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Rational design of polyaromatic ionomers for alkaline membrane fuel cells with >1 W cm -2 power density
Alkaline membrane fuel cells (AMFCs) show great potential as alternative energy conversion devices to acidic proton exchange membrane fuel cells (PEMFCs). Over the last decade, there has been significant progress in the development of alkaline-stable polyaromatic materials for membrane separators and ionomeric binders for AMFCs. However, the AMFC performance using polyaromatic ionomers is generally poor, ca . a peak power density of <400 mW cm -2 . We report a rational design for polyaromatic ionomers which can minimize undesirable phenyl group interaction with hydrogen oxidation catalysts. The AMFC using a newly designed aryl ether-free poly(fluorene) ionomer exhibits a peak power density of 1.46 W cm -2 , which is approaching that of Nafion-based PEMFCs. This study further discusses the remaining challenges of high-performing AMFCs.
Thermal Extraction Modeling within HYBRID: Nominal and Extraction Conditions in Advanced Reactor Systems
This document details continuing development of thermal extraction modeling within the HYBRID repository, the modeling repository of the Integrated Energy Systems program at Idaho National Laboratory. The focus of the thermal extraction work is setting up template energy conversion systems for advanced reactor systems. Based on these nominal conditions, the IES team is developing extraction capability maps that present the system thermal-to-electric efficiency of the remaining system and the mass extraction fraction capability of these systems when extracting steam at various pressures to send steam to applications at a lower given pressure. These curves are mapped on what has become termed “whale chart” due to the appearance of the results. Multiple advanced reactor systems are complete, and it is anticipated that all four of the main advanced reactor types: advanced light-water reactors, high temperature gas reactors, liquid metal fast reactors, and molten salt reactors, will be complete by the end of the fiscal year.
Energy conversion device and method of reducing friction therein
A device configured for converting energy includes a first surface, a second surface configured for moving with respect to the first surface during operation of the device, and a coating disposed on at least one of the first surface and the second surface. The coating includes a first layer of a ceramic alloy represented by the general formula AlMgB.sub.14--X, wherein X is present in an amount of from 0 to 70 parts by weight based on 100 parts by weight of the ceramic alloy and is a doping agent selected from the group of Group IV elements and borides and nitrides thereof, and a second layer disposed on the first layer and including carbon in a gradient concentration. The coating has a hardness of from 10 to 20 GPa and a coefficient of friction of less than or equal to 0.12.
Impact of sub-cell internal luminescence yields on energy conversion efficiencies of tandem solar cells: A design principle
To develop a realistic design principle, we calculated the maximum conversion efficiency η{sub sc} and optimized sub-cell band-gap energies E{sub g} in double-junction tandem solar cells via a detailed-balance theory, paying particular attention to their dependence on internal luminescence quantum yields y{sub int} of the top and bottom sub-cell materials. A strong drop in the maximum η{sub sc} occurs when y{sub int} slightly drops from 1 to 0.9, where the drop in y{sub int} of the bottom cell causes a stronger effect than that of the top cell. For low values of y{sub int}, the maximum η{sub sc} has a simple logarithmic dependence on the geometric mean of the two sub-cells'y{sub int}.
Template-stabilized oxidic nickel oxygen evolution catalysts
Earth-abundant oxygen evolution catalysts (OECs) with extended stability in acid can be constructed by embedding active sites within an acid-stable metal-oxide framework. In this paper, we report stable NiPbO x films that are able to perform oxygen evolution reaction (OER) catalysis for extended periods of operation (>20 h) in acidic solutions of pH 2.5; conversely, native NiO x catalyst films dissolve immediately. In situ X-ray absorption spectroscopy and ex situ X-ray photoelectron spectroscopy reveal that PbO 2 is unperturbed after addition of Ni and/or Fe into the lattice, which serves as an acid-stable, conductive framework for embedded OER active centers. The ability to perform OER in acid allows the mechanism of Fe doping on Ni catalysts to be further probed. Catalyst activity with Fe doping of oxidic Ni OEC under acid conditions, as compared to neutral or basic conditions, supports the contention that role of Fe 3+ in enhancing catalytic activity in Ni oxide catalysts arises from its Lewis acid properties.
Electrocatalysis in Alkaline Media and Alkaline Membrane-Based Energy Technologies
Hydrogen energy-based electrochemical energy conversion technologies offer the promise of enabling a transition of the global energy landscape from fossil fuels to renewable energy. Here, we present a comprehensive review of the fundamentals of electrocatalysis in alkaline media and applications in alkaline-based energy technologies, particularly alkaline fuel cells and water electrolyzers. Anion exchange (alkaline) membrane fuel cells (AEMFCs) enable the use of nonprecious electrocatalysts for the sluggish oxygen reduction reaction (ORR), relative to proton exchange membrane fuel cells (PEMFCs), which require Pt-based electrocatalysts. However, the hydrogen oxidation reaction (HOR) kinetics is significantly slower in alkaline media than in acidic media. Understanding these phenomena requires applying theoretical and experimental methods to unravel molecular-level thermodynamics and kinetics of hydrogen and oxygen electrocatalysis and, particularly, the proton-coupled electron transfer (PCET) process that takes place in a proton-deficient alkaline media. Extensive electrochemical and spectroscopic studies, on single-crystal Pt and metal oxides, have contributed to the development of activity descriptors, as well as the identification of the nature of active sites, and the rate-determining steps of the HOR and ORR. Among these, the structure and reactivity of interfacial water serve as key potential and pH-dependent kinetic factors that are helping elucidate the origins of the HOR and ORR activity differences in acids and bases. Additionally, deliberately modulating and controlling catalyst-support interactions have provided valuable insights for enhancing catalyst accessibility and durability during operation. The design and synthesis of highly conductive and durable alkaline membranes/ionomers have enabled AEMFCs to reach initial performance metrics equal to or higher than those of PEMFCs. We emphasize the importance of using membrane electrode assemblies (MEAs) to integrate the often separately pursued/optimized electrocatalyst/support and membranes/ionomer components. Operando/in situ methods, at multiscales, and ab initio simulations provide a mechanistic understanding of electron, ion, and mass transport at catalyst/ionomer/membrane interfaces and the necessary guidance to achieve fuel cell operation in air over thousands of hours. We hope that this Review will serve as a roadmap for advancing the scientific understanding of the fundamental factors governing electrochemical energy conversion in alkaline media with the ultimate goal of achieving ultralow Pt or precious-metal-free high-performance and durable alkaline fuel cells and related technologies.
Conversion of Coal Wastes and Coal Plus Other Opportunity Fuel Mixtures, Such as Coal Plus Municipal Solids, to Produce Electricity and/or Liquid Fuels
For the foreseeable future, the Nation’s energy demand will continue to come largely from indigenous fossil energy resources and hydrocarbon fuels. Specifically waste coal plus other opportunity fuels need to be utilized as a feedstock to eliminate a waste stream and optimized to maximize energy yield and cleanly minimize pollutant emissions. Modular equipment is needed for installation in coal preparation locations, military installations, and research park facilities. Thermal decomposition of coal, biomass, and mixed solid waste (MSW) have been shown to reduce a waste stream while providing liquid and gaseous fuel products with low pollutant emissions. However, thermal decomposition processes have several challenges associated with preprocessing biomass and MSW, feeding and conveying material into the reactor, and post processing of syngas to remove undesirable products while upgrading to increase yield of high value products. Increasing total energy output from power plants by utilizing biomass and mixed wastes ultimately lowers energy costs, harmful environmental impacts of emissions, and has significant impacts on the energy security and sustainability of the U.S. economy. Entrained flow gasifiers (EFGs) produce very little CH4 and a wide range of H2/CO ratios (0.5–2.0) but are limited in their ability to effectively feed large biomass or MSW particles into the reactor. A solution to the feeding problems is to use pyrolysis torrefaction (PT) for conversion of waste materials to create a feedstock similar to coal and capable of grinding down and mixing with the coal feed. Mainstream experimentally explored reaction pathways for the conversion of coal waste plus municipal solids (CWPMS) and demonstrated a bench-scale reactor used for torrefaction of the municipal solid waste (MSW) to create a coal-like feed for blending with the coal waste. The material was processed in a pilot-scale EFG to determine product yield and emissions with CWPMS fuels, as well as the ash content and slagging properties of these feedstocks. The PT-EFG system was experimentally validated, where emissions and yield data were used to develop a high-fidelity process model and economic analysis. The following was accomplished in the Phase I: Determined optimal torrefaction process conditions for MSW and biomass through TGA; maximized heating value of fuel while maximizing final mass of torrefied product Demonstrated torrefaction of MSW and biomass feedstocks at 334°C, pulverized to uniform 74 µm particle size, and processed into coal-like feedstocks Demonstrated 8 lb/h pilot-scale EFG using MSW and biomass blends with waste coal; demonstrated 100% biomass in EFG Determined major effects of MSW torrefaction and co-gasifying high-ash coal waste-MSW blends have on pilot-scale EFG Demonstrated blending low-ash, low-sulfur torrefied biomass with high-ash waste bituminous and anthracite refuse coals generates a higher quality syngas compared to syngas from high-ash waste coals Demonstrated a high carbon conversion (> 99.5%) and syngas with 29.47% H2 content, and 0% CH4 content; greater water–gas shift occurs in EFG than predicted by equilibrium ASPEN Plus model Blended lower-ash, high-alkali biomass MSW to lower slag viscosities of the high-ash coal refuse sufficiently for better slag flow compared to feeding the high-ash coal Used low-sulfur biomass to greatly reduce the EFG syngas H2S concentrations and produce non-leachable slag and quench water with very little organic and trace metal contamination Developed a process model and TEA showing the modular PT EFG is cost competitive to existing power plants with the advantage of using low- or negative-value feedstocks such as waste coal stockpiles and non-landfilled MSW; providing a large incentive to implement an economical PT-EFG process
Efficient electrocatalytic conversion of CO.sub.2 to CO using ligand-protected Au.sub.25 clusters
An apparatus and method for CO.sub.2 reduction using an Au.sub.25 electrode. The Au.sub.25 electrode is comprised of ligand-protected Au.sub.25 having a structure comprising an icosahedral core of 13 atoms surrounded by a shell of six semi-ring structures bonded to the core of 13 atoms, where each semi-ring structure is typically --SR--Au--SR--Au--SR or --SeR--Au--SeR--Au--SeR. The 12 semi-ring gold atoms within the six semi-ring structures are stellated on 12 of the 20 faces of the icosahedron of the Au.sub.13 core, and organic ligand --SR or --SeR groups are bonded to the Au.sub.13 core with sulfur or selenium atoms. The Au.sub.25 electrode and a counter-electrode are in contact with an electrolyte comprising CO.sub.2 and H+, and a potential of at least -0.1 volts is applied from the Au.sub.25 electrode to the counter-electrode.
A Dual-Stage Sodium Thermal Electrochemical Converter (Na-TEC)
The sodium thermal electrochemical converter (Na-TEC) is a heat engine that generates electricity via the isothermal expansion of sodium ions through a solid-electrolyte. The Na-TEC can ideally achieve conversion efficiencies above 45%, but thermal management limitations have constrained previous single-stage devices to thermal efficiencies below 20%. To mitigate some of these limitations, the isothermal expansion can be divided into two stages; one at the evaporator temperature (1150K) and another at an intermediate temperature (550K – 1050K). This dual-stage Na-TEC takes advantage of regeneration and reheating, and is amenable to improved thermal management through reduced parasitic losses. The dual-stage device can improve the efficiency by ~8% points over the best performing single-stage device. Generally, a single-stage Na-TEC should be used for applications requiring high power densities, whereas a dual-stage Na-TEC should be used for applications requiring high efficiency.
DOE Support for the North American meeting of the International Society for Microbial Electrochemistry and Technology
The objective of the North American meeting of the International Society for Microbial Electrochemistry and Technology (NA-ISMET 2021, postponed from 2020 due to COVID-19) was to provide a welcoming space for an interdisciplinary group of researchers, primarily based in North America, to discuss their latest discoveries and innovative ideas on both basic science and applied technology in the field of microbial electrochemistry. After two years of limited travel and research interactions due to COVID-19, an in-person meeting was urgently needed to facilitate conversations and collaborations that help move the field forward. NA-ISMET 2021 was co-organized by Moh El-Naggar from the University of Southern California (USC) and Orianna Bretschger from Aquacycl Inc. The meeting took place on November 17 – 19, 2021 at the Michelson Center for Convergent Biosciences of USC. We hosted a total number of 65 registered participants from across the United States and several international participants. Thanks to the generous support from the Department of Energy, Air Force Office of Scientific Research, Office of Naval Research, the Army Research Office, the ISMET organization, and Gamry Instruments Inc., we were able to waive registration fees for all participants and reduce travel cost for several early-career researchers. The scientific program included 28 talks (16 from early-career researchers) and 24 posters that highlighted recent advances in microbial electrochemistry.
Manifesto on the Thermochemistry of Nanoscale Redox Reactions for Energy Conversion
Advancements in the use of nanoscale materials for energy conversions will rely on a clear understanding of reaction thermochemistry. While band edge and Fermi energies can be rigorous thermodynamic descriptors of bulk materials, we show here that their application to nanoscale systems is problematic. A change of one electron at a 1000 atom nanoparticle or a localized surface site on a catalyst/electrode causes significant nuclear reorganization of the system. Electron transfer is often coupled with solvent reorganization and/or with the transfer of ions, including ion intercalation, surface binding, and movement within the surrounding double layer. These effects can be significant (even for some bulk materials). However, Fermi and band energies, as typically used, do not include the energetics of nuclear reorganizations or cation coupling. A comprehensive approach to nanoscale charge transfer thermodynamics must explicitly consider these effects in order to have a more complete understanding and greater control of nanoscale redox reactivity.
Performance characterization of metal-supported solid-oxide fuel cell stacks at elevated pressure
Here, in this paper, we present results on performance characterization of solid oxide fuel cell stacks at elevated pressures up to 6 bar a . Stacks are designed and built by Ceres Power, Ltd., and are rated at 1- and 5- kW e . Fuel streams include H 2 / N 2 mixtures, synthetic natural-gas reformate, and simulated anode tail-gas recycle. Elevated operating pressure serves to increase stack electrochemical performance, with the most-pronounced gains found up to 4 bar a . Pressurized operation reduces the extent of methane conversion, promoting more-uniform internal reforming and cooling within the stack. Such cooling is critical at higher-current conditions. A previously developed one dimensional computational stack model is used to provide insight into stack operation. Pressurization is found to slightly increase internal thermal gradients, while promoting more-uniform reactant-concentration profiles across the cell, reducing the likelihood of local fuel starvation. The high fuel dilution brought by anode recycle can modestly decrease stack performance; however, this decrease is recovered through elevated-pressure operation at 3 bar a . Anode recycle further promotes compositional uniformity across the cell. These results reflect that pressurized operation can promote stack performance, while potentially promoting long-term stack durability through uniformity in stack environmental conditions.
Performance enhancement of perovskite solar cells with Mg-doped TiO{sub 2} compact film as the hole-blocking layer
In this letter, we report perovskite solar cells with thin dense Mg-doped TiO{sub 2} as hole-blocking layers (HBLs), which outperform cells using TiO{sub 2} HBLs in several ways: higher open-circuit voltage (V{sub oc}) (1.08 V), power conversion efficiency (12.28%), short-circuit current, and fill factor. These properties improvements are attributed to the better properties of Mg-modulated TiO{sub 2} as compared to TiO{sub 2} such as better optical transmission properties, upshifted conduction band minimum (CBM) and downshifted valence band maximum (VBM), better hole-blocking effect, and higher electron life time. The higher-lying CBM due to the modulation with wider band gap MgO and the formation of magnesium oxide and magnesium hydroxides together resulted in an increment of V{sub oc}. In addition, the Mg-modulated TiO{sub 2} with lower VBM played a better role in the hole-blocking. The HBL with modulated band position provided better electron transport and hole blocking effects within the device.
Hybrid Solid Oxide Fuel Cell/Gas Turbine Model Development for Electric Aviation
A thermodynamic model was developed and validated to analyze a high-performance solid oxide fuel cell and gas turbine (SOFC-GT) hybrid power system for electric aviation. This study used a process simulation software package (ProMax) to study the role of SOFC design and operation on the feasibility and performance of the hybrid system. Standard modules, including compressor, turbine, heat exchanger, reforming reactor, and combustor were used from the ProMax tool suite while a custom module was created to simulate the SOFC stack. The model used an SOFC test data set as an input. Additional SOFC stack performance effects, such as pressure, temperature, and utilization of air and fuel, were added from open source data. System performance predictors were SOFC specific power, fuel-to-electricity conversion efficiency, and hybrid system efficiency. Using these input data and predictors, a static thermodynamic performance model was created that can be modified for different system configurations and operating conditions. Prior to creating the final aircraft performance model, initial demonstration models were developed to validate output results. We used the NASA SOFC model as a benchmark, which was created with their Numerical Propulsion System Simulator (NPSS) software framework. Our output results matched within 1% of both the NASA model and open source SOFC performance data. With confidence gained in the accuracy of this model, a 1-MW SOFC-GT hybrid power system was constructed for an aircraft propulsion concept. Overall hybrid system efficiencies of > 75% FTE were observed during standard 36,000 feet cruise flight conditions.
Photoinduced charge transfer in transition metal dichalcogenide heterojunctions – towards next generation energy technologies
Increasing interest in using two-dimensional transition metal dichalcogenides (2D TMDCs) in optical energy conversion technologies creates a demand for improving the yields and lifetimes of photogenerated charge carriers. Despite inherently fast photocarrier decay in neat 2D TMDCs, the unique photophysics in these quantum-confined systems motivates continued effort to control the evolution of photoexcited states and create functional devices. Here, an intriguing strategy to accomplish this goal is to employ TMDCs in heterojunctions with appropriate semiconductors, where energy level offsets drive photoinduced charge transfer (PCT) across material interfaces. PCT in TMDC-based systems can be optimized for many different applications, such as driving free carriers to photocatalytic sites for redox reactions like water splitting, extracting charge to perform work in photovoltaics or photodetectors, and manipulating the spin and momentum valley electronic degrees of freedom for quantum computing systems. Here, we review recent strides in optimizing PCT for such applications through greater fundamental understanding of the photophysics that occurs at TMDC/semiconductor interfaces. After giving an overview of isolated TMDC properties, synthetic methods, and the basics of PCT, we discuss TMDCs in heterojunctions with several classes of materials, including other TMDCs, small molecule semiconductors, polymers, single-walled carbon nanotubes, quantum dots, perovskites, and electrolytes. In addition to highlighting the unique benefits of each materials category, we also identify parallels across common themes, such as the roles of charge-transfer states, spin, electronic coupling, delocalization, interfacial atomic morphology, and the precise design of energy landscapes to direct charge and energy motion. We hope to capture a broad range of the valuable work in this fast-paced field to inspire new research directions for employing PCT in targeted TMDC-based systems.
Autogenic reaction synthesis of photocatalysts for solar fuel generation
In one preferred embodiment, a photocatalyst for conversion of carbon dioxide and water to a hydrocarbon and oxygen comprises at least one nanoparticulate metal or metal oxide material that is substantially free of a carbon coating, prepared by heating a metal-containing precursor compound in a sealed reactor under a pressure autogenically generated by dissociation of the precursor material in the sealed reactor at a temperature of at least about 600.degree. C. to form a nanoparticulate carbon-coated metal or metal oxide material, and subsequently substantially removing the carbon coating. The precursor material comprises a solid, solvent-free salt comprising a metal ion and at least one thermally decomposable carbon- and oxygen-containing counter-ion, and the metal of the salt is selected from the group consisting of Mn, Ti, Sn, V, Fe, Zn, Zr, Mo, Nb, W, Eu, La, Ce, In, and Si.
Thermoelectric Conversion of Waste Heat to Electricity in an IC Engine Powered Vehicle
The thermoelectric generator shorting system provides the capability to monitor and short-out individual thermoelectric couples in the event of failure. This makes the series configured thermoelectric generator robust to individual thermoelectric couple failure. Open circuit detection of the thermoelectric couples and the associated short control is a key technique to ensure normal functionality of the TE generator under failure of individual TE couples. This report describes a five-year effort whose goal was the understanding the issues related to the development of a thermoelectric energy recovery device for a Class-8 truck. Likely materials and important issues related to the utility of this generator were identified. Several prototype generators were constructed and demonstrated. The generators developed demonstrated several new concepts including advanced insulation, couple bypass technology and the first implementation of skutterudite thermoelectric material in a generator design. Additional work will be required to bring this system to fruition. However, such generators offer the possibility of converting energy that is otherwise wasted to useful electric power. Uur studies indicate that this can be accomplished in a cost-effective manner for this application.