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DOE OSTI2023

LipidOz enables automated elucidation of lipid carbon–carbon double bond positions from ozone-induced dissociation mass spectrometry data

Lipids play essential roles in many biological processes and disease pathology, but unambiguous identification of lipids is complicated by the presence of multiple isomeric species differing by fatty acyl chain length, stereospecifically numbered (sn) position, and position/stereochemistry of double bonds. Conventional liquid chromatography-mass spectrometry (LC-MS/MS) analyses enable the determination of fatty acyl chain lengths (and in some cases sn position) and number of double bonds, but not carbon-carbon double bond positions. Ozone-induced dissociation (OzID) is a gas-phase oxidation reaction that produces characteristic fragments from lipids containing double bonds. OzID can be incorporated into ion mobility spectrometry (IMS)-MS instruments for the structural characterization of lipids, including additional isomer separation and confident assignment of double bond positions. The complexity and repetitive nature of OzID data analysis and lack of software tool support have limited the application of OzID for routine lipidomics studies. Here, we present an open-source Python tool, LipidOz, for the automated determination of lipid double bond positions from OzID-IMS-MS data, which employs a combination of traditional automation and deep learning approaches. Our results demonstrate the ability of LipidOz to robustly assign double bond positions for lipid standard mixtures and complex lipid extracts, enabling practical application of OzID for future lipidomics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Mixing-Controlled CI Combustion and Fuel-Effects Research

This project is focused on developing advanced combustion strategies for mixing-controlled compressionignition (i.e., diesel-cycle) engines that are synergistic with renewable and/or unconventional fuels in a manner that enhances domestic energy security, economic competitiveness, and environmental quality. During this reporting period, the focus was on ducted fuel injection (DFI), a technology that differs from conventional diesel combustion (CDC) in that it involves injecting fuel along the axis of one or more small cylindrical ducts within the combustion chamber. Each duct performs a function similar to the tube on a Bunsen burner, helping to premix the fuel with the charge-gas before ignition, creating a stable flame that forms little to no soot. The purpose of the work conducted during Fiscal Year (FY) 2019 was to begin determining the extent to which the use of oxygenated fuels, when combined with DFI and charge-gas dilution, can simultaneously lower the soot and nitrogen-oxides (N0 x ) emissions from mixing-controlled compression-ignition engines, and what the corresponding impacts on other regulated emissions and efficiency are likely to be.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2026

Metallic Phase-Free Zn-Al Mixed Oxide Dual Function Materials Enable High Co Selectivity in Reactive Carbon Capture From Dilute Streams

Scaling conventional carbon capture and utilization methods can be limited by cost and permitting issues associated with transportation of captured CO2. Reactive carbon capture (RCC), in which a single solid-phase dual function material (DFM) is used to both capture CO2 from dilute streams (e.g., flue gas) and catalytically convert the bound species to products in a single unit operation, has the potential to reduce energy and capital costs by over 50% relative to separate capture and conversion. To incentivize adoption, high-value products such as methanol and CO should be targeted. Appealingly, CO can be produced at atmospheric pressure, thereby lowering overall H2 demand; however, high reaction temperatures (> 600 degrees C) and the use of oxidizable transition metals, such as Ni, are often necessary to drive the reverse water-gas shift (RWGS) during reactive desorption of the bound CO2. The sensitivity of these transition metals to oxygen undercuts their utility in point source RCC. To further derisk RCC, it is essential to develop metallic-phase free DFMs that are insensitive to residual oxygen in flue gas and can achieve selective reactive desorption to CO at moderate pressures (< 400 degrees C). To this end, we have developed K-modified Zn-Al mixed oxides (K/ZnAlOx) to convert captured CO2 to CO with > 97% selectivity and yields up to 53% of captured CO2 at 400 degrees C. Complementary in situ spectroscopy studies revealed the role of K-modification in improving RCC performance of unmodified ZnAlOx. The top performing DFM was also subjected to extended RCC cycling with oxygen co-fed with CO2 during the capture test to assess durability under simulated flue gas.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Development and Testing of an Advanced Cascaded Thermoelectric Residential Heat Pump

Electricity-driven heat pumps using vapor compression cycle are an energy-efficient solution to replace fossil fuel burning and reduce greenhouse gas emissions for space heating in residential buildings. However, heating capacity and Coefficient of Performance (COP) of heat pumps degrade significantly with increasing temperature difference between ambient and indoor environments. Residents and building owners are hence reluctant to fully embrace electric heat pumps. The use of conventional all-electric heat pumps also causes concern for electric utilities due to an increased winter peak demand arising from the use of supplemental electric resistance heaters. Our research is an attempt to alleviate these concerns by designing and laboratory testing a thermoelectric (TE) heat pump cascaded with a vapor compression cycle to enhance heating capacity and COP. TE modules increase the subcooling in the refrigerant liquid of the vapor compression cycle to enlarge the evaporating capacity and works at an efficiency greater than a conventional electric resistance strip. This results in a simple, affordable, efficient and highly controllable solution to adequately meet space heating needs in dwellings. The laboratory testing of the 3-stage cascaded TE heat pump performed in this research has exhibited a higher heating capacity by above 15%, while maintaining a heating COP of 2.0-3.6 in the ambient temperature range of -18˚C to 8˚C (0˚F to 47 ˚F), which represents more than 60% of winter temperatures observed in US. If successfully commercialized, this technology can advance space-heating electrification by overcoming consumer cost barrier of heat pumps.

Shen, Bo↗

DOE OSTI2022

CFD-DEM Modeling of Autothermal Pyrolysis of Corn Stover with a Coupled Particle- and Reactor-Scale Framework

Autothermal operation of fast pyrolysis is an efficient process-intensification technique wherein exothermic oxidation reactions are used to overcome the heat-transfer bottleneck of conventional pyrolysis. The development of accurate, reliable modeling toolsets is imperative to generating a deeper understanding of biomass autothermal pyrolysis systems to support scale-up and industrial deployment. This modeling effort describes the development of single-particle and reactor models which incorporate detailed reaction schemes and simultaneous exothermic oxidation reactions. The particle-scale model was parameterized for corn stover feedstock with particle morphology, density, ash content, and biopolymer composition, all of which impact the emergent conversion characteristics during pyrolysis. Results were then used to parameterize a reactor-scale autothermal pyrolysis model, which was developed using a coarse-grained computational fluid dynamic-discrete element method. The simulation results compared well with experimental results, with the predicted bio-oil, light gas, and biochar yield within 3.0 wt% of the experimental yields. Further analyses were performed to test the influence of equivalence ratio, biomass injection position, and particle size distribution on autothermal pyrolysis. The analysis of the physio-chemical properties of the fluid and solid phase inside the reactor and at the reactor outlet help reveal important process interactions of autothermal pyrolysis.

BIOMASS FUELS,INORGANIC, ORGANIC, PHYSICAL, AND AN↗

DOE OSTI2021

Ce stabilized Ni–SrO as a catalytic phase transition sorbent for integrated CO 2 capture and CH 4 reforming

Integration of carbon dioxide capture from flue gas with dry reforming of CH 4 represents an attractive approach for CO 2 utilization. The selection of a suitable bifunctional material serving as a catalyst/sorbent is the key. This paper reports Ni decorated and CeO x -stabilized SrO (SrCe 0.5 Ni 0.5 ) as a multi-functional, phase transition catalytic sorbent material. The effect of CeO x on the morphology, structure, decarbonation reactivity, and cycling stability of the catalytic sorbent was determined with TEM-EDX, XRD, in situ XRD, CH 4 -TPR and TGA. Here, cyclic process tests were conducted in a packed bed reactor. The results indicate that large Ni clusters were present on the surface of the SrNi sorbent, and the addition of CeO 2 promoted even distribution of Ni on the surface. Moreover, the Ce–Sr interaction promoted a complex carbonation/decarbonation phase-transition, i.e. SrCO 3 + CeO 2 ↔ Sr 2 CeO 4 + CO 2 as opposed to the conventional, simple carbonation/decarbonation cycles (e.g. SrCO 3 ↔ SrO + CO 2 ). This double replacement crystalline phase transition mechanism not only adjusts the carbonation/calcination thermodynamics to facilitate SrCO 3 decomposition at relatively low temperatures but also inhibits sorbent sintering. As a result, excellent activity and stability were observed with up to 91% CH 4 conversion, >72% CO 2 capture efficiency and ~100% residual O 2 capture efficiency from flue gas by utilizing the CeO 2 ↔ Ce 2 O 3 redox transition. This renders an intensified process with zero coke deposition. Moreover, the SLDRM with SrCe 0.5 Ni 0.5 has the flexibility to produce concentrated CO via CO 2 -splitting while co-producing a syngas with tunable H 2 /CO ratios.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Multi-scale model based design of membrane reactor/separator processes for intensified hydrogen production through the water gas shift reaction

This paper aims to first quantify the impact of various diffusion models (Maxwell-Stefan, Wilke, Dusty-Gas) on the predictions of a multi-scale membrane reactor/separator mathematical model, and to then demonstrate this model's use for the design and process intensification of membrane reactor/separator systems for hydrogen production. This multi-scale model captures velocity, temperature and species' concentration profiles along the catalyst pellet's radial direction, and along the reactor's axial direction, by solving the momentum, energy, and species transport equations, accounting for convection, conduction, reaction, and diffusion mechanisms. In the first part of work, the effect of pellet-scale design parameters (mean pore diameter, volumetric porosity, tortuosity factor, etc.) and various species' flux models on the model predictions is studied. In the second part, the study focuses on the comparison, in terms of their process intensification characteristics, of various hydrogen production processes. These include a conventional high-temperature shift reactor (HTSR)/low-temperature shift reactor (LTSR) sequence, a novel HTSR/membrane separator (MS)/LTSR/MS sequence, and a process that involves low-temperature shift membrane reactors-LTSMR in a series.

08 HYDROGEN↗

DOE OSTI2022

Hydrogen Crossover Flux through Two-Dimensional Nanomaterials

Energy storage and conversion devices require an ion-exchange membrane with high transmission of charge-balancing ions and separation of anode and cathode electrolytes/gases. This ensures optimum device performance. Most conventional membranes suffer huge cross-permeation resulting in low energy efficiency and material degradation. This work investigated hydrogen permeability and proton transmission through membrane electrode assemblies (MEAs) containing a monolayer of hexagonal boron nitride and single-layer and bi-layer graphene in a gas-phase small-scale cell and a liquid cell. Here we found that the hydrogen crossover flux through MEAs with 2D materials was inhibited by at least a factor of 5 compared to the one without. Single-layer graphene and boron nitride enabled high proton transmission, but bi-layer graphene inhibited proton conduction. Defect visualization of 2D materials revealed few atomic-scale defects in graphene. These findings suggest that a monolayer of 2D material may provide good selectivity for energy conversion and storage devices by blocking species crossover while allowing high proton transmission.

2D materials↗

DOE OSTI2025

Stacked-mosaic amplifier and diode delivery concept for kJ-class inertial fusion energy laser driver

We report on a laser amplifier architecture designed as a modular element for scaling to multi-megajoule laser facilities intended for inertial fusion energy (IFE) power plants. This kilojoule-class module features a stacked mosaic of gain media integrated with a diode delivery system for efficient optical pumping of the mosaic-structured gain medium, enabling high-repetition-rate operation at high wall plug efficiencies, necessary for an IFE driver. Details of a diode delivery system capable of pumping the mosaic architecture are presented. Comprehensive numerical modeling demonstrates that the stacked-mosaic approach reduces transverse gain by five orders of magnitude compared to a conventional full-aperture Yb:YAG based amplifier, substantially suppressing transverse amplified spontaneous emission (TASE) and enabling enhanced longitudinal energy extraction. Detailed analysis of thermal management and wavefront distortion in a 4 × 4 mosaic array indicates that temperature gradients and thermally induced aberrations are effectively controlled using gas cooling and commercially available phase-plate and deformable mirror technologies. We further discuss the applicability of a stacked-mosaic architecture to direct-drive IFE schemes, where broad spectral bandwidth is critical, and its compatibility with frequency conversion modules for up-conversion to blue wavelengths. Finally, an example point design for a 10 kJ, 10 Hz Yb:YAG module operating at 175 K with wall-plug efficiency exceeding 10 % is presented, underscoring the feasibility of this approach for next-generation high-energy lasers for IFE drivers. The results establish the stacked-mosaic amplifier as a scalable, robust platform not only for IFE but also for a broad range of advanced scientific and industrial laser applications.

Lasers↗

DOE OSTI2022

Cradle-to-Grave Lifecycle Analysis of U.S. Light-Duty Vehicle-Fuel Pathways: A Greenhouse Gas Emissions and Economic Assessment of Current (2020) and Future (2030-2035) Technologies

This study provides a comprehensive life cycle analysis (LCA), or cradle-to-grave (C2G) analysis, of the cost and greenhouse gas (GHG) emissions of a variety of vehicle-fuel pathways, the levelized cost of driving (LCD) and cost of avoided GHG emissions. The C2G analysis assesses light duty midsize sedans and small sport utility vehicles (SUVs) across a variety of vehicle-fuel technology pathways, including conventional internal combustion engine vehicles (ICEVs), flexible hybrid electric vehicles (HEVs), plug-in hybrid electric vehicles (PHEVs), battery electric vehicles (BEVs) with varying vehicle ranges, and fuel cell electric vehicles (FCEVs). Coming at a timely manner, given the marked increase, since 2016, in climate aspirations announced by governmental institutions and private firms both in the US and across the globe, this analysis builds on a previous comprehensive life cycle analysis, updating that study’s 2016 assumptions and methods (Elgowainy et al. 2016). These updates incorporate technological advances and changes in energy supply sources that have emerged during the intervening period. Utilizing these updated assumptions and methods, alongside more recent data, the present report accounts for a broader range of vehicle technologies and considers both current (2020) and expected future (2030-2035) conditions. Reflecting increased research interest in synthetic liquid fuels produced using renewable low-carbon electricity and CO 2 sources, electro-fuels (a.k.a. e-fuels) were added to the potential future fuel technologies that are evaluated. This study takes a “pathway” approach rather than a “scenario” approach; hence distinct, technically feasible, routes or sequences of processes starting with one or more feedstocks and ending with an intermediate or a final product are examined, not necessarily constrained by practical feedstock, economic, policy, and market considerations.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2023

Cradle-to-Grave Lifecycle Analysis of U.S. Light-Duty Vehicle-Fuel Pathways: A Greenhouse Gas Emissions and Economic Assessment of Current (2020) and Future (2030-2035) Technologies

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2022

A Large Eddy Simulation Study of Flow Turbulence, Alumina Transport, and Bath Temperature Evolution in Conventional Aluminum-Smelting Cell Using OpenFOAM

In this study, a Large Eddy Simulation (LES) of the aluminum-smelting process is performed using OpenFOAM. To understand the coupled behavior of heat transfer, mass transfer, and flow of the smelting process, a multi-physics computational fluid dynamics (CFD) model based on the Eulerian–Eulerian multi-fluid approach is adopted. The model accounts for CO 2 bubble and magnetohydrodynamics (MHD)-driven flow, along with alumina dissolution, transport, and bath temperature evolution. The simulation predictions show small-scale turbulent vortical structures in the anode–cathode space caused by combined effect of MHD and CO 2 bubble-bath interactions and relatively large-scale asymmetric vortices in the inter-anode space caused by the CO 2 bubble-bath interactions. The vortex formation at the edges of the anodes evidently aids in transporting alumina from the central channel to the bottom of the anodes and prevents accumulation of gas bubbles in the periphery of the anode bottom. Symmetric bath cold spots are observed in the vicinity of the feeder. Cold spots are also observed in the anode–cathode distance space below the anode bottom due to the transport of undissolved solid to this region by the flow. The findings from the work are useful in developing and designing alumina-feeding strategy leading to reduced anode effects and smooth operation of the cell. The work also highlights the important flow structures in conventional aluminum-smelting cell.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Superatomic chemistry

Superatoms are atomic clusters with tailored size and composition that mimic the chemistry of atoms in the periodic table. However, unlike the atoms whose chemistry is governed by their valence electron orbitals, the chemistry of superatoms is governed by their highest occupied molecular orbitals. In addition, due to their large size and non-spherical geometry, superatoms can promote unusual reactions and serve as the building blocks of cluster assembled materials with properties very different from conventional materials. This perspective highlights the unique role of superatoms in chemical and material sciences by focusing on superhalogens, which not only possess electron affinities larger than those of halogens but also can be stable when multiply charged. We discuss how these unique features of superhalogens enable noble gas atoms like argon to form chemical bonds at room temperature and zinc to exhibit an oxidation state of +3. Here, the advantages of using superhalogens in the synthesis of water-resistant materials for solar cells, halogen-free electrolytes for solid-state batteries, and multiferroic materials are also discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

SunLine Transit Agency Fuel Cell Electric Bus Progress Report (Data Period Focus Jan-Jun 2020) [Slides]

This report presents early results from a deployment of fuel cell electric buses (FCEBs) operated by SunLine Transit Agency in the Coachella Valley area of California. The five FCEBs, produced by New Flyer, feature an electric drive propulsion system powered by a Ballard fuel cell system. The project team is collaborating with the U.S. Department of Energy (DOE) and DOE's National Renewable Energy Laboratory (NREL) to evaluate the buses in revenue service. The goal of this evaluation is to compare the FCEB performance to that of conventional technology and to track progress over time toward meeting the technical targets set by DOE and the Department of Transportation (DOT). The FCEBs were delivered beginning in mid-2019. The data period covers January 2020 through July 2020. NREL collects data on five 2019 model year compressed natural gas (CNG) buses as a baseline comparison at SunLine. These new CNG buses were phased into service beginning in April 2020.

25 ENERGY STORAGE↗

DOE OSTI2022

SunLine Transit Agency Fuel Cell Electric Bus Progress Report - Data Period Focus: Jan. 2020 through Dec. 2021 [Slides]

This report presents early results from a deployment of fuel cell electric buses (FCEBs) operated by SunLine Transit Agency in the Coachella Valley area of California. The five FCEBs, produced by New Flyer, feature an electric drive propulsion system powered by a Ballard fuel cell system. The project team is collaborating with the U.S. Department of Energy (DOE) and DOE's National Renewable Energy Laboratory (NREL) to evaluate the buses in revenue service. The goal of this evaluation is to compare the FCEB performance to that of conventional technology and to track progress over time toward meeting the technical targets set by DOE and the Department of Transportation (DOT). The FCEBs were delivered beginning in mid-2019. The data period covers January 2020 through December 2021. NREL collects data on five 2019 model year compressed natural gas (CNG) buses as a baseline comparison at SunLine. These new CNG buses were phased into service beginning in April 2020.

08 HYDROGEN↗

DOE OSTI2024

Abstract for CRADA between National Energy Technology Laboratory and TOPTICA Photonics, Inc.

The National Energy Technology Laboratory (NETL) and Toptica Photonics (Participant) will collaborate to demonstrate the application of a frequency-comb laser (dual-comb spectroscopy) in an optically accessible rotating detonation engine (RDE). RDEs are a next-generation energy conversion technology which are well-suited to hydrogen usage and have the potential to significantly increase the efficiency of gas turbine engine power cycles. However, critical information is needed about the high temperature and pressure detonation wave, which represents an extremely challenging diagnostic environment. Dual-comb spectroscopy can be used to characterize the pressure-broadened IR absorption features at MHz rates, providing information not possible with conventional tunable diode laser (TDL) technologies. This collaboration will, for the first time, demonstrate application of dual-comb spectroscopy within the combustion annulus of a hydrogen-air RDE. If successful, the data generated will help to accelerate commercialization of RDE technologies in support of decarbonizing our nation’s energy sector.

08 HYDROGEN↗

DOE OSTI2020

An Arduino based automatic pressure evaluation system to quantify growth of non‐model anaerobes in culture

Abstract Measuring the growth rate of non‐model anaerobic microbes typically requires the use of time‐consuming and often destructive manual measurements. Here, an Arduino based automatic pressure evaluation system (A‐APES) was developed to automatically measure the rate of fermentation gas production as a proxy for microbial growth in anaerobic systems. The A‐APES system measures accumulated gas pressure in sealed cultures accurately at high‐resolution, while venting the system at programmed intervals to prevent over pressurization. The utility of A‐APES is demonstrated in this study by quantifying the growth rate and phases of a biomass‐degrading anaerobic gut fungus, which cannot be otherwise measured via conventional techniques due to its association with particulate substrates. Given the utility of the A‐APES approach, we provide a complete construction guide to fabricate the device, which is three times less expensive compared to existing commercial alternatives.

Wilken, St. Elmo↗

DOE OSTI2023

Environmental life cycle assessment of treatment and management strategies for food waste and sewage sludge

A consequential life cycle assessment (LCA) was utilized to compare the environmental impacts of food waste and sewage sludge management strategies. The strategies included a novel two-phase anaerobic digestion (AD) system and alternatives including landfill, waste-to-energy, composting, anaerobic membrane bioreactor, and conventional AD (wet continuous stirred-tank reactor [CSTR]). The co-management of food waste with sewage sludge was also considered for the two-phase AD system and for a conventional AD reactor. Further, a multidimensional LCA approach was taken, considering the five-midpoint impact categories of global warming, smog, human health particulate, acidification, and eutrophication estimated using the U.S. EPA Tool for the Reduction and Assessment of Chemical and Other Environmental Impacts. Co-management of food waste and sewage sludge using the novel two-phase AD system was shown to maximize energy recovery and had a net global warming benefit while reducing other environmental impacts compared with the alternative management strategies. It had similar relative environmental advantages across all categories as conventional AD, with the advantage of a smaller physical footprint. However, both approaches featured net environmental burdens when the background electric grid intensity fell below 0.25 kg CO 2 -eq kWh -1 , as could be expected in a decarbonized electric future. Upgrading the biogas produced from AD to renewable natural gas can displace the use of fossil natural gas for other non-electricity energy requirements that are difficult to decarbonize and may extend the time period of significant environmental benefits of utilizing AD for organic waste management. Treatment of the nutrient-rich supernatant generated by the novel two-phase AD system could be an obstacle for utilities with stringent nutrient discharge limits. Future research and full-scale implementation are needed to demonstrate the benefits of the two-phase AD system predicted through this analysis.

54 ENVIRONMENTAL SCIENCES↗