-tailed distribution. Scaled nationally using Monte Carlo methods accounting for sampling uncertainty and skewed distributions, residential interior piping contributes 12.30 [8.11, 18.55] Gg yr-1 to Germany's methane emissions. These results emphasize the need to include residential leak rates in emission inventories and highlight the efficiency potential of targeted mitigation strategies focused on high-emitting installations under evolving EU methane regulations.

Accurate methane emission estimates are essential for climate policy, yet current field methods often struggle with spatial constraints and source complexity. Ground-based mobile approaches frequently miss key plume features, introducing bias and uncertainty in emission rate estimates. This study addresses these limitations by using small unmanned aerial systems equipped with precision gas sensors to measure methane alongside co-released tracers. We tested whether arc-shaped flight paths and alternative ratio estimation methods could improve the accuracy of tracer-based emission quantification under real-world constraints. Controlled releases using ethane and nitrous oxide tracers showed that (1) arc flights provided stronger plume capture and higher correlation between methane and tracer concentrations than traditional flight paths; (2) the cumulative sum method yielded the lowest relative error (as low as 3.3%) under ideal mixing conditions; and (3) the arc flight pattern yielded the lowest relative error and uncertainty across all experimental configurations, demonstrating its robustness for quantifying methane emissions from downwind plume measurements. These findings demonstrate a practical and scalable approach to reducing uncertainty in methane quantification. The method is well-suited for challenging environments and lays the groundwork for future applications at the facility scale.

The quantification of methane concentrations in air is essential for the quantification of methane emissions, which in turn is necessary to determine absolute emissions and the efficacy of emission mitigation strategies. These are essential if countries are to meet climate goals. Large-scale deployment of methane analyzers across millions of emission sites is prohibitively expensive, and lower-cost instrumentation has been recently developed as an alternative. Currently, it is unclear how cheaper instrumentation will affect measurement resolution or accuracy. To test this, the Wireless Autonomous Transportable Methane Emission Reporting System (WATCH₄ERS) has been developed, comprising four commercially available sensing technologies: metal oxide (MOx,), Non-dispersion Infrared (NDIR), integrated infrared (INIR), and tunable diode laser absorption spectrometer (TDLAS). WATCHERS is the accumulated knowledge of several long-term methane measurement projects at Colorado State University’s Methane Emission Technology Evaluation Center (METEC), and this study describes the integration of these sensors into a single unit and reports initial instrument response to calibration procedures and controlled release experiments. Specifically, this paper aims to describe the development of the WATCH₄ERS unit, report initial sensor responses, and describe future research goals. Meanwhile, future work will use data gathered by multiple WATCH₄ERS units to 1. better understand the cost–benefit balance of methane sensors, and 2. identify how decreasing instrumentation costs could increase deployment coverage and therefore inform large-scale methane monitoring strategies. Both calibration and response experiments indicate the INIR has little practical use for measuring methane concentrations less than 500 ppm. The MOx sensor is shown to have a logarithmic response to methane concentration change between background and 600 ppm but it is strongly suggested that passively sampling MOx sensors cannot respond fast enough to report concentrations that change in a sub-minute time frame. The NDIR sensor reported a linear change to methane concentration between background and 600 ppm, although there was a noticeable lag in reporting changing concentration, especially at higher values, and individual peaks could be observed throughout the experiment even when the plumes were released 5 s apart. The TDLAS sensor reported all changes in concentration but remains prohibitively expensive. Our findings suggest that each sensor technology could be optimized by either operational design or deployment location to quantify methane emissions. The WATCH₄ERS units will be deployed in real-world environments to investigate the utility of each in the future.

The quantification of methane concentrations in air is essential for the quantification of methane emissions, which in turn is necessary to determine absolute emission and the efficacy of emission mitigation strategies. These are essential if countries are to meet climate goals. Large scale deployment of methane analyzers across the millions of emission sites is prohibitively expensive and lower-cost instrumentation has been recently developed as an alternative. Currently, it is unclear how cheaper instrumentation will affect measurement resolution or accuracy. To test this, the Wireless Autonomous Transportable Methane Emission Reporting System (WATCH4ERS) has been developed and comprises four sensing technologies: Metal Oxide (MOx,); Non-dispersion Infrared (NDIR); Integrated Infrared (INIR); and Tunable Diode Laser Absorption Spectrometer (TDLAS). This study describes the integration of these sensors to a single unit and test instrument response through calibration and downwind tests. Both calibration and response experiments indicate the INIR has little practical use for measuring methane concentrations less than 500 ppm. The MOx sensor is shown to have a logarithmic response to methane concentration change between background and 600 ppm but it is strongly suggested that passively sampling MOx sensor cannot respond fast enough to report concentrations that change on a sub-minute time frame. The NDIR sensor reported linear change to methane concentration between background and 600 ppm, although there was a noticeable lag in reporting changing concentration especially at higher values, and individual peaks could be observed throughout the experiment even when the plumes were released 5 s apart. The TDLAS sensor re-ported all changes in concentration but remains prohibitively expensive. Our findings suggest that each sensor technology could be optimized by either operational design or deployment location to quantify methane emissions and the WATCH4ERS units will be deployed in real-world environments to investigate the utility of each in the future.

Supercooled liquid clouds are ubiquitous over the Southern Ocean (SO), even to temperatures below −20°C, and comprise a large fraction of the marine boundary layer (MBL) clouds. Earth system models and reanalysis products have struggled to reproduce the observed cloud phase distribution and occurrence of cloud ice in the region. Recent simulations found the microphysical representation of ice nucleation and growth has a large impact on these properties, however, measurements of SO ice nucleating particles (INPs) to validate simulations are sparse. This study presents measurements of INPs from simultaneous aircraft and ship campaigns conducted over the SO in austral summer 2018, which include the first in situ observations in and above cloud in the region. Our results confirm recent observations that INP concentrations are uniformly lower than measurements made in the late 1960s. While INP concentrations below and above cloud are similar, higher ice nucleation efficiency above cloud supports model simulations that the dominant INP composition varies with height. Model parameterizations based solely on aerosol properties capture the mean relationship between INP concentration and temperature but not the observed variability, which is likely related to the only modest correlations observed between INPs and environmental or aerosol metrics. Including wind speed in addition to activation temperature in a marine INP parameterization reduces bias but does not explain the large range of observed INP concentrations. Direct and indirect inference of marine INP size suggests MBL INPs, at least during Austral summer, are dominated by particles with diameters smaller than 500 nm.

Supercooled liquid clouds are ubiquitous over the Southern Ocean (SO), even to temperatures below -20 °C, and comprise a large fraction of the marine boundary layer (MBL) clouds. Earth system models and reanalysis products have struggled to reproduce the observed cloud phase distribution and occurrence of cloud ice in the region. Recent simulations found the microphysical representation of ice nucleation and growth has a large impact on these properties, however, measurements of SO ice nucleating particles (INPs) to validate simulations are sparse. This study presents measurements of INPs from simultaneous aircraft and ship campaigns conducted over the SO in austral summer 2018, which include the first in situ observations in and above cloud in the region. Our results confirm recent observations that INP concentrations are uniformly lower than measurements made in the late 1960s. While INP concentrations below and above cloud are similar, higher ice nucleation efficiency above cloud supports model inferences that the dominant INP composition varies with height. Model parameterizations based solely on aerosol properties capture the mean relationship between INP concentration and temperature but not the observed variability, which is likely related to the only modest correlations observed between INPs and environmental or aerosol metrics. An updated parameterization for marine INPs is proposed, which reduces bias relative to existing methods by including wind speed as an additional variable. Direct and indirect inference of marine INP size suggests MBL INPs, at least those in the sub-2.5 μm range, are dominated by particles with diameters smaller than 500 nm.

Southern Ocean (SO) low‐level mixed phase clouds have been a long‐standing challenge for Earth system models to accurately represent. While improvements to the Community Earth System Model version 2 (CESM2) resulted in increased supercooled liquid in SO clouds and improved model radiative biases, simulated SO clouds in CESM2 now contain too little ice. Previous observational studies have indicated that marine particles are major contributor to SO low‐level cloud heterogeneous ice nucleation, a process that initiates a number of cloud processes that govern cloud radiative properties. In this study, we utilize detailed aerosol and ice nucleating particle (INP) measurements from two recent measurement campaigns to assess simulated aerosol abundance, number size distributions, and composition and INP parameterizations for use in CESM2. Our results indicate that CESM2 has a positive bias in simulated surface‐level total aerosol surface area at latitudes north of 58°S. Measured INP populations were dominated by marine INPs and we present evidence of refractory INPs present over the SO assumed here to be mineral dust INPs. Results highlight a critical need to assess simulated mineral dust number and size distributions in CESM2 in order to adequately represent SO INP populations and their response to long‐term changes in atmospheric transport patterns and land use change. We also discuss important cautions and limitations in applying a commonly used mineral dust INP parameterization to remote regions like the pristine SO.