CARBON FILTRATION FOR REDUCING EMISSIONS FROM CHEMICAL AGENT INCINERATION

Committee on Review and Evaluation of the Army Chemical Stockpile Disposal Program

Board on Army Science and Technology

Commission on Engineering and Technical Systems

National Research Council

National Academy Press
Washington, D.C.



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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration CARBON FILTRATION FOR REDUCING EMISSIONS FROM CHEMICAL AGENT INCINERATION Committee on Review and Evaluation of the Army Chemical Stockpile Disposal Program Board on Army Science and Technology Commission on Engineering and Technical Systems National Research Council National Academy Press Washington, D.C.

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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration NATIONAL ACADEMY PRESS 2101 Constitution Avenue, N.W. Washington, D.C. 20418 NOTICE: The project that is the subject of this report was approved by the Governing Board of the National Research Council, whose members are drawn from the councils of the National Academy of Sciences, the National Academy of Engineering, and the Institute of Medicine. The members of the committee responsible for the report were chosen for their special competencies and with regard for appropriate balance. The National Academy of Sciences is a private, nonprofit, self-perpetuating society of distinguished scholars engaged in scientific and engineering research, dedicated to the furtherance of science and technology and to their use for the general welfare. Upon the authority of the charter granted to it by the Congress in 1863, the Academy has a mandate that requires it to advise the federal government on scientific and technical matters. Dr. Bruce M. Alberts is president of the National Academy of Sciences. The National Academy of Engineering was established in 1964, under the charter of the National Academy of Sciences, as a parallel organization of outstanding engineers. It is autonomous in its administration and in the selection of its members, sharing with the National Academy of Sciences the responsibility for advising the federal government. The National Academy of Engineering also sponsors engineering programs aimed at meeting national needs, encourages education and research, and recognizes the superior achievements of engineers. Dr. William A. Wulf is president of the National Academy of Engineering. The Institute of Medicine was established in 1970 by the National Academy of Sciences to secure the services of eminent members of appropriate professions in the examination of policy matters pertaining to the health of the public. The Institute acts under the responsibility given to the National Academy of Sciences by its congressional charter to be an adviser to the federal government and, upon its own initiative, to identify issues of medical care, research, and education. Dr. Kenneth I. Shine is president of the Institute of Medicine. The National Research Council was organized by the National Academy of Sciences in 1916 to associate the broad community of science and technology with the Academy’s purposes of furthering knowledge and advising the federal government. Functioning in accordance with general policies determined by the Academy, the Council has become the principal operating agency of both the National Academy of Sciences and the National Academy of Engineering in providing services to the government, the public, and the scientific and engineering communities. The council is administered jointly by both Academies and the Institute of Medicine. Dr. Bruce M. Alberts and Dr. William A. Wulf are chairman and vice chairman, respectively, of the National Research Council. This is a report of work supported by Contract DAAD19-99-C-0010 between the U.S. Army and the National Academy of Sciences. Any opinions, findings, conclusions, or recommendations expressed in this publication are those of the author(s) and do not necessarily reflect the view of the organizations or agencies that provided support for the project. International Standard Book Number 0-309-06595-X Limited copies are available from: Board on Army Science and Technology National Research Council 2101 Constitution Avenue, N.W. Washington, D.C. 20418 (202) 334-3118 Additional copies of this report are available from: National Academy Press 2101 Constitution Avenue, N.W., Lockbox 285 Washington, D.C. 20055 (800) 624-6242 or (202) 334-3313 (in the Washington metropolitan area) http://www.nap.edu Copyright 1999 by the National Academy of Sciences. All rights reserved. Printed in the United States of America.

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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration COMMITTEE ON REVIEW AND EVALUATION OF THE ARMY CHEMICAL STOCKPILE DISPOSAL PROGRAM DAVID S. KOSSON, chair, Rutgers, The State University of New Jersey, New Brunswick CHARLES E. KOLB, vice chair, Aerodyne Research, Inc., Billerica, Massachusetts DAVID H. ARCHER, Carnegie Mellon University, Pittsburgh, Pennsylvania PIERO M. ARMENANTE, New Jersey Institute of Technology, Newark DENNIS C. BLEY, Buttonwood Consulting, Inc., Oakton, Virginia FRANK P. CRIMI, Lockheed Martin (retired), Saratoga, California ELISABETH M. DRAKE, Massachusetts Institute of Technology, Cambridge (until 3/31/99) J. ROBERT GIBSON, DuPont Agricultural Products, Wilmington, Delaware MICHAEL R. GREENBERG, Rutgers, The State University of New Jersey, New Brunswick KATHRYN E. KELLY, Delta Toxicology, Inc., Crystal Bay, Nevada RICHARD S. MAGEE, New Jersey Institute of Technology, Newark (until 1/27/99) JAMES F. MATHIS, Exxon Corporation (retired), Houston, Texas WALTER G. MAY, University of Illinois, Urbana ALVIN H. MUSHKATEL, Arizona State University, Tempe (until 3/31/99) H. GREGOR RIGO, Rigo & Rigo Associates, Inc., Berea, Ohio KOZO SAITO, University of Kentucky, Lexington ARNOLD F. STANCELL, Georgia Institute of Technology, Atlanta CHADWICK A. TOLMAN, National Science Foundation, Arlington, Virginia WILLIAM TUMAS, Los Alamos National Laboratory, Los Alamos, New Mexico Board on Army Science and Technology Liaison RICHARD A. CONWAY, Union Carbide Corporation, Charleston, West Virginia Staff DONALD L. SIEBENALER, Study Director HARRISON T. PANNELLA, Research Associate WILLIAM E. CAMPBELL, Senior Project Assistant

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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration BOARD ON ARMY SCIENCE AND TECHNOLOGY WILLIAM H. FORSTER, chair, Northrop Grumman Corporation, Baltimore, Maryland THOMAS L. MCNAUGHER, vice chair, RAND Corporation, Washington, D.C. RICHARD A. CONWAY, Union Carbide Corporation, Charleston, West Virginia GILBERT S. DECKER, Walt Disney Imagineering, Glendale, California LAWRENCE J. DELANEY, Delaney Group, Potomac, Maryland ROBERT J. HEASTON, Guidance and Control Information Analysis Center (retired), Naperville, Illinois ELVIN R. HEIBERG, III, Heiberg Associates, Inc., Mason Neck, Virginia GERALD J. IAFRATE, University of Notre Dame, Notre Dame, Indiana KATHRYN V. LOGAN, Georgia Institute of Technology, Atlanta JOHN H. MOXLEY, III, Korn/Ferry International, Los Angeles, California STEWART D. PERSONICK, Bell Communications Research, Inc., Morristown, New Jersey MILLARD F. ROSE, Auburn University, Auburn, Alabama GEORGE T. SINGLEY, III, Hicks & Associates, McLean, Virginia CLARENCE G. THORNTON, Army Research Laboratories (retired), Colts Neck, New Jersey JOHN D. VENABLES, Venables and Associates, Towson, Maryland JOSEPH J. VERVIER, ENSCO, Inc., Melbourne, Florida ALLEN C. WARD, Ward Synthesis, Inc., Ann Arbor, Michigan Staff BRUCE A. BRAUN, Director MICHAEL A. CLARKE, Associate Director MARGO L. FRANCESCO, Administrative Associate ALVERA G. WILSON, Financial Associate DEANNA P. SPARGER, Senior Project Assistant

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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration Preface The United States has maintained a stockpile of highly toxic chemical agents and munitions for more than half a century. In 1985, Public Law 99-145 mandated an "expedited" effort to dispose of M55 rockets containing unitary chemical warfare agents because of their unlikely, but plausible, potential for self-ignition. This program soon expanded into the Army Chemical Stockpile Disposal Program (CSDP), the mission of which is to eliminate the entire stockpile of unitary chemical agents and munitions. The current baseline incineration system was developed to carry out this mission. Since 1987, the National Research Council (NRC), through its Committee on Review and Evaluation of the Army Chemical Stockpile Disposal Program (Stockpile Committee), has overseen the Army's disposal program and has endorsed the baseline incineration system for destroying the stockpile. In 1992, after setting several intermediate goals and dates, Congress enacted Public Law 102-484, which directed the Army to dispose of the entire stockpile of unitary chemical agents and munitions by December 31, 2004. As a result of the subsequent implementation, on April 29, 1997, of the international Chemical Weapons Convention, which the United States has ratified, the date has been reset to April 29, 2007. Incineration processes raise concerns about potentially harmful emissions. Many people fear that substances in the exhaust gas could adversely affect their health and the environment, and some have remained resolutely opposed to the baseline incineration system. When properly operated, however, the incineration system with its pollution control devices releases mostly harmless products: carbon dioxide, water, and other completely oxidized products in their most stable state. However, incinerator emissions also contain small quantities of products of incomplete combustion and other trace contaminants, collectively known as substances of potential concern (SOPCs). For the CSDP, the presence of these SOPCs (and, potentially, trace quantities of chemical agents below the monitoring detection limits) have become matters of concern. At a workshop sponsored by the Stockpile Committee in 1991, the committee suggested that the Army evaluate a number of modifications to the pollution abatement systems (PASs) for cleaning the incinerator off-gases at sites in the continental United States. One of these technologies involved using activated carbon to adsorb SOPCs. At the time, this technology was already being routinely used at chemical processing plants for the separation and recovery of trace organic products, although it had not been used as an air pollution control system for incinerators in the United States. Hence, activated carbon filters were not included in the PAS at the first full-scale chemical agent disposal facility, the Johnston Atoll Chemical Agent Disposal System (JACADS), or at the Tooele Chemical Agent Disposal Facility (TOCDF). The Stockpile Committee described public concerns regarding emissions from the baseline incineration system in a 1992 letter report entitled, "Letter Report on Review of the Choice and Status of Incineration for Destruction of the Chemical Stockpile," and again in a February 1994 report, Recommendations for the Disposal of Chemical Agents and Munitions. The Stock-pile Committee found the baseline system to be adequate for the safe disposal of the stockpile but noted that adding activated carbon filter beds to polish all facility exhaust gases could further protect against emissions of chemical agent or trace organic materials,

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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration even in the unlikely event of a major upset. Consequently, the committee recommended that the use of activated charcoal beds to filter the discharge from baseline system incinerators be evaluated. The assessment was to include estimates of the magnitude and potential consequences of upsets and site-specific estimates of benefits and risks. If carbon filtration was found to have site-specific advantages, the committee recommended that the equipment be installed. This report reviews the Army's evaluation of carbon filters for use in the baseline incineration PAS, as well as the Army's change management process (the Army's tool for evaluating major equipment and operational changes to disposal facilities). In preparing this report, members of the Stockpile Committee evaluated exhaust gas emissions testing at the two operating baseline incineration systems, JACADS and the TOCDF; evaluated the development of the dilute SOPC carbon filter simulation model; and evaluated the conceptual design of a modified PAS with an activated carbon filter. The two major risk assessments conducted for each continental disposal site that use the baseline system, namely, (1) the quantitative risk assessment, which evaluates the risks and consequences of accidental agent releases, and (2) the health risk assessment, which evaluates the potential effects of nonagent emissions on human health and the environment, were also examined. In a 1997 NRC report, Risk Assessment and Management at Deseret Chemical Depot and the Tooele Chemical Agent Disposal Facility, the Stockpile Committee first reviewed carbon filters and included findings and recommendations concerning the addition of carbon filters to the baseline PAS. In the present report, the Stockpile Committee has evaluated continuing developments pertaining to these findings and recommendations. The committee greatly appreciates the support and assistance of NRC staff members, Donald L. Siebenaler, Harrison T. Pannella, William E. Campbell, Carol R. Arenberg, and Margo L. Francesco in the production of this report. David S. Kosson, chair Charles E. Kolb, vice chair Committee on Review and Evaluation of the Army Chemical Stockpile Disposal Program

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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration Acknowledgments This report has been reviewed by individuals chosen for their diverse perspectives and technical expertise, in accordance with procedures approved by the NRC's Report Review Committee. The purpose of this independent review is to provide candid and critical comments that will assist the authors and the NRC in making the published report as sound as possible and to ensure that the report meets institutional standards for objectivity, evidence, and responsiveness to the study charge. The content of the review comments and draft manuscript remain confidential to protect the integrity of the deliberative process. We wish to thank the following individuals for their participation in the review of this report: Gene H. Dyer, Bechtel Corporation (retired) Stan Kaplan, Bayesian Systems, Inc. George E. Keller II, Union Carbide Corporation Frank Mirer, United Auto Workers Mark J. Rood, University of Illinois Douglas M. Ruthven, University of Maine Harrison Shull, U.S. Naval Postgraduate School Leo Weitzman, LVW Associates, Inc. Ralph T. Yang, University of Michigan While the reviewers provided many constructive comments and suggestions, responsibility for the final content of this report rests solely with the authoring committee and the NRC.

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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration Contents     EXECUTIVE SUMMARY   1 1   INTRODUCTION AND BACKGROUND   6     Selection and Development of the Baseline Incineration System,   6     Role of the National Research Council,   7     Purpose of the Report,   9 2   TRACE GASEOUS EMISSIONS FROM AGENT INCINERATION   11     History of the Regulation of Trace Emissions,   11     Measuring Trace Emissions,   12     Emissions Concentrations in Exhaust Gas from JACADS and the TOCDF,   13     Emissions Sampling and Analysis Methodology,   14     Characteristics of Exhaust Gas Emissions,   15     Emission Rates,   16     Summary,   18 3   CONTROLLING TRACE ORGANICS WITH PASSIVE ACTIVATED CARBON FILTERS   20     Fundamentals of Adsorption,   21     Maximum Adsorption from the Gas Phase,   23     Operational Modes,   23     Application to the Incineration of Chemical Agents and Munitions,   23     Adsorption Equilibrium at Low Concentrations,   23     Adsorption Data,   24     Adsorption of Multicomponents,   25     Carbon Bed Breakthrough Times,   26     Filter Upsets,   28     Chemical Stability of Adsorbed Materials,   28     Summary,   29 4   FACILITY DESIGN WITH A CARBON FILTER SYSTEM   31     Gas Conditioning,   31     Alternative 1,   31     Alternative 2,   33

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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration     Comparison of Alternative Designs,   33     Performance of the Carbon Bed,   33     Water Balance,   34     Design of the Scrubber Tower,   34     Blower Equipment,   34     Summary of Gas Conditioning,   35     Description of the Carbon Filter,   35     Safety,   36     Sampling,   38     Maintenance,   38     Disposal,   38     Summary,   39 5   RISK ASSESSMENT AND CHANGE MANAGEMENT: AN EVALUATION OF THE ARMY'S DECISION-MAKING PROCESS   40     Background,   40     Focus of the Stockpile Committee's Review,   40     Documents Reviewed,   40     Risk Assessments for Anniston and Umatilla,   41     The Anniston PFS Risk Evaluations,   43     The Anniston Letter Report,   44     Change Management Process,   44     Future Evaluations of Major Design Changes,   47     Summary,   48 6   FINDINGS AND RECOMMENDATIONS   49     REFERENCES   52     APPENDICES         A Reports of the Committee on Review and Evaluation of the Army Chemical Stockpile Disposal Program (Stockpile Committee),   57     B Consolidated Exhaust Gas Characteristics for the JACADS and TOCDF Baseline Incineration Systems,   58     C Commercial Application of Carbon Bed Filters to Combustion Sources,   70     D Theoretical Modeling of Adsorption,   72     E Adsorption Separations: Alternative Modes of Operation,   80     F Alternative Flue Gas Cleaning Systems for Substances of Potential Concern,   82     G Biographical Sketches of Committee Members,   84

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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration Figures And Tables FIGURES 4-1   Schematic diagram of Alternative 1 for fixed-bed PFS,   32 4-2   The six PFS filter units and dampers,   37 4-3   PFS gas reheater,   39 D-1   Sketch of adsorption equilibrium,   73 E-1   Typical concentration profile of a material strongly adsorbed on a solid,   80 E-2   "Favorable" adsorption isotherm for strongly adsorbed species,   80 E-3   Comparison of maximum adsorption for fixed bed (q) and solids injection (qm) adsorption separation modes,   81 TABLES 2-1   Emissions Tests at the Two Operational Baseline Incineration Facilities, JACADS and the TOCDF,   13 2-2   Effect of Data Characteristics on Emissions Characteristics for Different Averaging Times,   18 3-1   Emission Levels of Chlorinated Dioxins for Some European Incinerators,   21 3-2   "Before" and "After" Data on Chlorinated Dioxin/Furan Cleanup with a Carbon Filter,   21 3-3   Chlorinated Dioxins Adsorbed on Powdered Activated Carbon,   25 3-4   Estimated Carbon Filter Breakthrough Times for Substances of Potential Concern in Stack Gases from the Chemical Agent Disposal Facility Liquid Incinerator,   26 3-5   Calculated Range of Carbon Adsorption of Agents,   27 4-1   Pressure Parameters for the Incineration of HD for a PFS-Equipped Baseline System,   35 4-2   Design Information for the PFS Carbon Filter Unit,   36 5-1   Effect of the Carbon Filter System on Risk at the Anniston Facility,   45

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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration B-1   Exhaust Gas Characteristics for the JACADS and TOCDF Baseline Incineration Systems,   59 C-1   Partial List of Activated Carbon Bed Filter Installations,   70 C-2   Performance of Activated Carbon Bed Filters,   71 D-1   Vapor Pressures for Various Chlorinated Dioxins,   73 D-2   Calculated Partial Pressures for Chlorinated Dioxins Based on 1 ng/m3,   73 D-3   Agent Detection Limits,   73 D-4   Agent Vapor Pressures and p/psat Ratios Based on Agent Detection Limits,   74

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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration Abbreviations And Acronyms ATV acute threshold value BIF boiler and industrial furnace CAMDS Chemical Agent Munitions Disposal System (Deseret Chemical Depot) CDF chlorinated dioxin/furan CFR U.S. Code of Federal Regulations CMP change management process CSDP Chemical Stockpile Disposal Program CWC Chemical Weapons Convention DCD Deseret Chemical Depot DFS deactivation furnace system D-R Dubinin-Radushkevich (adsorption equilibrium relation) DRE destruction and removal efficiency DUN dunnage incinerator EMPC estimated maximum possible concentration EPA Environmental Protection Agency GB satin (nerve agent) HD mustard agent (distilled) HE hazard evaluation HEPA high efficiency particulate air HRA health risk assessment ITEQ international toxic equivalence JACADS Johnston Atoll Chemical Agent Disposal System LC50 lethal concentration resulting in fatality of 50 percent of subjects in a given population LIC liquid incinerator MACT maximum achievable control technology MPF metal parts furnace MWC municipal waste incinerator NODA Notice of Data Availability NRC National Research Council NSPS new source performance standards PAS pollution abatement system PFS PAS (carbon) filter system PIC product of incomplete combustion POHC principal organic hazardous constituent PQL practical quantitation limit QRA quantitative risk assessment RAC reference air concentration RCRA Resource Conservation and Recovery Act RfD reference dose RsD Risk-Specific Dose SOPC substance of potential concern SOPEC substance of potential environmental concern TOCDF Tooele Chemical Agent Disposal Facility VX a type of nerve agent

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Carbon Filtration for Reducing Emissions from Chemical Agent Incineration ng/dnm3 at 7% O2 nanograms (10-9 grams) per dry normal (32°F [0°C], 1 atm) cubic meter adjusted to a diluent concentration of 7 percent oxygen ng/dsm3 at 7% O2 nanograms (10-9 grams) per dry standard (68°F [20°C], 1 atm) cubic meter adjusted to a diluent concentration of 7 percent oxygen