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At least 397 records · Page 22

Thermodynamic Limits of Redox-Based Thermochemical Processes (REDOTHERM)

Solar thermochemical fuel production is a potential pathway for the production of sustain liquid drop-in fuels, which can help decarbonize the aviation and maritime sectors. In an attempt to analyze the commercial viability of this technology, several studies have been conducted, including system and technoeconomic analysis (TEA) modeling. However, most studies to date simply assume a given redox reactor efficiency, which is significantly higher than demonstrated values to date. While it is widely recognized that utilizing a counter-current flow (CF) configuration could increase the redox reactor efficiency, an over-simplification in the thermodynamic modeling may lead to unphysical results which has been included in multiple publications. The fact that the solar redox reactor is the least developed component in the process chain makes it hard to identify technology gaps and evaluate pathways to deployment at scale using this approach. In this work, a thermodynamic model for a moving oxide system has been developed, in a general form that allows to analyze the system for different redox-active materials, under a wide range of operating conditions, for both parallel and countercurrent flows. The model capabilites are demonstrated, and the model's code will be shared as an open-source on GitHub in the next few months.

chemical looping↗

Creep suppression and fatigue in bio-based composites manufactured via conventional and large format additive manufacturing processes

The emergence of novel extrusion-based additive manufacturing (AM) processes has prompted the development of new thermoplastic composite feedstocks, and broadening sustainability initiatives have driven the development of bio-based and recyclable material for AM feedstocks. Poly(lactic acid) (PLA) with wood flour (WF) is one composite system that has been demonstrated in numerous AM applications, as well as traditional processing methods (i.e., compression and injection molding); however, there has been a need to understand how the variation in processing methodology impacts the material performance of these bio-based feedstocks from a fundamental perspective, with particular emphasis on creep for an extended application use-life. Herein, PLA/WF is explored as a feedstock material for large format additive manufacturing (LFAM) and the performance of additively manufactured materials is compared to those produced via more traditional processing methods. It is also demonstrated that the addition of WF decreases the material’s coefficient of thermal expansion (CTE) while increasing its Young’s modulus, susceptibility to water uptake, and creep fatigue resistance. Essentially, the addition of 20 wt% WF results in a 92 % decrease in rubbery regime CTE while simultaneously resulting in a 14 % increase in modulus, 190 % increase in water uptake, and a 31 % decrease in residual strain after cyclic creep tests. The processing method was also found to play a large role in the final part performance, with the printed material increasing the crystallinity by 183 % and 214 % compared to its compression and injection molded counterparts. Furthermore, the porosity of printed samples increased by two orders of magnitude compared to samples prepared via traditional processing methods.

36 MATERIALS SCIENCE↗

A novel peridynamics-based approach to predict pharmaceutical tablet robustness

The pharmaceutical drug product development process can be greatly accelerated through the use of modeling and simulation techniques to predict the manufacturability and performance of a given formulation. The anticipation and possible mitigation of tablet damage due to manufacturing stresses represents a specific area of interest in the pharmaceutical industry for predicting formulation and tableting performance. While the finite element method (FEM) has been extensively used for predicting the mechanical behavior of powder material in the compaction processes, a shortcoming of the approach is the inherent difficulty to predict discontinuities (e.g., damage or cracking) within a tablet as FEM is a continuum-based approach. In this work, we propose a novel method utilizing peridynamics (PD), a numerical method that can capture discontinuities such as tablet fracture, to predict the evolution of damage and breakage in pharmaceutical tablets. The approach links (1) the finite element method – to elucidate the behavior of powders during die compaction – with (2) the peridynamics modeling technique – to model the discontinuous nature of damage and predict tablet breakage during the critical stages of unloading and ejection from the compression die. This short communication presents a proof of concept including a workflow to calibrate the linked FEM-PD simulation models. Further, it demonstrates promising results from a preliminary experimental validation of the approach. Following further development, this approach could be used to guide the optimization of compression processes through targeted changes to formulation material properties, compression process conditions, and/or tooling geometries to deliver improved process efficiency and tablet robustness.

36 MATERIALS SCIENCE↗

Application of Raman Spectroscopy to Determine Uranium Content in ADUN Solution

The work presented in this report is part of the ongoing efforts to address the nuclear material control and accounting needs for advanced reactor fuel fabrication facilities. This work was supported by the Materials Protection, Accounting, and Control Technologies (MPACT) program under the US Department of Energy Office of Nuclear Energy‘s Nuclear Fuel Cycle and Supply Chain program. The activities and engagements under the MPACT program are designed to support a robust US civilian nuclear energy enterprise. In the work described in this report, we supported MPACT objectives by developing measurement techniques that could be used for material accounting and process monitoring and by working with industry partners to identify existing gaps and areas for improvement. Oak Ridge National Laboratory has been working with commercial tristructural isotropic (TRISO) fuel fabricators such as Standard Nuclear to develop technology for rapid and cost-effective uranium content assessment. This work has focused on demonstrating advanced measurement techniques (e.g., Raman spectroscopy) that can be used for rapid, reliable, and cost-effective routine measurements of uranium content in feed solutions and liquid waste streams as well as for monitoring in-line process measurements and product streams. Specifically, this report explores techniques for accurately determining uranium content in acid-deficient uranyl nitrate (ADUN) solutions and detecting low uranium concentrations in ammonia solutions. Developing such measurement techniques will benefit TRISO fuel fabrication facilities, facilities involved in other parts of the fuel cycle that require online monitoring of aqueous solutions, and potentially molten salt fuel reactors. This work supports developing Raman spectroscopy procedures to determine uranium concentrations in ADUN solutions, which are used as feedstock in the sol–gel process for creating TRISO fuel. Some additional benefits of using Raman spectroscopy for uranium quantification in fabrication facilities include enabling online monitoring of the chemical process, which would provide near real-time feedback; eliminating the need for sample transfers, preparation, or dilution; providing nondestructive measurements; and user friendliness. In this fiscal year, FY25, we determined the identity of the unknown Raman band at approximately 853 cm−1 that was discovered in ADUN Raman spectra in FY24, created calibration curves and determined uranium concentrations of two ADUN solutions, and compared the Raman results to results obtained from inductively coupled plasma mass spectrometry and Davies–Gray titration. Furthermore, we have identified focus areas for experimentation in future fiscal years. A key result is that the accuracy of using Raman can provide accuracy comparable to destructive analysist techniques, With a well-developed calibration curve, using standards and a large number of samples (more than five samples), uncertainty on the order of 1%–3% is achievable. Given that the uncertainties achieved by Raman spectroscopy were on the order of the uncertainties achieved using ICP-MS, we conclude that with a well-developed procedure Raman spectroscopy can be used to determine uranium concentrations in ADUN solutions for NMC&A applications. The benefits of such an approach are that the time and effort will be less than that of comparable destructive analysis techniques, with approximately the same level of technical expertise. This will be attractive to operators of fuel fabrication facilities as it will lower costs and improve efficiencies.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Transforming Public Housing with Deep Energy Retrofits

Open Market ESCO’s (OME) Transforming Public Housing through Deep Energy Retrofits project demonstrated new design and financing solutions for implementing deep energy retrofits (DERs) in occupied low-income multifamily housing. The Project performed an integrated project delivery process, including designing low-carbon retrofit solution packages, construction pricing, and financing. The Project developed a constructible and financeable DER scope for a 102-unit extremely low-income multifamily property in Boston. This Project demonstrated a replicable approach for streamlining and implementing DER projects in occupied housing, including real solutions for overcoming design complexities and cost barriers.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Advanced Fuels Campaign Execution Plan

The Advanced Fuels Campaign (AFC) Execution Plan details the strategy, mission, scope, and goals—both near-term and long-term—along with the structure and organization of nuclear fuels and materials research, development, and demonstration (RD&D) activities within the Fuel Cycle Technologies (FCT) program. The FCT program, tasked by the U.S. Department of Energy (DOE), employs a science-based approach to advance fuel technologies. This approach integrates theory, experiments, and multi-scale modeling and simulation (M&S) to develop a predictive understanding of fuel fabrication processes and fuel/cladding performance under irradiation, moving beyond traditional empirical methods. The long-term goals of the AFC are guided by the AFC Strategic Plan and align with the DOE Office of Nuclear Energy (NE) Roadmap [1], which outlines a multi-decade vision for demonstrating and qualifying advanced fuel forms to support diverse fuel cycle options. Near-term goals focus on enhancing accident tolerant fuels (ATF) for Light Water Reactors (LWR), a significant challenge that demands balancing immediate objectives with ongoing progress toward advanced reactor missions. Accelerating the traditional fuel qualification process to meet ATF objectives is another critical challenge. A detailed set of 5-year goals, summarized below, has been developed in line with the overarching science-based fuel development approach: • Advanced LWR Fuel Technologies: By 2027, support the development of advanced LWR fuel technologies with improved performance and enhanced accident tolerance. This includes high burnup (HBu), low enriched uranium (LEU)+, coated cladding, and doped fuel, aimed at complementing industry-led significant LWR uprates and plant refurbishments. • Tristructural Isotropic (TRISO) Fuel: Achieve qualification by 2028 and develop improved designs for emerging markets. • Metal Fuel: Achieve qualification by 2028 and develop improved designs for emerging markets. • Molten Salt Fuel: By 2027, deploy a robust program that enables fuel salt qualification technologies needed to support fuel salt research and development (R&D), focusing on emergent needs to derisk fuel salt production and utilization in advanced reactors. • Long-Term ATF: Develop fuel technologies that enable significant power uprates (~50%) in refurbished or new LWRs while optimizing fissile material utilization and waste disposal. The 5-year milestones in the AFC Execution Plan are contingent on an assumed budget. This Execution Plan will be updated annually to reflect actual funding profiles as budget guidance becomes available, ensuring milestones are adjusted accordingly. In summary, the AFC Execution Plan presents a comprehensive strategy to advance nuclear fuel technologies through a science-based approach, addressing both near-term and long-term goals while adapting to funding realities.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Real Time, In-line Monitoring of Hanford Tank Wastes - Year 1 Report

The team comprised of students, postdocs, early, mid and senior career scientists from Los Alamos National Laboratory, Savanah River National Laboratory, Georgia Tech and Florida International University, with the guidance of H2C, is developing a suite of in-line instruments for the Hanford high level waste (HLW) and low active waste (LAW) processes to provide near-real-time analysis of waste form physical properties and composition. The work builds on results from the recent DOE-ORP, EM Technology Development and other projects that demonstrated promise for the use of real-time in-line monitoring (RTIM) to measure chemical compositions of slurries of up to 20 weight % solids. The goal is for this instrument suite is to substantially reduce the need for sampling for process control. Sample waste, exposure associated with sample analysis, and the demand for an external laboratory facility would be greatly reduced. The throughput of waste treatment systems would be improved by elimination of the downtime caused by waiting for sample results. This translates into reduced process storage as process knowledge will be continuously updated in near-real-time. These breakthrough technologies would significantly reduce the life cycle cost and accelerate the schedule for the Hanford tank waste mission.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

A machine learning approach to determine the elastic properties of printed fiber-reinforced polymers

This work focuses on the simultaneous determination of the elastic constants and the fiber orientation state for a short fiber-reinforced polymer composite by performing a minimum of experimental tests. Here we introduce a methodology that enables the inverse determination of fiber orientation state and the in-situ polymer properties by performing tensile tests at the composite coupon level. We demonstrate the approach for the extrusion deposition additive manufacturing (EDAM) process to illustrate one application of the methodology, but the development is such that it can be applied to short fiber-reinforced polymer (SFRP) systems processed via other methods. Currently, developing composites additive manufacturing digital twins require extensive material characterization. In particular, the mechanical characterization of the orthotropic elastic properties of a composite involves extensive sample preparation and testing, therefore the elasticity tensor is generally populated using a micromechanics model. This, however, requires measuring the fiber orientation state in addition to knowing the constituent material properties. Experimentally measuring the fiber orientation state can be tedious and time consuming. Further, optical methods are limited to resolving the orientation of cylindrical fibers or cluster of non-cylindrical fibers, and computed tomography (CT) methods scan regions of volume that are much smaller than a full printed bead. Therefore, we propose a methodology, accelerated by machine learning, to identify the anisotropic mechanical properties and fiber orientation state at the same time. Early results show that inference of the fiber orientation and composite properties is possible with as few as three tensile tests. Our results show that a combination of the choice of the micromechanics model and reliable set of experiments can yield the nine elastic constants, as well as, the fiber orientation state.

36 MATERIALS SCIENCE↗

All-polymer organic solar cells with nano-to-micron hierarchical morphology and large light receiving angle

Distributed photovoltaics in living environment harvest the sunlight in different incident angles throughout the day. The development of planer solar cells with large light-receiving angle can reduce the requirements in installation form factor and is therefore urgently required. Here, thin film organic photovoltaics with nano-sized phase separation integrated in micro-sized surface topology is demonstrated as an ideal solution to proposed applications. All-polymer solar cells, by means of a newly developed sequential processing, show large magnitude hierarchical morphology with facilitated exciton-to-carrier conversion. The nano fibrilar donor-acceptor network and micron-scale optical field trapping structure in combination contributes to an efficiency of 19.06% (certified 18.59%), which is the highest value to date for all-polymer solar cells. Furthermore, the micron-sized surface topology also contributes to a large light-receiving angle. A 30% improvement of power gain is achieved for the hierarchical morphology comparing to the flat-morphology devices. These inspiring results show that all-polymer solar cell with hierarchical features are particularly suitable for the commercial applications of distributed photovoltaics due to its low installation requirement.

14 SOLAR ENERGY↗

Binary pseudo-random array standards for calibration of 3D optical surface profilers used for metrology with aspheric x-ray optics

High-accuracy surface metrology is vitally important in manufacturing ultra-high-quality free-form mirrors designed to manipulate x-ray light with nanometer-scale wavelengths. The current and potential capabilities of x˗ray mirror manufacturing are limited by inherent imperfections of the integrated metrology tools. Metrology tools are currently calibrated with super-polished flat test-standard/reference mirrors. This is acceptable for fabrication of slightly curved x-ray optics. However, for even moderately curved aspherical x-ray mirrors the flat-reference calibration is not sufficiently accurate. For micro-stitching interferometry developed for surface measurements with curved x-ray mirrors, the tool aberration errors are known to be transferred into the optical surface topography of x-ray mirrors. Our approach to improving metrology is to thoroughly calibrate the measuring tool and apply the results of the calibration to deconvolution of the measured data. Here we explore the application of a recently developed technique for calibrating the instrument transfer function (ITF) of 3D optical surface profilers to metrology with significantly curved x-ray optics. The technique, based on test standards patterned with two-dimensional (2D) binary pseudo-random arrays (BPRAs), employs the unique properties of the BPRA patterns in the spatial frequency domain. The inherent 2D power spectral density of the pattern has a deterministic white-noise-like character that allows direct determination of the ITF with uniform sensitivity over the entire spatial frequency range and field of view of an instrument. The high efficacy of the technique has been previously demonstrated in application to metrology with flat and slightly curved optics. Here, we concentrate on development of an efficient fabrication process for production of highly randomized (HR) BPRA test standards on flat and 500-mm spherical optical substrates. We also compare and discuss the results of the ITF calibration of an interferometric microscope when using the HR BPRA standards on flat and curved substrates.

Munechika, Keiko↗

Cryogenic C-band wavelength division multiplexing system using an AIM Photonics Foundry process design kit

Cryogenic environments make superconducting computing possible by reducing thermal noise, electrical resistance and heat dissipation. Heat generated by the electronics and thermal conductivity of electrical transmission lines to the outside world constitute two main sources of thermal load in such systems. As a result, higher data rates require additional transmission lines which come at an increasingly higher cooling power cost. Hybrid or monolithic integration of silicon photonics with the electronics can be the key to higher data rates and lower power costs in these systems. We present a 4-channel wavelength division multiplexing photonic integrated circuit (PIC) built from modulators in the AIM Photonics process development kit (PDK) that operate at 25 Gbps at room temperature and 10 Gbps at 40 K. We further demonstrate 2-channel operation for 20 Gbps aggregate data rate at 40 K using two different modulators/wavelengths, with the potential for higher aggregate bit rates by utilizing additional channels.

42 ENGINEERING↗

Performance Demonstration of Self-Powered Neutron Detectors for Steady-State Reactor Operations

The irradiation testing of sensors in reactors is a crucial step towards calibrating and qualifying sensors prior to their deployment in experiments. This report details the process toward qualifying and calibrating custom-designed rhodium-based self-power neutron detectors (Rh-SPNDs) for steady-state reactor irradiations. This process serves to both demonstrate the performance capabilities of Rh-SPNDs as well as to provide experimental data for development of a sensor sensitivity model. Two designs of Rh-SPNDs were tested in various reactors to demonstrate: detection resolution in a low neutron flux environment, a delayed-response compensation technique, output linearity in a large range of neutron flux, and measurement accuracy verified with dosimetry. The detection resolution and compensation technique was demonstrated in the AGN-201m reactor at Idaho State University. The irradiation confirmed the sensors’ capability to perform steady-state operations in a low neutron flux of ~2E8 n/cm 2 -sec. Sensor output linearity coupled with the delayed-response compensation was investigated at the neutron radiography reactor at Idaho National Laboratory. A Rh-SPND was irradiated to neutron fluxes ranging from 2E8 to 2E13 n/cm2-sec range. The measured data demonstrated a wide and linear range of operation with a measured linear sensitivity of 1.0129 ×10 -13 A/W with a correlation-squared value of r 2 =0.9927. The measurement accuracy was investigated at the Advanced Test Reactor Critical reactor. The SPNDs were inserted into a test vehicle with collocated flux wires. Two irradiations with different flux levels were performed, and the SPNDs relative measurement between the two irradiations was calculated to be 1.2613 ± 0.0153 for the small SPND design and 1.1809 ± 0.0108 for the large SPND design. Both SPND measurements fell between the co-axial dosimetry result, which reported 1.218 ± 0.047. Additionally, the preliminary MCNP model for calculating SPND sensitivity was developed in parallel to this work. Modeled neutron spectrum with measured magnitude was used for inputs to determine the simulated SPND output. The results showed an overestimation of signal strength by a factor of 5, which was expected because of model simplification. This leads to future modeling work to account for signal losses from additional physical properties, including high temperature environments for FY-21.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Thermochemical conversion of waste plastics with coal and biomass to generate value-added products

Co-gasification of waste plastic and waste coal/biomass in steam was investigated to evaluate the effects of operating conditions and low-cost catalyst compositions of coal ash on syngas production and tar mitigation. The results demonstrate the benefits of waste plastic conversion with coal or biomass. A better understanding of these processes will facilitate the development of more accurate kinetic models for industrial-scale chemical recycling.

co-gasification↗

Optimized Carbon Fiber Intermediate Development to Enable High-Volume Manufacturing of Lightweight Automotive Composites

The ongoing pursuit of improved fuel economy and reduced greenhouse gas emissions has resulted in sustained interest for lightweight materials technologies. In this context, carbon fiber composites have captured the imagination of automotive engineers due to the potential to achieve substantial mass reduction when compared to traditional steel construction. That stated, the use of carbon fiber composites in automotive has been limited for the most part to premium supercars and other derivative platforms. In these cases, manufacturing costs are less of an obstacle to implementation, and the performance benefits of carbon fiber have enabled production of structures offering more than 50% weight savings. In practice, translating these low-volume demonstrations onto high-volume vehicle platforms has remained challenging. This can be attributed to several factors, with the absence of suitable high throughput production methodologies being a key impediment. To date, structural, crash critical components have relied upon manufacturing techniques born out of the aerospace industry. This has created a disconnect between automotive production systems that are accustomed to manufacturing multiple parts per minute and the aerospace technologies that have cycle times in the order of hours. Consequently, the focus of this project is the development of manufacturing process technology for carbon fiber composites that can support a mainstream vehicle program at an assumed throughput of 100,000 vehicles per year. In practice, this translates to a part-to-part cycle time of less than 3 minutes. Project participation included contributions from a broad range of academic, industrial and national lab partners. The primary scope of work, being the development of new carbon fiber epoxy compounds that are stable at room temperature and suited to high throughput automated processing. For project management, the work streams were divided into six key areas, with the lead organization in parentheses. • Carbon fiber/epoxy materials formulation development and scale up (Dow) • Simulation of discontinuous near isotropic meso-structure intermediates (Purdue) • Simulation of mechanical performance of compression molded components (Purdue) • Meso-Scale morphological analysis and correlation with structural performance (UTK) • Paint and adhesion durability analysis (MSU) • Demonstrator part design, prototype production, and validation testing (Ford). The primary goal at the commencement of the project was development of a chopped carbon fiber sheet molding compound (SMC) that offered a three times improvement in tensile modulus over a comparable glass-based SMC. In addition to meeting mechanical performance targets, the resin kinetics were modified to achieve a processing cycle time of less than 3 minutes. Other critical-to-quality (CTQ) specifications were also stipulated to account for a broad range of materials and processing characteristics. To achieve the above, staff scientists at Dow Chemical created an extensive series of new epoxy blends for testing and validation. Throughout this development, a key challenge was attaining material performance goals without impacting processing behavior and paintability of finished components. The latter required a new internal mold release system being developed by Dow that was designed to complement the kinetics of the rapid cure epoxy. As a complement to work studies at the industrial partners, the teams from academia executed a series of analytical and experimental studies to investigate potential factors influencing CF-SMC performance. Unit cell models were developed to capture the meso-scale representations of the fiber matrix architecture. Results of this analysis and subsequent morphological investigations led to the design of a novel composite derivative comprising carbon fiber platelets embedded in an epoxy matrix; the platelet size and aspect ratio playing significant role in final composite properties. This approach was a departure from previous research in CF-SMC development whereby bulk filamentization or disassembly of the carbon fiber rovings had been considered the most effective means of achieving both fiber wet through and wet-out. As the course of the academia studies progressed, the aspect ratio of the fiber constituents was further optimized before finalizing material attributes and processing conditions. For the purposes of technology validation, the Ford team led a work stream devoted to the design, fabrication and testing of demonstration components. The carbon fiber SMC material has the potential to displace numerous stampings and castings on an automotive structure but ultimately vehicle closure applications were selected to showcase the abilities of the CF-SMC to achieve both mass reduction and business case for large complex structures. Using target properties established by the Dow staff scientists, the complete closure system for a full-size sedan decklid and a mid-size wagon liftgate were engineered. Prototypes for both applications were fabricated using production representative processing methods to allow for physical testing and performance validation of the CF-SMC structures. Following completion of a testing program that concluded with a FMVSS301 55 mph offset rear crash, the CF-SMC formulation was declared by the Ford team to have met all engineering requirements. To summarize, the joint development activities during this project led to significant technical breakthroughs and achievement of all milestones. The result was the development of a novel, tack-free carbon fiber molding compound that is suited to automated processing. This combined room temperature stability, fast cure kinetics, and internal mold release system facilitates cycle times that are conducive to high-volume production. The VORAFUSE M6400 successfully passed technology validation at Ford and is now eligible for consideration on future production commercial vehicle programs.

36 MATERIALS SCIENCE↗

Hydrogen Mitigation Process Testing at Nevada Solar One

The National Renewable Energy Laboratory (NREL) and Acciona Solar Power (ASP) developed and installed a process that addresses the issue of hydrogen buildup in Acciona's Nevada Solar One power plant. Our method selectively removes hydrogen from the expansion tanks of the power plant to control hydrogen levels in the circulating heat-transfer fluid (HTF). During previous work, we developed a sensor that measures hydrogen partial pressure in the expansion-tank headspace gas. We demonstrated that our sensor measures hydrogen levels over a wide range of partial pressure from 10 mbar down to 0.003 mbar. More recently, we conceived and developed an integrated process module that performs both hydrogen sensing and separating functions. The sensor/separator measures hydrogen partial pressure in the headspace gas in the same way as our original sensor design. Additionally, the integrated module separates hydrogen from the headspace gas to reduce hydrogen to the level needed to maintain the performance of receivers in the collector field. Laboratory testing at NREL showed that the sensor function had an accuracy of +/-7%, and the hydrogen extraction rate for separator function was consistent with our modeling predictions. The primary benefit of this module is its simple design, both in terms of function and incorporation into the HTF subsystem of the power plant. Most recently, NREL and ASP completed installation and initial testing of a mitigation process at ASP's Nevada Solar One power plant in Boulder City, Nevada. In this paper, we report on the completed installation, initial testing, and plans to bring the process to full automation, so that it can be operated unattended on a daily schedule.

chemical elements↗

Developing novel electrodes with ultralow catalyst loading for high-efficiency hydrogen production in proton exchange membrane electrolyzer cells

Hydrogen plays more crucial roles for decarbonizing the planets and meeting the climate challenges because of its high energy density and zero-emission. It can be produced with proton exchange membrane electrolyzer cells (PEMECs) driven by sustainable and renewable energy resources. Although PEMECs have a number of advantages, including high purity production, quick response, and the ability to operate at high pressure facilitating the gas delivering, their performance and cost greatly hinder their commercial-scale applications. To achieve high-efficiency and cost-reduced hydrogen production in PEMECs, we proposed thin engineered liquid/gas diffusion layers (LGDLs) and associated electrodes, i.e., catalyst-coated LGDLs (CCLGDLs), over conventional porous transport layers (PTLs) and catalyst-coated membranes (CCMs). The research approaches in this project are based on material synthesis, in-situ and ex-situ characterizations, component design and treatment, numerical modeling, and cost analysis. The thin and tunable LGDLs (TT-LGDLs) and CCLGDLs were successfully developed with great performance improvement as demonstrated in lab-scale, bench-scale, and system-scale electrolyzer tests. The electrode thickness was reduced from 370 µm to less than 100 µm with simplified fabrication processes. With the catalytically enhanced Ir-based catalyst coating, the as-developed CCLGDLs with a catalyst loading of 0.34 mg Ir /cm 2 achieved a cell performance of 1.77 V at 2 A cm -2 , exhibiting the catalyst mass activity enhanced by >20 times with significant catalyst saving over conventional catalyst cell design. In-situ PEMEC characterizations, including the current distribution mapping and high-speed and multiscale visualizations, were conducted for a deeper understanding of mass transport and electrochemical reactions within an electrolyzer with LGDLs and CCLGDLs. A 2D cell model was developed and validated for the enhanced performance on TT-LGDL through reducing ohmic losses due to nonuniform hydration and water transport. Further, the cost analysis results have shown a path to move beyond equivalency and surpass costs associated with the project baseline. In this project, the design and fabrication of TT-LGDLs and CCLGDLs will contribute to the performance enhancement, manufacturing simplification, and cost reduction for PEMECs and other energy conversion devices, thus shortening their pathways towards commercialization. This project also provides a good foundation for furthering the in-situ reaction interface research.

08 HYDROGEN↗

Cloud Radiative Effects on MJO Development in DYNAMO

Observed Madden-Julian Oscillation (MJO) events are examined with the aid of regional model simulations to understand the role of cloud radiative effects in the MJO development. The importance of this role is demonstrated by the absence of MJO in the model simulations that contain no cloud radiative effects. Comparisons of model simulations with and without the cloud radiative effects and observation help identify the major processes arising from those effects. Those processes develop essentially from heating in the upper-troposphere due to shortwave absorption within anvil clouds in the upper troposphere and the convergence of longwave radiation in the middle-upper troposphere, with a peak at 300-hPa, during deep convection. First, that heating adds extra buoyancy and accelerates the rising motion in the upper troposphere in deep convection. The vertical acceleration in the upper troposphere creates a vacuum effect and demands for more deep convection to develop. Second, in response to that demand and required by mass balance arises the large-scale horizontal and vertical mass, moisture, and energy convergence. It strengthens deep convection and, with the feedback from continuing cloud radiative effect, creates conditions that can perpetuate deep convection and MJO development. That perpetuation does not occur however because those processes arising from the cloud radiative heating in the upper troposphere stabilize the troposphere till it supports no further deep convection. Weakening deep convection reduces cloud radiative effects. The subsequent reduction of the vacuum effect in the upper troposphere diminishes deep convection completing an MJO cycle. These results advance our understanding of the development of the MJO in the radiative-convective system over warm waters in the tropics. They show that while the embryo of intraseasonal oscillation may exist in the system its growth/development is largely dependent on cloud radiative effects and feedbacks.

54 ENVIRONMENTAL SCIENCES↗

Microwave-assisted pyrolysis of hydrocarbons using iron-based alumina catalysts obtained via solution combustion synthesis

The demand for hydrogen is growing which makes the development of clean and efficient H2 synthesis technologies imperative. Microwave-assisted, thermocatalytic, dehydrogenation of hydrocarbons has demonstrated the ability to generate H2 with high yield and selectivity, leaving behind valuable solid carbon byproducts. However, this microwave-assisted process is unoptimized which prevents it from being utilized in industry. A critical component of optimization is the development of a catalyst that is catalytically active, a good microwave absorber, and can be regenerated for repeated dehydrogenation cycles. Previous studies that focused on plastic waste decomposition have used iron-based alumina (FeAlxOy) made via solution combustion synthesis (SCS). Unexplored is the effect of tuning SCS parameters on dehydrogenation performance, the use of these materials in hydrocarbon decomposition to H2, and the regeneration of these catalysts. This dissertation has three objectives: (1) characterize the relationship between SCS parameters and the material properties of FeAlxOy, (2) determine how differences in the material properties of FeAlxOy influence their performance as catalysts during microwave-assisted pyrolysis of fossil fuels, and (3) investigate the Boudouard reaction to regenerate the FeAlxOy post-dehydrogenation.

Chanoi, Zachary Aidan↗