given mass, as demonstrated in Table 8-9. However, it is clear, given <strong>the</strong> distributions <strong>of</strong>particle mass, particle surface area and particle number by particle size in ambient air,that particle mass falls dramatically as one enters <strong>the</strong> ultrafine size range: so much so, infact, that surface area begins to fall be<strong>for</strong>e getting down to <strong>the</strong> ultrafine range, and <strong>the</strong>nfalls dramatically once <strong>the</strong> ultrafine range is reached (as shown in <strong>the</strong> Whitby plot on p.2-7, Fig. 2-1). I would drop Table 8-9. It is conceivable that <strong>the</strong> Whitby plot is outdated,since it is at least 23 years old. It might be useful to have similar work repeated <strong>for</strong>modern-day atmospheres.8-82 The first paragraph describes a clinical study that has no place here. One couldalternatively note that, “Clinical studies have observed....”. Here is what <strong>the</strong>toxicological studies show:.....SummaryThis summary, as I noted above, is excellent.Chapter 9. Integrative syn<strong>the</strong>sis.I would recommend that this chapter, as <strong>the</strong> title suggests, serve <strong>the</strong> primary purpose <strong>of</strong>an integrative syn<strong>the</strong>sis ra<strong>the</strong>r than a stand-alone summary <strong>of</strong> <strong>the</strong> CD. Of course it is possible<strong>for</strong> it to partially serve as a summary, while still serving primarily as a syn<strong>the</strong>sis, but this wouldtake considerable thoughtfulness.In terms <strong>of</strong> organization, I would like to see <strong>the</strong> chapter focus on <strong>the</strong> big issues that werelargely unresolved at <strong>the</strong> time <strong>of</strong> <strong>the</strong> 1996 CD, and <strong>the</strong>n proceed to addressing how muchprogress has been made in answering <strong>the</strong>se questions. This should take <strong>the</strong> <strong>for</strong>m <strong>of</strong> integratingnew findings across discipline. For example, in addressing <strong>the</strong> issue <strong>of</strong> coarse fraction effects,<strong>the</strong> epidemiological findings in isolation would suggest that <strong>the</strong>re are effects <strong>of</strong> <strong>the</strong> coarsefraction, apart from those due to <strong>the</strong> fine fraction, and that strong consideration should be givento setting a coarse particle standard <strong>of</strong> some <strong>for</strong>m. However, this course is tempered somewhatwhen in<strong>for</strong>mation on coarse PM measurement issues and exposures are also considered.The chapter could end with posing questions that remain unanswered, and which stillneed fur<strong>the</strong>r work.Barbara Zielinska, PhDChapter 2: Physics, Chemistry, and Measurement <strong>of</strong> <strong>Particulate</strong> <strong>Matter</strong>In my opinion, this chapter requires more work. At present, <strong>the</strong> chapter makes <strong>the</strong>impression on <strong>the</strong> reader that it was written by several independent authors, without any attemptto integrate it into one consistent document. Following are <strong>the</strong> specific examples:1. On page 2-47, line 19-21 (Section 2.2.3), <strong>the</strong> authors state discussing <strong>the</strong> experimentswith two quartz fiber filters deployed in series in order to examine <strong>the</strong> artifacts connectedwith SVOC partitioning: “Unless <strong>the</strong> individual compounds are identified, <strong>the</strong>investigator does not know what to do with <strong>the</strong> loading value on <strong>the</strong> second filter (i.e. toadd or subtract from <strong>the</strong> first filter loading value)”. I agree with this statement -moreover, even if <strong>the</strong> individual compounds were identified on back-up filter, <strong>the</strong>decision concerning adding or subtracting back-up filter loading would not bestraight<strong>for</strong>ward. However, <strong>the</strong> authors discuss subsequently in detail (page 2-51 to 2-62)in several places throughout <strong>the</strong> Section 2.2.3 several experiments with Teflon-quartz orquartz-quartz back-up filters that produced conflicting results. The references <strong>of</strong> Turpinet al., 2000, and Kirchsteller et al, 2000, are discussed on p. 2-52 – 2-53 and again on p.2-61 – 2-62 (in addition, <strong>the</strong> reference <strong>of</strong> Turpin et al., 2000, is missing). This would beconfusing to <strong>the</strong> reader who is not very familiar with <strong>the</strong> problem <strong>of</strong> positive andnegative sampling artifacts. It would be desirable to organize <strong>the</strong> discussion in moreconsistent manner, shorten it significantly, and not scatter it throughout <strong>the</strong> wholeSection 2.2.3A - 17
2. There are repetitions <strong>of</strong> <strong>the</strong> same statements throughout <strong>the</strong> chapter. For example, <strong>the</strong>discussion <strong>of</strong> sulfate and nitrate in western and eastern U.S. on page 2-21 (line 12-22) isrepeated on page 2-51 (line 1-7).3. The discussion <strong>of</strong> <strong>the</strong> various denuder techniques and <strong>the</strong>ir limitations (Sections 2.2.3.2and 2.2.3.3) is certainly important, especially since <strong>the</strong> popularity <strong>of</strong> <strong>the</strong>se techniques hasincreased greatly recently. The selection <strong>of</strong> <strong>the</strong> correct denuder type, its dimensions, flowrate, etc., greatly influence <strong>the</strong> results and incorrect conclusions could be drawn if <strong>the</strong>user is not familiar with <strong>the</strong> denuder technique. It would be desirable if authors put moreemphasis on discussing <strong>the</strong>se factors and organize <strong>the</strong>m in more logical manner (instead<strong>of</strong> <strong>the</strong> extensive discussion <strong>of</strong> <strong>the</strong> front-back-up filters collection methods, which producedoubtful results anyway).Some statements or opinions express by authors are not accurate, <strong>for</strong> example:1. Page 2-19, line 18-19: “…some primary organic compounds … are found…in <strong>the</strong> fineparticle mode.” As a matter <strong>of</strong> fact, most <strong>of</strong> <strong>the</strong> combustion-generated organiccompounds are found in <strong>the</strong> fine particle mode.2. Page 2-24, line 13: “…adsorption <strong>of</strong> organic gases…(e.g. polycyclic aromatichydrocarbons)”. Only 2 ring PAH are gaseous at ambient temperature, with 3 and 4 ringPAH distributed between <strong>the</strong> gas- and particle-phases.3. Page 2-53, line 3-12: this discussion is impossible to follow, is <strong>the</strong>re part <strong>of</strong> <strong>the</strong> sentencemissing?4. The PC-BOSS and RAMS denuders are discussed extensively throughout <strong>the</strong> chapter(page 2-55, 2-58, 2-89, 2-103, 2-105). However, both devices use a virtual impactorupstream <strong>of</strong> <strong>the</strong> denuder that removes not only a majority <strong>of</strong> <strong>the</strong> gases from <strong>the</strong> aerosolflow, but also particles smaller than 0.1 um. Thus, <strong>the</strong> gas-particle distribution ischanged even be<strong>for</strong>e <strong>the</strong> aerosol enters <strong>the</strong> denuder! In addition, particulate OCestimates have to be corrected <strong>for</strong> particle losses in <strong>the</strong> inlet <strong>of</strong> 46 to 48%. Is this 46 to48% factor independent <strong>of</strong> temperature, pressure and o<strong>the</strong>r factors? How accurate are <strong>the</strong>measurements, taking into account <strong>the</strong>se corrections? It would be desirable if authorsdiscuss <strong>the</strong> limitations <strong>of</strong> <strong>the</strong>se denuders as well as put <strong>the</strong> results obtained with <strong>the</strong>sedevices in proper perspective.5. Page 2-95: The discussion <strong>of</strong> <strong>the</strong> commercially available automated carbon analyzerseems to be a little premature in this document, since no comparison data with o<strong>the</strong>restablished techniques is available yet. There is no clear understanding what <strong>the</strong>instrument really measures in comparison with TOR and TOT techniques.6. For completeness, a newly developed continuous photoacoustic technique <strong>for</strong> blackcarbon measurement should be included in Section 2.2.5. The technique and itsapplications are described by Moosmuller et al. (1998) and Arnott et al. (1999; 2000).7. Page 2-103, line 18-23: One has to be careful when expressing <strong>the</strong> opinion that <strong>the</strong>denuder technique is an improvement over <strong>the</strong> filter/adsorbent collection method. Itshould be followed by <strong>the</strong> caveat that this is not an “out <strong>of</strong> <strong>the</strong> shelf” technique, it is notstraight<strong>for</strong>ward and requires thorough understanding by <strong>the</strong> user. If not used properly, itis subject to numerous artifacts and may lead to erroneous conclusions. Also, onedoesn’t have to use a charcoal impregnated glass-fiber filter <strong>for</strong> SVOC collection(especially that it is not readily available commercially); o<strong>the</strong>r solid adsorbents (such asPUF/XAD plugs) are used as well.The minor problems that require corrections are as follows:1. Page 2-10, line 4-5: missing word, “<strong>the</strong> term ultrafine”, “<strong>the</strong> term nanoparticle”2. Page 2-13, line 13: prior to 19873. Page 2-20, line 22: “…or on or in..”?4. Page 2-21, line 7: “in” be<strong>for</strong>e SO4 not necessary5. Page 2-25, line 1: “are” is missing6. Page 2-33, line 29: what is “PNA organic compounds”?7. Page 2-56, line 19-21: an awkward sentence, instead <strong>of</strong> which method?A - 18
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