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i I L Comments with references on "Measuring exposure to Environmental Tobacco Smoke" Submitted by: Dr. Paul R. Nelson, R.J. Reynolds Tobac:co Co. A major problem with this text is the omission of the references. Without these, it is impossible to verify that the claims mada about selected pieces of research are indeed representative of the work t:hat has been performed. Additionally, it makes judgements about the completeness and balance of background research impossible. Overall, this chapter does not contain a full set of references for statements made throughout the chapter. Specific references which are missing are included with this document, and passages of text which the author should be required to substantiate with references or deleteare also indicated. In the introduction, the author makes refelrence to measurements of hydroproline, N-nitrosoproline, aromatic amines, genotoxicity, and protein or DNA adducts in biological fluids as indicators of exposure to ETS or mainstream smoke. As this chapter deals with measurement of exposure to ETS, only those methods which can be used to assess exposure to ETS should be included. Without access to the specific references, it is not possible to asses the relevance or specificity of these measures to ETS, and this shouLd be done by the author. Additionally genotoxici,ty of and DNA adducts in biological fluids may also be caused by non-ETS sources. This may render the use of these tests inappropriate for consideration or mention in this chapter. The validity of self reported data on questionnaires (p. 52, para. 2) should be taken into account. References•should be provided to demonstrate the validity of self-reported exposure to ETS. The modeling approach described on page 54 and detailed in chapter 7 is not based upon representative sampling, and its app:.icability to this chapter is questionable. Additionally there are many questions about the validity of the model and its underlying assumptions, which are tD be dealt with elsewhere. Furthermore, it should be pointed out that the model. of Repace et: al., is not the only model which had been proposed to model ETS behavior. Several additional models have been advanced [(Rickert,1988) (Robinson,1988) (Nazaroff,1989,2 refs.)] and these are included in the appendix 'to this text. Before any model is advocated (as on p. 54) the relative merits and applicability of the models to a wide variety of sampling conditions must be performed. The reference to over 4000 air contaminants in the gas and particulate phase of ETS requires reference and clarification. First (First,1985) reports that >2300, or perhaps >3000 compounds have been idi~ntified in tobacco smoke; however, in order to state that >4000 contaminants are present in ETS requires that positive confirmation of this many compounds in ETS be documented in the literature. The presence of these compounds at trace levels in mainstream and sidestr-eam smoke does not justify the conclusion that all are present in ETS, nor does the actual number bear particular relevance to measurement of ETS. Relatively few compounds are present in sufficient coilcentration to permit their measurement in ETS. A balanced selection of references should be provided for the compounds measured in ETS presented at the top of page 56. Since this chapter deals with exposure measurement to ETS, multiple references 1:o each analyte should be

L1 I L provided which include sensitivity, detection-limits, possible interferences and concentrations typically encountered in real world settings. Discussion of and proper references to the analysis of these compounds in ETS and the environment in general is relevant to this chapter, and it should be included in more detail. It should also be noted that the tables in chapter six referenced in the same paragraph are incomplete. Only nicotine and RSP measurements are reported in the tables for ETS measurements. Sterling et al. hare prepared an excellent review of results reported prior to 1982 (Sterling,198?.), which includes tables of many compounds measured in ETS, and also provides available information on sampling conditions as well. The author should either prepare similar tables based upon all available data generated to date, or seek Dr. Sterling's permission to include his table in this document. It :ahould also be noted that the data presented in the tables in chapter 6 represen-: only a small segment of the total amount of ETS research which has been performe:d to date. (For example, see references in review by Sterling et al.) Additionally, several recent developments in ETS markers have been overlooked. Solanesol has been proposed as a marker for the particulate phase of ETS [ (Ogden, 1988) (Benner,1989)]. This compound has an advantage in that it is tobacco specific, and can be used to estimate the contribution of ETS to RSP. UVPM and FPM have also been reported as being reasonably specific markers of ETS particulate [(Conner,in press), Dr. Michael Ogden has presented this several places also]. Additionally, ethenylpyridine has been used as a marker for the vapor phase of ETS [(Thome, 1986) (Eatough,1988,EPA/APCA)]. This compound is also tobacco specific, and does not suffer from son:e of the decay problems associated with nicotine [(Baker,1988) (Eatough,1988,Indoor&Ambient Air Quality)]. Other markers have also been evaluated by Eatough et al. (Eatough,1989). Item 2 in the section of page 56 on the use of RSP as a marker requires reference. Specifically, what compounds of health concern are found in the particulate phase of ETS, who found them, and how do those concentrations compare with exposure limits. If the concentrations are "insignificant" by comparison to exposure limits item two should be dropped from thi: text. Items 3 & 4 in the same section also require reference. These statements cannot be considered general knowledge, and specific re::erences which prove their veracity must be provided. If they cannot be substantiated, then they should be dropped from the manuscript. On page 57, items one and two under the heading drawbacks with the use of RSP are related and should be combined under one heading. Additionally it should be noted from the data in figure 3 and table 4 of chapter 6 that tobacco smoke generally contributed less than 50% of the respirable suspended particles detected in homes. RSP levels in homes with no smoker:: were only 33% lower that in homes with one smoker, and 50% lower in homes with 2+ smokers (based on table 4). On page 57, Item two in the discussion of nicotine needs a reference. Once again, this is not a"point of common knowledge. Also, smokers smoke cigarettes on a per cigarette basis, not a on gram of tobacco basis. Therefore it is important to relate emission of nicotine to the smoking of a number of cigarettes, not just to the actual mass of tobacco consumed.

Item four in the discussion of nicotine is untrue, and it is not supported by the balance of available literature. When Kentucky reference cigarettes were smokel in a static cham~er by Ogden et al. (Ogden,1988,), the ratio of RSP (µg/m ) to nicotine (µg/m ) was found to be 14.7. When the same cigarettes were smoked in the same chamber under different conditicns, a ratio of 5.5 was obtained by Nelson et al. (Nelson,1989) In the work by Dgden et al. (Ogden,1988) 5 different types of cigarette were smoked under identical conditions, and RSP/nicotine ratios varied between 13 and 23. When one examines field studies, the variation in nicotine/RSP ratios continues to increase. In offices and bars in which smoking had taken place, Kirk et al. (Kirk,1988) found RSP/nicotine ratios which varied from 11.5 to 53. Oldaker et al.(Oldaker,1989), found that ratios in offices, restaurants and airplane passenger cs.bins were 30.8:1 (n-118), 22.5:1 (n-153) and 4.4:1 (n-44). Additionally, for the case of restaurant and office data, the correlation coefficient between RSP a1d nicotine were .236 and .198 respectively. These results indicate that any relationship between RSP and nicotine concentrations in smokey atmospheres is tenuous at best. Based upon the above referenced literature, nicotine does not vary with ETS related RSP as stated in item four of the nicotine discussion. Other researchers have examined the decay rates of nicotine and other ETS constituents in environmental chambers [(Heavner,1986) (Baker,1988) (Tang et al, 1989 APCA,in press)] and found that nicotine does not behave in a manner similar to other ETS constituents. These results also contradict the con:lusion in item 6 of the nicotine discussion. Because nicotine is not truly z.ssociated with other ETS constituents, nicotine and cotinine in physiological fluids do not provide a link between air concentrations of ETS and internal dose. Item two in the discussion of drawbacks of the ratio of nicotine to other vapor and particulate phase ETS constituents under a variety of conditions does not take the large amount of data in the literature ii.z which a large number of constituents have been measured into account. Sterling's (Sterling,1982) review gives data for a large number of constituents, and same relationships between nicotine and other compounds can be derived from his report. Additionally, multiple components have been measured in a number of other literature reports. [(Proctor,1989) (Sterling,1989)] In the section on the measurement of nicotine ani RSP in the air on p. 58, the statement that nicotine may be indicative of out:gassing from surfaces of other volatile ETS components is speculative, anc. not backed up by the literature. On P. 60, it is stated that "Gravimetric particles mass measurement methods are considered a standard method on particle mass measurement." References to this statement should be given. no The review annular denuder method outlined on page 62 is not yet published, of its effectiveness had been made by indeDendent laboratories. and It is likely that there are a great number of unpublished methods for many ETS analytes, however, this document should be concerned only with those which have 'M been presented in the literature, and for which there Ls good agreement on their effectiveness. Cn ~ .~ N O W

REFERENCES All references in this section are cited in detail in the bibliography associated with responses prepared at R.J. Reynolds. R.R. Baker, et al., Indoor & Ambient AIr Quality, p.121 (1988) C.L. Benner, et al, Environ. Sci. Technol., 23, 688 (1989) D.J. Eatough, et al., Proceedings of the 1988 EPA/AP:A International Symposium on Measurement of Toxic and Related Air Pollutants, p. 739 (1988) D.J. Eatough, et al., Indoor Air & Ambient Air Qualii_y, p. 131 (1988) D.J. Eatough, et al., Environment International, 15, 19 (1989) M.W. First, Indoor Air and Human Health, p. 195 (1985) P.W.W Kirk, et al., Indoor & Ambient Air Quality, p. 99 (1988) D.L: Heavner, et al., Proceedings of 79th annual APCA meeting, 86-37.9 (1986) W.W. Nazaroff, et al., Environ. Sci. Technol., 23, 157 (1989) W.W. Nazaroff, et al., Environment International, 15, 567 (1989) P.R. Nelson, et al., Present and Future of Indoor Air Quality, p. 277 (1989) G.B. Oldaker, et al., Present and Future of Indoor Air Quality, p. 287 (1989) C.J. Proctor, et al., Present and Future of Indoor Air Quality, p. 169 (1989) W.S. Rickert, et al., Can. Journal of Pub. Health, 79, S33 (1988) D.P. Robinson, et al., Indoor & Ambient Air Quality, 1>. 67 (1988) T. Sterling, et a1.; J. Air Pollution Control Assoc., 32, 250 (1982) T. Sterling, Indoor & Ambient Air Quality, p. 89 (1988) F.A. Thome, et al., Proceedings of the 79th APCA confe.rence, 86-37.6 (1986)