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  1. Estimating Total Methane Emissions from the Denver-Julesburg Basin Using Bottom-Up Approaches

    Riddick, Stuart N. ; Mbua, Mercy ; Anand, Abhinav ; ... - Gases
    Methane is a powerful greenhouse gas with a 25 times higher 100-year warming potential than carbon dioxide and is a target for mitigation to achieve climate goals. To control and curb methane emissions, estimates are required from the sources and sectors which are typically generated using bottom-up methods. However, recent studies have shown that national and international bottom-up approaches can significantly underestimate emissions. In this study, we present three bottom-up approaches used to estimate methane emissions from all emission sectors in the Denver-Julesburg basin, CO, USA. Our data show emissions generated from all three methods are lower than historic measurements.more » A Tier 1/2 approach using IPCC emission factors estimated 2022 methane emissions of 358 Gg (0.8% of produced methane lost by the energy sector), while a Tier 3 EPA-based approach estimated emissions of 269 Gg (0.2%). Using emission factors informed by contemporary and region-specific measurement studies, emissions of 212 Gg (0.2%) were calculated. The largest difference in emissions estimates were a result of using the Mechanistic Air Emissions Simulator (MAES) for the production and transport of oil and gas in the DJ basin. The MAES accounts for changes to regulatory practice in the DJ basin, which include comprehensive requirements for compressors, pneumatics, equipment leaks, and fugitive emissions, which were implemented to reduce emissions starting in 2014. The measurement revealed that normalized gas loss is predicted to have been reduced by a factor of 20 when compared to 10-year-old normalization loss measurements and a factor of 10 less than a nearby oil and production area (Delaware basin, TX); however, we suggest that more measurements should be made to ensure that the long-tail emission distribution has been captured by the modeling. This study suggests that regulations implemented by the Colorado Department of Public Health and Environment could have reduced emissions by a factor of 20, but contemporary regional measurements should be made to ensure these bottom-up calculations are realistic.« less

  2. Chemical Recycling of Polybutadiene Rubber with Tailored Depolymerization Enabled by Microencapsulated Metathesis Catalysts

    Warner, Matthew J. ; Lassa, James P. ; Narcross, Hannah ; ... - ACS Sustainable Chemistry & Engineering
    The effective management of plastic waste streams to prevent plastic land and water pollution is a growing problem that is also one of the most important challenges in polymer science today. Polymer materials that are stable over their lifetime and can also be cheaply recycled or repurposed as desired could more easily be diverted from waste streams. However, this is difficult for most commodity plastics. It is especially difficult to conceive this with intractable, cross-linked polymers such as rubbers. In this work, we explore the utility of microencapsulated Grubbs’ catalysts for the in-situ depolymerization and reprocessing of polybutadiene (PB) rubber.more » Second-generation Hoveyda-Grubbs catalyst (HG2) contained within glassy thermoplastic microspheres can be dispersed in PB rubber below the microsphere’s glass transition temperature (Tg) without adverse depolymerization, evidenced by rubber with and without these microspheres obtaining similar shear storage moduli of ≈16 and ≈28 kPa, respectively. The thermoplastic’s Tg can be used to tune the depolymerization temperature, via release of HG2 into the rubber matrix. For example, using poly(lactic acid) (PLA) vs polysulfone results in an 85 and 162 °C depolymerization temperature, respectively. Liquefaction of rubber to a mixture of small molecules and oligomers is demonstrated using a 0.01 mol % catalyst loading using PLA as the encapsulant. Furthermore, at that same catalyst loading, depolymerization occurs to a greater extent in comparison to two ex-situ approaches, including a conventional solvent-assisted method, where it occurs at roughly twice the extent at each given catalyst loading. In addition, depolymerization of the microsphere-loaded rubbers was demonstrated for samples stored under nitrogen for 23 days. Lastly, we show that the depolymerized products can be reprocessed back into solid rubber with a shear storage modulus of ≈32 kPa. Thus, we envision that this approach could be used to recycle and reuse cross-linked rubbers at the end of their product lifetime.« less

  3. Concept for an irradiation experiment to test a laser-induced breakdown spectroscopy off-gas sensor for molten salt systems

    Andrews, Hunter B. ; Myhre, Kristian G. ; McFarlane, Joanna - Frontiers in Energy Research
    This paper focuses on laser-induced breakdown spectroscopy (LIBS) as an off-gas sensor and details a conceptual irradiation experiment to evaluate its performance in an environment that is more realistic of an operational molten salt reactor (MSR). MSRs are a promising advanced nuclear design that use high-temperature liquid salts as the coolant, fuel, or a combination of both. They will generate and subsequently evolve fission products into the reactor headspace during operation. These evolved fission products will necessitate an online off-gas system to treat the reactor cover gas before recycling it to the core. Such a system, especially during the earlymore » deployment phase, will benefit from online sensors to inform operators of the treatment system’s performance. Optical spectroscopy is well-suited to fit this task as it can be remotely deployed using fiber-optics and can detect most species at high frequencies. LIBS can detect nearly every element on the Periodic Table, stable or radioactive, making it an ideal candidate. The provided conceptual experiment discusses the facility requirements, salt capsule design, and detailed testing campaigns with corresponding simulated LIBS spectra.« less

  4. The effects of phosphorus pentoxide additions on the thermal, rheological, and structural properties of sodium borosilicate glass

    Skerratt-Love, K. L. ; George, J. L. ; Bell, A. M. T. ; ... - Journal of Non-Crystalline Solids

  5. Emergent Chemical Behavior in Mixed Food and Lignocellulosic Green Waste Hydrothermal Liquefaction

    LeClerc, Heather O. ; Page, Jeffrey R. ; Tompsett, Geoffrey A. ; ... - ACS Sustainable Chemistry & Engineering
    Hydrothermal liquefaction (HTL) is a promising strategy for the conversion of energy-dense waste streams to fuels. Mixed-feed HTL aggregates multiple feed streams to achieve greater scales that capitalize on local resources, hence lowering costs. The potential for new pathways and products upon feedstock blending becomes a compounding level of complexity when unlocking emergent chemistries. Here, food and green waste streams were evaluated under HTL conditions (300 °C, 1 h) to understand the effect of feed molecular composition on product distributions and mechanisms. Thousands of emergent chemical compounds were detected via Fourier transform ion cyclotron resonance mass spectrometry, ultimately leading tomore » the emergence of two dominant outcomes. First, the presence of small amounts of food waste into green waste results in substantial decarboxylation and subsequent polymerization to biocrude than chars. Second, in the other limit, small amounts of green waste promote the capping of oxygenates into the biodiesel range, such as with the emergence of fatty acid methyl esters.« less

  6. Expanding plastics recycling technologies: chemical aspects, technology status and challenges

    Li, Houqian ; Aguirre-Villegas, Horacio A. ; Allen, Robert D. ; ... - Green Chemistry
    This paper reviewed the entire life cycle of plastics and options for the management of plastic waste to address barriers to industrial chemical recycling and further provide perceptions on possible opportunities with such materials.

  7. Life Cycle Analysis of Renewable Natural Gas and Lactic Acid Production from Waste Feedstocks

    Lee, Uisung ; Bhatt, Arpit ; Hawkins, Troy Robert ; ... - Journal of Cleaner Production
    Producing fuels and chemicals from waste is considered economically favorable, due to low feedstock cost, and environmentally favorable, due to avoided emissions from conventional waste management practices. In this study, we evaluate the life cycle greenhouse gas (GHG) emission reduction benefits of renewable natural gas (RNG) and lactic acid (LA) production from four types of wet waste feedstocks (wastewater sludge, food waste, swine manure, and fats, oil, and grease [FOG]) via anaerobic digestion (AD) and LA fermentation, respectively. RNG can be used as an alternative to fossil natural gas, while LA from waste feedstocks can displace conventional LA production pathwaysmore » (mainly from corn via fermentation). Providing comprehensive life cycle GHG emissions of the combinations of waste feedstocks and products through different routes helps identify the GHG hotspots and show where emissions savings come from. The results show that the carbon intensities (CIs) of waste-derived RNG and LA are much lower than those of their counterparts. We estimated the life cycle GHG emissions for RNG to be between -146 and 27 g carbon dioxide equivalent (CO2e)/MJ, much lower than the CI of fossil fuels. Waste-derived LA pathways also show substantially lower CIs, ranging from -4.2 to -1.4 kgCO2e/kg LA, compared to the CIs of LA from corn and corn stover (1.2 and 0.3 kgCO2e/kg LA, respectively). We will also discuss that the low CIs of waste-derived products can come from low yields leading to high emission credits. Thus, life cycle analysis results presented per weight of treated waste can be used to support decisions about which waste feedstocks and products are to be used for sustainable waste valorization. In addition, we found that monetary emission reduction credits can play an important role in driving waste valorization.« less

  8. Variation of lead isotopic composition and atomic weight in terrestrial materials (IUPAC Technical Report)

    Zhu, Xiang-Kun ; Benefield, Jacqueline ; Coplen, Tyler B. ; ... - Pure and Applied Chemistry (Online)
    The isotopic composition and atomic weight of lead are variable in terrestrial materials because its three heaviest stable isotopes are stable end-products of the radioactive decay of uranium (238U to 206Pb; 235U to 207Pb) and thorium (232Th to 208Pb). The lightest stable isotope, 204Pb, is primordial. These variations in isotope ratios and atomic weights provide useful information in many areas of science, including geochronology, archaeology, environmental studies, and forensic science. While elemental lead can serve as an abundant and homogeneous isotopic reference, deviations from the isotope ratios in other lead occurrences limit the accuracy with which a standard atomic weightmore » can be given for lead. In a comprehensive review of several hundred publications and analyses of more than 8000 samples, published isotope data indicate that the lowest reported lead atomic weight of a normal terrestrial materials is 206.1462 ± 0.0028 (k = 2), determined for a growth of the phosphate mineral monazite around a garnet relic from an Archean high-grade metamorphic terrain in north-western Scotland, which contains mostly 206Pb and almost no 204Pb. The highest published lead atomic weight is 207.9351 ± 0.0005 (k = 2) for monazite from a micro-inclusion in a garnet relic, also from a high-grade metamorphic terrain in north-western Scotland, which contains almost pure radiogenic 208Pb. When expressed as an interval, the lead atomic weight is [206.14, 207.94]. It is proposed that a value of 207.2 be adopted for the single lead atomic-weight value for education, commerce, and industry, corresponding to previously published conventional atomic-weight values.« less

  9. Assessment of municipal solid waste for valorization into biofuels

    Thompson, Vicki S. ; Ray, Allison E. ; Hoover, Amber ; ... - Environmental Progress and Sustainable Energy
    Abstract Almost 36 million tons of paper and yard trimmings are not currently being recycled or composted annually and likely end up in landfills. One approach to valorize these resources would be for biofuels production. Nonrecyclable municipal solid waste (MSW) paper and yard trimmings were assessed for their suitability as feedstocks to produce biofuels from sugars. Both materials met the cost target of less than $85.51/ton ($2016) with MSW paper ranging from $36.40 to $62.18/dry ton and grass clippings from $25.64 to $45.86/dry ton. MSW paper exceeded the carbohydrate requirement of 59% while grass clippings had significantly lower amounts of carbohydratesmore » (30%). However, both types of MSW had ash contents significantly above the required 5% total ash with paper at 22% ash and grass clippings at 16%. While neither waste material was individually found to be suitable for biofuels production based on compositional requirements, it was determined that blending either waste with corn stover would produce materials that met carbohydrate, ash, and cost targets. The higher carbohydrate and lower ash stover compensated for the lower carbohydrates and high ash of the waste materials, while the lower cost waste materials offset the higher cost of corn stover.« less

  10. Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses

    Bingham, Paul A. ; Vaishnav, Shuchi ; Forder, Sue D. ; ... - Journal of Alloys and Compounds
    In this paper, the capacity of simulated high-level radioactive waste borosilicate glasses to incorporate sulfate has been studied as a function of glass composition. Combined Raman, 57Fe Mössbauer and literature evidence supports the attribution of coordination numbers and oxidation states of constituent cations for the purposes of modelling, and results confirm the validity of correlating sulfate incorporation in multicomponent borosilicate radioactive waste glasses with different models. A strong compositional dependency is observed and this can be described by an inverse linear relationship between incorporated sulfate (mol% SO42-) and total cation field strength index of the glass, Σ(z/a2), with a highmore » goodness-of-fit (R2 ≈ 0.950). Similar relationships are also obtained if theoretical optical basicity, Λth (R2 ≈ 0.930) or non-bridging oxygen per tetrahedron ratio, NBO/T (R2 ≈ 0.919), are used. Finally, results support the application of these models, and in particular Σ(z/a2), as predictive tools to aid the development of new glass compositions with enhanced sulfate capacities.« less
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