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Locating and Estimating Air Emissions from Sources of 1,3-Butadiene

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Locating and Estimating Air Emissions from Sources of 1,3-Butadiene EPA 454/R-96-008 November 1996 LOCATING AND ESTIMATING AIR EMISSIONS FROM SOURCES OF 1,3-BUTADIENE Prepared for: Mr. Dennis Beauregard Work Assignment Manager Emission Factor and Inventory Group U. S. Environmental Protection Agency Research Triangle Park, North Carolina 27711 Prepared by: Eastern Research Group Post Office Box 2010 Morrisville, North Carolina 27560-2010 November 1996 This report has been reviewed by the Office of Air Quality Planning and Standards, U.S. Environmental Protection Agency, and has been approved for publication. Mention of trade names and commercial products does not constitute endorsement or recommendation for use. EPA-454/R-96-008 EXECUTIVE SUMMARY The 1990 Clean Air Act Amendments contain a list of 189 hazardous air pollutants (HAPs) which the U.S. Environmental Protection Agency must study, identify sources of, and determine if regulations are warranted. One of these HAPs, 1,3-butadiene (butadiene), is the subject of this document. This document describes the properties of butadiene as an air pollutant, defines its production and use patterns, identifies source categories of air emissions, and provides butadiene emissions data in terms of emission factors and national inventory estimates. The document is a part of an ongoing EPA series designed to assist the general public at large, but primarily State/local air agencies, in identifying sources of HAPs and determining emissions estimates. Butadiene is primarily used in the manufacture of synthetic elastomers (rubbers, latexes) and for producing raw materials for nylon. Butadiene is emitted into the atmosphere from its production, its use as a chemical feedstock in the production of other chemicals, the use of these other chemicals, mobile sources, and from a wide variety of miscellaneous processes involving fossil fuel and biomass combustion, petroleum refining, secondary lead smelting, and wastewater treatment. Including only sources for which estimates are available or can be calculated, total nationwide emissions are estimated at 121,002 tons per year (109,775 Mg/yr). The primary sources of butadiene emissions on a national level are on-road mobile (47%) and off-road mobile (35%). Table ES-1 illustrates the national emissions estimates developed for the more predominant butadiene categories. The main butadiene air emissions sources are on-road mobile, off-road mobile, biomass burning, butadiene users, and petroleum refining. Some of these estimates for the non-fuel combustion sources were obtained from the reports required under the Superfund Amendment and Reauthorization Act (SARA), Title III, Section 313. Other estimates are a function of national activity data combined with the best available emission factors. iii Table ES-1. National Emission Estimates by Source Categorya Applicable Source Year Tons (Mg) Percent Mobile On-road 1992 56,786 (51,517) 47.3 Off-road 1990 41,883 (37,996) 34.9 General aviation and air taxis 1994 107 (97) 0.1 Stationary Biomass burning (forest fires & prescribed burning) 1989 19,931 (18,082) 16.0 Major butadiene usersb 1992 1,405 (1,275) 1.2 Petroleum refining 1992 219 (199) 0.2 Butadiene production 1992 191 (173) 0.2 Secondary lead smelting 1990 134 (122) 0.1 Miscellaneous other sourcesc 1992 106 (96) 0.1 Total 121,049 (109,004) 100.1 a Only sources for which estimates were available or could be calculated are included. For example, emissions from open burning of tires have not been included. b Includes following SIC Codes: 28 Chemicals and allied products 2812 Alkalies and chlorine 2819 Industrial inorganic chemicals, nec 2821 Plastics materials synthetic resins and nonvulcanizable elastomers 2822 Synthetic rubber (vulcanizable elastomers) 2865 Cyclic organic crudes and intermediates, and organic dyes and pigments 2869 Industrial organic chemicals, nec 2879 Pesticides and agricultural chemicals, nec 2891 Adhesives and sealants 2899 Chemicals and chemical preparations, nec c Other sources reporting under SARA 313 include facilities identified with the following SIC Codes. Also included are two facilities without SIC Codes but which account for 15 tons per year (14 Mg/yr) combined, and one facility with an SIC Code that is not listed but which reported 0.04 tons per year (0.04 Mg/yr). 2046 Wet corn milling 2369 Girl's, children's, and infant's outwear, nec 2621 Paper mills 3312 Steel works, blast furnaces (including coke ovens), and rolling mills 3579 Office machines, nec 8731 Commercial physical and biological research iv TABLE OF CONTENTS Section Page EXECUTIVE SUMMARY ................................................... iii LIST OF TABLES ........................................................ viii LIST OF FIGURES ....................................................... xii 1.0 PURPOSE OF DOCUMENT .......................................... 1-1 2.0 OVERVIEW OF DOCUMENT CONTENTS .............................. 2-1 3.0 BACKGROUND .................................................... 3-1 3.1 NATURE OF THE POLLUTANT ................................. 3-1 3.2 OVERVIEW OF PRODUCTION AND USE ......................... 3-3 3.3 OVERVIEW OF EMISSIONS .................................... 3-5 4.0 EMISSIONS FROM BUTADIENE PRODUCTION ......................... 4-1 4.1 BUTADIENE PRODUCTION .................................... 4-2 4.1.1 Process Descriptions ...................................... 4-2 4.1.2 Emissions ............................................. 4-11 5.0 EMISSIONS FROM MAJOR USES OF BUTADIENE ...................... 5-1 5.1 STYRENE-BUTADIENE COPOLYMER PRODUCTION .............. 5-2 5.1.1 Process Description ...................................... 5-3 5.1.2 Emissions .............................................. 5-5 5.2 POLYBUTADIENE PRODUCTION .............................. 5-10 5.2.1 Process Description ..................................... 5-10 5.2.2 Emissions ............................................. 5-11 5.3 ADIPONITRILE PRODUCTION ................................ 5-16 5.3.1 Process Description ..................................... 5-16 5.3.2 Emissions ............................................. 5-16 5.4 NEOPRENE PRODUCTION .................................... 5-20 5.4.1 Process Description ..................................... 5-21 5.4.2 Emissions ............................................. 5-23 5.5 ACRYLONITRILE-BUTADIENE-STYRENE COPOLYMER PRODUCTION .............................................. 5-26 5.5.1 Process Description ..................................... 5-27 5.5.2 Emissions ............................................. 5-34 5.6 NITRILE ELASTOMER PRODUCTION .......................... 5-36 v TABLE OF CONTENTS, continued Section Page 5.6.1 Process Description ..................................... 5-37 5.6.2 Emissions ............................................. 5-40 6.0 BUTADIENE EMISSIONS FROM MOBILE SOURCES ..................... 6-1 6.1 ON-ROAD MOBILE SOURCES .................................. 6-1 6.2 OFF-ROAD MOBILE SOURCES ................................. 6-4 6.2.1 Marine Vessels .......................................... 6-9 6.2.2 Locomotives ........................................... 6-11 6.2.3 Aircraft ............................................... 6-12 6.2.4 Rocket Engines ......................................... 6-15 7.0 EMISSIONS FROM MISCELLANEOUS SOURCES OF BUTADIENE ......... 7-1 7.1 MISCELLANEOUS USES OF BUTADIENE IN CHEMICAL PRODUCTION ............................................... 7-1 7.1.1 Product and Process Descriptions ............................ 7-2 7.1.2 Emissions ............................................. 7-10 7.2 INDIRECT SOURCES OF BUTADIENE .......................... 7-13 7.2.1 Vinyl Chloride Monomer and Polyvinyl Chloride Production ...... 7-13 7.2.2 Publicly Owned Treatment Works .......................... 7-14 7.2.3 Secondary Lead Smelting ................................. 7-14 7.2.4 Petroleum Refining ...................................... 7-15 7.2.5 Combustion Sources ..................................... 7-16 7.3 OTHER BUTADIENE SOURCES ............................... 7-22 8.0 SOURCE TEST PROCEDURES ........................................ 8-1 8.1 EPA REFERENCE METHOD 18 ................................. 8-1 8.2 NIOSH METHOD 1024 ......................................... 8-4 8.3 FEDERAL TEST PROCEDURE .................................. 8-5 8.4 AUTO/OIL AIR QUALITY IMPROVEMENT RESEARCH PROGRAM SPECIATION METHOD ....................................... 8-7 9.0 REFERENCES ..................................................... 9-1 APPENDICES Appendix A - Emission Factor Summary Table ................................ A-1 Appendix B - Estimating Methods for National Butadiene Emission Sources .......... B-1 References for Appendix B ....................................B-15 vi TABLE OF CONTENTS, continued Appendix C - Facility-Specific Emissions Data from EPA Section 114 Responses ................................................. C-1 References for Appendix C ....................................C-30 Appendix D - Estimation Methods for Equipment Leaks ......................... D-1 References for Appendix D .................................... D-7 Appendix E - Summary of 1992 TRI Air Emissions Data for 1,3-Butadiene .......... E-1 vii LIST OF TABLES Table Page ES-1 National Emission Estimates by Source Category ............................ iv 3-1 Physical and Chemical Properties of 1,3-Butadiene .......................... 3-2 4-1 Butadiene Production Facilities ......................................... 4-3 4-2 Butadiene Yields from Recovery Using a Mixed-C4
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