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

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At least 415 records · Page 23
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Pyrolysis of high-density polyethylene: Degradation behaviors, kinetics, and product characteristics

Pyrolysis is a promising technology for converting plastic waste into valuable raw materials while offering a potential solution to the global plastic pollution crisis. In this study, the thermal pyrolysis of high-density polyethylene (HDPE) is investigated in a drop tube reactor under nearly isothermal conditions. The impact of reaction temperature and gas/volatile residence time on carbon conversion and product distribution is examined across a range of 500–900°C and 3.6–32.2s, respectively. Non-condensable gas products detected by online mass spectrometry are H 2 , CH 4 , C 2 H 4 , C 2 H 6 , C 3 H 6 , and C 3 H 8 . At elevated temperatures and prolonged residence time, H 2 yield reaches as high as 8.6 wt% of the initial HDPE mass due to intensified cracking reactions of C 2 –C 3 hydrocarbons and long-chain aliphatic compounds. Consequently, pyrolysis tars consist mainly of polycyclic aromatic hydrocarbons (PAHs) with 5–7 rings, accompanied by visible coke deposition within the reactor. HDPE decomposition to volatiles is an endothermic process and it is complete at a temperature between 492°C and 525°C, depending on the heating rate employed, from non-isothermal thermogravimetric analysis and differential scanning calorimetry (TGA-DSC) measurements. The thermal degradation of HDPE pellets follows the two-dimensional nucleation growth model for conversion levels up to 0.8 with an apparent activation energy of 259–270 kJ/mol and a pre-exponential factor of 4.83 × 10 17 –1.37 × 10 19 min -1 , determined from various isoconversional methods such as Flynn-Wall-Ozawa (FWO), Kissinger-Akahira-Sunose (KAS), and Starink, along with Criado's master plots. Further, these findings provide valuable insights into optimizing process parameters and refining reactor design for pyrolysis, which can be integrated with gasification and reforming processes to enhance hydrogen production on a larger scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Coupling of Adhesion and Anti-Freezing Properties in Hydrogel Electrolytes for Low-Temperature Aqueous-Based Hybrid Capacitors

Solid-state zinc-ion capacitors are emerging as promising candidates for large-scale energy storage owing to improved safety, mechanical and thermal stability and easy-to-direct stacking. Hydrogel electrolytes are appealing solid-state electrolytes because of eco-friendliness, high conductivity and intrinsic flexibility. However, the electrolyte/electrode interfacial contact and anti-freezing properties of current hydrogel electrolytes are still challenging for practical applications of zinc-ion capacitors. Here, we report a class of hydrogel electrolytes that couple high interfacial adhesion and anti-freezing performance. The synergy of tough hydrogel matrix and chemical anchorage enables a well-adhered interface between hydrogel electrolyte and electrode. Meanwhile, the cooperative solvation of ZnCl 2 and LiCl hybrid salts renders the hydrogel electrolyte high ionic conductivity and mechanical elasticity simultaneously at low temperatures. More significantly, the Zn||carbon nanotubes hybrid capacitor based on this hydrogel electrolyte exhibits low-temperature capacitive performance, delivering high-energy density of 39 Wh kg –1 at –60 °C with capacity retention of 98.7% over 10,000 cycles. With the benefits of the well-adhered electrolyte/electrode interface and the anti-freezing hydrogel electrolyte, the Zn/Li hybrid capacitor is able to accommodate dynamic deformations and function well under 1000 tension cycles even at –60 °C. This work provides a powerful strategy for enabling stable operation of low-temperature zinc-ion capacitors.

25 ENERGY STORAGE↗
DOE OSTI2020

Synthesis of nickel selenide thin films for high performance all-solid-state asymmetric supercapacitors

As a significant semiconductor, nickel selenide shows enormous potential and extensive application prospects in the field of sensor, photocatalysis and supercapacitor. In this paper, nickel selenide (Ni 3 Se 2 , NiSe) thin films were successfully fabricated on stainless-steel sheet using a facile, effective electrodeposition technique. The morphologies, microstructures and chemical compositions of the thin films are characterized systematically. Electrochemical tests exhibit that the Ni3Se2 and NiSe possess high specific capacitance of 581.1 F/g and 1644.7 F/g, respectively. A flexible, all-solid-state asymmetric supercapacitor is assembled by utilizing NiSe film as positive electrode and activated carbon as negative electrode. The solid device delivers a high areal capacitance of 27.0 mF/cm 2 at the current density of 0.7 mA/cm 2 . Furthermore, the maximum volumetric energy density and power density of the NiSe//AC asymmetric SCs can achieve 0.26 mWh/cm 3 and 33.35 mW/cm 3 , respectively. The device shows robust cycling stability with 84.6% capacitance retention after 10000 cycles, outstanding flexibility and satisfactory mechanical stability. Moreover, two devices in series can light up a red light-emitting diode, which displayed great potential applications for energy storage.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Long-term carbon intensity reduction potential of K-12 school buildings in the United States

School buildings have a great potential for carbon emission reduction since their annual emission is about 72 million metric tons. Currently, more than 30% of school buildings were built before 1960 and are underperforming. To effectively reduce carbon emissions via school building retrofits, it is critical for policymakers to understand the carbon intensity reduction potential of retrofitting school buildings in different regions. Hence, this study develops a method to comprehensively assess the long-term carbon intensity reduction potential of aggregated commercial buildings on a county-by-county basis in the continental U.S. We apply this method to the K-12 school buildings including primary and secondary school buildings. Here, this paper predicts the carbon intensity reduction potential of K-12 school buildings with eight building retrofit measures from 2022 to 2050 in the continental U.S. The results reveal several interesting findings: (1) In the approximately 3,000 counties of the U.S. from 2022 to 2050, the carbon intensity reduction potential of retrofitting K-12 school buildings in each county ranges from 0.41 kg/m 2 to 40.00 kg/m 2 . (2) Even in the same climate zone, the trends of carbon intensity reduction potential from 2022 to 2050 are different depending on their electricity sources. For example, in a hot and humid climate zone, the carbon intensity reduction potential in Florida will decrease from 2044 to 2048. However, in Mississippi, the carbon intensity reduction potential from 2044 to 2046 will increase due to the termination of the nuclear energy usage. (3) Generally, reducing lighting power density leads to more carbon intensity reduction in most states, but it might not be applicable for states with high clean energy penetration, such as Washington.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2023

Bridging adsorption behavior of confined CH 4 -CO 2 binary mixtures across scales

An accurate understanding of the competitive adsorption of CH 4 -CO 2 binary mixtures in nano-confined systems is critical for engineering CO 2 storage in shale gas reservoirs. Due to difficulties in making reliable experimental observations in nano-scale, atomistic simulations (ASs), such as the Grand Canonical Monte Carlo (GCMC) method, provide a viable approach to studying the adsorption behavior of confined fluids. ASs are, however, limited in the size of the compositional domain due to the high computational cost. This work proposes a framework that combines AS and the lattice Boltzmann (LB) method to bridge the physics of confined fluids across scales. The Peng–Robinson equation of state (PR-EoS) produces fugacity coefficients, which serve as input for conducting multi-component GCMC simulations. These GCMC simulations explore the competitive adsorption behavior of CH 4 -CO 2 in nano-slits at various composition, pressure, and channel-width conditions. Both components generate adsorption layers with high densities near the walls with CO 2 preferentially adsorbing compared to CH 4 on the organic walls of carbon sheets. At the mesoscale, a pseudopotential model represents the intermolecular forces in multi-component, multiple-relaxation-time LB simulations. The LB simulations are in good agreement with the GCMC results, allowing us to obtain values for tunable LB parameters. We then extend the use of LB to simulate adsorption behavior in complex networks with nano-sized channels. The phase behavior and fluid properties in the complex geometries of nano-channels differ from nano-slits and bulk systems. Furthermore, the bridging of physics from GCMC (microscale) to LB (mesoscale) via the macroscale PR-EoS connects the adsorption behavior of binary systems across scales.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Performance and cost analysis of liquid fuel production from H 2 and CO 2 based on the Fischer-Tropsch process

Electro-fuels can be produced from concentrated sources of carbon dioxide and hydrogen using electricity generated from renewable sources; this process enables energy storage at high volumetric energy density. Among the electro-fuels options, FT (Fischer-Tropsch) fuel is attractive for heavy-duty trucks and non-road transportation applications. This study conducts a techno-economic analysis of FT liquid fuel production from H 2 and CO 2 using a detailed performance analysis. Minimum fuel selling price is estimated for a broad range of H 2 and CO 2 prices and for a range of potential CO 2 credits. The analysis indicates that H 2 price has the largest impact on the minimum selling price of FT fuel. FT fuel production with a CO 2 price of $17.3/metric ton requires an H 2 price of $0.8/kg to be cost-competitive with the pre-tax petroleum diesel price of $3.1/gal in 2050 (before the application of any CO 2 credits). When the H 2 price is $2.0/kg from central water electrolysis (2020 target), the minimum selling price of the FT fuel is $5.4–5.9/gal. A sensitivity analysis shows that future system optimization of FT fuel production could focus on improving the H 2 and CO 2 recycle contributions and FT fuel conversion ratio. The analysis results can be combined with various upstream systems for H 2 and CO 2 production.

08 HYDROGEN↗
DOE OSTI2021

Degradation mechanisms of 1.3 μm C-doped quantum dot lasers grown on native substrate

Here, the aim of this paper is to analyse the degradation modes of 1.3 μm InAs quantum dot laser diodes (QD LDs) grown by using carbon as a p-type dopant, as an alternative to beryllium. The devices were stressed at high current densities, to favor the onset of excited-state (ES) emission, and to study the related degradation phenomena. The study of QD LDs is of fundamental importance for the photonic integrated circuits (PICs). The investigation is based on two types of stress tests: 1) a current step stress and 2) a constant current stress. With these experiments we demonstrate that a) the current is a determining factor for the onset of the ES during the operation of such devices. b) the onset of ES is responsible for a rapid quenching of the ground state (GS) emission. c) stress induces a significant increase in the threshold current of the devices, that is ascribed to the lowering of the injection efficiency, which in turn can be explained by the easier escape of carriers from quantum dots (QDs) from ES energy levels. d) the contribution of defects on the optical and electrical degradation is also discussed.

42 ENGINEERING↗
NASA NTRS1992

Pulsed power molten salt battery

It was concluded that carbon cathodes with chlorine work well. Lithium alloy chlorine at 450 C, 1 atm given high power capability, high energy density, DC + pulsing yields 600 pulses, no initial peak, and can go to red heat without burn-up. Electrochemical performance at the cell and cell stack level out under demanding test regime. Engineering and full prototype development for advancing this technology is warranted.

Argade, Shyam D.↗
NASA NTRS2016

Functional Responses in Otolith Structures from Micro- to Hyper-Gravity

Vertebrates and invertebrates sense gravito-inertial acceleration by mechanoreceptors in the otolith and statolith organs, respectively. These structures consist of ciliated sensory hair cells surmounted by biomineral grains of calcium carbonate (CaCO3) called oto-orstato-conia. The grains provide mechanical loading of hair cell cilia, and their high density increases sensitivity to acceleration. A widely considered mechanism by which the animal responds to a chronic change in amplitude of gravity is a change in weight lending otoconia. In G, it is argued, the organism counters the loss of gravity by increasing CaCO3 production, thereby increasing otolith mass, as a means to increase system gain. In hypergravity (HG), the converse is argued. Here, we present the results obtained in 3 species exposed both to G and HG. Adult toadfish, Opsanus tau, were exposed to G in 2 short-duration shuttle missions and to 1.24 1.73G centrifugation for 1-32 days; re-adaptation was studied following 1-8 days of 1G. Results show a biphasic pattern in response to 1.73G: initial hypersensitivity, similar to that observed after G exposure, followed by transition to a significant decrease at 16-32 days. Recovery from HG exposure is 4-8 days. Next, we examined directly the responses of statocyst receptors in the land snail after exposure to G on two unmanned Russian Orbital missions and at 1.24G. Similar to vertebrate afferents snail receptors increased their sensitivity to tilt after G exposure, and decrease it after 16-32 days of HG. Two major pieces of information are still needed: vertebrate hair cell response to altered gravity and impact of longer duration exposures on sensory plasticity. To address the latter, we applied electron microscopic techniques to image otoconia mass obtained from 1) mice subjected to 91-days of weightlessness in the Mouse Drawer System (MDS) flown on International Space Station, 2) mice subjected to 91-days of 1.24G centrifugation on ground, and 3) mice flown on 2 short-duration orbital missions. Images indicate a clear restructuring of individual otoconia, suggesting deposition to the outer shell. Images from their HG counterparts indicate the converse - an ablation of the otoconia mass. For shorter duration exposures to weightlessness on 13-day shuttle missions, mice otoconia appear normal. Despite the permanence of 1G in evolution, the animal senses exposure to a novel, non-1G, environment and adaptive mechanisms are initiated - in the short term, compensation is likely confined to the peripheral sensory receptors, the brain or both. For longer exposures structural modifications of the endorgan may also result. Support Contributed By: NASA 03-OBPR-04 and 11-11_Omni_2-0002

Vertebrates↗
DOE OSTI2020

Development of a Testbed for Pipeline Flushing - 20425

Pipelines which carry high-level waste within the DOE complex should be properly flushed in the cases where stationary or moving beds of solid sediment occur, or lines are prone to hydrogen gas buildup. Present guidelines establish a minimum for the amount of water (flush volume) and flush velocity values used for post-transfer flushing operations to achieve satisfactory cleaning of pipelines. However, further studies are needed to find optimal operating velocity modes/values in order to minimizing the flush volume and consequent downstream waste. These efforts are significantly helpful to DOE waste remediation sites by preserving tank storage, preventing additional waste processing, and minimizing dilution and changes in waste chemistry. An experimental test loop was recently developed for study of non-Newtonian slurry flushing at the Florida International University (FIU). This loop was designed to create sediment beds of various materials and bed heights and investigate parameters that effect the efficiency of flushing operations. The objective is to find flush velocity values/modes which lead to satisfactory cleaning of transport lines with a minimum amount of water usage. A 165 ft experimental test loop made of 3-inch carbon steel pipes was constructed and used in initial testing campaigns. This pipe loop was equipped with real-time monitoring instruments to record variation of pressure, density, mass flow rate, and temperature during testing. Post-flush in-situ no-flow evaluations were performed using ultrasonic, endoscopy, and visual inspection. Additional post-flush evaluations were conducted using filtration and density monitoring of residuals within a designated circulations loop. These provisions enable comparison of pipeline cleanness before the start and after termination of flushing operations for efficiency evaluation. This paper presents efforts associated with flushing of kaolin-water mixtures at different concentrations and with various flush volume and flush velocity values/modes. In initial testing, efforts focused on creating repeatable sediment beds inside the pipeline in both fully-flooded (no pre-flush drainage) and gravity-drained (pre-flush drained) systems. Bed characterization (i.e., measurement of sediment height and solids concentration) was conducted to ensure about consistency of initial conditions between tests. Preliminary results for flushing study of 10% vol. kaolin-water mixtures starting from a fully-flooded initial condition showed that flushing with 1-line volume (65 gallons) could remove up to 72 percent of solids from the pipeline. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Hierarchically Structured Catalysts Toward Sustainable Hydrogen Economy: Electro‐ and Thermo‐Chemical Pathways

Abstract Hydrogen, as an important clean energy source, plays a more and more crucial role in decarbonizing the planet and meeting the global climate challenge due to its high energy density and zero‐emission. The demand for sustainable hydrogen is increasing drastically worldwide as driven by the global shift towards low‐carbon energy solutions. Thermochemical catalysis process dominates hydrogen production at scale given its relatively mature technology and commercialization status, as well as the established manufacturing infrastructure. While due to its environmentally friendly nature and growing abundant sources of renewable electricity, the electrochemical path for hydrogen production is rising as a major alternative to the thermochemical means. Nevertheless, hierarchically structured catalysts and devices have gradually taken the center stage toward replacing the traditional counterparts, especially with the rapid advancement of the design and manufacture of such ordered nanostructure assemblies toward high activity, efficient mass transport, and superb stability. In this review, the latest progress of the hierarchically structured catalysts for hydrogen production have been surveyed on electro‐ and thermo‐ chemical pathways comparatively. It covers the structure designs of atomic dispersion, nanoscale surfaces and interfaces for achieving highly active and durable catalysts, components, and devices. Both electrochemical and thermochemical approaches are reviewed in terms of the vast design details, engineered benefits, and understandings of various Pt‐group metal (PGM) and non‐PGM based transition metal catalysts for hydrogen production. As the growing trend, brief discussions are also presented toward the high‐level assembly and manufacture of complexly structured components and devices at scale in the electrochemical and thermochemical energy systems.

Deng, Chenxin↗
DOE OSTI2020

Real Time 3D Observations of Portland Cement Carbonation at CO2 Storage Conditions

Depleted oil reservoirs are considered a viable solution to the global challenge of CO 2 storage. A key concern is whether the wells can be suitably sealed with cement to hinder the escape of CO 2 . Under reservoir conditions, CO 2 is in its supercritical state, and the high pressures and temperatures involved make real-time microscopic observations of cement degradation experimentally challenging. Here, we present an in situ 3D dynamic X-ray micro computed tomography (μ-CT) study of well cement carbonation at realistic reservoir stress, pore-pressure, and temperature conditions. The high-resolution time-lapse 3D images allow monitoring the progress of reaction fronts in Portland cement, including density changes, sample deformation, and mineral precipitation and dissolution. By switching between flow and nonflow conditions of CO 2 -saturated water through cement, we were able to delineate regimes dominated by calcium carbonate precipitation and dissolution. For the first time, we demonstrate experimentally the impact of the flow history on CO 2 leakage risk for cement plugging. In-situ μ-CT experiments combined with geochemical modeling provide unique insight into the interactions between CO 2 and cement, potentially helping in assessing the risks of CO 2 storage in geological reservoirs.

58 GEOSCIENCES↗
NASA NTRS2002

Characterization on C/SiC Ceramic Matrix Composites with Novel Fiber Coatings

Ceramic Matrix Composites (CMCs) are attractive candidate materials in the aerospace industry due to their high specific strength, low density and higher temperature capabilities. The National Aeronautics and Space Administration (NASA) is pursuing the use of CMC components in advanced Reusable Launch Vehicle (RLV) propulsion applications. Carbon fiber-reinforced silicon carbide (C/SiC) is the primary material of interest for a variety of RLV propulsion applications. These composites offer high- strength carbon fibers and a high modulus, oxidation-resistant matrix. For comparison, two types of carbon fibers were processed with novel types of interface coatings (multilayer and pseudoporous). For RLV propulsion applications, environmental durability will be critical. The coatings show promise of protecting the carbon fibers from the oxidizing environment. The strengths and microstructures of these composite materials are presented.

Petko, Jeanne↗
DOE OSTI2020

Engineering Surface Oxygenated Functionalities on Commercial Carbon toward Ultrafast Sodium Storage in Ether-Based Electrolytes

The pursuit of a high-capacity anode material has been urgently required for commercializing sodium-ion batteries with a high energy density and an improved working safety. In the absence of thermodynamically stable sodium intercalated compounds with graphite, constructing nanostructures with expanded interlayer distances is still the mainstream option for developing high-performance carbonaceous anodes. In this regard, a surface-functionalized and pore-forming strategy through a facile CO 2 thermal etching route was rationally adopted to engineer negligible oxygenated functionalities on commercial carbon for boosting the sodium storage process. Benefitted from the abundant ionic/electronic pathways and more active reaction sites in the microporous structure with noticeable pseudocapacitive behaviors, the functionalized porous carbon could achieve a highly reversible capacity of 505 mA h g -1 at 50 mA g -1 , an excellent rate performance of 181 mA h g -1 at 16,000 mA g -1 , and an exceptional rate cycle stability of 176 mA h g -1 at 3200 mA g -1 over 1000 cycles. These outstanding electrochemical properties should be ascribed to a synergistic mechanism, fully utilizing the graphitic and amorphous structures for synchronous intercalations of sodium ions and solvated sodium ion compounds, respectively. Finally, the controllable generation and evolution of a robust but thin solid electrolyte interphase film with the emergence of obvious capacitive reactions on the defective surface, favoring the rapid migration of sodium ions and solvated species, also contribute to a remarkable electrochemical performance of this porous carbon black.

25 ENERGY STORAGE↗
DOE OSTI2026

Enhanced cycling stability of Ni-rich Li-metal cells enabled by dual vinylene carbonate and tris(trimethylsilyl)borate electrolyte additives

NMC811 (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) and other high-Ni chemistries are promising cathode candidates for high-performance electric vehicles, owing to their high energy density and reduced cobalt content. However, their long-term cycling stability is hindered by surface degradation, particularly when paired with conventional electrolytes and a lithium metal anode. Electrolyte additives represent a practical approach to enhance interfacial stability and improve overall battery performance by promoting the formation of a robust electrolyte–electrode interphase (EEI). In this study, we revisit the effects of vinylene carbonate (VC) and tris(trimethylsilyl)borate (TMSB) additives on single-crystal SC-NMC811||Li cells. While TMSB only increases the open-circuit voltage and initial overpotential, it delivers superior capacity retention at C/3 compared to cells containing only VC or a dual additive system (VC and TMSB). Notably, under fast-charging conditions (1C, 2C, and 5C), the dual-additive system significantly outperforms other formulations, achieving markedly enhanced long-term capacity retention. Comprehensive electrochemical and spectroscopic analyses reveal that the VC/TMSB dual-additive system suppresses surface transition in NMC811, mitigates structural degradation by forming a thin, LiF-deficient cathode-electrolyte interface (CEI) layer. Moreover, they promote smooth and dense Li deposition and generate a LiF-deficient solid-electrolyte interphase (SEI). Consequently, the synergistic stabilization of both the CEI and SEI effectively limits the overall cell impedance growth during extended cycling. These findings provide key insights into co-additive strategies for engineering stable interfaces in high-energy Ni-rich Li-metal batteries.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Development of coal-derived carbon-based structural unit as a potential new building material

Coal combustion for energy has not only wasted the hydrogen-rich volatile matters but also results in CO 2 emission causing serious environmental issues. An integrated coal pyrolysis and solvent extraction process under elevated temperatures in an inert atmosphere is implemented to convert as-mined coal from Wyoming Powder River Basin to functional carbon elements such as pyrolysis char (PC). This paper presents the development and fabrication of new carbon-based structural unit (CSU) using pulverized PC and two coal-derived pitches (mesophase pitch and tar pitch) to attain high compressive strength greater than 30 MPa, low thermal conductivity less than 0.30 W/m.K, and low density less than 1.25 g/cm 3 . CSUs have the potential to overcome the current challenges with cement and concrete through pressurized fabrication followed by carbonization. This study aims to develop CSU with nearly 100% coal-derived carbon material for structural application in buildings. The effects of pressing pressures, carbonization temperatures, and binder contents on the density and mechanical and thermal properties of CSU samples are investigated. The study concludes that mesophase pitch produces a better performance of CSU samples, a combination of 100 MPa pressing pressure and carbonization temperature of 900 ⁰C yields the highest compressive strength, and a 25% MP content is recommended for low-cost CSU fabrication. Furthermoer, CSU has a much lower density, lower thermal conductivity, higher compressive strength, and higher strength-to-density ratio than normal concrete.

36 MATERIALS SCIENCE↗
NASA NTRS2002

Characterization of C/SiC Ceramic Matrix Composites (CMCs) with Novel Interface Fiber Coatings

Ceramic Matrix Composites (CMCs) are attractive candidate materials in the aerospace industry due to their high specific strength, low density and higher temperature capabilities. The National Aeronautics and Space Administration (NASA) is pursuing the use of CMC components in advanced Reusable Launch Vehicle (RLV) propulsion applications. Carbon fiber-reinforced silicon carbide (C/SiQ is the primary material of interest for a variety of RLV propulsion applications. These composites offer high-strength carbon fibers and a high modulus, oxidation-resistant matrix. For comparison, two types of carbon fibers were processed with novel types of interface coatings (multilayer and pseudoporous). For RLV propulsion applications, environmental durability will be critical. The coatings show promise of protecting the carbon fibers from the oxidizing environment. The strengths and microstructures of these composite materials are presented.

Petko, Jeanne F.↗
DOE OSTI2024

Carbonate Management to Enable Energy- and Carbon-Efficient CO 2 Electrolysis (Final Technical Report)

The rapid growth and plummeting cost of solar energy have spurred growing interest in using CO 2 electrolysis to produce chemicals and fuels as an alternative to conventional petrochemical processes. High-temperature (>800 °C) solid oxide electrolyzers that convert CO 2 into CO and O 2 have recently become commercially available. Low-temperature electrolysis cells offer the prospect of more convenient and flexible operation, which is critical for utilizing intermittent solar energy, and provide access to more valuable C 2+ products such as ethylene, ethanol, and propanol. Over the past 10 years, research in this area has yielded substantial progress in both fundamental understanding of the requisite electrocatalytic reactions and design of prototype devices. Leveraging insights from fuel cells and membrane water electrolyzers, researchers have developed electrolysis cells with gas diffusion electrodes (GDE) that have demonstrated high CO 2 electrolysis current densities (>100 mA cm –2 ) as well as promising selectivity and stability. Despite these advances, the energy efficiency (electrical energy-to-product) and carbon efficiency (CO 2 -to-product) of low-temperature CO 2 electrolysis remain far too low for large-scale deployment. A preponderance of evidence indicates that the principal source of efficiency losses is the rapid and thermodynamically favorable reaction of CO 2 with hydroxide (OH – ) to form carbonate (CO 3 2– ). Carbonate formation imposes steady-state electrolysis conditions that result in large voltage and CO 2 losses for all known (photo)electrochemical CO 2 cells. While much current research remains focused on CO 2 reduction catalyst design, this largely overlooked CO 3 2– problem presents a fundamental scientific barrier to creating a viable electrochemical option for converting solar energy into chemicals and fuels. The project pursues an integrated, multi-PI research effort that establishes a fundamental science of CO 3 2– management. PI Kanan and Co-PI Mani’s contribution to the project is to evaluate strategies to mitigate the CO 3 2– problem by changing the properties of the electrolyte and the environment in which CO 2 reduction catalysis takes place. Experimental studies showed that electrolytes composed of a high concentration of both CO 3 2– and HCO 3 – , which serve as moderately alkaline buffers, improved the cell voltage by compared to all-HCO 3 – electrolytes, but these buffered systems still show substantial CO 2 uptake that reduces pH over time. Computational studies developed a homogenized model of a CO 2 reduction catalyst layer that permits a low-cost exploration of the high-dimensional parameter space associated with catalyst layers on gas diffusion electrodes. The model was validated by accurately reproducing experimental data for the related but simpler reaction of CO reduction and then used to probe the effects of catalyst layer architecture on CO 2 reduction. Minimizing the size of catalyst and hydrophobic domains in the catalyst layer is predicted to mitigate CO 3 2– formation and thereby enable prolonged operation at elevated pH. In support of the CO 2 electrolysis studies, a new method for rapidly prototyping electrochemical cells was developed and validated. The method uses a combination of 3D printing and electroless plating to generate conductive cell components for evaluating new cell designs. The carbonate problem encompasses mass transport processes and acid-base reactions that are relevant to many other electrochemical systems. Investigation of strategies to address the carbonate problem led to an additional line of inquiry into the physicochemical phenomena that determine the efficiency of electrochemical acid-base production, which has numerous applications in the broader field of carbon management. New strategies for using the supporting electrolyte to inhibit H + /OH – recombination in electrochemical acid-base production were evaluated, leading to the development of a novel acid-base producing system that eliminates the need for ion exchange membranes and exhibits promising efficiency and current densities for scalable applications.

25 ENERGY STORAGE↗