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At least 181 records · Page 10

Spatio-Temporal Variability of Atmospheric CO2 as Observed from In-Situ Measurements over North America during NASA Field Campaigns (2004-2008)

Regional-scale measurements were made over the eastern United States (Intercontinental Chemical Transport Experiment - North America (INTEX-NA), summer 2004); Mexico (Megacity Initiative: Local and Global Research Observations (MILAGRO), March 2006); the eastern North Pacific and Alaska (INTEX-B May 2006); and the Canadian Arctic (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS), spring and summer 2008). For these field campaigns, instrumentation for the in situ measurement of CO2 was integrated on the NASA DC-8 research aircraft providing high-resolution (1 second) data traceable to the WMO CO2 mole fraction scale. These observations provide unique and definitive data sets via their intermediate-scale coverage and frequent vertical profiles (0.1 - 12 km) for examining the variability CO2 exhibits above the Earth s surface. A bottom-up anthropogenic CO2 emissions inventory (1deg 1deg) and processing methodology has also been developed for North America in support of these airborne science missions. In this presentation, the spatio-temporal distributions of CO2 and CO column values derived from the campaign measurements will be examined in conjunction with the emissions inventory and transport histories to aid in the interpretation of the CO2 observations.

Choi, Yonghoon↗

Improving Efficiency of Off-Road Vehicles by Novel Integration of Electric Machines and Advanced Combustion Engines

Modern off-road equipment will increasingly rely on electrified implements that will deliver precision control with a smaller footprint than hydraulics. The primary energy converter, however, will be an onboard reciprocating internal combustion engine because of the power density of hydrocarbon fuels in comparison to electrical energy storage and the remote locations where much of this equipment is deployed. Adding energy storage and electric machines creates opportunities to improve efficiency while reducing emissions. This program investigated approaches to take advantage of the extra flexibility that an enhanced electrical system to enable high-efficiency, low-emissions combustion technologies. The current program evaluated hybridization of both the torque application and air-handling systems to maximize efficiency while minimizing cost. This program designed, analyzed and tested a hybrid off-road vehicle consisting of a series electric powertrain with energy storage, an electrified air system, and a 33% downsized diesel engine. Detailed comparisons were made between the base powertrain and the developed powertrain using powertrain simulations, engine testing, and vehicle testing. The key results of the study are: • The resulting vehicle reduces fuel consumption by 5% to 15% at equal productivity. The primary improvements were due to recovery of regenerative braking losses for cycles where large transients are encountered. • The electrified air system was an enabler to allow engine downsizing. This was most important for duty-cycles where the engine primarily operated at moderate loads and had few low speed high torque conditions. • Engine level improvements showed re-optimization of the powertrain is possible when electrified air handing is available. Increased exhaust gas recirculation and advanced injection timing allowed up to a 15% reduction in brake specific fuel consumption at equal NOx and transient response. Compared to the larger engine, the downsized engine achieves up to an 18% reduction in brake specific fuel consumption over the non-road transient cycle. • The life cycle analysis and total cost of ownership study showed that the hybrid powertrain has the potential to reduce 5-year CO2 and total cost of ownership by ~6% over the baseline vehicle. The results also indicated that a pure battery electric vehicle is not feasible in this application and is likely to increase the CO2 emissions due to the CO2 from battery production. A hybrid powertrain with low carbon fuels shows the potential to substantially reduce CO2 and total cost of ownership.

02 PETROLEUM↗

Coal-based Bricks & Blocks (CBBs): Process Development to Prototype Fabrication Coupled with Techno-Economic Analysis and Market Survey

The decline of coal use for energy production provides an abundance of local feedstock for new innovative uses and value-added products. Expanding the U.S. coal-value chain to manufacture high-value carbon products can strengthen the nation’s energy and mineral security, enhance the U.S. national defense security, increase the United States’ economic prosperity, while achieving U.S. environmental objectives. The primary project goal is a relatively light-weight composite product with superior (or comparable) compressive strength. Both virgin and, where available, post-consumer recycled thermoplastic versions are tested for each thermoplastic species. A useful attribute of thermoplastics as binders is that they can be heated to their melting point, cooled, and reheated again without significant degradation. A key advantage of thermoset CBBs is that they require only mixing and molding. CBB advantages include low cost, availability, binding ability and processability. Coal-based bricks and blocks (CBBs) weigh about 50% less than clay bricks and can be manufactured with an interlocking design to promote ease of use for the novice builder. CBB formulation is evaluated according to a design-of-experiments (DoE) approach. DoE variables are a) relative weight fractions of binder, b) relative proportions of large versus small (milled) anthracite size fractions, and c) additive percentage. Fabrication methods include hot-press molding and extrusion, the later being the most commercially viable. CBBs are tested for compressive strength, modulus of rupture (by flexure test) and water absorption per ASTM C67, with density determined by the Archimedes drainage method. Fractured interfaces are examined by SEM (Scanning Electron Microscopy) to resolve fracture dynamics and interior microstructure uniformity. Differential scanning calorimetry (DSC) is used to compare plastic transition temperatures i.e., glass and melting temperatures to contrast virgin with post-consumer recycled thermoplastics and optimize their usage. These results are used in the DoE analysis to identify the binder and relative weight percentages for optimum strength, density, and porosity. Overall, CBBs possess strength comparable to clay-based bricks but are non-permeable and hydrophobic, and hence resistant to degradation by freeze-fracturing, corrosion, and efflorescence. The strongest composites have been made with the following thermoplastic binders (in order of strength): thermoset, high-density polyethylene crosslink resin, high-density polyethylene, nylon 6/6, and polypropylene. Results from a techno-economic analysis TEA show economy of scale for CBBs by modularization and reveal the binder as the cost driver for material costs. Ideally, the incorporation of post-consumer recycled thermoplastic will decrease material acquisition costs and increase product sustainability. Notably, CBBs do not require the high temperature calcination needed to produce cement, nor do they require firing in the 1600-2400 °F range for three days using natural gas, as do clay brick equivalents. Instead, CBBs are heated to a modest <600 °F according to the melt flow index of the thermoplastic binder. Existing anthracite mines can be expanded to produce CBBs to reduce aggregate transportation costs and emissions that exist for clay bricks. TEA reflects this reduced energy cost while a comparative CO2 emission analysis quantifies the reduced environmental footprint. The market survey identifies several commercialization opportunities, dependent upon the brick classification.

01 COAL, LIGNITE, AND PEAT↗

Hybrid Capture for Net-Negative Emissions

The Energy & Environmental Research Center, in partnership with the U.S. Department of Energy and North Dakota ethanol producer Red Trail Energy, LLC (RTE), completed an initial engineering design (IED) for a potential hybrid capture system at the RTE CCS (carbon capture and storage) site. The RTE CCS Project is currently operating a CO2 capture facility, adjacent to the RTE ethanol facility in western North Dakota, and injecting the CO2 more than a mile below RTE property for permanent storage. This novel process would add capturing CO2 produced from natural gas boilers to the existing bioprocessing capture system to achieve a net-negative CO2 emissions industrial process at commercial scale (~310,000 tonnes/yr CO2). Initial findings of the IED showed the hybrid system to be technically viable with a moderate estimated cost of $55/tonne CO2 captured for the hybrid system. A cradle-to-gate life cycle assessment (LCA) was also conducted, showing preliminary net-negative carbon emissions potential anticipated from implementing a hybrid CCS system at a commercial scale. Recommended next steps toward potential implementation include hybrid capture system demonstration testing for detailed engineering and LCA model comparisons with low-carbon fuel incentive programs for financial support.

01 COAL, LIGNITE, AND PEAT↗

Increasing anthropogenic methane emissions arise equally from agricultural and fossil fuel sources

Climate stabilization remains elusive, with increased greenhouse gas concentrations already increasing global average surface temperatures 1.1°C above pre-industrial levels (World Meteorological Organization 2019). Carbon dioxide (CO2) emissions from fossil fuel use, deforestation, and other anthropogenic sources reached ~ 43 billion metric tonnes in 2019 (Friedlingstein et al 2019, Jackson et al 2019). Storms, floods, and other extreme weather events displaced a record 7 million people in the first half of 2019 (IDMC 2019). When global mean surface temperature four million years ago was 2°C–3°C warmer than today (a likely temperature increase before the end of the century), ice sheets in Greenland and West Antarctica melted and parts of East Antarctica’s ice retreated, causing sea levels to rise 10–20 m (World Meteorological Organization 2019). Methane (CH4) emissions have contributed almost one quarter of the cumulative radiative forcings for CO2, CH4, and N2O (nitrous oxide) combined since 1750 (Etminan et al 2016). Although methane is far less abundant in the atmosphere than CO2, it absorbs thermal infrared radiation much more efficiently and, in consequence, has a global warming potential (GWP) ~86 times stronger per unit mass than CO2 on a 20-year timescale and 28- times more powerful on a 100-year time scale (IPCC 2014). Global average methane concentrations in the atmosphere reached ~1875 parts per billion (ppb) at the end of 2019, more than two-and-a-half times preindustrial levels (Dlugokencky 2020). The largest methane sources include anthropogenic emissions from agriculture, waste, and the extraction and use of fossil fuels as well as natural emissions from wetlands, freshwater systems, and geological sources (Kirschke et al 2013, Saunois et al 2016a, Ganesan et al 2019). Here, we summarize new estimates of the global methane budget based on the analysis of Saunois et al (2020) for the year 2017, the last year of the new Global Methane Budget and the most recent year data are fully available. We compare these estimates to mean values for the reference ‘stabilization’ period of 2000–2006 when atmospheric CH4 concentrations were relatively stable. We present data for sources and sinks and provide insights for the geographical regions and economic sectors where emissions have changed the most over recent decades.

fossil fuel sources↗

Geologic Carbon Storage of Anthropogenic CO2 under the Colorado Plateau in Emery County, Utah

Geologic Carbon Storage (GCS) is a promising technology for storing large volumes of anthropogenic CO2 effectively and permanently. Numerical simulations are an integral part of site selection and characterization for any potential GCS site. As part of the DOE-funded CarbonSAFE Rocky Mountains Phase I project, a regional GCS analysis was undertaken to understand the efficacy of storing CO2 emissions from the power generation and heavy industry in central Utah’s favorable geology. In this study, the injection of CO2 for geologic storage was simulated in the Navajo Sandstone Formation in Emery County, Utah. Carbon dioxide was sourced from regional power generation stations and heavy industries throughout Utah, with an emphasis on emissions reduction at the Hunter Power Plant near Castle Dale, Utah. A simulation grid was extracted from the project’s geological model encompassing an area around Price, Huntington, and Castle Dale in central Utah. The Navajo Sandstone Member of the Glen Canyon Group was the target of CO2 injection with the overlying Carmel formation providing the primary seal. A suite of simulations was performed assessing the viability of this area for permanent CO2 storage. Results indicate that the area can not only store 46 million metric tons of anthropogenic CO2, meeting the project goals, but this area has the capacity to securely store at least 1.3 billion tons of CO2, suggesting the injection site and surrounding geology are suitable locations for commercial-scale GCS.

58 GEOSCIENCES↗

Data for Carbon-negative Hydrogen: Aqueous Phase Reforming (APR) of Glycerol over NiPt Bimetallic Catalyst Coupled with CO2 Sequestration

Herein we report the production of high-pressure (19.3 bar), carbon-negative hydrogen (H2) from glycerol with a purity of 98.2 mol% H2, 1.8 mol% light hydrocarbons (mainly methane), and 400 ppm of CO. Aqueous phase reforming (APR) of 10 wt% glycerol solution was studied with a series of NiPt alumina bimetallic catalysts supported on alumina. The Ni8Pt1-450 catalyst had the highest hydrogen selectivity (95.6%) and the lowest alkanes selectivity (3.7%) of the tested catalysts. The hydrogen selectivity decreased in the order of Ni8Pt1-450 > Ni8Pt1-260 > Ni1Pt1-260 > Pt-260. The CO2 was sequestered with CaO adsorbent which formed CaCO3. We measured the adsorption capacity of the CaO adsorbent at different temperatures. Life cycle analysis showed that the APR of glycerol coupled with CO2 capture has net negative CO2 equivalent greenhouse gas emissions. The CO2 emissions are −9.9 kg CO2 eq./kg H2 and −50.1 kg CO2 eq./kg H2 when grid electricity and renewable electricity are used, respectively, and the CO2 is allocated respectively to the mass of products produced. The cost of this H2 (denoted as “green-emerald”) was estimated to be 2.4 USD per kg H2 when grid electricity is used and 2.7 USD per kg H2 when using renewable electricity. The cost of glycerol has the highest contribution of 1.71 USD per kg H2. Participation in the carbon credit markets can further decrease the price of the produced H2.

Catalysis↗

CarbonSAFE North Dakota – Early Successes

Conference presentation for American Institute of Chemical Engineers (AIChE) Annual Meeting, Boston, MA and virtual, November 5–11 and 15–19, 2021. As part of the U.S. Department of Energy’s (DOE’s) CarbonSAFE program, the Energy & Environmental Research Center (EERC) is conducting commercial-scale site characterization and permitting of up to two geologic horizons for the geologic storage of anthropogenic CO2 emissions. These storage horizons would collectively and permanently store nearly 4 million metric tons (MMt) of CO2 per year captured as part of Minnkota Power Cooperative’s (Minnkota’s) Project Tundra. Minnkota’s ambitious initiative to build the world’s largest postcombustion carbon capture and storage facility in central North Dakota demonstrates the existence of a business case for carbon capture, and storage (CCS).

20 FOSSIL-FUELED POWER PLANTS↗

Low-GWP Refrigerants Status and Outlook

Refrigeration - including air conditioning (AC) – contributes substantially to the modern life of the 21st century and its economy. The food cold chain, air conditioning, healthcare and energy are examples of sectors for which refrigeration is indispensable. About 5 billion refrigeration systems – of different types and sizes– operate worldwide in different applications [1]. The dominant share of equipment providing refrigeration operate on the vapor-compression-cycle principle and use fluorocarbon refrigerants. Concerns about the environmental safety have become the driving force for refrigerant changes within the last 35 years. The phased-out schedule of stratospheric-ozone-depleting fluids was first formulated by the Montreal Protocol (MP) in 1987 and was made more stringent during the follow-up international meetings [2]. The affected chlorofluorocarbon (CFC) and hydrochlorofluorocarbon (HCFC) refrigerants were largely replaced by hydrofluorocarbons (HFCs).The 2016 Kigali Amendment to the MP [3] responses to the concerns about the Earth climate change. The refrigeration and AC sectors are attributed with about 7.8 % of global greenhouse gas emissions [4]. This contribution comes in the form of direct effect, which is related to refrigerant emissions from refrigeration systems (37 %), and in the form of indirect effect, which is related to CO2 emissions from fossil fuel power plants producing electricity to power refrigeration systems (63 %) [4]. The Kigali Amendment aims at reducing the direct effect. The effect a given molecule has on the climate change is quantified in a simplified manner by its Global Warming Potential (GWP), a relative index referencing the effect produced to that of the same mass of carbon dioxide released to the atmosphere. By definition, GWP of carbon dioxide is equal to one.While HFC refrigerants have on average a lower GWP than the CFCs and HCFCs they replaced, they are still potent greenhouse gases (GHGs). The Kigali Amendment phases down the use of HFCs by imposing a schedule for reducing a weighted GWP value to be implemented by a country through the year 2047 (Figure 1). It provides four paths depending on the country location and category assigned in the MP, and also prescribes a method for establishing the baseline consumption used for calculating GWP reductions. For developing countries, it is expected to bring the weighed GWP across all refrigeration applications down to about 300 from the baseline value of about 2000. The implementation of Kigali Amendment aims at reducing the future warming due to HFCs from the range of 0.3 °C to 0.5 °C to less than 0.1 °C [5]. While this reduction may seem to be small, it must be viewed in the context of the 2015 Paris Agreement [6], which calls for holding global warming to well below 2 °C and pursuing to limit global warming to 1.5 °C relative to pre-industrial levels [6]. Considering that average global temperatures reached 1 °C above pre-industrial levels for the first time in 2015 [7], the Earth is already within 1 °C of the “2 °C limit”.The low-GWP requirement narrows the pool of fluids that can be considered for application as a refrigerant [8]. This Informatory Note discusses low-GWP refrigerant options for major applications and presents their selection merits.

Yana Motta, Samuel↗

The Industrial Efficiency and Decarbonization Office

The Industrial Efficiency and Decarbonization Office (IEDO) supports innovation technologies and the adoption of practices to enable the industrial sector to cost-effectively reduce greenhouse gas (GHG) emissions. IEDO and its programs are critical to putting the Nation on a pathway to reduce CO2 emissions by 50% by 2030 when compared to 2005 levels, and to achieve net-zero carbon emissions by 2050. With 30% of primary energy-related emissions attributable to the industrial sector, IEDO builds upon a foundation of energy efficiency as a decarbonization pathway to include process electrification, use of low carbon fuels and feedstocks, and carbon capture to meet industrial emissions reductions targets. IEDO provides planning, management, and direction necessary for a balanced national program of research, development, demonstration, technical assistance, and workforce development to drive energy, materials and production efficiency, and decarbonization across the industrial sector.

Energy-Intensive Industries, Cross-Sector Technolo↗

New Approach to Characterize CO2 and CH4 Emissions over Sacramento, California Using an Airborne Aircraft Measurement

Emission fluxes of carbon dioxide (CO2) and methane (CH4) over Sacramento, California, USA, are estimated using an aircraft equipped with a cavity ring-down greenhouse gas sensor through the Alpha Jet Atmospheric eXperiment (AJAX). To better quantify the emission fluxes over the entire city and two small point sources within the area, we designed flights in a cylindrical pattern and computed the emission fluxes from 9 flights over all seasons using the Kriging method based on Gausss divergence theorem. The concentrations at the downwind side of Sacramento show somewhat persistent patterns among the 9 flights, but the magnitudes and locations of the fluxes vary depending on the individual weather conditions and seasonality on a given flight day. The net emission fluxes tend to be smaller in summer (July) than winter (November). Both trace gas mixing ratios as well as the wind speed and direction show high spatial variability both horizontally and vertically. The local maximum emission fluxes over a landfill and a rice field measured on July 29, 2015, were 2-3 times lower than the maximum measured over the entire city. These low emission fluxes suggest that not only the local source but also the transport of greenhouse gases due to diurnal and seasonal variation in winds have a strong effect on the CO2 and CH4 flux estimation of the both local emissions and city-size emissions. Our results highlight that the aircraft-based approach is effective and useful for capturing city-size emission fluxes and estimating the greenhouse gas emissions and its sources.

airborne↗

On the Discovery of CO Nighttime Emissions on Titan by Cassini/VIMS: Derived Stratospheric Abundances and Geological Implications

We present a quantitative analysis of CO thermal emissions discovered on the nightside of Titan by Baines et al. [2005. The atmospheres of Saturn and Titan in the near-infrared: First results of Cassini/VIMS. Earth, Moon, and Planets, 96, 119-147] in Cassini/VIMS spectral imagery. We identify these emission features as the P and R branches of the 1-0 vibrational band of carbon monoxide (CO) near 4.65 microns. For CH3D, the prominent Q branch of the nu(2) fundamental band of CH3D near 4.55 microns is apparent. CO2 emissions from the strong nu(3) vibrational band are virtually absent, indicating a CO2 abundance several orders of magnitude less than CO, in agreement with previous investigations. Analysis of CO emission spectra obtained over a variety of altitudes on Titan's nightside limb indicates that the stratospheric abundance of CO is 32 +/- 15 ppm, and together with other recent determinations, suggests a vertical distribution of CO nearly constant at this value from the surface throughout the troposphere to at least the stratopause near 300 km altitude. The corresponding total atmospheric content of CO in Titan is similar to 2.9 +/- 1.5 x 10(exp 14) kg. Given the long lifetime of CO in the oxygen-poor Titan atmosphere (similar to 0.5-1.0 Gyr), we find a mean CO atmospheric production rate of 6 +/- 3 x 10(exp 5) kg yr(exp -1). Given the lack of primordial heavy noble gases observed by Huygens [Niemann et al., 2005. The abundances of constituents of Titan's atmosphere from the GCMS on the Huygens probe. Nature, 438, 779-784], the primary source of atmospheric CO is likely surface emissions. The implied CO/CH4 mixing ratio of near-surface material is 1.8 +/- 0.9 x 10(exp -4), based on an average methane surface emission rate over the past 0.5 Gyr of 1.3 x 10(exp -13) gm cm(exp -2) s(exp -1) as required to balance hydrocarbon haze production via methane photolysis [Wilson and Atreya, 2004. Current state of modeling the photochemistry of Titan's mutually dependent atmosphere and ionosphere. J. Geophys. Res. 109, E06002 Doi: 10.1029/2003JE002181]. This low CO/CH4 ratio is much lower than expected for the sub-nebular formation region of Titan and supports the hypothesis [e.g., Atreya et al., 2005. Methane on Titan: photochemical-meteorological-hydrogeochemical cycle. Bull. Am. Astron. Soc. 37, 735] that the conversion of primordial CO and other carbon-bearing materials into CH4-enriched clathrate-hydrates occurs within the deep interior of Titan via the release of hydrogen through the serpentinization process followed by Fischer-Tropsch catalysis. The time-averaged predicted emission rate of methane-rich surface materials is approximately 0.02 km(exp 3) yr (exp -1), a value significantly lower than the rate of silicate lava production for the Earth and Venus, but nonetheless indicative of significant geological processes reshaping the surface of Titan.

carbon compounds↗

Effects of spatial variability in vegetation phenology, climate, landcover, biodiversity, topography, and soil property on soil respiration across a coastal ecosystem

Coastal terrestrial-aquatic interfaces (TAIs) are crucial contributors to global biogeochemical cycles and carbon exchange. A systematic evaluation of the interaction between coastal catchment properties and carbon dioxide (CO2) emission by soil respiration is significant for assessing carbon dynamics and predicting the future trajectory of atmospheric CO2 concentrations in coastal TAIs. The soil CO2 efflux in these transition zones is however poorly understood due to the high spatiotemporal dynamics of TAIs, as various sub-ecosystems in this region are compressed and expanded by complex influences of tides, changes in river levels, climate, and land use. We focus on the Chesapeake Bay region to (i) investigate the spatial heterogeneity of the coastal ecosystem and identify spatial zones with similar environmental characteristics based on the spatial data layers, including vegetation index (kNDVI), climate, landcover, diversity, topography, soil property, and relative tidal elevation; (ii) understand the primary driving factors affecting soil respiration within sub-ecosystems of the coastal ecosystem. Specifically, we employed hierarchical clustering analysis to identify spatial regions with distinct environmental characteristics, followed by the determination of main driving factors using Random Forest regression and SHapley Additive exPlanations. Maximum and minimum temperature are the main drivers common to all sub-ecosystems, while each region also has additional unique major drivers that differentiate them from one another. Precipitation exerts an influence on vegetated lands, while soil pH value holds importance specifically in forested lands. In croplands characterized by high clay content and low sand content, the significant role is attributed to bulk density. Wetlands demonstrate the importance of both elevation and sand content, with clay content being more relevant in non-inundated wetlands than in inundated wetlands. The topographic wetness index significantly contributes to the mixed vegetation areas, including shrub, grass, pasture, and forest. Additionally, our research reveals that dense vegetation land covers and urban/developed areas exhibit distinct soil property drivers. Overall, there is no one-size-fits-all approach to modeling carbon fluxes in coastal TAIs, and our study highlights the importance of further research and monitoring practices to improve our understanding of carbon dynamics and promote the sustainable management of coastal TAIs.

54 ENVIRONMENTAL SCIENCES↗

A Broad Bank Lidar for Precise Atmospheric CO2 Column Absorption Measurement from Space

Accurate global measurement of carbon dioxide column with the aim of discovering and quantifying unknown sources and sinks has been a high priority for the last decade. In order to uncover the "missing sink" that is responsible for the large discrepancies in the budget the critical precision for a measurement from space needs to be on the order of 1 ppm. To better understand the CO2 budget and to evaluate its impact on global warming the National Research Council (NRC) in its recent decadal survey report (NACP) to NASA recommended a laser based total CO2 mapping mission in the near future. That's the goal of Active Sensing of CO2 Emissions over Nights, Days, and Seasons (ASCENDS) mission - to significantly enhance the understanding of the role of CO2 in the global carbon cycle. Our current goal is to develop an ultra precise, inexpensive new lidar system for column measurements of CO2 changes in the lower atmosphere that uses a Fabry-Perot interferometer based system as the detector portion of the instrument and replaces the narrow band laser commonly used in lidars with a high power broadband source. This approach reduces the number of individual lasers used in the system and considerably reduces the risk of failure. It also tremendously reduces the requirement for wavelength stability in the source putting this responsibility instead on the Fabry- Perot subsystem.

Georgieva, E. M.↗

Advanced Intensity-Modulation Continuous-Wave Lidar Techniques for ASCENDS O2 Column Measurements

Global atmospheric carbon dioxide (CO2) measurements for the NASA Active Sensing of CO2 Emissions over Nights, Days, and Seasons (ASCENDS) space mission are critical for improving our understanding of global CO2 sources and sinks. Advanced Intensity- Modulated Continuous-Wave (IM-CW) lidar techniques are investigated as a means of facilitating CO2 measurements from space to meet the ASCENDS measurement requirements. In recent numerical, laboratory and flight experiments we have successfully used the Binary Phase Shift Keying (BPSK) modulation technique to uniquely discriminate surface lidar returns from intermediate aerosol and cloud contamination. We demonstrate the utility of BPSK to eliminate sidelobes in the range profile as a means of making Integrated Path Differential Absorption (IPDA) column CO2 measurements in the presence of optically thin clouds, thereby eliminating the need to correct for sidelobe bias errors caused by the clouds. Furthermore, high accuracy and precision ranging to the surface as well as to the top of intermediate cloud layers, which is a requirement for the inversion of column CO2 number density measurements to column CO2 mixing ratios, has been demonstrated using new hyperfine interpolation techniques that takes advantage of the periodicity of the modulation waveforms. This approach works well for both BPSK and linear swept-frequency modulation techniques. The BPSK technique under investigation has excellent auto-correlation properties while possessing a finite bandwidth. A comparison of BPSK and linear swept-frequency is also discussed in this paper. These results are extended to include Richardson-Lucy deconvolution techniques to extend the resolution of the lidar beyond that implied by limit of the bandwidth of the modulation, where it is shown useful for making tree canopy measurements.

Campbell, Joel F.↗

Development of Thermostable Carbonic Anhydrases Using Structure-Guided Recombination for Use in CO2 Removal Systems on Spacecraft

Carbon capture and storage has been a research area of great interest in recent years as a method for mitigation of CO2 emissions, due to the effects of climate change. The development of technologies for the efficient capture of CO2 are also of great interest for human spaceflight applications. One of the most promising technologies in this area is CO2 scrubbing using liquid amines, unfortunately, liquid amines with low heats of desorption tend to have slow CO2 binding kinetics. One potential solution to this problem is to use the enzyme carbonic anhydrase (CA) to enhance the kinetics of CO2 binding to liquid amines, allowing the overall process to be more energy efficient. Interest in using carbonic anhydrase as a biocatalyst has led to a number of efforts to improve the thermostability and solvent tolerance of several distinct carbonic anhydrase enzymes. In the work described here, we screened through a diverse set of natural carbonic anhydrases to identify candidates for protein engineering aimed at increased stability and activity in various liquid amines. We then used SCHEMA structure-guided recombination to develop a set of chimeric carbonic anhydrases with high thermostability and activity. These chimeras were used as the starting points for further protein engineering work targeting activity in liquid amine systems. Our ultimate goal is to test the engineered enzymes in a liquid amine system for cabin air revitalization on ISS or other spacecraft.

Life Support, Carbon dioxide, Carbonic anhydrase, ↗

Multi-century dynamics of the climate and carbon cycle under both high and net negative emissions scenarios

Abstract. Future climate projections from Earth system models (ESMs) typically focus on the timescale of this century. We use a set of five ESMs and one Earth system model of intermediate complexity (EMIC) to explore the dynamics of the Earth's climate and carbon cycles under contrasting emissions trajectories beyond this century to the year 2300. The trajectories include a very-high-emissions, unmitigated fossil-fuel-driven scenario, as well as a mitigation scenario that diverges from the first scenario after 2040 and features an “overshoot”, followed by a decrease in atmospheric CO2 concentrations by means of large net negative CO2 emissions. In both scenarios and for all models considered here, the terrestrial system switches from being a net sink to either a neutral state or a net source of carbon, though for different reasons and centered in different geographic regions, depending on both the model and the scenario. The ocean carbon system remains a sink, albeit weakened by carbon cycle feedbacks, in all models under the high-emissions scenario and switches from sink to source in the overshoot scenario. The global mean temperature anomaly is generally proportional to cumulative carbon emissions, with a deviation from proportionality in the overshoot scenario that is governed by the zero emissions commitment. Additionally, 23rd century warming continues after the cessation of carbon emissions in several models in the high-emissions scenario and in one model in the overshoot scenario. While ocean carbon cycle responses qualitatively agree in both globally integrated and zonal mean dynamics in both scenarios, the land models qualitatively disagree in zonal mean dynamics, in the relative roles of vegetation and soil in driving C fluxes, in the response of the sink to CO2, and in the timing of the sink–source transition, particularly in the high-emissions scenario. The lack of agreement among land models on the mechanisms and geographic patterns of carbon cycle feedbacks, alongside the potential for lagged physical climate dynamics to cause warming long after CO2 concentrations have stabilized, points to the possibility of surprises in the climate system beyond the 21st century time horizon, even under relatively mitigated global warming scenarios, which should be taken into consideration when setting global climate policy.

54 ENVIRONMENTAL SCIENCES↗

Broadband Lidar Technique for Precision CO2 Measurement

Presented are preliminary experimental results, sensitivity measurements and discuss our new CO2 lidar system under development. The system is employing an erbium-doped fiber amplifier (EDFA), superluminescent light emitting diode (SLED) as a source and our previously developed Fabry-Perot interferometer subsystem as a detector part. Global measurement of carbon dioxide column with the aim of discovering and quantifying unknown sources and sinks has been a high priority for the last decade. The goal of Active Sensing of CO2 Emissions over Nights, Days, and Seasons (ASCENDS) mission is to significantly enhance the understanding of the role of CO2 in the global carbon cycle. The National Academy of Sciences recommended in its decadal survey that NASA put in orbit a CO2 lidar to satisfy this long standing need. Existing passive sensors suffer from two shortcomings. Their measurement precision can be compromised by the path length uncertainties arising from scattering within the atmosphere. Also passive sensors using sunlight cannot observe the column at night. Both of these difficulties can be ameliorated by lidar techniques. Lidar systems present their own set of problems however. Temperature changes in the atmosphere alter the cross section for individual CO2 absorption features while the different atmospheric pressures encountered passing through the atmosphere broaden the absorption lines. Currently proposed lidars require multiple lasers operating at multiple wavelengths simultaneously in order to untangle these effects. The current goal is to develop an ultra precise, inexpensive new lidar system for precise column measurements of CO2 changes in the lower atmosphere that uses a Fabry-Perot interferometer based system as the detector portion of the instrument and replaces the narrow band laser commonly used in lidars with the newly available high power SLED as the source. This approach reduces the number of individual lasers used in the system from three or more to one - considerably reducing the risk of failure. It also tremendously reduces the requirement for wavelength stability in the source putting this responsibility instead on the Fabry-Perot subsystem.

Heaps, William S.↗