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Papers by Philip Schonewill

Aiche Journal, 2008

ABSTRACT The direct methanol fuel cell experiences performance decay at high current densities du... more ABSTRACT The direct methanol fuel cell experiences performance decay at high current densities due to mass transfer limitations. The dominant mass transfer limiting mechanism at high methanol/water feed rates and low methanol feed concentrations has been attributed to the slow diffusion of methanol through the porous diffusion layer of the anode. In this study, fluid oscillations were induced in the feed to the anode of a DMFC and significant performance improvements were observed at high current densities. It was found that the improvement in measured limiting current densities over steady flow operation was as large as twofold and the peak power density increased by as much as 30%. A model is presented which predicts the experimental values of limiting current density as a function of the Peclet number in the porous diffusion layer of the DMFC anode. © 2008 American Institute of Chemical Engineers AIChE J, 2008

CRC Press eBooks, Nov 15, 2019

Philip P. Schonewill Oscillatory flow has numerous interesting and useful applications, many of w... more Philip P. Schonewill Oscillatory flow has numerous interesting and useful applications, many of which take advantage of oscillatory flow's unique features. Two processes which benefit from oscillatory flow are investigated herein: the first, using oscillatory flow to enhance mass transport in a porous medium, and the second, developing separation strategies from the study of inertial migration of particles and bubbles in oscillatory flow. The effect of oscillatory flow on mass transport in a porous medium was studied both fundamentally, in a model porous medium, and specifically, in the direct methanol fuel cell (DMFC). In the limit where the oscillatory flow could be considered quasi-steady, it was found that the transverse diffusivity of a solute could A.

The Direct Feed Low-Activity Waste (DFLAW) process has been proposed to support early production ... more The Direct Feed Low-Activity Waste (DFLAW) process has been proposed to support early production of immobilized low-activity waste (ILAW). In the DFLAW process, Hanford tank waste supernatant is sent to the Low-Activity Waste Pretreatment System (LAWPS) for filtration and cesium removal. The resultant treated waste is delivered to the Hanford Tank Waste Treatment and Immobilization Plant (WTP) Low-Activity Waste (LAW) Vitrification Facility for immobilization. The conceptual design and ongoing technology maturation of the LAWPS facility are being conducted by Washington River Protection Solutions, LLC (WRPS), but the DFLAW process also necessitates interfaces between WRPS and Bechtel National, Inc. to deliver the treated LAW from the LAWPS facility to the WTP for vitrification. This report describes simulant development work that was conducted to support the technology maturation of the LAWPS facility. Desired simulant physical properties (density, viscosity, solids concentration, solids particle size), sodium concentrations, and general anion identifications were provided by WRPS. The simulant recipes, particularly a "nominal" 5.6M Na simulant, are intended to be tested at several scales, ranging from bench-scale (500 mL) to full-scale (upwards of 6,000 gallons). Each simulant formulation was selected to be chemically representative of the waste streams anticipated to be fed to the LAWPS system, and used the current version of the LAWPS waste specification as a formulation basis. After simulant development iterations, four simulants of varying sodium concentration (4.0M, 5.6M, 6.0M, and 8.0M) were prepared and characterized. The formulation basis, development testing, and final simulant recipes and characterization data for these four simulants are presented in this report. All of the simulants described in this report fall within the physical property target ranges specified for processing in the LAWPS, but they do not span the entire range of specified physical properties. Simulants that are bounding with respect to a particular physical property or result in specific processing performance would have to be adjusted from these recipes or developed separately.

This success criterion was met. Kinetics tests were performed with simulants with varying OH conc... more This success criterion was met. Kinetics tests were performed with simulants with varying OH concentrations using SRF resin in a column. It was found that the kinetics and Cs loading were not affected by OH concentration. 6) Provide Cs load performance data collected after the resin has been stored at variable temperatures including (>45°C) in 0.5 M HNO 3. This success criterion was met. Several samples of resin were placed in 0.5 M HNO 3 and held at 25°C, 45°C, or 55°C for 70 days. One set of samples was held at 25°C in de-ionized water (DIW) for 70 days as a control batch. Then each sample was removed and loaded with Cs in a batch contact at 25°C for 24 hours with periodic samples taken to assess the level of Cs loading. The results showed that the acid did not seem to affect the loading of the resin at 25°C. However, at 45°C the kinetics of the resin loading were significantly reduced with a lower overall loading and at 55°C the resin had completely disintegrated and was unable to be loaded for a comparison. vii Quality Requirements The PNNL Quality Assurance (QA) Program is based on the requirements defined in the U.S. Department of Energy Order 414.1D, Quality Assurance, and 10 CFR 830, Energy/Nuclear Safety Management, and Subpart A-Quality Assurance Requirements (a.k.a. the Quality Rule). PNNL has chosen to implement the following consensus standards in a graded approach:

The Direct Feed Low-Activity Waste (DFLAW) process has been proposed to support early production ... more The Direct Feed Low-Activity Waste (DFLAW) process has been proposed to support early production of immobilized low-activity waste (LAW) at the Hanford Site. The tank farm contractor Washington River Protection Solutions, LLC (WRPS) is developing the Tank-Side Cesium Removal (TSCR) system to accomplish the treatment objectives. The TSCR system is being designed and built by AVANTech, Inc. for WRPS and will use a filter to remove entrained solids in the LAW and will use columns of crystalline silicotitanate (CST) ion exchange media to remove 137 Cs.

The PNNL Quality Assurance (QA) program is based on requirements defined in DOE Order 414.1D, Qua... more The PNNL Quality Assurance (QA) program is based on requirements defined in DOE Order 414.1D, Quality Assurance, and Title 10 of the Code of Federal Regulations (CFR) Part 830, Energy/Nuclear Safety Management, and Subpart A-Quality Assurance Requirements (a.k.a., the Quality Rule). PNNL has chosen to implement the following consensus standards in a graded approach:

(PNNL) conducted a scoping study to investigate supplemental technologies for supplying vertical ... more (PNNL) conducted a scoping study to investigate supplemental technologies for supplying vertical fluid motion and enhanced mixing in Waste Treatment and Immobilization Plant (WTP) vessels designed for high solids processing. The study assumed that the pulse jet mixers adequately mix and shear the bottom portion of a vessel. Given that, the primary function of a supplemental technology should be to provide mixing and shearing in the upper region of a vessel. The objective of the study was to recommend a mixing technology and configuration that could be implemented in the 8-ft test vessel located at Mid-Columbia Engineering (MCE). Several mixing technologies, primarily airlift circulator (ALC) systems, were evaluated in the study, first by reviewing the available literature and then performing tests with a simple Newtonian simulant (water and glass beads). The experimental study was performed in a 90-in. diameter tank with a maximum liquid operating level of ~108 in. The initial testing evaluated the ability of ALC configurations to lift, transport, and distribute solid particles to near-surface locations in the test vessel. This testing established that ALCs generated significant liquid flows (several hundred gallons per minute) at air flow rates of 5 to 20 standard cubic feet per minute (scfm), and solid particles were readily transported up the riser tube at air flow rates as low as ~5 scfm. The principal outcome of the Newtonian testing was that candidate ALC systems were identified and recommended for testing in a non-Newtonian fluid. The candidate ALC system had the following features: a nominally 10-in. riser tube diameter, 5-ft riser tube length, positioned 5 in. off the tank floor, and an air distributor centrally located at the bottom of the riser tube (tube inlet). An alternative technology, a Geyser Hybrid Pump (GHP), was also identified as a possible candidate. Both of the recommended systems were confirmed to be capable of lifting and dispersing very large solid particles up to approximately 6 mm in size.

Industrial & Engineering Chemistry Research, Sep 15, 2011

Boehmite dissolution experiments were conducted at NaOH concentrations of 10 M and 12 M to determ... more Boehmite dissolution experiments were conducted at NaOH concentrations of 10 M and 12 M to determine whether the increased aluminum solubility at high hydroxide concentration would offset the increase in added sodium, leading to an overall decrease in the amount of sodium added during the boehmite dissolution process. A shrinking-core dissolution rate model that assumed reversible reaction was used to fit the test data. The resulting model accounted for the effects of temperature, hydroxide concentration, and dissolved aluminum concentration. The rate was found to be dependent on the 1.5 power of hydroxide molarity. When the dissolution rate model was used in simulations of batch boehmite dissolution, a concentration range of 7 to 9 M NaOH was found to minimize the mass of sodium needed to dissolve a given mass of aluminum, potentially reducing it by as much as two-thirds. The time required to dissolve the boehmite was also found to be decreased by using hydroxide concentrations greater than 10 M.

In an e-mail from Matthew Landon of WRPS to Philip Schonewill on May 9, 2016, PNNL was directed t... more In an e-mail from Matthew Landon of WRPS to Philip Schonewill on May 9, 2016, PNNL was directed to use 55 °C as the upper temperature limit for testing and this assumed a 12 hr duration for loss of flow.

The Waste Treatment and Immobilization Plant (WTP) at Hanford is being designed and built to pret... more The Waste Treatment and Immobilization Plant (WTP) at Hanford is being designed and built to pretreat and vitrify waste currently stored in underground tanks at Hanford. One of the postulated events in the hazard analysis for the WTP is a breach in process piping that produces a pressurized spray with small droplets that can be transported into ventilation systems. Literature correlations are currently used for estimating the generation rate and size distribution of aerosol droplets in postulated releases. These correlations, however, are based on results obtained from small engineered nozzles using Newtonian liquids that do not contain slurry particles and thus do not represent the fluids and breaches in the WTP. A test program was developed to measure the generation rate, and the release fraction which is the ratio of generation rate to spray flow rate, of droplets suspended in a test chamber and droplet size distribution from prototypic sprays. A novel test method was developed to allow measurement of sprays from small to large breaches and also includes the effect of aerosol generation from splatter when the spray impacts on walls. Results show that the release fraction decreases with increasing orifice area, though with a weaker dependence on orifice area than the currently-used correlation. A comparison of water sprays to slurry sprays with 8 to 20 wt% gibbsite or boehmite particles shows that the presence of slurry particles depresses the release fraction compared to water for droplets above 10 μm and increases the release fraction below this droplet size.

Industrial & Engineering Chemistry Research, Feb 8, 2023

Aiche Journal, 2008

ABSTRACT The direct methanol fuel cell experiences performance decay at high current densities du... more ABSTRACT The direct methanol fuel cell experiences performance decay at high current densities due to mass transfer limitations. The dominant mass transfer limiting mechanism at high methanol/water feed rates and low methanol feed concentrations has been attributed to the slow diffusion of methanol through the porous diffusion layer of the anode. In this study, fluid oscillations were induced in the feed to the anode of a DMFC and significant performance improvements were observed at high current densities. It was found that the improvement in measured limiting current densities over steady flow operation was as large as twofold and the peak power density increased by as much as 30%. A model is presented which predicts the experimental values of limiting current density as a function of the Peclet number in the porous diffusion layer of the DMFC anode. © 2008 American Institute of Chemical Engineers AIChE J, 2008

CRC Press eBooks, Nov 15, 2019

Philip P. Schonewill Oscillatory flow has numerous interesting and useful applications, many of w... more Philip P. Schonewill Oscillatory flow has numerous interesting and useful applications, many of which take advantage of oscillatory flow's unique features. Two processes which benefit from oscillatory flow are investigated herein: the first, using oscillatory flow to enhance mass transport in a porous medium, and the second, developing separation strategies from the study of inertial migration of particles and bubbles in oscillatory flow. The effect of oscillatory flow on mass transport in a porous medium was studied both fundamentally, in a model porous medium, and specifically, in the direct methanol fuel cell (DMFC). In the limit where the oscillatory flow could be considered quasi-steady, it was found that the transverse diffusivity of a solute could A.

The Direct Feed Low-Activity Waste (DFLAW) process has been proposed to support early production ... more The Direct Feed Low-Activity Waste (DFLAW) process has been proposed to support early production of immobilized low-activity waste (ILAW). In the DFLAW process, Hanford tank waste supernatant is sent to the Low-Activity Waste Pretreatment System (LAWPS) for filtration and cesium removal. The resultant treated waste is delivered to the Hanford Tank Waste Treatment and Immobilization Plant (WTP) Low-Activity Waste (LAW) Vitrification Facility for immobilization. The conceptual design and ongoing technology maturation of the LAWPS facility are being conducted by Washington River Protection Solutions, LLC (WRPS), but the DFLAW process also necessitates interfaces between WRPS and Bechtel National, Inc. to deliver the treated LAW from the LAWPS facility to the WTP for vitrification. This report describes simulant development work that was conducted to support the technology maturation of the LAWPS facility. Desired simulant physical properties (density, viscosity, solids concentration, solids particle size), sodium concentrations, and general anion identifications were provided by WRPS. The simulant recipes, particularly a "nominal" 5.6M Na simulant, are intended to be tested at several scales, ranging from bench-scale (500 mL) to full-scale (upwards of 6,000 gallons). Each simulant formulation was selected to be chemically representative of the waste streams anticipated to be fed to the LAWPS system, and used the current version of the LAWPS waste specification as a formulation basis. After simulant development iterations, four simulants of varying sodium concentration (4.0M, 5.6M, 6.0M, and 8.0M) were prepared and characterized. The formulation basis, development testing, and final simulant recipes and characterization data for these four simulants are presented in this report. All of the simulants described in this report fall within the physical property target ranges specified for processing in the LAWPS, but they do not span the entire range of specified physical properties. Simulants that are bounding with respect to a particular physical property or result in specific processing performance would have to be adjusted from these recipes or developed separately.

This success criterion was met. Kinetics tests were performed with simulants with varying OH conc... more This success criterion was met. Kinetics tests were performed with simulants with varying OH concentrations using SRF resin in a column. It was found that the kinetics and Cs loading were not affected by OH concentration. 6) Provide Cs load performance data collected after the resin has been stored at variable temperatures including (>45°C) in 0.5 M HNO 3. This success criterion was met. Several samples of resin were placed in 0.5 M HNO 3 and held at 25°C, 45°C, or 55°C for 70 days. One set of samples was held at 25°C in de-ionized water (DIW) for 70 days as a control batch. Then each sample was removed and loaded with Cs in a batch contact at 25°C for 24 hours with periodic samples taken to assess the level of Cs loading. The results showed that the acid did not seem to affect the loading of the resin at 25°C. However, at 45°C the kinetics of the resin loading were significantly reduced with a lower overall loading and at 55°C the resin had completely disintegrated and was unable to be loaded for a comparison. vii Quality Requirements The PNNL Quality Assurance (QA) Program is based on the requirements defined in the U.S. Department of Energy Order 414.1D, Quality Assurance, and 10 CFR 830, Energy/Nuclear Safety Management, and Subpart A-Quality Assurance Requirements (a.k.a. the Quality Rule). PNNL has chosen to implement the following consensus standards in a graded approach:

The Direct Feed Low-Activity Waste (DFLAW) process has been proposed to support early production ... more The Direct Feed Low-Activity Waste (DFLAW) process has been proposed to support early production of immobilized low-activity waste (LAW) at the Hanford Site. The tank farm contractor Washington River Protection Solutions, LLC (WRPS) is developing the Tank-Side Cesium Removal (TSCR) system to accomplish the treatment objectives. The TSCR system is being designed and built by AVANTech, Inc. for WRPS and will use a filter to remove entrained solids in the LAW and will use columns of crystalline silicotitanate (CST) ion exchange media to remove 137 Cs.

The PNNL Quality Assurance (QA) program is based on requirements defined in DOE Order 414.1D, Qua... more The PNNL Quality Assurance (QA) program is based on requirements defined in DOE Order 414.1D, Quality Assurance, and Title 10 of the Code of Federal Regulations (CFR) Part 830, Energy/Nuclear Safety Management, and Subpart A-Quality Assurance Requirements (a.k.a., the Quality Rule). PNNL has chosen to implement the following consensus standards in a graded approach:

(PNNL) conducted a scoping study to investigate supplemental technologies for supplying vertical ... more (PNNL) conducted a scoping study to investigate supplemental technologies for supplying vertical fluid motion and enhanced mixing in Waste Treatment and Immobilization Plant (WTP) vessels designed for high solids processing. The study assumed that the pulse jet mixers adequately mix and shear the bottom portion of a vessel. Given that, the primary function of a supplemental technology should be to provide mixing and shearing in the upper region of a vessel. The objective of the study was to recommend a mixing technology and configuration that could be implemented in the 8-ft test vessel located at Mid-Columbia Engineering (MCE). Several mixing technologies, primarily airlift circulator (ALC) systems, were evaluated in the study, first by reviewing the available literature and then performing tests with a simple Newtonian simulant (water and glass beads). The experimental study was performed in a 90-in. diameter tank with a maximum liquid operating level of ~108 in. The initial testing evaluated the ability of ALC configurations to lift, transport, and distribute solid particles to near-surface locations in the test vessel. This testing established that ALCs generated significant liquid flows (several hundred gallons per minute) at air flow rates of 5 to 20 standard cubic feet per minute (scfm), and solid particles were readily transported up the riser tube at air flow rates as low as ~5 scfm. The principal outcome of the Newtonian testing was that candidate ALC systems were identified and recommended for testing in a non-Newtonian fluid. The candidate ALC system had the following features: a nominally 10-in. riser tube diameter, 5-ft riser tube length, positioned 5 in. off the tank floor, and an air distributor centrally located at the bottom of the riser tube (tube inlet). An alternative technology, a Geyser Hybrid Pump (GHP), was also identified as a possible candidate. Both of the recommended systems were confirmed to be capable of lifting and dispersing very large solid particles up to approximately 6 mm in size.

Industrial & Engineering Chemistry Research, Sep 15, 2011

Boehmite dissolution experiments were conducted at NaOH concentrations of 10 M and 12 M to determ... more Boehmite dissolution experiments were conducted at NaOH concentrations of 10 M and 12 M to determine whether the increased aluminum solubility at high hydroxide concentration would offset the increase in added sodium, leading to an overall decrease in the amount of sodium added during the boehmite dissolution process. A shrinking-core dissolution rate model that assumed reversible reaction was used to fit the test data. The resulting model accounted for the effects of temperature, hydroxide concentration, and dissolved aluminum concentration. The rate was found to be dependent on the 1.5 power of hydroxide molarity. When the dissolution rate model was used in simulations of batch boehmite dissolution, a concentration range of 7 to 9 M NaOH was found to minimize the mass of sodium needed to dissolve a given mass of aluminum, potentially reducing it by as much as two-thirds. The time required to dissolve the boehmite was also found to be decreased by using hydroxide concentrations greater than 10 M.

In an e-mail from Matthew Landon of WRPS to Philip Schonewill on May 9, 2016, PNNL was directed t... more In an e-mail from Matthew Landon of WRPS to Philip Schonewill on May 9, 2016, PNNL was directed to use 55 °C as the upper temperature limit for testing and this assumed a 12 hr duration for loss of flow.

The Waste Treatment and Immobilization Plant (WTP) at Hanford is being designed and built to pret... more The Waste Treatment and Immobilization Plant (WTP) at Hanford is being designed and built to pretreat and vitrify waste currently stored in underground tanks at Hanford. One of the postulated events in the hazard analysis for the WTP is a breach in process piping that produces a pressurized spray with small droplets that can be transported into ventilation systems. Literature correlations are currently used for estimating the generation rate and size distribution of aerosol droplets in postulated releases. These correlations, however, are based on results obtained from small engineered nozzles using Newtonian liquids that do not contain slurry particles and thus do not represent the fluids and breaches in the WTP. A test program was developed to measure the generation rate, and the release fraction which is the ratio of generation rate to spray flow rate, of droplets suspended in a test chamber and droplet size distribution from prototypic sprays. A novel test method was developed to allow measurement of sprays from small to large breaches and also includes the effect of aerosol generation from splatter when the spray impacts on walls. Results show that the release fraction decreases with increasing orifice area, though with a weaker dependence on orifice area than the currently-used correlation. A comparison of water sprays to slurry sprays with 8 to 20 wt% gibbsite or boehmite particles shows that the presence of slurry particles depresses the release fraction compared to water for droplets above 10 μm and increases the release fraction below this droplet size.

Industrial & Engineering Chemistry Research, Feb 8, 2023