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Alumel Thermocouples for High-Temperature Gas-Cooled Reactor Applications

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Alumel Thermocouples for High-Temperature Gas-Cooled Reactor Applications cjl-* ;\ • . Tt LA-NUREG-6768-MS L Informal Report A Thermocouple Evaluation Model and Evaluation of Chromel-Alumel Thermocouples for High-Temperature Gas-Cooled Reactor Applications Issued: April 1977 I o s vA -a lamos scientific laboratory of the University of California LOS ALAMOS. NEW MEXICO 87545 / \ An AHitmative Action/Equal Opporlunily Employer UNITED STATES ENENCV RESEARCH AND DEVELOPMENT ADMINISTRATION CONTRACT W-74M-ENC. 1* or,;. This work was supported by the US Nuclear Regulatory Commission's Office of Nuclear Regulatory Research, Division of Reactor Safety Research. Primed in the United States of America. Available from National Technical lnfojmation Savice U.S- Department of Commerce 5285 Port Royal Road Springfield, VA 22161 Price: Printed Copy 54.50 Microfiche $3.00 NOTICE This report was prepared as an account of work sponsored by the United States Government. Neither the United States nor the United States Nuclear Regulatory Commission, nor tiny of their employees, nor any of their contractors, subcontractors, or their employees, makes any warranty, expiess oi implied, oi assumes any legal liability or responsibility fat the accuracy, completeness or usefulness of any information, apparatus, product or process disclosed, or represents that its use would not infringe privately owned rights. LA-NUREG-6768-MS Informal Report NRC-8 losvv/VcHamos icientlfic laboratory of the University of California LOS AlAMOS. N(W MEXICO B754S A Thermocouple Evaluation Model and Evaluation of Chromel-Alumel Thermocouples for High-Temperature Gas-Cooled Reactor Applications by 3ev. W. Washburn Manuscript completed: March 1977 Issued: April 1977 >.VP* Proparod lor the US Nuclear Regulatory Comminiun Offlco of Nuclear Regulatory Roiearch :v. Cf rms DDCAJ:. CONTENTS ABSTRACT 1 I. INTRODUCTION 1 II. MODEL 2 A. Discussion / B. Illustrations and Examples 8 III. METHOD FOR DETERMINING INHOMOGENEITIES 9 IV. FACTORS AFFECTING RELATIVE SEEBECK COEFFICIENTS 10 V. SPECIFIC FACTORS AFFECTING CHROMEL-ALUMEL PERFORMANCE 11 A. As-received Inhomogeneities 11 B. Short-Range Ordering 12 C. Short-Term and Reversible Effects 13 1. Cold Working 13 2. Heat Treatment 13 D. Non-Reversible Effects 14 1. Oxidation 16 2. Reduction 18 3. Irradiation 19 E. Factors Affecting Long-Term Performance 22 1. General Considerations for Chromel-Alumel 22 2. HTGR-Related Factors 26 F. Long-Term Stability 27 G. Insulation and Sheath 30 VII. EXPERIMENTAL DATA 32 A. Bare Elements 32 B. Sheathed Elements 33 C. Combined Disturbing Effects Including Irradiation 34 VIII. SUMMARY AND CONCLUSIONS 35 REFERENCES 38 iv List of Tables I. Irradiation-Induced Con.position Changes 20 II. Errors Introduced by Heat Treatments 33 List of Figures 1. Circuit model 43 Z. Temperature and emf distributions 43 3. Scanning gradient 44 4. Cumulative heat treatment, typical 90 Ni-iO Cr alloys 44 5. Effects of cold work 44 6. Heat treatment of bare Alumel in air 45 7a. Effect of chromium in Ni-Cr alloy on the deviation of thermo-emf from an arbitrary standard at 1273 K 45 7b. Effect of Cr in a Ni-Cr alloy (Tophel) on the thermo-emf 45 7c. Effect of Cr content on thermo-emf of Ni-Cr alloy vs Pt 45 7d. Effect of Cr content on thermo-emf of Ni-Cr alloys vs Pt 46 7e. Effect of Cr content on thermo-emf of Ni-Cr alloy 46 7f. Effect of Co on the emf change of Ni-/H alloy (WfaiJ 46 7g. Effect of Mn on the emf change of Ni-Al alloy (Nial) 46 7h. Effect of Si on the emf change of Ni-Al alloy (Nial) 47 7i. Effect of Al on the emf change of Ni-Al alloy (Nial) 47 8a. Cr concentration in the zone of solute depletion in Chromel after heating in air 47 8b. Comparison of calculated and measured values of thermo-emf drift in Ni-Cr alloy 47 9. Reaction equilibrium: relation between Pog and temperature 48 10. Changes in inc'xated temperature of 1.0-mm Chromel-Alumel thermocouples in protection tubes and exposed to rich exothermic gas at 1366 K. 48 11a. Chrome1, composition changes by transmutation 49 lib. Alumel composition changes by transmutation 49 12a. Change in Seebeck coefficient with Cr depletion in Ni-Cr alloy 49 12b. Change in Seebeck coefficient with solute depletion in Ni-Cr and Ni-Al alloys 50 12c. Change in Seebeck coefficient with Cr depletion 1n Ni-Cr alloy 50 13. Short-range ordering error in Chromel and standard Chromel- Alumel error limits 51 v List of Figures (cont) 11a. Change in thermo-emf with Cr depletion in Ni-Cr alloy 51 14b. EMF and teropHrature errors with Cr depletion in Ni-Cr alloy (10 wt* Cr initial concentration) 52 14c. Temperature measurement error for typical solute depletions in Chrome! (C) and Alumel (A) 52 15. Therao-emf errors for solute depletions and nuclear transmutations in Chromel (C) and Alumel (A) 53 16a. In situ calibration; correct method , 53 16b. In situ calibration; incorrect method 54 17. Observed errors for unprotected Chromel-Alumel thermocouples heated in air 54 18. Observed errors for sheathed Chromel-Alumel thermocouples 55 19. Temperature measurement errors for aluminum depletion in Alumel (A) and chromium depletion in Chromel (C) 55 20. Observed errors for irradiated Chromel-Alumel thermocouples 56 vi A THERMOCOUPLE EVALUATION MODEL AND EVALUATION OF CHROMEL-ALUMEL THERMOCOUPLES FOR HIGH- TEMPERATURE GAS-COOLED REACTOR APPLICATIONS by Bev. W. Washburn ABSTRACT Factors affecting the performance and reli• ability of thermocouples for temperature measure• ments in High-Tsmperature Gas-Cooled Reactors are investigated. A model of an Inhomogeneous thermo• couple, associated experimental technique, and a method of predicting measurement errors are de• scribed. Error drifts for Type K materials are predicted and compared with published stability measurements. I. INTRODUCTION The Los Alamos Scientific Laboratory is carrying out a broad program of research in High-Temperature Gas-Cooled Reactor (HTGR) safety under the direction of the Division of Reactor Safety Research of the U.S. Nuclear Regulatory Com• mission. A part of that program was the study of the suitability and reliability of thermocouples selected for reactor-safety-related temperature measurements. The program for satisfying this objective encompassed studies of the conductor materials, insulation, sheaths, assembly fabrication, quality control, reliabi• lity, and failure modes. This report primarily discusses factors relating to the performance and reliability of Type K conductor materials; however, some data on sheathed assemblies are also included. A model of a thermocouple with inhomogeneous conductors and an experimental technique for determining the model parameters are presented. Examples are given 1 to illustrate application of the model to the prediction of thermocouple measure• ment errors under service conditions. The Inadequacy of conventional thermo• couple calibration concepts applied to the quantitive Investigation and predic• tion of stability is discussed. The methods discussed in this report are general aid can be applied to other thermocouple investigation and application situations. II. MODEL. Classical laws relate specifically to linear homogeneous* conductors of dif• ferent materials connected in a continuous circuit. These laws relate the net generated emf, junction temperatures, and conductor materials. 2 3 Purely thermodynamic reasoning or the free electron theory of metals may be used to derive the following equation for the net emf generation of a thermo• couple, T2 T2 Enet=/ eldT + X e2dT« Ti M where e, and £- represent the absolute values of the emf1 s of the two metals. If the two materials each have one end at T, and one end at T,, r* Enet=i tei-'zW. Tl In general, thermocouples are found to exhibit a degree of nonrepeatability and in-service instabilities in their emf-temperature characteristics. These deviations from the Ideal performance are believed to result from inhomogenelties in the conductors. Experimental evidence indicates that inhomogenelties range from those present in as-received materials (some of which are fixed and likely to remain so) to those that are created by service conditions such as atmosphere, temperature, nuclear radiation, and time. *A homogeneous thermocouple is one In which each conductor Is homogeneous, in both chemical composition and physical condition, throughout Its length. 2 A model of the thermoelectric circuit must be developed in order to under• stand the performance of a nonldeal thermocouple in a working environment. Fig• ure 1 presents the elements of a thermocouple circuit that is compatible v.'ith the ideal circuit while also Including provision for perturbations 1n the ideal conductors. The difference voltage, Ae , generated in section n is related to the rela• tive Seebeck coefficient for the section and the temperature differential, iT , across the section by A s + As AT e„n = (* „n Jn „ n, and E = e = s + As AT (i) n *=/ n * = / n n' n N N = £ S-AT„ V £ AS„AT„ • n = 1 n = 1 If conductors A and B are connected at 0 to form a junction, eQ = 0. The rela• tive Seebeck coefficients, s, are determined by 5 = E E (la) A " B and (lb) s„ - (^ . 4«„ j where e. and e„ represent the absolute values of the thermal emf coefficients of the conductors A and B. 3 The emf contribution in each section is determined by the absolute thermal emf coefficient in each wire and the temperature difference across the section. Tn corresponds to the temperature of the nth isothermal line intersecting both conductors. The physical lengths of the sections may be variable and should be chosen compatible with the problem parameters and spatial resolution of the data being used.to construct the model. Only those portions of the conductors which are subjected to a temperature gradient need be included in a section, i.e., portions of conductors under isothermal conditions, throughout the analysis, may appear as a node between sections of the model.
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