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At least 577 records · Page 32

Surrogate Model Development of Spent Fuel Degradation for Repository Performance Assessment

In model simulations of deep geologic repositories, UO 2 fuel matrix degradation typically begins as soon as the waste package breaches and groundwater contacts the fuel surface. The initial degradation rate depends on the timing of these events, burnup of the fuel, temperature, and concentrations of dissolved reactants. Estimating the initial rate of degradation is fairly straightforward, but as UO 2 corrosion products precipitate on the fuel surface and the movement of dissolved species between the fuel surface and environment is impeded by the precipitated solids, the rate is more difficult to quantify. At that point, calculating the degradation rate becomes a reactive-transport problem in which a large number of equations must be solved by iteration for a large number of grid cells at each time step. The consequence is that repository simulations, which are already expensive, become much more expensive, especially when hundreds or thousands of waste packages breach. The Fuel Matrix Degradation (FMD) model is the process model of the Spent Fuel and Waste Science and Technology (SFWST) campaign of the US Department of Energy (DOE). It calculates spent fuel degradation rates as a function of radiolysis, redox reactions, electrochemical reactions, alteration layer growth, and diffusion of reactants through the alteration layer. Like other similar fuel degradation process models, it is a complicated model requiring a large number of calculations and iterations at each time step.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Iron Porphyrins Embedded into a Supramolecular Porous Organic Cage for Electrochemical CO 2 Reduction in Water

Here, a porous organic cage composed of six iron tetraphenylporphyrins was used as a supramolecular catalyst for electrochemical CO 2 -to-CO conversion. This strategy enhances active site exposure and substrate diffusion relative to the monomeric catalyst, resulting in CO generation with near-quantitative Faradaic efficiency in pH 7.3 water, with activities reaching 55 250 turnovers. These results provide a starting point for the design of supramolecular catalysts that can exploit the properties of the surrounding matrix yet retain the tunability of the original molecular unit.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

SiO2-TiO2 doped with Er3+/Yb3+/Eu3+ photoluminescent material: A spectroscopy and structural study about potential application for improvement of the efficiency on solar cells

Highlights: • Intense downconversion emission of Eu{sup 3+} under Uv excitation. • Upconversion emission assigned to the Er{sup 3+}/Yb{sup 3+} under 980 laser pump. • Double excitation simultaneous providing emission in visible range. • Potential application on improvement of solar cells. - Abstract: The various synthesis conditions to obtain a material based on SiO{sub 2}-TiO{sub 2} co-doped with Er{sup 3+}/Yb{sup 3+}/Eu{sup 3+} were investigated, searching for those that present the greatest potential to improve the efficiency of solar cells. Conditions adjusted included heat-treatment temperatures, concentrations of matrix, and concentrations of dopants. Raman spectroscopy results demonstrated the effect of the annealing temperatures on the TiO{sub 2} phase transition and the crystalline phase of the materials, which interfere with the photoluminescence of the materials. The band gap of the materials was evaluated by diffuse reflectance and it decreased due to the doping. The materials were able to absorb UV and IR energy and emit in the visible region, verified by the down conversion, up conversion and the double excitation of the materials. The results showed that the materials may be used as a strategy to use a greater portion of the solar spectrum, improving solar cell efficiency.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Extraordinary role of Hg in enhancing the thermoelectric performance of p-type SnTe

We report several synergistic effects in Hg alloying of SnTe to enhance the power factor and overall figure of merit ZT. Hg alloying decreases the energy separation between the two valence bands, leading to pronounced band convergence that improves the Seebeck coefficient. Hg alloying of SnTe also significantly enlarges the band gap thereby effectively suppressing the bipolar diffusion. Collectively, this results in high ZT of similar to 1.35 at 910 K for 2% Bi-doped SnTe with 3% HgTe. The solubility limit of Hg in SnTe is less than 3 mol%, and above this level we observe HgTe precipitates in the SnTe matrix, typically trapped at grain boundary triple junctions. The strong point defect scattering of phonons caused by Hg alloying coupled with mesoscale scattering via grain boundaries contributes to a great reduction of lattice thermal conductivity. The multiple synergistic roles that Hg plays in regulating the electron and phonon transport in SnTe provide important new insights into continued optimization of SnTe-based and related materials.

Tan, Gangjian↗

Controlled release of entrapped nanoparticles from thermoresponsive hydrogels with tunable network characteristics

Thermoresponsive hydrogels have been studied intensively for creating smart drug carriers and controlled drug delivery. Understanding the drug release kinetics and corresponding transport mechanisms of nanoparticles (NPs) in a thermoresponsive hydrogel network is the key to the successful design of smart drug delivery systems. Here, we construct a mesoscopic model of rigid NPs entrapped in a hydrogel network in an aqueous solution, where the hydrogel network is formed by cross-linked semiflexible polymers of thermoresponsive poly(N-isopropylacrylamide) (PNIPAM). By varying the temperature crossing the lower critical solution temperature of PNIPAM, we can significantly change the hydrogel network characteristics. We systematically investigate how the matrix porosity and the nanoparticle size affect the transport kinetics of NPs at different temperatures. Quantitative results on the mean-squared displacement and the van Hove displacement distributions of NPs show that all NPs entrapped in the smart hydrogels undergo subdiffusion at both low and high temperatures. For a coil state, the transport of NPs in the hydrogels can be enhanced by decreasing the matrix porosity of the polymer network and NPs' size. However, when the solution temperature is increased above the critical temperature, the hydrogel network collapses following the coil-to-globule transition, with the NPs tightly trapped in some local regions inside the hydrogels. Consequently, the NP diffusion coefficient can be reduced by two orders of magnitude, or the diffusion processes can even be completely stopped. These findings provide new insights for designing controlled drug release from stimuli-responsive hydrogels, including autonomously switch on/off drug release in response to physical and chemical stimuli.

42 ENGINEERING↗

Coarsening dynamics of ternary polymer solutions with mobility and viscosity contrasts

Using phase-field simulations, we investigate the bulk coarsening dynamics of ternary polymer solutions undergoing a glass transition for two models of phase separation: diffusion only and with hydrodynamics. The glass transition is incorporated in both models by imposing mobility and viscosity contrasts between the polymer-rich and polymer-poor phases of the evolving microstructure. For microstructures composed of polymer-poor clusters in a polymer-rich matrix, the mobility and viscosity contrasts significantly hinder coarsening, effectively leading to structural arrest. For microstructures composed of polymer-rich clusters in a polymer-poor matrix, the mobility and viscosity contrasts do not impede domain growth; rather, they change the transient concentration of the polymer-rich phase, altering the shape of the discrete domains. This effect introduces several complexities to the coarsening process, including percolation inversion of the polymer-rich and polymer-poor phases—a phenomenon normally attributed to viscoelastic phase separation.

Chemistry↗

Power-Law Entanglement and Hilbert Space Fragmentation in Nonreciprocal Quantum Circuits

Quantum circuits utilizing measurement to evolve a quantum wave function offer a new and rich playground to engineer unconventional entanglement dynamics. Here, in this work, we introduce a hybrid, nonreciprocal setup featuring a quantum circuit, whose updates are conditioned on the state of a classical dynamical agent. In our example the circuit is represented by a Majorana quantum chain controlled by a classical N-state Potts chain undergoing pair flips. The local orientation of the classical spins controls whether randomly drawn local measurements on the quantum chain are allowed or not. This imposes a dynamical kinetic constraint on the entanglement growth, described by the transfer matrix of an N-colored loop model. It yields an equivalent description of the circuit by an SU(N)-symmetric Temperley-Lieb Hamiltonian or by a kinetically constrained surface growth model for an N-component height field. For N = 2, we find a diffusive growth of the half-chain entanglement toward a stationary profile S(L) ~ L 1/2 for L sites. For N ≥ 3, the kinetic constraints impose Hilbert space fragmentation, yielding subdiffusive growth toward S(L) ~ L 0.57 . This showcases how the control by a classical dynamical agent can enrich the entanglement dynamics in quantum circuits, paving a route toward novel entanglement dynamics in nonreciprocal hybrid circuit architectures.

1-dimensional spin chains↗

Slides for MS&T2022: Carbon-Carbon Composites from 3D Printed Preforms Graphitized by Electric Field Assisted Sintering

Formation of Carbon-Carbon (C-C) composite materials requires putting a carbon fiber preform through a cycle of densification, carbonization, and graphitization. This cycle is then repeated until the desired properties are achieved. The graphitization phase is particularly energy demanding as it involves heating the components to in excess of 2000°C. In traditional furnaces this is also quite time consuming as typical heating rates are low, and the actual heat treatment may be limited by component dimensions, as heat is conducted throughout the part primarily by thermal diffusion. Joule heating by means of Electric Field Assisted Sintering (EFAS) systems enables high heating rates and causes the part to be heated from the inside, which eliminates the thermal diffusion time constraint. In our process, C-C composites are formed by pyrolyzation of 3D-printed carbon fiber preforms, vacuum infiltration of naphthalene based mesophase pitch, and carbonization. The part is then graphitized in the EFAS system. By this method graphitization of the composite matrix was achieved in less than an hour. A part density of greater than 1.6g/cc (up to 1.9g/cc demonstrated) was achieved after only two rounds of infiltration and a single graphitization. Overall the process took less than a week which is significantly faster than traditional methods. Optical microscopy and XRD results are discussed to elucidate the internal porosity and characterize the degree of graphitization. Testing was performed showing the impact on fiber direction to electrical and thermal properties of the final part.

36 MATERIALS SCIENCE↗

Development of FeCrAl-ODS steels for ATF cladding

As an enhanced accident tolerant fuel (ATF) for LWR at severe accident condition, FeCrAl-ODS ferritic steels have been developed, and their applicability is being studied under the Japanese MEXT program. Alloying design of FeCrAl-ODS ferritic steels has been conducted, focusing on effect of mutual interaction of Cr-Al on oxidation resistance and α'-embrittlement. Effects of co-addition of Zr and excessive oxygen have also been studied to improve high-temperature strength. The ring tensile test of the manufactured claddings showed that tensile strength increases by Zr-addition and Zr-added FeCrAl-ODS steels have the highest strength among the existed steels at entire temperature range from room temperature up to 1000 Celsius degrees. Although Zr-addition sometimes leads to growth of alumina scale by rapid inward diffusion of oxygen through zirconia inside alumina, oxidation rate of Zr-added FeCrAl-ODS steels was successfully reduced to the level of Zr-free specimen by controlling oxygen content to form Y{sub 2}Zr{sub 2}O{sub 7} inside ODS steel matrix. This finding makes possible to improve not only high-temperature strength but also steam oxidation resistance in the Zr-added FeCrAl-ODS steels. (authors)

36 MATERIALS SCIENCE↗

Hydrogen uptake in graphite matrix at high temperature

Tritium management is a critical challenge for the next generation of nuclear reactors, such as Fluoride Salt Cooled High Temperature Reactors (FHRs) and High Temperature Gas-cooled Reactors (HTGRs), due to the higher production rate (up to 10,000 times) than conventional Light Water Reactors (LWRs). Graphitic materials employed as moderator, reflector, and fuel pebbles offer a potential pathway for tritium recovery by serving as a sink for tritium. Prediction of uptake capacity under reactor relevant conditions remains a challenge due to a lack of low partial pressure data and significant inter-grade variability of graphite. This study addresses these gaps by providing a comprehensive characterization of hydrogen (as a tritium surrogate) uptake and release behavior in the A3-3 graphite matrix (GM) used in fuel pebbles. Uptake measurements are performed at reactor relevant temperatures of 600- 800 °C, 1-200 Torr hydrogen pressure, and 15-120 min equilibration time, followed by thermal desorption spectroscopy up to 1100 °C. Uptake experiments at different equilibration times demonstrate the role of kinetics in hydrogen uptake, which can be modeled as a diffusion-with-trapping process. In the thermodynamics limit, the Sips adsorption model is shown to capture the uptake in A3-3 GM well. Our campaign provides a set of new results for hydrogen uptake in A3-3, including limiting uptake capacity at 600 °C, apparent diffusion coefficient at 600 °C, and the first estimates of the FHR/HTGR relevant (600 °C, 20 Pa partial pressure) equilibrium uptake capacity and time to saturation. Desorption data highlights a new site for hydrogen uptake, not observed in nuclear graphite, which we attribute to the non-graphitized binder. Using the Kissinger method, we estimate activation energy for release from the desorption peaks, confirming the activation energy for release from the basal planes and providing the first estimate for the activation energy of release from the binder.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Identifying Suitable Front Contacts for High‐Efficiency Cd(Se,Te) Solar Cells on Space‐Qualified Cover Glass

Deployment of photovoltaics in space requires devices that combine high-efficiency, low areal mass, and resilience to harsh environments. Historically, high-efficiency multijunction III–V materials have dominated space power systems; however, their high cost and limited manufacturing throughput motivate the exploration of scalable alternatives. While CdTe-based thin-film photovoltaics offer an attractive option, their performance on non-conventional substrates can suffer from front contact instability under higher-temperature processing. Here, the role of front contact chemistry in limiting cell performance is investigated using CdTe-based devices fabricated on 150 μm thick Ceria-doped space-qualified 0214 Corning glass. A matrix of four transparent conducting oxides (TCOs: CTO, AZO, ITO, IZO) combined with two n-type emitters (MZO, IGO) reveals chemical stability at the front interface—rather than absorber composition alone—governs recombination losses, voltage deficits, and device reproducibility. Chemically stable front contact combinations suppress elemental diffusion and interfacial degradation, resulting in significantly improved carrier lifetimes and junction quality. These insights are validated through record-certified Cd(Se,Te) cell efficiencies of 18.4% under AM1.5G and 16.2% under AM0 illumination on ultra-thin glass. Beyond CdTe, this work provides a general framework for the rational selection of TCO/emitter interfaces in superstrate thin-film photovoltaics, including emerging technologies like metal halide perovskites, while enabling high-efficiency, lightweight photovoltaics for space applications.

14 SOLAR ENERGY↗

Collaborative or competitive phase transformation processes in an additively manufactured-maraging steel M300

Although retained austenite is present in minor amounts in as-built additively manufactured-maraging steels, its evolution during ageing is key to controlling the final microstructure. This study investigates the relationship between austenite reversion and precipitation evolution during ageing, particularly whether these processes compete or cooperate. Using Scanning/Transmission Electron Microscopy, Atom Probe Tomography and Thermo-Calc® PRISMA simulations, the presence and evolution of retained austenite, Ni 3 Ti and Fe 7 Mo 6 intermetallic phases was characterised across different ageing conditions. Experimental results revealed the presence of non-enriched austenite in the as-built condition. Nevertheless, with increasing ageing temperature, Ni and Mo segregation became evident. High-Resolution Transmission Electron Microscopy revealed that Ni 3 Ti precipitation primarily occurred within the martensitic matrix, while Fe 7 Mo 6 nucleated preferentially at the austenite-martensite interface. PRISMA simulations indicated early and rapid precipitation in solute-enriched areas (i.e., intercellular regions), with Ni 3 Ti forming prior to Fe 7 Mo 6 . Both experimental and simulation results suggested Ni diffusion controls retained austenite growth, while Ti and Mo drive Ni 3 Ti and Fe 7 Mo 6 precipitation, respectively. The evidence reported in this work supports a both collaborative and independent phase transformation mechanism, where austenite reversion and precipitation co-evolve.

42 ENGINEERING↗

Fundamental Study of Disposition and Release of Methane in a Shale Gas Reservoir

The recent boom in shale gas production through hydrofracturing has reshaped the energy production landscape in the United States. Wellbore production rates vary greatly among the wells within a single field and decline rapidly with time, thus bring up a serious concern with the sustainability of shale gas production. Shale gas production starts with creating a fracture network by injecting a pressurized fluid in a wellbore. The induced fractures are then held open by proppant particles. During production, gas releases from the mudstone matrix, migrates to nearby fractures, and ultimately reaches a production wellbore. Given the relatively high permeability of the induced fractures, gas release and migration in low-permeability shale matrix is likely to be a limiting step for long-term wellbore production. Therefore, a clear understanding of the underlying mechanisms of methane disposition and release in shale matrix is crucial for the development of new technologies to maximize gas production and recovery. Shale is a natural nanocomposite material with distinct characteristics of nanometer-scale pore sizes, extremely low permeability, high clay contents, significant amounts of organic carbon, and large spatial heterogeneities. Our work has shown that nanopore confinement plays an important role in methane disposition and release in shale matrix. Using molecular simulations, we show that methane release in nanoporous kerogen matrix is characterized by fast release of pressurized free gas (accounting for ~ 30 - 47% recovery) followed by slow release of adsorbed gas as the gas pressure decreases. The first stage is driven by the gas pressure gradient while the second stage is controlled by gas desorption and diffusion. The long-term production decline appears controlled by the second stage of gas release. We further show that diffusion of all methane in nanoporous kerogen behaves differently from the bulk phase, with much smaller diffusion coefficients. The MD simulations also indicate that a significant fraction (3 - 35%) of methane deposited in kerogen can potentially become trapped in isolated nanopores and thus not recoverable. We have successfully established experimental capabilities for measuring gas sorption and desorption on shale and model materials under a wide range of physical and chemical conditions. Both low and high pressure measurements show significant sorption of CH 4 and CO 2 onto clays, implying that methane adsorbed on clay minerals could contribute a significant portion of gas-in-place in an unconventional reservoir. We have also studied the potential impact of the interaction of shale with hydrofracking fluid on gas sorption. We have found that the CH 4 -CO 2 sorption capacity for the reacted sample is systematically lower (by a factor of ~2) than that for the unreacted (raw) sample. This difference in sorption capacity may result from a mineralogical or surface chemistry change of the shale sample induced by fluid-rock interaction. Our results shed a new light on mechanistic understanding gas release and production decline in unconventional reservoirs.

04 OIL SHALES AND TAR SANDS↗

Data-driven linear time advance operators for the acceleration of plasma physics simulation

In this study, we demonstrate the application of data-driven linear operator construction for time advance with a goal of accelerating plasma physics simulation. We apply dynamic mode decomposition (DMD) to data produced by the nonlinear SOLPS-ITER (Scrape-off Layer Plasma Simulator - International Thermonuclear Experimental Reactor) plasma boundary code suite in order to estimate a series of linear operators and monitor their predictive accuracy via online error analysis. We find that this approach defines when these dynamics can be represented by a sequence of approximate linear operators and is essential for providing consistent projections when compared to an unconstrained application. For linear diffusion and advection–diffusion fluid test problems, we construct and apply operators within explicit and implicit time advance schemes, demonstrating that stability can be robustly guaranteed in each case. We further investigate the use of the linear time advance operators within several integration methods including forward Euler, backward Euler, and the matrix exponential. The application of this method to simulation data from SOLPS-ITER, with varying levels of Markov chain Monte Carlo numerical noise, shows that constrained DMD operators yield a capability to identify, extract, and integrate a (slow) subset of the present timescales. Example applications show that for projected speedup factors of [Formula: see text], and [Formula: see text], a mean relative error of 3%, 5%, and 8% and maximum relative error less than 20% are achievable, which appears acceptable for typical SOLPS-ITER steady-state simulations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Signatures of QCD conductivities in heavy-ion collisions

Dissipative processes are pivotal for understanding the hydrodynamic evolution of hot and dense quantum chromodynamics (QCD) matter created in relativistic nuclear collisions. The interplay of multiple conserved charges—net baryon, strangeness, and electric charge—is of particular interest. Here, we simulate the longitudinal hydrodynamic evolution with the three diffusion currents in a hydrodynamic model with a lattice-QCD-based equation of state, NEOS -4 D , and estimate rapidity distributions including diffusive corrections to the phase-space distribution in the presence of multiple charges, which ensure charge conservation at particlization. We determine the response of particle yields at midrapidity to changes in the diagonal and off-diagonal conductivities. Inversely, we find that most components of the conductivity matrix can be constrained experimentally using identified particle multiplicities at different collision energies.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Coupled Gel/Seeded Growth of Cs2AgBiBr6 Single Crystals for Radiation Detection

Abstract— The all-inorganic lead free Cs2AgBiBr6 perovskite represents a highly promising environment-friendly radiation detector material. The first attempt to grow Cs2AgBiBr6 single crystals using the unique gel growth method is reported in this study. This technique enables controlled reagent diffusion in a gel medium at room temperature, fostering the growth of visible single crystals. It offers advantages over conventional methods, leading to fewer equilibrium and non-equilibrium defects and simplified execution. Interestingly, the as-grown crystals exhibited variations in size and colors within the gel matrix, indicating the influence of Bi solutes in Bi-poor and Bi-rich Cs2AgBiBr6 crystals. Once the crystals were confirmed by powder xray diffraction, a series of comprehensive material characterizations was performed. The resistivity of Cs2AgBiBr6 single crystals was measured at 1.12x107 Ω•cm. Trap density analysis yielded a value of 2.82 x1010 cm-3. The charge carrier mobility was determined to be 32.9 cm2V-1S-1, suggesting the suitability for radiation detector applications. Additional growth optimization is going on and further characterization will be reported during the presentation. Our work helps accelerate the development of lead-free perovskite materials toward radiation detector applications.

James, Ralph B.↗

Data Associated with "Identifying Suitable Front Contacts for High-Efficiency Cd(Se,Te) Solar Cells on Space-Qualified Cover Glass"

This is data associated with the publication " Identifying Suitable Front Contacts for High-Efficiency Cd(Se,Te) Solar Cells on Space-Qualified Cover Glass " by Aesha P. Patel, Ryan Muzzio, Matthew R. Young, Robert Morrissey, Suresh Chaulagain, B. Edward Sartor, Prabodika N. Kaluarachchi, Christian Velez, Joshua A. Brown, Joel N. Duenow, Stephen Glynn, Michael J. Heben, Zhaoning Song, Nikolas J. Podraza, Adam B. Phillips, Randy J. Ellingson, Matthew O. Reese. All data associated with each figure in the manuscript and supplementary should be available in this dataset. A readme file is also included to provide some guidance. Abstract: Deployment of photovoltaics in space requires devices that combine high-efficiency, low areal mass, and resilience to harsh environments. Historically, high-efficiency multijunction III–V materials have dominated space power systems; however, their high cost and limited manufacturing throughput motivate the exploration of scalable alternatives. While CdTe-based thin-film photovoltaics offer an attractive option, their performance on non-conventional substrates can suffer from front-contact instability under higher-temperature processing. Here, the role of front-contact chemistry in limiting cell performance is investigated using CdTe-based devices fabricated on 150 μm thick Ceria-doped space-qualified 0214 Corning glass. A matrix of four transparent conducting oxides (TCOs: CTO, AZO, ITO, IZO) combined with two n-type emitters (MZO, IGO) reveals chemical stability at the front interface—rather than absorber composition alone—governs recombination losses, voltage deficits, and device reproducibility. Chemically stable front-contact combinations suppress elemental diffusion and interfacial degradation, resulting in significantly improved carrier lifetimes and junction quality. These insights are validated through record-certified Cd(Se,Te) cell efficiencies of 18.4% under AM1.5G and 16.2% under AM0 illumination on ultra-thin glass. Beyond CdTe, this work provides a general framework for the rational selection of TCO/emitter interfaces in superstrate thin-film photovoltaics, including emerging technologies like metal halide perovskites, while enabling high-efficiency, lightweight photovoltaics for space applications.

14 SOLAR ENERGY↗

Beyond the effectiveness factor: Multi-step reactions with intraparticle diffusion limitations

Though common in many industrial chemical processes, multi-step reactions occurring within porous catalyst particles provide significant challenges to previously established modeling frameworks. In this work, a system of reaction-diffusion equations is solved analytically via eigenanalysis. The intraparticle concentration profiles are integrated over the particle volume to obtain effectiveness factors for each reacting species, referred to herein as a multi-step effectiveness vector (MEV). The MEV solution is tested for the case of uniform flow past a stationary catalyst particle with a state-of-the-art, multi-step reaction scheme for fluid catalytic cracking (FCC). Outputs from particle-resolved direct numerical simulation (DNS) are compared to outputs from ordinary differentials with effective reaction closures coming from the MEV solution, the classic single-step effectiveness factor (SEF) (R. Aris, 'The mathematical theory of diffusion and reaction in permeable catalysts: The theory of the steady state,' Oxford University Press, 1975), and utilizing the intrinsic rates as-is. When compared to DNS, the MEV solution shows excellent agreement for the formation of all species and quantitatively captures the intraparticle concentration profiles. By contrast, the intrinsic treatment shows an over-prediction for product formation and the SEF treatment shows mixed levels of accuracy that depend upon the reaction coupling. Specifically, the SEF treatment accurately characterizes product formation if the kinetic scheme is weakly coupled but shows significant departure if stronger coupling is present. The computational cost associated with the MEV solution is associated with eigendecomposition of the Thiele matrix, an N x N matrix where N is the number of reacting components. Overall, the method is shown to be relatively easy to implement and may significantly enhance the fidelity of chemical reactor simulations that employ multi-step reaction schemes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗