EPA-450/4-74-005
I September 1974
 (OAQPS No.  1.2-018)
                      GUIDELINE SERIES
                      DESIGNATION
               OF UNACCEPTABLE
           ANALYTICAL METHODS
                OF MEASUREMENT
     FOR CRITERIA POLLUTANTS
      U.S. ENVIRONMENTAL PROTECTION AGENCY
        Office of Air and Waste Management
      Office of Air Quality Planning and Standards
      Research Triangle Park, North Carolina 27711

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                             EPA-450/4-74-005

                           (OAQPS No. 1.2-018)
          DESIGNATION

      OF UNACCEPTABLE

   ANALYTICAL METHODS

       OF MEASUREMENT

FOR  CRITERIA POLLUTANTS
                     L Froteirjiu:..
                     Ti-)-.^ TV"?
      Monitoring and Data Analysis Division
    Office of Air Quality Planning and Standards
                 and
Quality Assurance and Environmental Monitoring Laboratory
      National Environmental Research Center

      Research Triangle Park, North Carolina

             September 1974

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                    OAQPS GUIDELINE SERIES

The guideline series of reports is being issued by the Office of Air Quality
Planning and Standards (OAQPS) to provide information to state and local
air pollution control agencies; for example, to provide guidance on the
acquisition and processing of air quality data and on the planning and
analysis requisite for the maintenance of air quality.  Reports published in
this series will be available - as supplies permit - from the  Air Pollution
Technical Information Center, Research Triangle Park, North Carolina
27711; or, for a nominal fee, from the National Technical Information Ser-
vice,  5285 Port Royal Road, Springfield, Virginia 22151.
                Publication No.  EPA-450/4-74-005
                  (OAQPS Guideline No.  1.2-018 )
                                   --.^Ci^c^,^

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                      TABLE OF CONTENTS



                                                                Page

INTRODUCTION					   ]

CATEGORIES OF ANALYTICAL METHODS -			-		   1

REFERENCE AND EQUIVALENCY REGULATIONS		-	   2

ACCEPTABILITY OF ANALYTICAL METHODS -		   3

DISCUSSION OF CRITERIA POLLUTANTS 	   3

  1.  Total Suspended Parti culates					   3

  2.  Carbon Monoxide 	   3

  3.  Sulfur Dioxide			   5

  4.  Nitrogen Dioxide 	   5

  5.  Photochemical Oxidants  (Ozone) 			   5

  6.  Total Hydrocarbons  Corrected for Methane 	   5

POLLUTANT  METHOD  CODE	—	-			   6

SUMMARY  OF REGIONAL OFFICE  RESPONSIBILITIES 	   6

APPENDIX A.  FEDERAL REFERENCE  METHODS, UNAPPROVED METHODS,
             UNACCEPTABLE METHODS		—   25

APPENDIX B.  RATIONALE  FOR RANKING THE METHODS AS
             UNACCEPTABLE-		—		   39

BIBLIOGRAPHIC  DATA SHEET			   41
                                m

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Designation of Unacceptable Analytical Methods of Measurement For
                     Criteria Pollutants
Introduction
     It is well known to all who analyze the air to measure criteria
pollutants that some techniques or methods are better than others.
Because important decisions, such as air quality standards achievement
and State Implementation Plan (SIP) revisions, are based on data
derived from these methods, it is imperative that only good quality data
be used.  Toward this end, we are designating 14 analytical methods
as unacceptable for continued use for these purposes.  Accordingly,
the objective of this guideline is to present the rational for those
methods which are being designated unacceptable, and to provide guidance
on the acceptability of methods for future measurements.  This will
enable the Regional Offices and the State agencies to make decisions
concerning implementation of monitoring network requirements, consistent
with the objectives and needs of their monitoring program.

Categories of Analytical Methods
     Methods for measuring air pollutants fall into one of three
categories:  (1) approved,  (2) unacceptable, and (3) those methods
which are neither approved nor unacceptable (unapproved).  At present,
the only officially approved methods are the Federal reference methods
described in appendices to 40 CFR Part 50, originally promulgated
on April 30, 1971 (36FR8186) with the National Ambient Air Quality
Standards (NAAQS).  This Federal Register also introduced the concept
of an "equivalent method", which is any method which can be demonstrated to
be "equivalent" to the reference method.  Thus, unapproved methods may
become approved only by demonstrating equivalence to the reference
method.

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     Those methods designated as unacceptable are not equivalent to the
reference methods because-they are known to yield measurements of
poor accuracy and reliability.  They are considered to be obsolete.
In each case, suitable analytical methods which produce measurements
of greater reliability are available to replace the unacceptable
methods.
Reference and Equivalency Regulations
     Regulations governing the procedures and criteria by which unapproved
methods may be determined to  be  equivalent  were  proposed  in  the
Federal Register on October 12, 1973 (38 FR 28438) as a new Part 53.
Pending revision based on comments from interested persons, the new
regulations, when finally promulgated, will require that a method
must be tested according to prescribed procedures and meet certain
prescribed specifications to be approved as an equivalent method.  In
essence, manual methods must demonstrate a consistent relationship
to the reference method in side-by-side measurements of ambient air.
Automated methods (automatic air analyzers) must demonstrate such a
consistent relationship as well  as meet certain performance specifications,
The new regulations will also cover reference methods which are automated
methods (i.e., CO and oxidants).   An analyzer must meet prescribed
performance specifications before it can be determined to be approved
as a reference method.
     Unapproved methods must be tested according to the prescribed
procedures and submitted with an application for approval to the
Quality Assurance and Environmental Monitoring Laboratory, NERC, RTP.
Approved methods are to be published  in  the  Federal  Register.  The
regulations will  apply to S02,  CO,and oxidants  corrected  for S02
and N02-

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Acceptability of Analytical Methods
     Table I lists those analytical methods for which data were
submitted by the States in 1972.  We have listed the individual
methods as "approved", "unapproved" and "unacceptable".  Use of
methods designated "unacceptable" should be discontinued as soon
as possible.  Data derived from those methods will not be accepted
or used by the NADB after September 1974.
     For S02, CO, and oxidants corrected for SO? and N02, unapproved
methods may be used until the equivalency regulations are promulgated.
After promulgation of  those regulations and additional approved
methods become available, unapproved methods may be used only until
they can be replaced with approved methods, and not later than 5 years
after promulgation after which  time only approved methods are to be
used.  For NCL and hydrocarbons corrected for methane, guidance for
selecting adequate automated methods may be found in the forthcoming
EPA Environmental Monitoring Series document (EPA-650/4-74-018),
Guidelines for Determining Performance Characteristics  of Automated
Methods for Measuring Nitrogen Dioxide and Hydrocarbons Corrected  for
Methane in Ambient Air.
     Until  these regulations and  guidelines become  available,  the
following guidance should  be considered:
Discussion  of Criteria Pollutants
     1.   TSP  - The high-volume  method is the Federal reference method
for total suspended  particulates.  Since  the air  quality standard
is defined  by the method,  the  high-volume  sampler is  the only  acceptable
method.   No procedures for determining  equivalency  of  alternate methods
have been developed-,  so all  other methods  are  to  be considered unacceptable,
     2.   Carbon  Monoxide - The non-dispersive  infrared (NDIR)  is  the
 Federal  reference method for CO.   Automated  analyzers  based on other
 principles  have  not  yet been tested with  respect  to equivalency,
 and  are  therefore unapproved.

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              Table  I.    1972-1973  POLLUTANT-METHOD-STATIONS  SUMMARY


Pollutant
TSP 11101
CO 42101



S02 42401










NO. 42602











Photochemical
Ox 44101
(Oxone)





44201




Code
91
11
12
21

11
13
14
15
16
31
33
91
92
93

n
12
13
14
71
72
84
91
94
95
96


11
13
14
15
51
81
82
11
13



Method
Hi-Vol (FRM)a
NDIR (FRM)
Coulometnc
Flame lonization

Colori metric
Conduct! metric
Coulometri c
Autometerc
Fl ame Photometric
Hydrogen Peroxide0
Sequential Conductimetric
West-Gaeke-Sulfamic Acid (FRM)
West-Gaeke Bubbler
Conductimetric Bubbler

Colori metric
Colori metric
Coulometri c
Chemi luminescence
J-H Bubbler (orifice)
Saltzman
Sodium Arsenite (orifice)
J-H Bubbler (frit)
Sodium Arsenite (frit)
TEA
TGS


Alkaline KI Instrumental
Coulometric"
Neut KI Colon metric
Coulometri c
Phenol phthal in
Alkaline KI Bubbler
Ferrous Oxidation
Chemi 1 uminescence (FRM)
Coulometri cd

1972
No. of
Stations
^28 —
223
1
2
~Z2E~
68
80
76
1
12
38
3
1040
45
2
1365
110
15
5
36
11
11
5
816
28


1037

49
10
75
13
5
64
85
62
1
364
1972
Percent
of Total
100
99
0
1
100
5
7
6
0
0
3
0
76
3
0
TOO"
12
1
0
3
1
1
0
79
3


100

13
3
21
4
1
18
23
17
0
100
1973
No. of
Stations
~1B02~
278
2
10
290
89
108
172
1
29
38
6
1510
11
0
T953
136
14
10
8
14
5
26
995
456


1664

10
10
89
22
3
79
91
131
1
436
1973
Percent
of Total
TD'CT
96
0
4
100
5
6
9
0
1
2
0
77
0
0
TTJO~
8
1
1
0
1
0
1
60
28


100

2
2
21
5
1
18
21
30
0
100
                                                                              Approved  Unapproved  Unacceptable
                                                                                         X
                                                                                         X
                                                                                         X
                                                                                         xc
                                                                                         X
                                                                                         xc
                                                                                         X
FRM = Federal Reference Method.
See Appendix B for an explanation of why these methods are unacceptable.
Thesa methods should be reported under method code 42401 13.
These methods should be under method code 44101 15.

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3.  Sulfur Dioxide -  The manual  West-Gaeke - sulfamic acid (24-hour
bubbler) method is the Federal reference method for S02.  The other
manual methods listed are unacceptable.  The similarly named "West-Gaeke"
method (SAROAD method code 42401  92) is not equivalent to the
reference method (SAROAD method code 42401 91).  Since no continuous
method has yet been tested for equivalency, they are classified as
unapproved.
4.  Nitrogen Dioxide - The manual NASN bubbler method is the Federal
reference method for N02-  However, in the June 8, 1973,issue of
the Federal Register (38 FR 15174), it was proposed that the NASN
method be withdrawn as the reference method and a new one designated
after testing of proposed candidate methods.  Although  the method
was not officially withdrawn, the problems with variable collection
efficiency and NO interferences are such  that it must be considered
unacceptable.  All other methods, both manual and continuous,
have  been classified as unapproved.
5. Photochemical Oxidants (Ozone) -  The  reference method for photochemical
oxidants  is a continuous chemiluminescence method based on the gas-phase
reaction  of ozone with ethylene.  This method is specific for ozone.
All other methods listed in Table I are total oxidant methods.  Six
of these  methods  for total oxidants are being designated unacceptable.
While the remaining automated methods  are not being designated
unacceptable, strong consideration  should be given to replacing them
with  the  reference  method.
6. Total  Hydrocarbons  Corrected  for Methane  -  This category  is
unique  in that, while  hydrocarbons  corrected for methane is  a
criteria  pollutant,  the  ambient  air quality standard  is only
a guide for  achieving  the oxidant standard.  A  gas chromatographic
flame ionization  technique  is the federal reference method  for
hydrocarbons  corrected for  methane, but this method is  difficult  and
expensive to use.   Other methods  are  now  becoming  available  and,  as
mentioned before,  guidance  for selection  of adequate  automated
methods may  be  obtained  in  the EPA  Environmental  Monitoring  Series
document (EPA-650/4-74-018),  Guidelines for Determining Performance
 Characteristics of Automated  Methods  for Measuring N02  and Hydrocarbons
 r.nrrpct.ed for Methane  in the  Ambient  Air.
                                 5

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 Pollutant Method Code
      Correct identification of the pollutant method is of utmost
 importance in the reporting of air quality data.  It will be of little
 help to upgrade the West-Gaeke bubbler procedure (SAROAD method code
 42401 92) for example, to the West-Gaeke-Sulfamic Acid method (SAROAD
 method code 42401 91) unless the method codes under which the data are
 reported to the NADB are also changed.  See OAQPS Guideline  #1.2-017,
 A Description of the Analytical  Techniques  and  Associated SAROAD Method
 Codes Used in Storing Data in the National  Aerometric  Data Bank, for  a
 description of the analytical technique associated with  the  SAROAD method
 code.
      After the  equivalency regulations are  promulgated,  the  pollutant
 method  code will  become  even more important since there  may  be  a unique
 identification  code  for  each method which passes  the equivalency testing
 and  becomes approved as  a  reference or equivalent method.  This new
 code may identify not only the method  principle but also  the instrument
 model and  manufacturer.
 Summary of Regional  Office Responsibilities
      The  Regional  Offices  should  see that those methods designated in
 Table 1  as unacceptable  are  replaced with approved methods as soon as
 practical.  This will  insure  adequate  data  for air quality trend analyses
 and  compliance with  NAAQS  after 9/1/74  when data from unacceptable methods
will no  longer be used.  After promulgation of the equivalency regulations,
 EPA  Regional Offices should assist in  the conversion to the  exclusive use
of approved methods  for S02>  CO and "oxidants corrected for S02 and N0?
and  similarly assistance should be provided for selecting adequate methods
for  ^ and total hydrocarbons corrected for methane  according to the
 available  guidelines.
     To help the Regional Offices identify which states reported data
by which method in 1972,  we have included Table II, a printout of
the data from which Table  I was prepared.  Note that the printout is
by pollutant code and method.  Appendix A, which  is an  extract from OAQPS
Guideline #1.2-017, presents a description of the  analytical  technique
associated with the SAROAD method  code.   Lastly,  Appendix  B,  contains  a
short paragraph for each  method which has been designated  unacceptable,
giving the rationale for  that designation.

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Table II.  INVENTORY OF AIR POLLUTANT MONITORING  SITES,  BY  STATE,  1972

STATE
STATE
STATE
STATE
STATE
STATE
STATE"
STATE
STATE
STATE
STATE
STATE
STATF
STATE
STATE
STATE
STATE
STATF
STATE
STATE
STATE
STATE
STATE

STATE
STATE

COUNT
'"COUNT ~
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT ""
COUNT "
COUNT
COUNT
COUNT"
COUNT
COUNT
COUNT"
COUNT
COUNT"
COUNT""

COUNT
"COUNT
POLLUTANT
CODE
uiof
111 01
11 101
11101
11101 "
11101 '
111 01
11101 ""
iii'oT""
mo!
1 1 1 0 1
moi
11101
11101
"ill 01
11101
111 01
11 101
11 101
11101
~ Tiioi
moi"
11101

11101
11101
METH
C'iDE
91
"9l"
91

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TABLE II
POLLUTANT MPTH
CODE CDDE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STAT£ 	
STATE
STATE
STATE
STATE
STATE
STATE
COUNT
CUUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
11 101
11101
11101
11101
11101
11101
11101
11101
11101
11101
11101
11101
11101
11101
11101
11101
11101
11 10 I
11101
11101
11101
11101
11101
11101
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
MISSOURI
MONTANA
NEBRASKA
NEVADA
NEW HAMPSHIRE
NEW JERSEY
NEW MEXICO
NFW YORK
NORTH CAROLINA
NORTH DAKOTA
OHIO
OKLAHOMA
OREGON
PENNSYLVANIA
PUERTO RICO
RHODE ISLAND
SOUTH CAROLINA
SOUTH DAKOTA
TENNESSEE
TEXAS
UTAH
VERMONT
VIRGINIA
WASHINGTON
NUMBER OF
SITES
49
2
36
41
26
79
28
233
199
16
137
95
48
105
5
23
75
2
98
192
8
2
i22
57

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TABLE II



STATE
STATE
STATE
STATE
STATE
POLUTCOD
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STAf E
STATE



COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT"
COUNT"
COUNT
COUNT
C"OUNT"
COUNT"
COUNT
COUNT"
COUNT "
COUNT
"CO'JNT
COUNT
"COUNT
""con NT"

POLLUTANT
CODE
11101
11101
" 11 101
11101
11101
11 101
42101
""42101
42L01
42101
42101
42ToT
-42TOT--
42101
42101
42101
4?101
42101
42101
4~2~1 01
42101
42TOI
42101
42101 "
42101

MFTH
CODE
91-
91
91
91
91
91
lT~~
11
11
11
11
"" 11
1 1 "
11
11
11
11
11
11
"11
11
11
11
1 1
11



WEST VIRGINIA
WISCONSIN
WYOMING
GUAM
VIRGIN ISLANDS

ALABAMA
ALASKA
ARIZONA
CALIFORNIA
COLORADO
DIST COLUMBIA
FLORIDA
GEORGIA
HAWAII
ILLINOIS
"INDIANA
IOWA
KANSAS
KENTUCKY
LOUISIANA
MARYLAND
MASSACHUSETTS
MICHIGAN
MINNESOTA

NUMBER OF
SITES
38
7
4
11
4
2828
2
1
3
51
1
2
6
2
1
1
3
2
5
7
3
19
5
3
3

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TABLE II

STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
POLUTCOO
STATE
POLUTCOD
STATE
POLUTCOO

COUNT
COUNT
CO'JNT
COUNT
COUNT
CO'JNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
POLLUTANT
CODE
42101
42101
42101
42101
42101
42101
42101
42101
42101
4?101
42101
42101
42101
42101
42101
42101
42101
42101
42i01
42101
42101
42101
42101
42101
METH
CODE
il
11
11
11
11
11
11
11
11
11
11
11
11
11
11
11
11
11
11
11
12
12
21
21

MISSOURI
NEBRASKA
NEVADA
NEW JERSEY
NtW MEXICO
VFW YORK
NORTH CAROLINA
OHIO
OKLAHOMA
OREGON
PENNSYLVANIA
RHODE ISLAND
TENNESSEE
TEXAS
UTAH
VIRGINIA
WASHINGTON
WEST VIRGINIA
WISCONSIN

OHIO
*•
KENTUCKY

NUMBER OF
SITES
10
1
1
22
1
13
2
13
4
2
2
2
4
1
4
9
10
1
1
223
1
1
2
2
  10

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TABLE II
POLLUTANT
CODfc
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
POLUTCOD
STATF
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE""""
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
"COUNT
"COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
" COUNT" ""
COUNT
"COUNT
COUNT
COUNT
"COUNT
COUNT
COUNT
"COUNT
COUNT
42401
42401
42401
42401
42401
42401
42401
~4240l
"42401
42401
42401
"~424~6 1
42401
42401
42401
42401
"42401
42401
42401
42401
"""42401""
42401
42401
—42461
~ 42 401
METH
cone
11
Ti
11
11
11
~"H"
11
~TY
11
11
il
11
11
11
11
11
13
13
13
13
13
13
13
13
l"3~"

"ARIZONA
COLORADO
" DELAWARE
DIST COLUMBIA
F'LOR i DA
ILLINOIS
KENTUCKY
MARYLAND
MASSACHUSETTS
MISSOURI
NEW JERSEY
NEW YORK
OHIO
PENNSYLVANIA
WASHINGTON

ARIZONA
CALIFORNIA
COLORADO
CONNECTICUT
DELAWA'RE
DIST COLUMBIA
FLORIDA
"ILL I NCI'S
INDIANA
NUMBER OF
SITES
2
1
6
2
3
1
5
1
4
5
22
7
4
4
1
68
2
18
1
I
7
2
i~
1
8

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TABLE II
POLLUTANT
CODE
STATE
STATE
STATE
STATE
STATf
STATED
STATE
STATE
STATE
POLUTCOD
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
JSTATE
J5TATE
STATE
STATE
STATE
COUNT
COUNT
COUNT
„ COUNT
COUNT
_ COUNT
COUNT
COUNT
COUNT
COUNT
_COUNT
_COUNT_
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
42401
42401
42401
4240 1
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
METH
CODE
13
13
U
13
13
13
13
13
13
13
14
14
14
14
14
14
14
14
14
14
14
14
14
14

MARYLAND
MINNESOTA
MISSOURI
NEW YORK
OHIO
OREGON
PENNSYLVANIA
VIRGINIA
WASHINGTON
ALABAMA
ARIZONA
DIST COLUMBIA
FLORIDA
GJORGIA
INDIANA
KANSAS
KENTUCKY
MASSACHUSETTS
MICHIGAN
MINNESOTA
MISSOURI
NEW YORK
NORTH CAROLINA
NUMBER OF
SITES
12
2
2
1
7
2
2
2
9
80
2
8
2
2
2
4
3
6
2
22
4
1
12
1
   12

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TABLE II
POLLUTANT
CODE
STATE
STATE
STATE
STATE
POLUTCOO
STATE
POLUTCOD
STATE
STATE
POLUTCOD
STATE
POLUTCOD"
STATE
poLuTcob"
STATE
STATE "
STATE
STATE "
STAT6
STATE —
STATE
STATE
	 	 - -
$T AT E
-ctAfT
-"e
COUNT
COUNT
COUNT
COUNT
COUNT^
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
"COUNT
"COUNT
"COUNT
COUNT
"COUNT
"COUNT
COUNT
COUNT
COUNT
-COUNT
COUNT
COUNT

--COUNT'
-"COUNT
42401
42401
42401
42401
41401
"42401"
~42401
42401
4240T
42401
42401
"42401
-4240T™
"~42 401
-42401-

42401
~~42401~
42401
"42401


	 _r



— 42401
METH
CODE
14
14
14
14
14
15
15
16
iV
16
31
31 "
33
"33"
- "gjf-
91
91
"~9i
	
91
01
91
91

-"" 91


NUMBER OF
SITES
OHIO
PENNSYLVANIA
TENNESSEE
VIRGINIA

"TENNESSEE

MARYLAND
VIRGINIA

NEW YORK
._..
"MI'S SOUR i "
"""
"ALABAMA
ALASKA
ARIZONA
" ARKANSAS
CALIFORNIA
—cOiORADO^
-CONNECTICUT
OEtAVI^E _.
-OiSf-COLOHBlA
"pTtiRToA
^ ._--"'
" ^GEORGIA

1
i
1
2
76
I
1
11
1
12
38
38
3
3
13
1
7
""2
16
4
3
—r~~~
34 "
._- 	
13
	 	 — 	 ' "" "
„_. 	 	 "••"

-------
         TABLE II



— — 	 _ _
STATE COUNT
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
-STATF
STATE
STATE
- TE
STATE

STATE

STATE
_?T4fE
___COUNT
COUNT
. COUNT
COUNT
COUNT
C OUN T
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
- ..COUNT
COUNT
-.COUNT
COUNT

'--'UtyT .

"UN T ,
COUNT
4<
COUNT
PCLLUTAN
CODE
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
42401
,42401
42401
42401
42
—
V4o!

4240 1
'^•y f n
^40j
"> /. A .
t40l
-401

IT METH ~
CODF NUMBER OF
— - SITES
91 HAWAII
12
91 ILLINOIS
- . 38
91 INDIANA
66
91 IOWA
2
91 KANSAS
30
91 KENTUCKY
98
91 LOUISIANA
17
91 ^ A I N £
6
91 MARYLAND
-- _. 49
91 MASSACHUSETTS
91 MICHIGAN
24
91 MINNESOTA
91 MISSISSIPPI
--?-1. MISSOURI
9l- MONTANA 4
NERRASKA
-9L, NEVADA ' _ 4
91
NEW lr-
CWJC»S£y 4
9)
N t~ w
™ r x i r n 8
9|
N6w YORK a
H CARQL r M ^^

92

-------
TABLE II
POLLUTANT
CODE
STATE
STATE
STATF
STATE
STATF
STATE
STATE
STATE
STATE
ST AT E
STATE
STATE
STATE
STATE
STATE
STATE
"POLUTCOD
STATE
STATE
P GLUT COD
STATE
POLUTCOO
STATE
"STATE
"STATE
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
"COUNf
COUNT
COUNT
COUNT" ""
~C~0'JN~T "
COUNT
COUNT
"COUNT
"COUNT
COUNT
"COUNT"
COUNT
42401
42401
42401
42401
42401
42401
42401
42401
42401"
4240 1
42401 "
42401
424QT
4T40I "
424~ol~ ~
~4240~i~
42401
42401
42401
"42401
"424 Ol
42401
42602
"42602" """
42602
METH
CODE
91
91
91
91
91
91
91
91
~~9\
91
91
91
91
-----
91
91
91
92
92
"~92
" 93
93
11
11
11
OREGON
PENNSYLVANIA
PUERTO PICO
RHODfc ISLAND
SOUTH CAROLINA
SOUTH DAKOTA
"TENNESSEE
TEXAS
UTAH
VIRGINIA
"~ WASHINGTON
WEST VIRGINIA
WISCONSIN
WYOMING
GUAM
VIRGIN ISLANDS
"~ '
"FLORIDA
MASSACHUSETTS

"INDIANA

ALABAMA
ARIZONA
CALIFORNIA
NUMBER OF
SITES
1
14
4
18
38
1
37
13
1
49
4
15
3
2
9
3
1040
1
44
45
2
2
2
3
50
  15

-------
TABLE II
POLLUTANT METH

STATE
jHTATj;
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
POLUTCOD
STATE
STATE
STATE
STATE

COUNT
__CO'JNT_
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
CODE
42602
	 .42602
_ 42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
CODE
11
	 11
11
11
11
11
11
11
11
11
11
11
11
li
11
11
11
11
11
11
12
12
12
12
CONNECTICUT
__PJ_S! COLUMBIA
FLORIDA
GEORGIA
KENTUCKY
MAINE
MARYLAND
MASSACHUSETTS
MINNESOTA
MISSOURI
NEVADA
NEW YORK
NORTH CAROLINA
UHIO
OKLAHOMA
OREGON
PENNSYLVANIA
TENNESSEE
VIRGINIA

COLORADO
DIST COLUMBIA
ILLINOIS
MISSOURI
NUMBER OF
SITES
1
1
4
1
8
1
6
1
1
8
1
13
1
2
1
1
1
1
2
110
1
1
1
1
      16

-------
TABLE II
-
STA^E
STATE
STATE
STATE
STATE
POLtlTCOD
STATE
STATE
STATE
STATE
POLUTCOD
STATE
STATE
STATE
STATF
STATE
STATE
STATE
STATE
Sf ATE
STATF
STATE
STATE
STATE
STATE
!
COUNT
COUNT
COUNT
COUNT "
COUNT
COUNT "
COUNT
COUNT"
COUNT
COUNT
"COUNT
COUNT ""
COUNT"
~ccuNf"~
COUNT
COUNT
COUNT
COUNT
COUNT
"COUNT
COUNT
COUNT
COUNT
COUNT""
"COUNT"
3OLLUTANT
CODE
42602 """"
42602
42602
42602
42602
426 0"2
42602
~42~602
42602
42602
42602
"42602
"42602
~42602~"
42602
42602
42602
42602
"42602
""42602
42602
42602
42602
"" 42602
42602"""
METH
CODE
12
12
12
12
12
12
13
13 "
13
- y3
-3~
14
14
14
14
14
14
14
14
14
14
14
14
14
14
--
NEW JERSEY
OHIO
PfcNNSYLVANIA
RHODE ISLAND
VIRGINIA

KANSAS
MINNESOTA
NEVADA
TENNESSEE

ARIZONA
COLOR ADO
CONNECTICUT
DIST COLUMBIA
ILLINOIS
INDIANA
IOWA
KENTUCKY
MARYLAND
MASSACHUSETTS
MINNESOTA
MISSOURI
NEBRASKA
NEW MEXICO
NUMBER OF
SITES
5
1
1
2
2
15
2
1
1
1
5
1
1
1
2
2
1
1
3
1
1
1
2
1
1
 17

-------
    TABLE II
-

STATE
, STATE, 	
STATE
STATE 	
STATED
STATE
POLUTCOO
STATE
POLUTCOD
STATE
POLUTCOO
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
_SJATE 	
STATE
STATE
P

COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
'OLLUTANT
CODE

42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
METI
CODI

14
14
14
14
14
14
14
71
71
72
72
91
91
91
91
9i
91
91
91
91
91
91
91
91
-1

NEW" YORK
OHIO
PENNSYLVANIA
TEXAS
UTAH
VIRGINIA

MINNESOTA

INDIANA

ALABAMA
ALASKA
ARIZONA
ARKANSAS
CALIFORNIA
COLORADO
CONNECTICUT
DELAWARE
DIST COLUMBIA
FLORIDA
GEORGIA
HAWAII
ILLINOIS
NUMBER OF
SITES

2
5
5
2
1
2
36
11
11
11
11
13
1
5
2
16
2
4
3
2
22
13
11
4
18

-------
	

STATE
STATE
STATE"
STATE
STATE
STATE
STAfE~
STATE
STATE "
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
	 -
	
"" COUNT"
COUNT
" "COUNT
COUNf
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT

POLLUTANT
CODE
42602
42602
" 42602"
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
TABL
METH
CODE
9 r
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
91
E II

	 	
INDIANA
IOWA
""KANSAS
KENTUCKY
LOUISIANA
"MAINE
MARYLAND
MASSACHUSETTS
MICHIGAN
MINNESOTA
MISSISSIPPI
MISSOURI
MONTANA
NEBRASKA
NEW HAMPSHIRE
NEW JERSEY
NEW MEXICO
NEW YORK
NORTH CAROLINA
OHIO
OKLAHOMA
OREGON
PENNSYLVANIA
PUERTO RICO
RHODE ISLAND
- - - 	

NUMBER OF
SITES
41
2
29
87
4
1
49
54
6
3
. ^ 	 ._
4
1
3
4
8
7
9
~ ~155
67
19
.__ ..._
4
18
19

-------



STATE
STATE 	
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STAT E
POLUTCOD
STATE
POLUTCOD
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE



COUNT
^COUNT
COUNT
COUNT
COJJNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT

POLLUTANT
CODE
42602
	 _42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
42602
44101
44101
44101
44101
44101
44101
44101
44101
44101
44101

METf
CO Of
91
?1
91
91
91
91
91
91
91
91
91
91
94
94
11
11
11
11
11
11
11
11
11
11

1

SOUTH CAROLINA
SOUTH DAKOTA
TENNESSEE
TEXAS
UTAH
VIRGINIA
WASHINGTON
WEST VIRGINIA
WISCONSIN
WYOMING
GUAM

KENTUCKY

ARIZONA
COLORADO
OIST COLUMBIA
FLORIDA
ILLINOIS
INDIANA
IOWA
KANSAS
MISSOURI
NEW JERSEY

NUMBER OF
SITES
TO
1
41
13
1
7
10
1
3
2
9
816
28
28
1
1
1
2
1
2
1
1
1
4
20

-------
TABLE II
OOLLUTANT MFTH
CODE CODE
STATE
STATE
STATE
ST AT E
STATE
STATE
STATE
STATE
STATE ~
POLUTCOD
STATE
STATE
STATE
STATE
POLUTCOD"
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
"COUNT
COUNT
COUNT
COUNT"
COUNT
COUNT
COUNT
"COUNT"
coWr
COUNT
"44101
"44161
44101
44101
44101
44101
44101
44101
44101
44i01
44101
44101
44101
44101
"44101
"44101
44101
"44101
~44TOF
44101
44101
44101
~~44l6T~
44i01
44101
1 1
ii
11
1 1
if"
if
11
11
11
11
13
13
13
13
~~13
14
14
14
14
14
14
14
14 ~
14
14
NEW YORK
NORTH CAROLINA
OHIO
PENNSYLVANIA
TENNESSEE
TEXAS
VIRGINIA
WASHINGTON
WISCONSIN
KANSAS
NEVADA
NEW MEXICO
WASHINGTON

ALABAMA
ARIZONA
CALIFORNIA
COLORADO
KENTUCKY
MINNESOTA
MISSOURI
OHIO
OREGON
PENNSYLVANIA
NUMBER OF
SITES
12
2
8
1
4
1
4
1
1
49
3
1
1
5
10
1
1
56
1
"1
1
8
2
1
i
21

-------
     TABLE II

STATE
STATE
P'lLJTCO',
STATE
STATF
POLUTCOD
STATE
POLUTCOD
STATE
STATF
STATE
STATE
POLUTCOD
STATE
STATE
STATE
POLUTCOD
STATE
STATE
STATE
STATE
STATE
STATE
STATE

COUNT
COUNT
COUNT
C OU N T
CUIJNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
POLLUTANT
CODF
44101
44101
44101
44101
441ui
44101
44101
44101
44101
44101
44101
44101
44101
44101
44101
44101
44101
44201
44201
44201
44201
44201
44201
44201
'^Th
rnOE
u
14
14
15
i'j
15
51
51
81
81
31
81
81
82
32
82
32
il
11
11
11
11
11
11
1
TciMMiISSF-
VIRGINIA

C/L I FURN IA
VIRGINIA

OKLAHOMA

MINNESOTA
NORTH CAROLINA
OKLAHOMA
SOUTH CAROLINA

KANSAS
KENTUCKY
JHIO

ALABAMA
COLORADO
DIST COLUMBIA
FLORIDA
GEORGIA
HAWAI I
ILLINOIS
NUMBER OF
SITES
1
1
75
12
1
13
5
5
7
7
13
37
64
3
76
6
85
2
1
1
4
1
1
1
22

-------
TABLE II

STATE
STATE
STATF
STATE
STATE
STATE
STATE
STATE
STATF
STATE
STATE
STATE
STATE
STATE
STATE
STATE
STATE
POLUTCOO
STATE
POLUTCOD

COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT
COUNT"
COUNT
COUNT
COUNT""
COUNT
"COUNT
COUNT""
COUNT
POLLUTANT
C 0 0 E
44201
44201
442U1
Xt420i
44201
44201
44201
44201
4420~1
44201
~442T)T
44201
44201
44201
44201
44201
44201
44201
~44~201
44201
'-I t T H
CODE
11
H
11
11
11
11
11
11
11
11
11
11
11
11
il
11
11
ii
13
1~3"~

INDIANA
KANSAS
KENTUCKY
LOJISUNA
MARYLAND
MICHIGAN
MISSOURI
NEBRASKA
NEW YORK
NORTH CAROLINA
OHIO
OKLAHOMA
PENNSYLVANIA
SOUTH CAROLINA
TENNESSEE
TEXAS
VIRGINIA

OREGON

NUMBER OF
SITES
1
2
2
3
6
1
1
3
12
2
7
2
1
1
1
1
5
62
1
1
 23

-------

-------
                             APPENDIX A.*
                       FEDERAL REFERENCE METHODS
                          UNAPPROVED METHODS
                         UNACCEPTABLE METHODS
                             APPENDIX B.
                  RATIONALE FOR RANKING THE METHODS
                            AS UNACCEPTABLE
*Extracted from Guideline Document OAQPS 1.2-017, A Description of the
 Analytical Techniques and Associated SAROAD Method Codes Used in StbTing
 Data in the National Aerometric Data Bank.
                                 25

-------
              Federal Reference Methods

 11101  91   SUSPENDED PARTICULATE - HI-VOL - GRAVIMETRIC
           Air is drawn at 40 to 60 ft3/min through a glass
           fiber filter, by means of a blower, and the sus-
           pended particles having a diameter between 100
           and 0.1 ym are collected.  The suspended particulate
           is  calculated by dividing the net weight of the
           particulate by the total air volume sampled and
           reported in density units as yg/m3.  Heavy
           loading of suspended particulate, oily particulates,
           or  high humidity can cause reduced air flow
           through the filter.   Therefore, flow rates should
           be  measured before and after the sampling period.
           1.   "Rules and Regulations," Federal Register,
           Vol 36,  No.  228,  U.S.  Government Printing Office,
           Washington,  D.C.,  (Nov.  25,  1971), p 22388.
           2.   Intersociety Committee,  "Methods of Air
           Sampling and Analysis,"  American Public Health
           Association,  Washington, D.C.,  1972, p 356.
           3.  "Air Quality Data for  1967,  "APTD-0741,
           APTIC,  Research Triangle Park, North Carolina,
           1971, p. 17.
42101 11  CARBON MONOXIDE - INSTRUMENTAL  - NON-DISPERSIVE
          INFRA-RED
          The non-dispersive infrared  instrument has a sample
          cell, a rererence. cell,  and a detector.   The detector
          is divided by a flexing  diaphragm into two equal
          cells filled with equal  concentrations of CO.  The
          reference cell is filled with a CO-free  air.
          When infrared radiation is passed into the  sample
          cell some of the radiation is absorbed by CO
          in  this  cell in  proportion to the concentration
                              26

-------
          of CO and the rest is transmitted to the detector.  In the
          detector, the radiation causes the CO to expand flexing the
          diaphragm in proportion to the transmitted infrared radiation.
          Since the reference cell is filled with zero CO air, the
          reference cell side of the detector exerts a constant pres-
          sure on the diaphragm.  When the CO is introduced into the
          sample cell, unequal amounts of residual radiation reach
          the two compartments of the detector causing an unequal
          expansion of the detector gas.  This unequal expansion
          causes the diaphragm to deflect, creating a change of
          electrical capacitance in an external circuit, and ultimate-
          ly an amplified signal which is suitable for input to a
          servo-type recorder.  The detector is calibrated by placing
          CO standards in the sample cell and recording the electrical
          signals.
          1.  "Rules and Regulations," Federal  Register, Vol.  36,
          No. 228,  (Nov. 25, 1971), p. 22391.
42401  91  SULFUR DIOXIDE-GAS BUBBLER WEST-GAEKE-SULFAMIC ACID'
          Sulfur dioxide is collected in a tetrachloromercurate solution,
          forming a stable dichlorosulfitomercurate complex.  When acid-
          bleached  pararosaniline is added to the collected S02 together
          with formaldehyde, the amino groups (-NH3) form a red violet
          compound  called pararosaniline methylsulfonic acid which is
          measured  spectrophotometrically.   The method is described in
          the Federal  Register.   (The NASN procedure,  however,  uses
          1.725 g/1  sulfamic acid rather than  6 g/1  and does not use
          EDTA).  The  sulfamic acid eliminates  interference from oxides
          of nitrogen.
          1.  "Rules  and Regulations," Federal  Register.  Vol.  36,
          No.  228,  U.  S.  Government Printing Office,  Washington,  D.  C.,
          (Nov.  25,  1971),  p.  22385.
          2.  West,  P.  W.  and G  C.  Gaeke, (1956),  "Fixation of  Sulfur
          Dioxide as Disulfito-Mercurate (II)  and Subsequent Colori-
          metric  Estimation,"  Anal.  Chem.  28,  1819.
                                   27

-------
          3.   Intersociety Committee,  "Methods  of  Air Sampling  and
          Analysis," American Public Health  Association,  Washington,  D.  C.,
          1972, p.  447.
          4.   "Air Quality Data for 1967, "APTD 0741, APTIC,  Research
          Triangle Park, N. C., 1971,  p.  20.
44201 11   OZONE - INSTRUMENTAL-CHEMILUMINESCENCE
          Ambient air to be measured and  ethylene  are delivered
          simultaneously to a mixing cell where ozone reacts  with
          the ethylene to emit light which is measured by a photomul-
          tiplier tube.   If the air and ethylene flow rates are constant,
          the resulting  photomultiplier signal  can be related to the  input
          ozone concentration.   Analyzers are calibrated  with known
          ozone concentration standards.
          1.   "Rules and Regulations,  "Federal  Register,  Vol. 36,
          No. 228, U. S. Government Printing Office, Washington, D.C.,
          (Nov. 25, 1971), p. 22392.
          2.   "A Chemiluminescence Detector for Ozone Measurement,"
          Bureau of Mines Report of Investigation  RI-7650, United States
          Department of the Interior, U.  S.  Government Printing Office,
          Washington, D. C., 1972.
                                     28

-------
                 Unapproved Methods

42101 21  CARBON MONOXIDE - INSTRUMENTAL - FLAME IONIZATION
          Ambient air is passed through two gas chromatographic
          columns in series, the first retains most pollutants
          but passes CO and CH4, and the second passes only
          CO.  The CO then flows through a Ni catalyst where
          it is converted to CH4 which is measured by a flame
          ionization detector.  The resulting measured current
          is related to the CO  concentration of the input
          ambient air by dynamic calibration with known CO
          concentration standards.
          1.  Rotterdam, Warsaw, and Bucharest,  "The Status
          of Instrumentation in Air Pollution Control," Environ-
          mental Control Seminar Proceedings, U. S.Department
          of Commerce,  (May  5-June 4,  1971),  p  217.

42401  11  SULFUR DIOXIDE-INSTRUMENTAL-WEST  GAEKE-COLORIMETIC
          A  continuous  analyzing system  is  set up such that
          the ambient air  flows through  a  glass beaded absorp-
          tion  column concurrently with  0.02M sodium tetrachloro-
          mercurate.  Dichlorosulfitomercurate  ion  is  formed
          reacted with  acid-bleached  pararosaniline and
          formaldehyde  to  produce  a  red-purple  pararosaniline
          methylsulfonic  acid  which  is quantitatively measured
          colorimetrically.   The  zero (100%T)   baseline is
          established with pure reagents for 1  hr and the in-
          strument  is then dynamically calibrated with known
          S02  concentration standards.  Air flow rate and
          reagent  flow  rate must be  calibrated and maintained
          accurately.

 42401 13 SULFUR DIOXIDE-INSTRUMENTAL-CONDUCTIMETRIC
          Sulfur dioxide is absorbed -in acidic H202 which
          oxdizes  the S02 to H2S04.   The resulting change
           in conductivity can be measured, compensated for
                              29

-------
           temperature,  and related to the input S02 concentration
           by dynamic calibration with known S02 concentration
           standards. However,  specificity is  poor because any
           materials  that alter  the conductivity of the reagent
           are potential interfering agents.
           1.   Beckman Air Quality Acralyzer Operating and
           Service  Manual,  Scientific and  Process Inst.  Div.,
           Fullerton, California,  16TW352,  (Aug.  1966).
           2.   Thomas, M.D.,  (1932),  "Automatic Apparatus for
           the Determination  of  Small Concentrations of Sulfur
           Dioxide  in Air," Anal.  Chem.  5,  253.
           3.   M. B.  Jacobs,  "The  Chemical  Analysis of Air
           Pollutants,"  Chemical Analysis,  Vol  10,  Interscience
           Publishers, Inc.,  New York, N.Y.,  (1960),  p 394.
           4.   Water,  Atmospheric  Analysis,  (1971),  "Annual Book
           of  ASTM  Standards," American  Society for Testing and
           Materials,  Philadelphia, Pa., Part 23, p 272.

42401 14   SULFUR DIOXIDE-INSTRUMENTAL-COULOMETRIC
           The  air  to be measured  is  passed through a  cell
           containing a neutral buffered iodide or  bromide
           electrolyte where  an electrical current  or  potential
          maintains  a constant concentration of  free  12 or Br2.
          When SO2 in the input air  reacts with  the I2 or Br2,
           the change in electrical current or potential necessary
           to restore or maintain the original concentration of
           12 or Br2  (coulometric titration) is a quantitative
          measure of the S02 input.  If the input flow rate is
          constant, the S02 concentration can be related to
          the electrical signal by dynamic calibration with
          known S02 concentration standards.

42401 16  SULFUR DIOXIDE-INSTRUMENTAL-GC FLAME PHOTOMETRIC
          Chromatographic columns are used to separate SOo,
          H2S, CS2, and CH3SH.   Effluent from the columns is
                            30

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          burned in a hydrogen-rich flame.   A photomultiplier
          tube is used to detect the 395 run emission band
          characteristic of sulfur.  The electrical signal is
          related to the input concentration by dynamic cali-
          bration with known S02> H2S, CS2/ or CH3SH concen-
          tration standards.
          1.   H. H. Willard, L. L. Merritt, and J. A. Dean,
          "Instrumental Methods of Analysis," D. Van Nostrand
          Company, Inc., 4th Edition, 1965, p 309.

42401 33  SULFUR DIOXIDE-DAVIS INSTRUMENT-SEQUENTIAL-CONDUCTIMETRIC
          Water is deionized by passage through an amberlite
          resin column; then its conductivity is measured.
          Ambient air, having first passed through a scrubber
          of amberlite resin and soda-lime to remove C02/ is
          next passed through the deionized water where  the S02
          is absorbed.  The increased conductivity of the water
          is a measure of the SC>2 concentration of the air.
          1.  Thomas, M.D. and J. N. Abersold,  (1929), "Automatic
          Apparatus for the Determination of Small Concentrations
          of Sulfur Dioxide in Air," Anal. Chem. 1,  14.

42602 11  NITROGEN DIOXIDE-INSTRUMENTAL-COLORIMETRIC
          The Lyshkow modification of the Griess-Saltzman
          reagent  is used in various continuous NO2  analyzers.
          Users should consult the manufacturer's  literature
          for details of reagent preparation.
          1.  "Rules and Regulations" Federal Register,  Vol 38,
          No. 110, USGPO Wash., D.C.,  (June  8,  1973), p  15176.
          2.  Lyshkow, N. A.,  (1965), "A Rapid  Sensitive Colori-
          metric Reagent for Nitrogen Dioxide in Air" J. Air
          Poll. Control Assoc. 15  (No.  10) 481.
42602 12  NITROGEN DIOXIDE-INSTRUMENTAL-COLORIMETRIC
          The original Griess-Saltzman reagent  is used  in
          various continuous N02 analyzers.  Users  should
                              31

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           consult  the manufacturer's  literature for details
           of  reagent preparation.
           1.   "Rules and  Regulation,"  Federal Register,  Vol 38,
           No.  110, USGPO,  Wash., D.C.,  (June 8, 1973)  p  15176.
           2.   Saltzman, B.  E.,  (1954)  "Colorimetric Micro
           Determination of Nitrogen Dioxide in the Atmosphere"
           Anal. Chem. 26,  1949.

42602 13   NITROGEN DIOXIDE-INSTRUMENTAL-COULOMETRIC
           Air  to be measured  is  passed through a cell  containing
           neutral buffered iodide-iodine  solution causing an
           established equilibrium between iodine and iodide
           to be unbalanced.   The current  required to re-
           establish the equilibrium  (coulometric titration)
           is a measure of  the input NO? concentration.   If
           the  input  flow rate is  constant, the  N02 concentration
           can be related to the electrical  signal by dynamic
           calibration with known N02 concentration standards.

42602 14   NITROGEN DIOXIDE-INSTRUMENTAL-CHEMILUMINESCENCE
           The ambient air  to be measured  is  drawn over a heated
           catalytic converter which reduces  NO2  to NO.   The
          NO is then analyzed by method 42601 14,  and  the
          original N02 concentration is obtained by subtracting
           the concurrent NO concentration.
           1.   "Rules and Regulation," Federal Register,  Vol  38,
          No.  110,  USGPO, Wash., D.C.,  (June 8,  1973)  p  15176.
           2.  NO/NOX/N02 Analyzer Bulletin,  Bulletin 4133,
          Beckman Instruments, Inc., Fullerton,  Calif.

42602 84  NITROGEN DIOXIDE-GAS BUBBLER-NASN  SODIUM ARSENITE-
          ORIFICE
          The method is much like method  42602  71  except for
          the absorber (l.Og of NaAs02).  Ambient  air  is in-
          troduced  into the absorber by means  of  an orifice
                               32

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          in  the bubbler.   The  orifice  is  usually not cali-
          brated.
          1.   "Rules and Regulation," Federal Register,  Vol 38,
          No. 110,  USGPO,  Wash.,  D.C.,  (June 8,  1973), p 15175.
          2.   Christie,  A. A.,  R. G.  Lidzey, and D.  W. F.  Radford
          (1970),  "Field Methods  for  the Determination of Nitrogen
          Dioxide  in Air."  Analyst 95, 519.
          3.   Merryman,  E. L.,  et.al.,  "Effects of NO, C02,
          CH4/ H2O and Sodium Arsenite  on NO2 Analysis,"
          presented at the Second Conference on Natural Gas
          Research and Technology. Atlanta, Georgia, June 5, 1972.

42602 94  NITROGEN DIOXIDE-GAS BUBBLER-NASN-SODIUM ARSENITE-
          FRIT
          This method is identical to method 42602 71 except
          that l.Og/1 of NaAs02 is added to the absorbing
          solution, and a fritted bubbler is used instead of
          an orifice bubbler.
          1.   Christie, A. A., R. G.  Lidzey, and D. W. F. Radford,
          (1970),  "Field Methods for the Determination of Nitrogen
          Dioxide in Air." Analyst 95,  519.
          2.   Merryman, E. L.  et al.,  "Effects of NO, C02,
          CH., H2O and Sodium Arsenite on N02 Analysis,"
          presented at the Second Conference on Natural Gas
          Research and Technology.  Atlanta, Georgia, June 5, 1972,
          3.   "Selected Method for the Measurement of Air
          Pollutants," U.S. Department of Health, Education,
          and Welfare 999-AP-ll, Robert A.  Taft Sanitary
          Engineering Center, Cincinnati, Ohio, May  1965,
          p  C-4.

44101 11  TOTAL OXIDANT-INSTRUMENTAL-ALKALINE KI
          Identical to method 44101 14 except 1 N sodium
          hydroxide is used instead of the  phosphate buffer
          in the absorbing solution.
                             33

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44101 14  TOTAL OXIDANT-INSTRUMENTAL-COLORIMETRIC-NEUTRAL KI
          Air to be measured is contacted with nuetral
          phosphate buffered potassium iodide.  Oxidants
          convert the KI  to 12  or  KIg  which is measured
          spectr©photometrically at 352 nm.  If the input
          air flowrate is constant, the color density can
          be related to the oxidant concentration.  Analyzers
          are calibrated dynamically with known standard
          concentrations of ozone.  Sulfur dioxide inter-
          ference may be minimized by use of a Cr03 pre-
          scrubber, which also causes an NO interference.
          1.  Intersociety Committee, "Methods of Air
          Sampling and Analysis," American Public Health
          Association, Wash., B.C., 1972, p 356.
          2.  Water, Atmospheric Analysis,  (1971), "Annual
          Book of ASTM Standards," American Society for Testing
          and Materials, Philadelphia, Pa., Part 23, p 518.
          3.  Wartburg, A. F.,  and B. E. Saltzman, (1965),
          "Absorption Tube for Removal of Interfering SO2
          in Analysis of Atmospheric Oxidant" Anal. Chem. 37,
          779.

44101 15  TOTAL OXIDANT-INSTRUMENTAL-COULOMETRIC-NEUTRAL KI
          Air to be measured is passed though  a cell containing
          potassium iodide and two electrodes.  Oxidants
          convert iodide ions to I2 which is reduced at the
          cathode of the cell causing a current to flow through
          an external circuit.   If the flow rate is constant,
          this electrical signal can be related to the input
          concentration of oxidants.  Analyzers are calibrated
          dynamically with known standard concentrations of
          ozone.
                               34

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                  Unacceptable Methods
42101 12   CARBON MONOXIDE - INSTRUMENTAL - COULOMETRIC
           Atmospheric air  is  drawn through a heated
                                                            column
          where I2 is liberated.
                                    The I~ is directed
                                                   is measured
           into an electrochemical cell where
           coulometrically .
           1.   Beckman  Instrumentation, Bulletin 3000 4411-4,
           Beckman Instruments,  Inc., Fullerton,  California.
42401 15   SULFUR DIOXIDE-INSTRUMENTAL-THOMAS AUTOMETER
           The  Thomas Autometer is a conduc time trie analyzer
           developed in 1929.   There are later models.  The
           method is similar to method 42401 13.

42401 31   SULFUR DIOXIDE-DAVIS INSTRUMENT-HYDROGEN PEROXIDE
           The  Davis instrument is a conductimetric instrument,
           and, as such, this method is much  like method 42401 13.

42401 92   SULFUR DIOXIDE-GAS  BUBBLER-WEST-GAEKE
           This method is similar to method 42401 91 except
           that the sample absorbing reagent is 0.1M tetra-
           chloromercurate*,  the starch which is used for
           standardization is made with mercuric iodide;
           and sulfamic acid is not used except when high con-
           centrations of N02 are expected.   The sulfamic
           acid is added to  the sample after collection.
           1.   "Selected Methods for the Measurement of Air
           Pollutants" U.S. Department of Health,  Education,
           and  Welfare 999 AP-11, Robert A. Taft  Sanitary
           Engineering Center,  Cincinnati, Ohio,  May 1965,
           p A-l.
           2.   Nauman, R. V.,  et al. ,  (1960), Anal Chem. 32,
           1307.
                              35

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          3.   West, P.  W. and F. Ordoveza, (1962), Anal. Chem. 34,
          1324.
42401 93  SULFUR DIOXIDE-GAS BUBBLER-CONDUCTIMETRIC
          This manual conductimetric method uses the same
          principle as the instrumental conductimetric
          method.  The absorber is a multiple-jet bubbler
          system and the sampling is not continuous.  The
          details are described in the reference.
          1.  Intersociety Committee, "Methods of Air Sampling
          and Analysis," American Public Health Association,
          Washington, D.C., 1972, p 456.

42602 71  NITROGEN DIOXIDE-GAS BUBBLER-JACOBS-HOCHHEISER-
          50 ml TUBE + ORIFICE
          Ambient air to be measured is bubbled through a.
          sodium hydroxide solution where N02 forms a stable
          solution of sodium nitrite.  The nitrite ion pro-
          duced is reacted with phosphoric acid, sulfanilamide,
          and N-l naphthylethylenediamine dihydrochloride;
          and measured colorimetrically at 540 nm.
42602 72  NITROGEN DIOXIDE-GAS BUBBLER-SALTZMAN  (50 ml TUBE +
          ORIFICE)
          The sample is absorbed in the Griess-Saltzman reagent
          and after 15 min the stable pink color is measured
          colorimetrically at 550 nm; cannot be used for
          sampling period over 30 minutes.
          1.  Intersociety Committee, "Methods of Air Sampling
          and Analysis," American Public Health Association,
          Washington, D.C., 1972, p 329.
          2.  Saltzman, B. E., (1954), "Colorimetric Micro-
          Determination of Nitrogen in the Atmosphere," Anal.
          Chem. 26, 1949.

44101 81  TOTAL OXIDANT-GAS BUBBLER-ALKALINE KI
          Oxidants in sampled ambient air are absorbed in
          an alkaline KI solution in a bubbler.  A stable

                               36

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          product is formed which can be stored with little
          loss  for several days.   Analysis is completed
          by addition of phosphoric acid-sulfuric acid
          reagent/ liberating iodine, which is then determined
          spectrophotometrically at 352 nm.
          1.  Selected Methods for the Measurement of Air
          Pollutants U.S. DHEW 999-AP-ll, RATSEC Cincinnati,
          Ohio, 1965, p E-l.
          2.  Water, Atmospheric Analysis, (1971), "Annual
          Book of ASTM Standards," American Society for Testing
          and Materials, Philadelphia, Pa., Part 23, p 391.
          3.  M. B. Jacobs,  (1960),  "The Chemical Analysis of
          Air Pollutants," Chemical Analysis, Vol 10, Inter-
          science Publishers, Inc., New York, N. Y., p 219.
44101 82  TOTAL OXIDANT-GAS BUBBLER-FERROUS OXIDATION
          Air to be measured is filtered through a Whatman
          No. 4 paper at 1  ft3/min; then bubbled through two
          impingers in series containing acidified  ferrous
          ammonium  sulfate absorbing  solution.  After sampling
          ammonium  thiocyanate is  added, and  the resultant
          color  is measured with a colorimeter  and  green  filter,
          1.  M.  B. Jacobs,  (1960),  "The Chemical Analysis of
          Air Pollutants,"  Chemical  Analysis,  Vol  10,  Inter-
          science Publishers, Inc.,  New York,  N.  Y.,  p 228.

44201 13  OZONE  - INSTRUMENTAL  -  COULOMETRIC
          This method is identical to method 44101 15.
          1.   Mast, G.  M.  and H.  E.  Saunders, (Oct. 1962),
          "Research and Development of the Instrumentation of
          Ozone Sensing," Instrument Soc.  of Amer. Trans.,
          !_, 375.
          2.  Bufalini, J. J.,  (1968), "Gas Phase Titration of
          Atmospheric Ozone," Environ. Sci. Tech. 2, 703.
           3.  wartburg, A. P., and B. E.  Saltzman,  (1965),
            "Absorption Tube for Removal of Interfering S02 in
           Analysis of Atmospheric Oxidant" Anal. Chem. 37, 779,
                              37

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 42602  91   NITROGEN DIOXIDE-GAS BUBBLER-JACOBS-HOCHHEISER (100
           ml  TUBE + FRIT)
           This method is  identical to method 42602 71,  except
           that a fritted  bubbler is used instead of an  orifice
           bubbler and the volume of the absorbing solution is
           doubled.
           1.   "Selected Methods for the Measurement of  Air
           Pollutants/1 U.S.  Department of Health, Education,
           and Welfare 999-AP-ll, Robert A.  Taft Sanitary
           Engineering Center,  Cincinnati, Ohio, May 1965,  p C-4.
           2.   Purdue, L.  J.,  et.al.,  (1972), "Reinvestigation
           of  the Jacobs-Hochheiser Procedure for Determining
           Nitrogen Dioxide in  Ambient Air," Environ.  Sci.
           and Tech.  6, 152.

44101 13  TOTAL OXIDANTS-INSTRUMENTAL-MAST MODEL  742-2
          Identical to method 44101-15.
          1.  Mast, G. M.  and H. E. Saunders,  (Oct. 1962),  "Research
          and Development of the Instrumentation  of Ozorui Sensing,"
          Instrument Soc.  of Amer. Trans., 1, 375.
          2.  Bufalini, J. J.,  (1968), "Gas Phase Titration of
          Atmospheric  Ozone," Environ Sci Technol 2, 703.
          3.  Wartburg, A. P., and B. E. Saltzman,  (1965),
          "Absorption Tube for Removal of Interfering SO2 in
          Analysis of Atmospheric Oxidant" Anal.  Chem. 37, 779,

44101 51  TOTAL OXIDANT-GAS BUBBLER-PHENOLPHTHALIN
          Phenolphthalin,  in the presence of CuSO/}, is
          oxidized to phenolphthalein by ambient  air oxidants.
          Air is passed through 10 ml of reagent  at 800
          ml/min for 10 min.  The color is read using a
          colorimeter and a green filter.
          1.  M. B. Jacobs, (1960), "The Chemical Analysis
          of Air Pollutants," Chemical Analysis, Vol 10,
          Interscience Publishers,  Inc., New York, N.  Y.,
          p 226.
                             38

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                           APPENDIX B
          Rationale  for Ranking the Methods  as   Unacceptable
CO 42101 12
  COULOMETRIC
  Interferences with this method include mer-
  captans, hydrogen sulfide, olefins, acetylenes,
  and water vapor.  In addition, the slow response,
  need  for careful column preparation, and the
  need  for well controlled  temperatures and flow
  rates make  this  an unreliable  procedure.
S02 42401 15
   THOMAS  AUTOMETER
   This  is a conductimetric analyzer.   Data  collected
   using this analyzer should be  reported as 42401-13.
S02 42401 31
   DAVIS INSTRUMENT
   This is a conductimetric analyzer.   Data collected
   using this analyzer should be reported as 42401-13.
 S02  42401
92 WEST-GAEKE BUBBLER
   This method differs only slightly from 42401-91  and
   offers no substantial advantages.  Method 42401-91
   should thus be used for uniformity.
 S02 42401
93 CONDUCTIMETRIC BUBBLER
   The method lacks specificity; Method 42401-91 should
   be used to obtain better measurements.
 N02 42602-71  J-H BUBBLER (orifice)

 N02 42602 91  J-H BUBBLER (frit)
               The objections to these methods have been detailed in
               38 FR 15174 (June 8, 1973):  The collection
               efficiency is a function of N02 concentration and
               the presence of NO  introduces a positive interference,
                                 39

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 N02 42602 72  SALTZMAN
               This  manual  method suffers  from interferences
               from  SO^,  ozone,  PAN,  and prolonged  exposure
               to  light,  and  cannot be  used  for periods
               over  30  minutes.

 TOTAL 0Y  44101  11   ALKALINE  KI-INSTRUMENTAL
        A
               The alkaline KI method produces  such  variable
               results  in different hands  that  data  from one
               site  cannot be compared with  data from another.

 TOTAL Ov  44101  13   MAST MODEL 742-Z
        A
               This  method is identical to method 44101-15.  Data
               collected using this analyzer should be reported
               as 44101-15.
TOTAL Ox 44101 51 PHENOLPHTHALIN
              Results of this method do not agree with those
              obtained by other total oxidant methods,.

TOTAL Ov 44101 81  ALKALINE KI BUBBLER
       A
              The alkaline KI method produces such variable
              results in different hands that data from one
              site cannot be compared with data from another.
TOTAL Ov 44101 82  FERROUS OXIDATION
       A
              Results of this method do not agree with those
              obtained by other total oxidant methods,,

OZONE 44201  13 COULOMETRIC
              This method is identical  to method 44101-15.
              Data collected using this method should be
              reported as 44101-15.
                           40

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                               TECHNICAL REPORT DATA
                        (Please read Instructions on the reverse before completing)
. REPORT NO.
EPA-450/4-74-005
                                                    3. RECIPIENT'S ACCESSION
. TITLE AND SUBTITLE
Designation of Unacceptable  Analytical Methods
of  Measurement for  Criteria  Pollutants
           5. REPORT DATE
            September 1974
           6. PERFORMING ORGANIZATION CODE
            MDAD, OAQPS, QAEML,  NERC-
                                                                                  .TP
. AUTHOR(S)
                                                    8. PERFORM
 PERFORMING ORG \NIZATION NAME AND ADDRESS
 Monitoring and Data Analysis Division
 Office of Air Quality planning and Standards
 Research Triangle Park,  N.C. 27711
                                                     10. PROGRAM ELEMENT
           11. CONTRACT/GRANT NO.
12. SPONSORING AGENCY NAME AND ADDRESS
Office of Air Quality Planning and Standards
Environmental Protection Agency
Research Triangle Park,  N.C. 27711
                                                     13. TYPE OF REPORT AND PERIOD COVERED
           14. SPONSORING AGENCY CODE
15. SUPPLEMENTARY NOTES
is. ABSTRACT  This report contains a designation  of the  acceptability of
various  analytical measurement methods currently in use.  Each monitorinj
method  is placed  into one  of three  categories i.e.,  approved-Federal
Reference Method  (FRM) or  equivalent;  unapproved -  not yet  determined
to be equivalent  to the FRM; and  unacceptable - known to yield measure-
ments of poor accuracy and reliability and  in most  cases obsolete.
                            KEY WORDS AND DOCUMENT ANALYSIS
                DESCRIPTORS
                                         b.IDENTIFIERS/OPEN ENDED TERMS
                                                                 c. COS AT I Field/Group
 Federal Reference Methods
 Unapproved Methods
 Unacceptable Methods
 S02
 TSP
 CO
 N02 and Photochemical  Oxidants
18. DISTRIBUTION STATEMENT
 Release unlimited
19. SECURITY CLASS (This Report!
   None
                                                                 21. NO. OF PAGES
                                         20. SECURITY CLASS (Thispage)
                                             None
                                                                 22. PRICE
EPA Form 2220-1 (9-73)

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