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DOE OSTI2021

Carbon dioxide and nitrogen reduction reactions using 2D transition metal dichalcogenide (TMDC) and carbide/nitride (MXene) catalysts

Improving the carbon dioxide and nitrogen reduction reactions (CO 2 RR and NRR) can reduce anthropogenic greenhouse gas emissions while selectively producing chemicals needed for the fuel, plastic, and chemical industries. Efficient CO 2 RR can be used to replace fossil fuels as well as repurpose captured CO 2 , while new NRR pathways can be used to supplement or replace the energy intensive Haber–Bosch process for NH 3 generation with no CO 2 emissions. Therefore, this review article focuses on (photo)electrocatalytic and photocatalytic conversion of CO 2 and N 2 molecules into useful products, such as carbon monoxide, methanol, formic acid, and ammonia, using 2D transition metal dichalcogenides (TMDCs) and metal carbides/nitrides (MXenes). Additionally, these highly tunable 2D catalysts will be evaluated for their ability to selectively and efficiently undergo CO 2 RR and NRR by controlling defects, phases, edge sites, interfaces, and functional groups. We first address the CO 2 RR and NRR challenges, with a particular focus on theoretical mechanisms and minimum energy pathways. We follow this discussion with a detailed review of state-of-the-art 2D TMDC and MXene experimental catalysts for CO 2 RR and NRR (photo)electrocatalytic and photocatalytic reactions, and then address areas of opportunity for these catalytic reactions.

14 SOLAR ENERGY↗

DOE OSTI2023

Low-carbon fuels for spark-ignited engines: A comparative study of compressed natural gas and liquefied petroleum gas on a CFR engine with exhaust gas recirculation

Decades of work on low-carbon fuels have established their potential for substantial emissions reductions; however, their adoption is still limited by infrastructure concerns and engine efficiency deficits. As infrastructures have begun to evolve, research on strategies that maximize engine efficiency through interactions with fuel properties must also now take center place. This paper compares the performance, emissions, and combustion characteristics of two forefront low-carbon fuels: compressed natural gas (CNG) and liquefied petroleum gas (LPG) in a cooperative fuel research (CFR) engine over a range of compression ratios and engine loads. The effects of exhaust gas recirculation (EGR), end-gas auto-ignition, and a novel combustion control tool, the combustion intensity metric (CIM), were also evaluated at different stoichiometric engine operating conditions. In comparison to LPG, CNG operation demonstrated an extended knock-free regime, allowing engine operation at higher engine loads and compression ratios, but LPG operation exhibited enhanced combustion characteristics with higher peak pressures and faster apparent heat release rates (AHRR). LPG operation achieved higher brake thermal efficiencies and lower equivalent CO 2 emissions compared to CNG operation at the tested engine loads and compression ratios. LPG demonstrated significantly higher EGR tolerance limits compared to CNG, with a maximum of 28% EGR rate, compared to 23% for CNG. This improved EGR dilution tolerance was responsible for a 90% reduction in NOx emissions for LPG compared to a maximum of 70% with CNG. EGR dilution also exhibited more effective knock mitigation potential with LPG, suppressing knock intensity values by up to 98% and transitioning the engine operation towards normal combustion from heavy knocking conditions. As a result, the CIM was found to decrease burn durations and improve the quality of combustion by controlling the desired fraction of end-gas auto-ignition.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2025

High Power Density, Carbon Neutral Electrical Power Generation for Air Vehicles

The synergistic integration of a Solid Oxide Fuel Cell-Combustor (SOFC-C) with a turbogenerator (TG) will provide a very high fuel-to-electricity conversion efficiency while maintaining high power-to-weight ratio during high-altitude flight. The proposed SOFC-C-TG power generation technology exceeds the REEACH technical performance targets (TPT). This unique concept addresses many of the challenges faced in all electric propulsion-based aviation. The system has high part-load efficiency (more than 65% lower heating value (LHV)) during long cruise times, load following capability, high-power capacity at high altitudes adapting to low temperatures and pressures, rapid startup time of less than 30 minutes (proven with current SOFC technology), high power density (more than 3.2 kW/kg), efficient thermal management, and a foundation for a compact, efficient electrical storage and power generation system (ESPG). The SOFC-C concept achieves the technology targets by reducing the complexity of traditional fuel cell-gas turbine hybrid systems (FC-GT). The SOFC-C does not require heat exchangers and dramatically reduces the balance of plant increasing power density and performance in efficiency. The reduction in mass through elimination of heat exchangers, external reformer, and other components dramatically decreases the overall thermal dampening of the system which enables rapid startup and load following capability. Direct control of the cathode inlet temperature of the SOFC-C enables rapid warm-up of the SOFC tubes with the ability to reach operating temperature and full power in less than 30 minutes.

03 NATURAL GAS↗

DOE OSTI2020

Effects of blending C3-C4 alcohols on motor gasoline properties and performance of spark ignition engines: A review

Supplementing petroleum fuels with sustainable and renewable alternatives is a good option for increasing the sustainability of transportation fuels. Alcohols are particularly attractive blendstocks for spark ignition engines, mainly due to their desirable fuel properties including high octane, evaporative cooling, and reduced sooting propensity. Although the use of SI engines is widespread around the world, predominately for light duty vehicles, concerns about CO2 emissions and other sustainability issues necessitate increased engine efficiencies, reduced tailpipe pollutants, and lower lifecycle carbon emissions. The intelligent blending of C2-C4 alcohols into motor gasoline is a viable method for achieving these goals. There are a multitude of ways to produce renewable alcohols such as through fermentation from first-generation feedstocks (sugar and corn) and second-generation feedstocks (lignocellulosic biomass), or by gasification and mixed alcohol fuel synthesis routes from lignocellulosic biomass. Currently ethanol is extensively used in motor gasoline fuels worldwide and although many have proposed the use of C3 and C4 alcohols in motor gasoline as an improvement over ethanol, the higher cost of production and lack of clear definition as to their benefit over ethanol when blended into motor gasoline have led to slow acceptance into the market. In this review, special emphasis is placed on the effects of blending C3 and C4 alcohols into motor gasoline in terms of physicochemical properties, volatility behavior, and engine performance when compared to ethanol blends. Furthermore, the impact of blending C3 and C4 alcohols with gasoline on emission (particulate matter, nitrogen oxides, carbon monoxide, hydrocarbons, and unregulated oxygenates) and combustion (volumetric efficiency, thermal efficiency, fuel consumption, and cold performance) characteristics is discussed. Although there are some disagreements in the literature over the effect of alcohols predominately around the type of SI engine, i.e., port fuel injected versus direct fuel injected and engine operating mode, generally it is stated that alcohols can potentially reduce soot, unburned hydrocarbons and CO emissions while increasing thermal efficiency when proper engine configuration/calibration is used. Lastly, research that must be conducted to find the optimum combination of alcohol blends and engine configurations is highlighted and discussed.

09 BIOMASS FUELS↗

DOE OSTI2022

Fuel Composition Influences on Reciprocating Engine Performance

The introduction of new fuels into the market is a unique opportunity to take advantage of new fuel compositions to improve the efficiency and emissions of internal combustion reciprocating engines and alternative fuel feedstocks. However, there are numerous challenges that introductions of new fuels face before they can become first legal, then ubiquitous. This chapter reviews four different case studies related to changing fuel composition. In some circumstances, the fuel formulation was changed in seemingly minor ways, and resulted in the unanticipated consequences. In other cases, a fuel change was desired, but an unexpected barrier slowed the introduction of the fuel change. These case studies should be viewed as opportunities to understand the interdependencies that exist and factors that need to be considered when trying to change the fuel in the marketplace.

Szybist, James↗

DOE OSTI2022

High-Fidelity Heavy-Duty Vehicle Modeling Using Sparse Telematics Data

Heavy-duty commercial vehicles consume a significant amount of energy due to their large size and mass, directly leading to vehicle operators prioritizing energy efficiency to reduce operational costs and comply with environmental regulations. One tool that can be used for the evaluation of energy efficiency in heavy-duty vehicles is the evaluation of energy efficiency using vehicle modeling and simulation. Simulation provides a path for energy efficiency improvement by allowing rapid experimentation of different vehicle characteristics on fuel consumption without the need for costly physical prototyping. The research presented in this paper focuses on using real-world, sparsely sampled telematics data from a large fleet of heavy-duty vehicles to create high-fidelity models for simulation. Samples in the telematics dataset are collected sporadically, resulting in sparse data with an infrequent and irregular sampling rate. Captured in the dataset was geospatial information, time series measurements, and vehicle-specific metadata from a subset of 96 vehicles from varied geographic regions across North America. A series of custom algorithms was developed to process vehicle data and derive both vehicle model input parameters and representative drive cycles. Derived models provide a basis on which to simulate real-world vehicles and iterate on vehicle aerodynamics, auxiliary power loads, transmission shift schedules, and other parameters to achieve reduced fuel consumption and increase energy efficiency. Notably, these models were developed without the use of expensive field data collection, using only data collected through fleet telematics. Processed representative drive cycles are used to validate the fuel economy of derived models. The models developed through this research allow for more representative vehicle simulations with increased flexibility regarding vehicle-to-vehicle variations.

ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2022

Rational design of photosynthetic reaction center protein maquettes

New technologies for efficient solar-to-fuel energy conversion will help facilitate a global shift from dependence on fossil fuels to renewable energy. Nature uses photosynthetic reaction centers to convert photon energy into a cascade of electron-transfer reactions that eventually produce chemical fuel. The design of new reaction centers de novo deepens our understanding of photosynthetic charge separation and may one day allow production of biofuels with higher thermodynamic efficiency than natural photosystems. Recently, we described the multi-step electron-transfer activity of a designed reaction center maquette protein (the RC maquette), which can assemble metal ions, tyrosine, a Zn tetrapyrrole, and heme into an electron-transport chain. Here, we detail our modular strategy for rational protein design and show that the intended RC maquette design agrees with crystal structures in various states of assembly. A flexible, dynamic apo-state collapses by design into a more ordered holo-state upon cofactor binding. Crystal structures illustrate the structural transitions upon binding of different cofactors. Spectroscopic assays demonstrate that the RC maquette binds various electron donors, pigments, and electron acceptors with high affinity. We close with a critique of the present RC maquette design and use electron-tunneling theory to envision a path toward a designed RC with a substantially higher thermodynamic efficiency than natural photosystems.

09 BIOMASS FUELS↗

DOE OSTI2023

Real-time control of connected vehicles in signalized corridors using pseudospectral convex optimization

Recent advances in Connected and Automated Vehicle (CAV) technologies have opened up new opportunities to enable safe, efficient, and sustainable transportation systems. However, developing reliable and rapid speed control algorithms in highly dynamic environments with complex inter-vehicle interactions and nonlinear vehicle dynamics is still a daunting task. In this paper, we develop a novel speed control method for CAVs to produce optimal speed profiles that minimize the fuel consumption and avoid idling at signalized intersections. To this end, an optimal control problem is formulated using the information of the upcoming traffic signal to adapt vehicles' speeds to avoid frequent stop-and-go driving patterns. Here, by applying the pseudospectral discretization method and the sequential convex programming method, the computational efficiency is greatly improved, enabling potential real-time on-vehicle applications. In addition, the algorithm is implemented under a model predictive control framework to ensure online control with instant response for collision avoidance and robust vehicle coordination. The proposed algorithm is verified through numerical simulations of three different traffic scenarios. The convergence and accuracy of the proposed approach are demonstrated by comparing with a popular nonlinear solver. Furthermore, the benefit of the proposed method in both traffic mobility and fuel efficiency is validated using the speed profile determined from a traffic following model in a simulation software as the baseline.

42 ENGINEERING↗

DOE OSTI2025

Reducing Coke and Increasing Bio-Oil Yield during Catalytic Fast Pyrolysis of Biomass Using Phosphorus-Modified Zeolite Catalysts

Catalytic fast pyrolysis (CFP) is a promising strategy for producing hydrocarbon transportation fuels from biomass feedstocks. However, catalyst development is needed to increase bio-oil yields and enhance process economics. In this work, we demonstrate how post synthetic modification of formed ZSM-5 with phosphorus shifts CFP selectivity from coke and light gases toward the desired bio-oil product. Microscale experiments demonstrated reduced coke production relative to unmodified ZSM-5 and identified an optimal P loading. Extensive catalyst characterization revealed that P interacted with Al sites to reduce the acid site density, with preferential binding to the strongest acid sites. Insights from the microscale experiments were leveraged to produce kilogram quantities of formed P-ZSM-5 for evaluation in a larger semi-integrated process. These experiments generated liters of bio-oil that was hydrotreated and fractionated into gasoline, diesel, and jet cuts. The phosphorus-modified ZSM-5 improved CFP bio-oil yield, resulting in an 11% relative increase in the carbon yield from biomass to aviation fuel and a 14% decrease in the minimum fuel selling price. These results highlight the impact targeted changes in catalyst acidity, achieved by adding 2.5 wt % P, can have on the carbon efficiency and feasibility of fuel production from biomass feedstocks.

09 BIOMASS FUELS↗

DOE OSTI2024

Size Up or Size Down? National Analysis of Heat Pump Sizing and Impacts

Electrification of on-site fossil fuel combustion in buildings is recognized as a key component of achieving global greenhouse gas emissions targets. Air-source heat pumps are an efficient approach for space heating electrification. However, a major barrier to heat pump adoption is the high installation cost relative to furnaces and air conditioners. Because the installation cost of heat pumps - especially cold climate models - is dependent on their size, it is important to understand the distribution of heat pump sizes using different sizing methods and factors that impact heat pump sizing. In this study, we use sub-hourly physics simulations of 550,000 statistically representative dwelling units to analyze the distribution of heat pump size in the U.S. for three different efficiency levels of heat pumps, with and without building insulation and air sealing upgrades. We will present results from the national analysis of different factors affecting heat pump sizing along with the impact of sizing decisions on upgrade costs and operating costs.

electrification↗

DOE OSTI2020

Chapter 21: Sustainable Technologies for Seaweed Conversion to Biofuels and Bioproducts

Seaweeds are attractive candidates to supply the future sustainable, photosynthetic, bioenergy feedstocks thanks to their cultivation promise in offshore marine farms, with year-round production, and no external nutrient requirements. Despite this potential, there are significant challenges associated with realizing both the cultivation and harvesting logistics, as well as in developing an efficient conversion platform to fuels and products. Effective and scalable and economically viable conversion processes tailored to a seaweed are discussed in detail and gaps on identified needs for yield and efficiency improvements. Among the conversion processes discussed here, anaerobic fermentation of seaweeds to bioenergy products, including organic acids and biomass, is promising to disrupt the current bioenergy landscape.

anaerobic digestion↗

DOE OSTI2024

Impact of Heaters on Molten Salt Reactors Dynamics

Recently, there has been renewed interest in the Molten Salt Reactor (MSR) concept. This interest is mainly due to its advantages over Light Water Reactors (LWRs). Among these advantages are the flexibility in the fuel choice and the possibility to burn actinides [1]. Currently, two molten research reactors are under development. A 2 MW molten salt experimental reactor has been constructed and is planned for operation in China. A 1 MW Molten Salt Research Reactor is under construction in the United States [2]. Thus, Research and Development (R&D) programs are needed for the MSR technology. Reactor dynamics studies are crucial safety evaluation studies. The development of reactor dynamics tools for MSRs started during the Molten Salt Reactor Program (MSRP) at ORNL, focusing on the Molten Salt Reactor Experiment (MSRE) [3]. Although various dynamic simulation tools are available, R&D efforts to develop specialized tools for MSRs are still ongoing [4]. The primary motivation for this interest is the goal of commercializing MSRs. Developing a dynamics tool for MSRs is crucial for analyzing their safety and supporting their demonstration efforts. A crucial safety issue in MSRs is ensuring that the fuel salt in the primary loop remains molten. This concern becomes particularly important when the reactor operates at lower power levels. Most chloride and fluoride salts used as fuel have a melting point of approximately 450 °C [5]. Therefore, maintaining fuel salt temperatures above this melting point is essential to prevent it from freezing. Freezing of the fuel salt can lead to volume expansion, potentially causing damage to reactor components [6]. Moreover, it can create local blockages within fuel salt channels, reducing cooling efficiency and resulting in hot spots [7]. Various methods can prevent fuel salt from freezing at low power levels. These include reducing the fuel mass flow rate in the primary loop, decreasing heat exchange between the primary and secondary loops in the reactor, and using electric fuel salt heaters. Reducing the mass flow rate of fuel salt in the primary loop can increase the fuel salt transit time in the core, enhancing heat production and increasing temperature. However, it can potentially lead to challenges. These include increasing the potential for fuel salt deposition on the reactor channel walls [8], affecting the overall heat transfer processes. Thus, alternative methods should be used [9]. This research investigates the effects of fuel salt heaters on the dynamics and stability during MSR operation. The investigation includes studying the reactor stability with the fuel salt heaters on and off. In addition, the reactor response to transients is compared with and without the operation of fuel salt heaters. These transients include reactivity insertion, primary and secondary pump failure, and heat sink temperature increase. The results of the reactivity insertion transient are presented in the summary.

73 - NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

Beyond Energy Efficiency: A clustering approach to embed demand flexibility into building energy benchmarking

The intermittency of carbon-free renewables and the demand changes associated with the widespread push for electrifying the transportation and building sectors provides an opportunity for buildings to go beyond energy efficiency and push towards providing demand flexibility to the electricity grid. The duality of energy efficiency and demand flexibility is necessary for success in a sustainable and reliable energy transition. Current building energy benchmarking models are limited in their ability to integrate concepts of demand flexibility and/or utilize granular smart meter data. Thus, current benchmarking methods are focused annual energy usage and fail to incorporate how the time of use of energy consumption impacts emissions in a quickly changing energy grid. Without a more comprehensive view of energy usage and associated real-time emissions, current benchmarking methods are unlikely to realize the full decarbonization potential of buildings. New emerging data streams provide an opportunity to develop a new generation of benchmarking energy models that embed dimensions of energy efficiency, grid interactivity, and demand flexibility into their analysis. In this paper, we propose a four-step method for embedding grid interactivity and demand flexibility into building benchmarking models that utilizes emerging building and time-series electricity data streams. We first engineer features to produce a mix-type dataset that encompasses many attributes of grid-interactive and efficient buildings, and then we apply K-medoids using Gower's Distance to produce peer-group clusters. We apply the method to a case study of 306 primary and secondary schools in southern California, USA. The results show that the method effectively clusters buildings by attributes of demand flexibility and energy efficiency. The clustering results reveal patterns in inefficient building operations and demand inflexibility at the building peer group level. In conclusion, the interpretation of clusters can serve as an integrated energy efficiency and demand flexibility benchmarking model and inform performance-specific policy targeting for buildings that go beyond traditional efficiency measures.

24 POWER TRANSMISSION AND DISTRIBUTION↗

DOE OSTI2024

Integration of Concentrating Solar Power with High Temperature Electrolysis for Hydrogen Production: Preprint

Hydrogen (H2) has been identified as a leading sustainable contender to replace fossil fuels in transportation and electricity generation. H2 production can be achieved by concentrating solar thermal power (CSP) systems collecting thermal energy from the sun to various chemical processes for fuel production. Fuel production via solar thermal chemical processes integrated with CSP uses the full spectrum of sunlight compared with photovoltaic power conversion and stores solar energy directly and efficiently [1]. The solar fuel production can be realized by thermochemical processes (e.g., water splitting for H2 production, carbon dioxide reduction, or methane reforming) or thermal electrochemical methods (e.g., integration with solid oxide electrolysis cell). Technology development for CSP-integrated solar fuel production requires broad technological bases from solar energy collection to chemical energy conversion. H2 generated from renewable sources can be an energy carrier for a carbon-free economy. Integrating CSP with high temperature electrolysis (HTE) using solid oxide electrolysis cells (SOEC) provides a renewable path for H2 generation. The CSP-HTE integration approach provides the benefit of thermal energy storage (TES) for continuous operation, improved capacity, and SOEC life. H2 gas has low energy density for transportation, pipeline networks are expensive, and H2 liquefaction is energy intensive. However, an alternative method for H2 distribution is to use carbon dioxide (CO2) capture and liquid hydrocarbon synthesis to convert solar energy into liquid fuels that are compatible with the existing fossil fuel infrastructure.

concentrating solar thermal power↗

DOE OSTI2024

Decarbonizing Cooking Appliances With Hydrogen

A novel hydrogen compatible heterogeneous burner prototype was engineered, fabricated, and evaluated for applications in cooking appliances. The key features targeted and accomplished under this effort included fuel flexibility, tolerance to high hydrogen concentrations (up to 85% in atmospheric design and 100% in premixed design), wide range of thermal power ratings, thermal cycling, reliability, and most importantly safety. The burner was operated in the range of 3000 – 12,000 Btu/h under all practical operating conditions (cold start, hot restart, fuel concentration variance). The heterogeneous oxidation burner technology was evaluated for overall performance targeting safety, reliability, emissions, fuel flexibility, and energy efficiency in a commercial RV and residential cooking range appliance prototypes. The burner demonstrated safe and reliable performance generating infrared heating energy without the consumption of any parasitic energy while using low-cost materials. Performance evaluation testing of the novel IR burner demonstrated fuel flexibility with hydrogen blended natural gas while significantly eliminating air pollutants like NOx and methane and increasing the energy efficiency by up to 20%.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Computationally Guided Design of Multiple Impurities Tolerant Cathode for Solid Oxide Fuel Cell Applications

Solid oxide fuel cells (SOFCs) have been recognized as promising candidates in the demand of reducing the dependence on fossil fuels, which is one of the solutions to the threat of global warming. It was reported that the direct chemical-to-electrical energy conversion in SOFCs comes with negligible emission of greenhouse gases and up to 60% working efficiency. SOFC has unique advantages over traditional power generation technologies and other types of fuel cells due to the use of relatively inexpensive materials, low sensitivity to poisoning impurities in fuels, relatively high conversion efficiency, and fuel flexibility (like carbon-based fuels). However, during the SOFC operation, the cathode is exposed to intrinsic and extrinsic airborne contaminants at high temperatures (600–900°C), leading to their reaction with electrode materials, irreversible chemical and structural changes, and electrochemical performance degradation. of which CO2, SO2, Cr6+ and H2O are known to be concerns. Thus, developing a comprehensive understanding of the multiple impurities poisoning of SOFC cathodes in the presence of single or multiple impurities is necessary to address the long-term degradation of the SOFC cathode systems at operating conditions. An integrated computational and experimental approach has been utilized in the current work aiming at the comprehensive investigation of the cathode materials under single or multiple impurities poisoning effects, understanding the multiple impurities poisoning mechanism(s), and improving the long-term durability of the SOFC cathodes to develop better performing impurity-tolerant cathode materials. We first examined the agreement between the simulation approach and the experimental observations at various atmospheric and temperature conditions to confirm the reliability of CALPHAD for poisoning simulations in these cathodes. Then, using this approach, we investigated the accelerated testing protocol, which has become the standard method for conducting impurity poisoning experiments involving these cathode materials. We found our simulation approach is able to predict in which systems, i.e., cathode material and treatment environment, the accelerated testing protocols reflect actual operating conditions. Finally, in-depth simulations were done for these three candidate cathodes under different experimental conditions and suggested directions toward alternative cathode materials that have superior impurity tolerance.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Gas-phase stability of large lanthanide:diglycolamide clusters evaluated using collision-induced dissociation

Efficient utilization of long-term deep geologic storage repositories is critical for the large-scale deployment of nuclear energy. As the minor actinides (americium and curium) are the largest contributor to the decay heat of used nuclear fuel after a few hundred years, their removal from used fuel prior to disposal can significantly increase the amount of waste that can be stored in a given volume. The development of ligands that can effectively separate the minor actinides from other components of used nuclear fuel are crucial to efficient utilization of geological storage repositories. N,N,N’,N’-tetraoctyl diglycolamide (TODGA) is a promising extractant for the separation of lanthanides and the minor actinides from other components of used nuclear fuel. While the use of TODGA in f-element separations has been investigated in process-based formulations, gas-phase metal ion cluster experiments enable the study of covalent interactions in reprocessing systems absent from solvent effects. Exploring fundamental differences in lanthanide-ligand covalent interactions can impact the development and implementation of actinide-lanthanide separation systems in nuclear fuels reprocessing. In this study, lanthanide-TODGA clusters were synthesized in the gas-phase and identified using mass spectrometry fragmentation experiments. Large europium and samarium clusters were identified that contained up to 8 and 10 bound TODGA ligands, respectively; this was surprising due to the size and multidentate binding that is normal for TODGA. In addition, while smaller clusters showed evidence of sequential ligand fragmentation, larger clusters displayed the loss of neutral TODGA with applied collision voltage. Interestingly, the voltage required for this removal decreased as more TODGA ligands were bound to the metal, suggesting that the metal coordination sphere was becoming more saturated and TODGA ligands were more weakly bound as the clusters got larger.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

From Atom to Engine: Understanding Fundamental Effects of Structure on Combustion Using Tandem Experiment and Computation

The ability to tie structural features to a fuel candidate’s ignition properties provides a path for rational design of advantaged fuels that facilitate higher-efficiency, lower-emitting combustion in engines. The time evolution of a fuel’s radical population directly correlates with global combustion parameters, and because the generated radicals depend on the initial structure and reaction pathways of the fuel molecule, it follows that the molecular structure of a fuel has a direct impact on this cascade, and therefore salient ignition-tied fuel properties. This work aims to understand the impact of structural features in the context of global combustion properties for direct application to emerging engine technologies. Specifically, we highlight the ability to identify potential fuel blendstocks for specific engine strategies by examining and elucidating the radical cascade tied to ignition. A representative subset of alcohols possessing a variety of structural features (e.g. branching, chain length) was selected for study using a robust combination of experimental and computational methods. The approach begins with identifying short-lived radicals and likely abstraction sites upon pyrolysis in a microreactor coupled with photoionization mass spectrometry for direct detection of product species. In tandem, electronic structure calculations were performed to calculate the relevant potential energy surfaces for fuel pyrolysis as well as the subsequent O2 addition-isomerization reactions, which govern ignition behavior. Furthermore, the theoretical energetic and ro-vibrational data are used to calculate rate constants for direct ignition modeling to explore how structural effects impact NTC behavior. The microreactor data combined with electronic structure theory calculations provide a well-informed picture of the reactions relevant to ignition for each fuel in this study, as well as the most likely radicals generated under engine conditions. This thorough fundamental picture of fuel decomposition and ignition chemistry is used to correlate the observed ignition behavior to molecular structural effects.

advanced biofuels↗