Tritium Formation and Mitigation in High-Temperature Reactors

Tritium is a radiologically active isotope of hydrogen. It is formed in nuclear reactors by neutron absorption and ternary fission events and can subsequently escape into the environment. To prevent the tritium contamination of proposed reactor buildings and surrounding sites, this study examines the root causes and potential mitigation strategies for permeation of tritium (such as: materials selection, inert gas sparging, etc...). A model is presented that can be used to predict permeation rates of hydrogen through metallic alloys at temperatures from 450–750 degrees C. Results of the diffusion model are presented for a steady production of tritiu

Tritium Formation and Mitigation in High-Temperature Reactor Systems

Tritium is a radiologically active isotope of hydrogen. It is formed in nuclear reactors by neutron absorption and ternary fission events and can subsequently escape into the environment. To prevent the tritium contamination of proposed reactor buildings and surrounding sites, this study examines the root causes and potential mitigation strategies for permeation of tritium (such as: materials selection, inert gas sparging, etc...). A model is presented that can be used to predict permeation rates of hydrogen through metallic alloys at temperatures from 450–750 degrees C. Results of the diffusion model are presented for a steady production of tritiu

Hydrogen Production Performance of a 10-Cell Planar Solid-Oxide Electrolysis Stack

An experimental study is under way to assess the performance of solid-oxide cells operating in the steam electrolysis mode for hydrogen production over a temperature range of 800 to 900ºC. Results presented in this paper were obtained from a ten-cell planar electrolysis stack, with an active area of 64 cm2 per cell. The electrolysis cells are electrolytesupported, with scandia-stabilized zirconia electrolytes (~140 µm thick), nickel-cermet steam/hydrogen electrodes, and manganite air-side electrodes. The metallic interconnect plates are fabricated from ferritic stainless steel. The experiments were performed over a range of steam inlet mole fractions (0.1 - 0.6), gas flow rates (1000 - 4000 sccm), and current densities (0 to 0.38 A/cm2). Steam consumption rates associated with electrolysis were measured directly using inlet and outlet dewpoint instrumentation. Cell operating potentials and cell current were varied using a programmable power supply. Hydrogen production rates up to 100 Normal liters per hour were demonstrated. Values of area-specific resistance and stack internal temperatures are presented as a function of current density. Stack performance is shown to be dependent on inlet steam flow rate

Three-Dimensional Computational Fluid Dynamics Modeling of Solid Oxide Electrolysis Cells and Stacks

A three-dimensional computational fluid dynamics (CFD) electrochemical model has been created for detailed analysis of a high-temperature electrolysis stack (solid oxide fuel cells operated as electrolyzers). Inlet and outlet plenum flow distributions are discussed. Maldistribution of plena flow show deviations in per-cell operating conditions due to non-uniformity of species concentrations. Models have also been created to simulate experimental conditions and for code validation. Comparisons between model predictions and experimental results are discussed. Mass, momentum, energy, and species conservation and transport are provided via the core features of the commercial CFD code FLUENT. A solid-oxide fuel cell (SOFC) model adds the electrochemical reactions and loss mechanisms and computation of the electric field throughout the cell. The FLUENT SOFC user-defined subroutine was modified for this work to allow for operation in the electrolysis mode. Model results provide detailed profiles of temperature, Nernst potential, operating potential, activation over-potential, anode-side gas composition, cathode-side gas composition, current density and hydrogen production over a range of stack operating conditions. Variations in flow distribution, and species concentration are discussed. End effects of flow and per-cell voltage are also considered. Predicted mean outlet hydrogen and steam concentrations vary linearly with current density, as expected. Contour plots of local electrolyte temperature, current density, and Nernst potential indicate the effects of heat transfer, reaction cooling/heating, and change in local gas composition

Test Plan for Long-Term Operation of a Ten-Cell High Temperature Electrolysis Stack

This document defines a test plan for a long-term (2500 Hour) test of a ten-cell high-temperature electrolysis stack to be performed at INL during FY09 under the Nuclear Hydrogen Initiative. This test was originally planned for FY08, but was removed from our work scope as a result of the severe budget cuts in the FY08 NHI Program. The purpose of this test is to evaluate stack performance degradation over a relatively long time period and to attempt to identify some of the degradation mechanisms via post-test examination. This test will be performed using a planar ten-cell Ceramatec stack, with each cell having dimensions of 10 cm × 10 cm. The specific makeup of the stack will be based on the results of a series of shorter duration ten-cell stack tests being performed during FY08, funded by NGNP. This series of tests was aimed at evaluating stack performance with different interconnect materials and coatings and with or without brazed edge rails. The best performing stack from the FY08 series, in which five different interconnect/coating/edge rail combinations were tested, will be selected for the FY09 long-term test described herein

HT2005-72565 THERMAL AND ELECTROCHEMICAL THREE DIMENSIONAL CFD MODEL OF A PLANAR SOLID OXIDE ELECTROLYSIS CELL

ABSTRACT A three-dimensional computational fluid dynamics (CFD) model has been created to model high-temperature steam electrolysis in a planar solid oxide electrolysis cell (SOEC). The model represents a single cell, as it would exist in an electrolysis stack. Details of the model geometry are specific to a stack that was fabricated by Ceramatec 1 , Inc. and tested at the Idaho National Laboratory. Mass, momentum, energy, and species conservation and transport are provided via the core features of the commercial CFD code FLUENT 2 . A solid-oxide fuel cell (SOFC) model adds the electrochemical reactions and loss mechanisms and computation of the electric field throughout the cell. The FLUENT SOFC user-defined subroutine was modified for this work to allow for operation in the SOEC mode. Model results provide detailed profiles of temperature, Nernst potential, operating potential, anode-side gas composition, cathode-side gas composition, current density and hydrogen production over a range of stack operating conditions. Mean model results are shown to compare favorably with experimental results obtained from an actual ten-cell stack tested at INL

SYNGAS PRODUCTION VIA HIGH-TEMPERATURE CO-ELECTROLYSIS OF STEAM AND CARBON DIOXIDE IN A SOLID-OXIDE STACK

This paper presents results of recent experiments conducted at the INL studying coelectrolysis of steam and carbon dioxide in a 10-cell high-temperature solid-oxide electrolysis stack. Coelectrolysis is complicated by the fact that the reverse shift reaction occurs concurrently with the electrolytic reduction reactions. All reactions must be properly accounted for when evaluating results. Electrochemical performance of the stack was evaluated over a range of temperatures, compositions, and flow rates. The apparatus used for these tests is heavily instrumented, with precision mass-flow controllers, on-line dewpoint and CO2 sensors, and numerous pressure and temperature measurement stations. It also includes a gas chromatograph for analyzing outlet gas compositions. Comparisons of measured compositions to predictions obtained from a chemical equilibrium co-electrolysis model are presented, along with corresponding polarization curves. Results indicate excellent agreement between predicted and measured outlet compositions. Coelectrolysis significantly increases the yield of syngas over the reverse water gas shift reaction equilibrium composition. The process appears to be a promising technique for large-scale syngas production

Progress In High Temperature Electrolysis At The Idaho National Laboratory

The United States is considering the development of a domestic hydrogen-based energy economy. Hydrogen is of particular interest as a secondary energy carrier because it has the potential to be storable, transportable, environmentally benign, and useful in many chemical processes. Obviously, before a hydrogen economy can be implemented, an efficient and environmentally friendly means for large scale hydrogen production must be identified, proven, and developed. Hydrogen is now produced primarily via steam reforming of methane. However, from a long-term perspective, methane reforming is not a viable process for large-scale production of hydrogen since such fossil fuel conversion processes consume non-renewable resources and emit greenhouse gases. The U. S. National Research Council has recommended the use of water-splitting technologies to produce hydrogen using energy derived from a nuclear reactor. For the past several years, the Idaho National Laboratory has been actively studying the use of solid oxide fuel cells in conjunction with nuclear power for large-scale, high-temperature, electrolytic hydrogen production

THERMAL AND ELECTROCHEMICAL THREE DIMENSIONAL CFD MODEL OF A PLANAR SOLID OXIDE ELECTROLYSIS CELL

A three-dimensional computational fluid dynamics (CFD) model has been created to model high-temperature steam electrolysis in a planar solid oxide electrolysis cell (SOEC). The model represents a single cell, as it would exist in an electrolysis stack. Details of the model geometry are specific to a stack that was fabricated by Ceramatec , Inc. and tested at the Idaho National Laboratory. Mass, momentum, energy, and species conservation and transport are provided via the core features of the commercial CFD code FLUENT2. A solid-oxide fuel cell (SOFC) model adds the electrochemical reactions and loss mechanisms and computation of the electric field throughout the cell. The FLUENT SOFC user-defined subroutine was modified for this work to allow for operation in the SOEC mode. Model results provide detailed profiles of temperature, Nernst potential, operating potential, anode-side gas composition, cathode-side gas composition, current density and hydrogen production over a range of stack operating conditions. Mean model results are shown to compare favorably with experimental results obtained from an actual ten-cell stack tested at INL

3D CFD Model of High Temperature H2O/CO2 Co-electrolysis

3D CFD Model of High Temperature H2O/CO2 Co-Electrolysis Grant Hawkes1, James O’Brien1, Carl Stoots1, Stephen Herring1 Joe Hartvigsen2 1 Idaho National Laboratory, Idaho Falls, Idaho, [email protected] 2 Ceramatec Inc, Salt Lake City, Utah INTRODUCTION A three-dimensional computational fluid dynamics (CFD) model has been created to model high temperature co-electrolysis of steam and carbon dioxide in a planar solid oxide electrolyzer (SOE) using solid oxide fuel cell technology. A research program is under way at the Idaho National Laboratory (INL) to simultaneously address the research and scale-up issues associated with the implementation of planar solid-oxide electrolysis cell technology for syn-gas production from CO2 and steam. Various runs have been performed under different run conditions to help assess the performance of the SOE. This paper presents CFD results of this model compared with experimental results. The Idaho National Laboratory (INL), in conjunction with Ceramatec Inc. (Salt Lake City, USA) has been researching for several years the use of solid-oxide fuel cell technology to electrolyze steam for large-scale nuclear-powered hydrogen production. Now, an experimental research project is underway at the INL to produce syngas by simultaneously electrolyzing at high-temperature steam and carbon dioxide (CO2) using solid oxide fuel cell technology. A strong interest exists in the large-scale production of syn-gas from CO2 and steam to be reformed into a usable transportation fuel. If biomass is used as the carbon source, the overall process is climate neutral. Consequently, there is a high level of interest in production of syn-gas from CO2 and steam electrolysis. With the price of oil currently around $60 / barrel, synthetically-derived hydrocarbon fuels (synfuels) have become economical. Synfuels are typically produced from syngas – hydrogen (H2) and carbon monoxide (CO) -- using the Fischer-Tropsch process, discovered by Germany before World War II. High-temperature nuclear reactors have the potential for substantially increasing the efficiency of syn-gas production from CO2 and water, with no consumption of fossil fuels, and no production of greenhouse gases. Thermal CO2-splitting and water splitting for syn-gas production can be accomplished via high-temperature electrolysis, using high-temperature nuclear process heat and electricity. A high-temperature advanced nuclear reactor coupled with a high-efficiency high-temperature electrolyzer could achieve a competitive thermal-to-syn-gas conversion efficiency of 45 to 55%