Search NASA⌕ Search

SEARCH · Search NASA

Results for “hydroxyl radicals”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 235 records · Page 13

The Global Methane Budget 2000–2017

Understanding and quantifying the global methane (CH 4 ) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH 4 are continuing to increase, making CH 4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO 2 ). Assessing the relative importance of CH 4 in comparison to CO 2 is complicated by its shorter atmospheric lifetime, stronger warming potential, and atmospheric growth rate variations over the past decade, the causes of which are still debated. Two major difficulties in reducing uncertainties arise from the variety of geographically overlapping CH 4 sources and from the destruction of CH 4 by short-lived hydroxyl radicals (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations).

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Global Methane Budget 2000–2020

Abstract. Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. CH4 is the second most important human-influenced greenhouse gas in terms of climate forcing after carbon dioxide (CO2), and both emissions and atmospheric concentrations of CH4 have continued to increase since 2007 after a temporary pause. The relative importance of CH4 emissions compared to those of CO2 for temperature change is related to its shorter atmospheric lifetime, stronger radiative effect, and acceleration in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in quantifying the factors responsible for the observed atmospheric growth rate arise from diverse, geographically overlapping CH4 sources and from the uncertain magnitude and temporal change in the destruction of CH4 by short-lived and highly variable hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to improve, synthesise, and update the global CH4 budget regularly and to stimulate new research on the methane cycle. Following Saunois et al. (2016, 2020), we present here the third version of the living review paper dedicated to the decadal CH4 budget, integrating results of top-down CH4 emission estimates (based on in situ and Greenhouse Gases Observing SATellite (GOSAT) atmospheric observations and an ensemble of atmospheric inverse-model results) and bottom-up estimates (based on process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). We present a budget for the most recent 2010–2019 calendar decade (the latest period for which full data sets are available), for the previous decade of 2000–2009 and for the year 2020. The revision of the bottom-up budget in this 2025 edition benefits from important progress in estimating inland freshwater emissions, with better counting of emissions from lakes and ponds, reservoirs, and streams and rivers. This budget also reduces double counting across freshwater and wetland emissions and, for the first time, includes an estimate of the potential double counting that may exist (average of 23 Tg CH4 yr−1). Bottom-up approaches show that the combined wetland and inland freshwater emissions average 248 [159–369] Tg CH4 yr−1 for the 2010–2019 decade. Natural fluxes are perturbed by human activities through climate, eutrophication, and land use. In this budget, we also estimate, for the first time, this anthropogenic component contributing to wetland and inland freshwater emissions. Newly available gridded products also allowed us to derive an almost complete latitudinal and regional budget based on bottom-up approaches. For the 2010–2019 decade, global CH4 emissions are estimated by atmospheric inversions (top-down) to be 575 Tg CH4 yr−1 (range 553–586, corresponding to the minimum and maximum estimates of the model ensemble). Of this amount, 369 Tg CH4 yr−1 or ∼ 65 % is attributed to direct anthropogenic sources in the fossil, agriculture, and waste and anthropogenic biomass burning (range 350–391 Tg CH4 yr−1 or 63 %–68 %). For the 2000–2009 period, the atmospheric inversions give a slightly lower total emission than for 2010–2019, by 32 Tg CH4 yr−1 (range 9–40). The 2020 emission rate is the highest of the period and reaches 608 Tg CH4 yr−1 (range 581–627), which is 12 % higher than the average emissions in the 2000s. Since 2012, global direct anthropogenic CH4 emission trends have been tracking scenarios that assume no or minimal climate mitigation policies proposed by the Intergovernmental Panel on Climate Change (shared socio-economic pathways SSP5 and SSP3). Bottom-up methods suggest 16 % (94 Tg CH4 yr−1) larger global emissions (669 Tg CH4 yr−1, range 512–849) than top-down inversion methods for the 2010–2019 period. The discrepancy between the bottom-up and the top-down budgets has been greatly reduced compared to the previous differences (167 and 156 Tg CH4 yr−1 in Saunois et al. (2016, 2020) respectively), and for the first time uncertainties in bottom-up and top-down budgets overlap. Although differences have been reduced between inversions and bottom-up, the most important source of uncertainty in the global CH4 budget is still attributable to natural emissions, especially those from wetlands and inland freshwaters. The tropospheric loss of methane, as the main contributor to methane lifetime, has been estimated at 563 [510–663] Tg CH4 yr−1 based on chemistry–climate models. These values are slightly larger than for 2000–2009 due to the impact of the rise in atmospheric methane and remaining large uncertainty (∼ 25 %). The total sink of CH4 is estimated at 633 [507–796] Tg CH4 yr−1 by the bottom-up approaches and at 554 [550–567] Tg CH4 yr−1 by top-down approaches. However, most of the top-down models use the same OH distribution, which introduces less uncertainty to the global budget than is likely justified. For 2010–2019, agriculture and waste contributed an estimated 228 [213–242] Tg CH4 yr−1 in the top-down budget and 211 [195–231] Tg CH4 yr−1 in the bottom-up budget. Fossil fuel emissions contributed 115 [100–124] Tg CH4 yr−1 in the top-down budget and 120 [117–125] Tg CH4 yr−1 in the bottom-up budget. Biomass and biofuel burning contributed 27 [26–27] Tg CH4 yr−1 in the top-down budget and 28 [21–39] Tg CH4 yr−1 in the bottom-up budget. We identify five major priorities for improving the CH4 budget: (i) producing a global, high-resolution map of water-saturated soils and inundated areas emitting CH4 based on a robust classification of different types of emitting ecosystems; (ii) further development of process-based models for inland-water emissions; (iii) intensification of CH4 observations at local (e.g. FLUXNET-CH4 measurements, urban-scale monitoring, satellite imagery with pointing capabilities) to regional scales (surface networks and global remote sensing measurements from satellites) to constrain both bottom-up models and atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) integration of 3D variational inversion systems using isotopic and/or co-emitted species such as ethane as well as information in the bottom-up inventories on anthropogenic super-emitters detected by remote sensing (mainly oil and gas sector but also coal, agriculture, and landfills) to improve source partitioning. The data presented here can be downloaded from https://doi.org/10.18160/GKQ9-2RHT (Martinez et al., 2024).

54 ENVIRONMENTAL SCIENCES↗

SCILLA Secondary Aerosol Volume Concentration Airborne Data

This data set contains secondary aerosol volume concentration in cubic micrometers per cubic centimeter (um^3/cm^3). The aerosol was generated in an oxidation flow reactor (OFR) and its volume concentration measured with a scanning mobility particle sizer (SMPS). Both components were designed and built at the University of California Riverside. Ambient particles were removed with a Teflon filter upstream of the OFR and then pure ammonium sulfate particles were added to create a stable aerosol surface area on which low-volatility oxidation products condense. High concentrations of hydroxyl radical (OH) formed inside the OFR accelerate the oxidative chemistry that would typically occur over a period of several days in the atmosphere, resulting in the production of secondary aerosol from precursor gases present in the ambient air. Concentrations of added ozone and water vapor were controlled to produce the desired and approximately constant level of photochemical aging. The reactor temperature was controlled, while the pressure was not, and was always slightly lower than that of the sampled outside air. Sampled air was pulled from above the Naval Postgraduate School’s (NPS) Twin Otter aircraft through a rear-facing, ¼” OD PFA Teflon tube. The sample stream was split between the OFR and several gas analyzers (NOx, CO, O3, and H2O). Though not contained in these files, data from an aerosol mass spectrometer intermittently operated downstream of the OFR are also available.

{"secondary aerosol concentration",aerosol_concent↗

Physics

Auroral arcs, gas phase ozonation of ethylene and acetylene, prediction of hydroxyl radical microwave transitions, helium escape from earth atmosphere, and shape of magnetosphere

Source record↗

Characterization of hot hydrogen-atom reactions by kinetic spectrography.

The flash photolysis of hydrogen iodide in the presence of nitrous oxide, carbon dioxide, and water has been investigated by kinetic spectroscopy. Although the fraction of hydrogen iodide dissociated was very large, the only observable intermediate was imidogen. It was demonstrated that the rapid removal of imidogen and the apparent absence of hydroxyl radicals in each case is a result of the following two reactions, respectively: (1) NH + HI yields NH2 + I; and (2) OH + HI yields H2O + I.

Tomalesky, R. E.↗

Shock tube study of the reaction H plus O2 plus Ar yields HO2 plus Ar

Rate coefficient data for the recombination reaction H + 02 + Ar yields H02 + Ar have been determined from studies of lean hydrogen-oxygen mixtures behind incident shock waves over the temperature range of 948 to 1125 K. Hydroxyl radical concentration profiles were measured by ultraviolet absorption spectroscopy, and rate data were obtained through analysis of induction time and exponential growth parameter data. Analysis of the data yielded a rate coefficient which was generally lower than most of the more recent values obtained from shock tube studies. The effect of boundary layer formation on the conditions behind the shock was also examined and found to be negligible.

Jachimowski, C. J.↗

Diffusive ignition and combustion in a wall jet

Hydrogen is injected from a downstream facing step in a wall into a high-temperature stream. Temperature and hydroxyl radical concentration are measured downstream of the injection plane by means of ultraviolet absorption spectroscopy. The experimental results are compared with theory which is based on a finite-difference solution of boundary-layer equations. Finite-rate kinetics equations are included in the analysis. The analytic predictions are also compared with previously obtained experimental results which are based on probe measurements. Comparison is made between calculated and observed ignition distances.

Kurkov, A. P.↗

The molecular dynamics of atmospheric reaction

Detailed information about the chemistry of the upper atmosphere took the form of quantitative data concerning the rate of reaction into specified states of product vibration, rotation and translation for exothermic reaction, as well as concerning the rate of reaction from specified states of reagent vibration, rotation and translation for endothermic reaction. The techniques used were variants on the infrared chemiluminescence method. Emphasis was placed on reactions that formed, and that removed, vibrationally-excited hydroxyl radicals. Fundamental studies were also performed on exothermic reactions involving hydrogen halides.

Polanyi, J. C.↗

Diffusive ignition and combustion in a wall jet

Hydrogen is injected from a downstream facing step in a wall into a high-temperature stream. Temperature and hydroxyl radical concentration are measured downstream of the injection plane by means of ultraviolet absorption spectroscopy. The experimental results are compared with theory which is based on a finite-difference solution of boundary-layer equations. Finite-rate kinetics equations are included in the analysis. The analytic predictions are also compared with previously obtained experimental results which are based on probe measurements. Comparison is made between calculated and observed ignition distances.

Kurkov, A. P.↗

Some observations on the oscillatory behavior of carbon monoxide oxidation

The oscillatory behavior of the oxidation of carbon monoxide was experimentally studied in an attempt to further elucidate the reaction at low pressure. The phenomenon is observed as multiple explosions and involves successive flashes of light accompanying the slow reaction in a static system, including over 450 flashes in one case. Electronically excited hydroxyl radicals (water impurity) and carbon dioxide have been identified as components of the emission. The phase difference between the two was seen to be negligible. The nature of the temperature and pressure changes during a cycle indicates that the oscillation is purely kinetic rather than thermokinetic. A procedure is presented whereby sustained oscillations can be obtained for particular regions in the pressure-temperature plane, vessel surface pretreatments, and H2O-containing reactants.

Mccaffrey, B. J.↗

Balloon stratospheric research flights, April 1976 to December 1976

These flights were designed to measure the vertical concentration profile of trace stratospheric species which form major links in the chlorine photochemical system of the upper atmosphere, to measure the vertical concentration profiles of atomic oxygen, the hydroxyl radical and ozone in the stratosphere. An overview of the scientific goals of the program, a statement of program management and support functions, a brief description of the instrumentation flown, pertinent engineering and payload operations data, and a summary of the scientific data obtained for four flights are presented.

Allen, N. C.↗

Nightglow emissions of OH/X 2 pi/ - Comparison of theory and measurements in the /9-3/ band

The visible airglow experiments on the Atmosphere Explorer C and E satellites have viewed the (9-3) band nightglow emission of the excited hydroxyl radical in the lower thermosphere at tropical latitudes. The surface brightnesses observed at similar local times vary by approximately a factor of 2. Comparison of the measurements with time-dependent photochemical calculations shows reasonable agreement and indicates that temporal changes in atmospheric transport processes are the most likely explanation of the nightglow variations.

Frederick, J. E.↗

Three methods for in situ cross-linking of polyvinyl alcohol films for application as ion-conducting membranes in potassium hydroxide electrolyte

Three methods of in situ cross-linking polyvinyl alcohol films are presented. They are: (1) acetalization with a dialdehyde such as glutaraldehyde, (2) acetalization with aldehyde groups formed by selective oxidative cleaving of the few percent of 1,2 diol units present in polyvinyl alcohol, and (3) cross-linking by hydrogen abstraction by reaction with hydrogen atoms and hydroxyl radicals from irradiated water. For the third method, improvement in film conductivity in KOH solution at the expense of mechanical strength is obtained by the presence of polyacrylic acid in the polyvinyl alcohol films. Resistivities in 45 percent KOH are given for in situ cross-linked films prepared by each of the three methods.

Philipp, W. H.↗

The impact of chlorofluoromethane and NO/x/ injections on stratospheric ozone

The chlorofluoromethane problem and the SST problem have been subject to continuing evaluation by the use of one-dimensional stratospheric photochemistry models. The problems to some extent appear to be inversely related to one another through hydroxyl radical reactions; in other words, processes which tend to increase the amount of OH in a model tend to increase the sensitivity of the ozone column to ClX perturbations, while at the same time decreasing the sensitivity to NO(x) perturbations. Evaluations of sensitivity to ClX and NO(x) have varied as new input information has become available and modeling techniques have improved. It is clear that either NO(x) or ClX, or both, will affect the distribution of ozone with altitude.

Stolarski, R. S.↗

Sensitivity of the predicted CO-OH-CH4 perturbation to tropospheric NOx concentrations

Measurements indicate that ambient NOx(NO + NO2) concentrations vary over at least an order of magnitude in the troposphere. Thus it is of interest to study atmospheric chemistry with NOx concentrations covering this range. In this paper we present steady state calculations which show that as NOx concentrations are increased from very low values, the hydroxyl radical concentration increases at first and then decreases. This change of behavior occurs at a concentration of NO2 of about 0.23 ppb in the model. Also, the response of the atmosphere to increased CO fluxes undergoes a qualitative change as a function of the concentration of NOx. At low levels of NOx concentration, an increase in CO fluxes into the atmosphere depletes the OH concentration and increases the concentrations of CH4 and H2, as reported in the literature. However, at high values of NOx concentration, increased CO fluxes give rise to an increase in the OH concentration and, consequently, a decrease in the concentrations of CH4 and H2.

Hameed, S.↗