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TRANSBOUNDARY AIR POLLUTION

UN/ECE INTERNATIONAL CO-OPERATIVE PROGRAMME ON EFFECTS ON MATERIALS, INCLUDING HISTORIC AND CULTURAL MONUMENTS

Report No. 10:

ENVIRONMENTAL DATA REPORT SEPTEMBER 1990 TO AUGUST 1991

DECEMBER 1992

PREPARED BY THE ENVIRONMENTAL SUB-CENTRE

I eh I NORWEGIAN INSTITUTE FOR AIR RESEARCH

LILLESTRØM/NORWAY

DATE ISBN

DECEMBER 1992 82-425-0448-2

International Co-operative

Programme on Effects on Materials, including Historic and Cultural

Monuments

Environmental data report September 1990 to August 1991

Jan F. Henriksen, Alena Bartonova, Kari Arnesen and Arild Rode

Prepared by the Environmental Sub-Centre

Norwegian Institute for Air Research

P.O. Box 64, N-2001 Lillestrøm, Norway

Table of Contents

Page

1 Introduction 3

2 The measuring programme 4

3 Data from the monitoring test sites 4

4 Monthly mean concentrations 5

4.1 Gases, temperatures and relative humidity 5

4.2 Precipitation components 5

4.3 TOW and sunshine hours 5

5 Yearly mean concentrations 6

5.1 Yearly mean values 6

5.2 TOW, sunshine hours and amount of precipitation 6

6 Calculations of monthly values 6

7 Results and discussions 8

8 Characterization of the gas data 9

9 References 10

Tables and Figures 11

Annex l 23

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International Co-operative Programme on Effects on Materials, including Historic and Cultural

Monuments

Environmental data report September 1990 to August 1991

1 Introduction

Airborne acidifying pollutants are known to be one major cause of corrosion of different materials including the extensive damage that has been observed on historic and cultural monuments. In order to fill some important gaps of knowledge in this field the Executive Body for the Convention on Long-range Transboundary Air Pollution decided to launch an international co-operative programme. The programme started in September 1987 and involves exposure at 39 test sites in 12 European countries and in the United States and Canada.

The aim of the programme is to perform a quantitative evaluation of the effect of sulphur pollutants in combination with NOx and other pollutants as well as climatic parameters on the atmospheric corrosion of important materials. For this purpose measurements of gaseous pollutants, precipitation and climate parameters have been initiated at or nearby each test site, together with evaluation of corro- sion of the exposed test materials at each site.

A Task Force is organizing the programme with Sweden as lead country and the Swedish Corrosion Institute serving as the Main Research Centre. Sub-centres in different countries have been appointed, each responsible for their own materials group. The materials groups are:

Structural metals, including steel, weathering steel, zinc and aluminium (Sub- centre responsible for evaluation: National Research Institute for Protection of Materials, Prague, Czechoslovakia), copper and cast bronze (Bayerisches Landesamt flir Denkmalpflege, Munich, Germany).

Stone materials, including Portland limestone and White Mansfield dolomitic sandstone (Building Research Establishment, Department of Environment, Watford, United Kingdom).

Paint coatings, including coil coated steel with alkyd melamine,steel with silicon alkyd paint, wood with alkyd paint system and wood with primer and acrylate (Norwegian Institute for Air Research, Lillestrøm, Norway).

Electric contact materials, including nickel, copper, silver and tin as coupons;

Eurocard connectors of different performance classes (Swedish Corrosion Institute and Royal Institute of Technology, Stockholm, Sweden).

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Environmental data storing, reporting and evaluation are the responsibility of the Norwegian Institute for Air Research. The aim of this report is to present all envi- ronmental data available from the fourth year of exposure, September 1990 to August 1991.

The yearly values for all test-sites for all four years are included in this report. To illustrate the quality of the data reported a statistical treatment of some of the environmental data was performed in the environmental report no. 9 (Henriksen et al., 1992). In this report some of the most important conclusions drawn, are sum- marized in chapter 8.

2 The measuring programme

The measuring programme includes a normal programme and an extended pro- gramme.

The measuring programme.

Components to be measured

Normal Gas S02, N02

programme Precipitation mm, pH, S0 ₄ -S, N03-N, c1-, conductivity Climate Temperature, relative humidity, time of

wetness (TOW) and sunshine hours

Extended Gas 03

proqrarnrne Precipitation NH4-N, Na, Ca, Ma, K

The data are to be reported to the environmental sub-centre as daily, weekly or monthly mean values, except for TOW, sunshine hours and mm precipitation which are reported as the sum of the daily values. The data will be presented as monthly and yearly values.

3 Data from the monitoring test sites

The data are sent to the environmental sub-centre on special reporting forms.

Some sites have given the results in ASCII files on diskette.

All data presented by the environmental sub-centre, as in this report, are given with the same accuracy -as in the filled-in reporting forms. For data series which include values "below the detection limit", these are, by convention, replaced with one half of the reported detection limits when calculating the mean values.

The monthly mean values are calculated from the daily or weekly values or used directly if monthly values are the only reported. Information about the data sets used for calculation of the mean values reported in this report is given by letter code

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D = daily records W = weekly records M = monthly records.

Information about the original measuring system for each test site is given the report "Description of test sites".

4 Monthly mean concentrations

The monthly and yearly values are given in the tables in Annex 1. The data have been subject to the following restrictions and classifications:

4.1 Gases, temperatures and relative humidity

For monthly mean values calculated from daily measurements, the percentage of data used in the calculations is listed together with mean values.

A monthly mean value with more than 75% data for a given component is accepted without any remarks.

A monthly mean value for a component with between 50% and 75% of avail- able data has been marked with an asterisk.

A monthly mean value with less than 50% data is reported with an (X).

Monthly values with less than 50% of the data included in the calculations are not recommended used for statistical dose-response treatment.

4.2 Precipitation components

For monthly mean values calculated from daily or weekly rain results, the percentages of the total amount of rain used in the calculations are listed to- gether with the mean values.

A monthly mean value for a component with more than 75% of the amount of rain used in the calculations is accepted without any remarks.

A monthly mean value for a component with between 50% and 75% of the amount of rain used in the calculations has been marked with an asterisk.

A monthly mean value with less than 50% of the amount of rain used in the calculations is reported with an (X). Monthly values with less than 50% of the total rain included in the calculations are not recommended used for further data treatment.

4.3 TOW and sunshine hours

The total sum from the recorded days is adjusted to a complete month by dividing the sum with the numbers of records and multiply with the number of days in the month. The percentage of data used for these adjustment is listed together with the monthly value.

With more than 75% of the values reported, the monthly value will be reported without any remarks.

With between 50% and 75% of the values reported, the monthly value will be reported with an asterisk.

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With less than 50% of the values reported, a monthly value is reported with

an (X). For further data treatment these data are often replaced by estimated

values, see chapter 5.

5 Yearly mean concentrations

5.1 Yearly mean values

All values given for yearly mean values are treated in the same way as the monthly values. If daily results are reported during the whole year, all available daily values are used for the calculation of the mean value. The percentage of available data is also calculated and listed together with the yearly values.

A yearly mean value for observations including 75% of the monthly values is accepted without any remarks. A yearly mean value including between 50%

and 75% of the monthly values is accepted with an asterisk.

A yearly mean value including less than 50% is reported with an (X).

If weekly or monthly values are reported, the monthly values are used in the cal- culations and the percentage is not listed.

5.2 TOW, sunshine hours and amount of precipitation

TOW, sunshine hours and amount of precipitation are reported as the total sum and must be completed to a full year if the results shall be of any use. Since there are seasonal variations in the climatic factors the use of average values for adjusting the results can be incorrect. To complete the yearly results estimated values were used. The estimated values were formed by comparing similar sites, by looking at reported values for other months from the same season or from meteorologic statistics. Only 4 estimated values are accepted for each parameter, and the estimated values are marked with a plus ( + ). If monthly values are available from the previous years, the missing monthly value is substituted with the mean value from the same month for the available years and marked with a (+).

If more than 4 of the monthly values are missing no yearly value is reported.

6 Calculations of monthly values

Mean temperature (TM)

Ti = measured values i = number of records

Mean relative humidity (RHM)

i

LRH;

RHM=-0~- i

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Time of wetness (TOW) (for incomplete data sets see chapter 4.3 and 5.2)

Sunshine hours (sh) (for incomplete data sets see chapter 4.3 and 5.2)

i

TOW=~. TOW

L.,;' '

0

i

sh= L ^sh;

0

Sunshine hours shall report the number of hours where the test panels have been exposed to sunlight. So far no efforts have been made to transform different sun radiation measurements to sunshine hours.

Mean gas concentrations GM

LG; ;

G =-o __

M .

l

For some sites where complete informations of the sampling period exist, another equation is used

n; = sampling period

Precipitation (for incomplete data sets see chapter 4.3 and 5.2)

weighted mean pH (pHM)

;

mm= Lmm;

0

f ^[mm;· (10-pH, )]

pHM =+log- ⁰ - -;- - - -

Lmm;

0

weighted mean values for cations, anions and conductivity (CM)

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7 Results and discussions

The yearly results for the first, second, third and fourth year, are given in Table 1 and the monthly and yearly results from September 1990 to August 1991 in Annex 1. The regularity of the environmental data is comparable to the good results from the third year. However, still there are sites where the influx of data is slower and lower than expected. Corrections of the yearly mean TOW values for sites 24 and 25 have been included in Table 1 for the first, second and third year.

For calculating dose-response equation it is crusial to have complete data sets and

sufficient spread in the values for the most important parameters. If gaps in the

data occur, estimated values must sometimes be generated. To illustrate the quality of the data measured and their yearly fluctuation, scatter plots of the most important parameters are made.

The pattern of the fourth year results is similar to them of the previous years. In

Figure 1-4 scatter plots of TOW, SO2, NO2 and pH for the third versus the fourth year results are presented. The figures show that the environmental condition at the sites do not change too much from one year to the next.

The NO2 results were clustered around the y=x line in the same way as the previous years. The Milan result for the fourth year was somewhat lower than the third year and similar to the first and second year.

The SO2 results were clustered around the y=x line when the fourth year results are compared with the third year. The sites with high SO2-concentrations had higher concentrations the first and second year compared with the two last years.

The TOW results clustered around the y=x line for the fourth and third year. The largest deviations were observed at site 8 Aschaffenburg and site 33 Toledo.

Yearly values for time of wetness are missing for six test sites the fourth year, which is twice as much as for the third year. The main reason is that either too few monthly values are reported or the percentage of values for each month is too low for generating a reliable yearly value.

For pH the largest deviation is observed at the sites Madrid (pH= 6.14), Venice (pH= 6.12) and Wells Cathedrals (pH= 6.22), which had higher values than the year before, and Stoke Orchard (pH= 3.18), which has had a trend towards lower values the last years. By comparing the observed yearly values for each site, it shows that the variation normally is low from one year to the next. 19 of the sites have a variation lower than 0.25 pH units, 14 sites are between 0.25 and 0.80 and only 6 sites have variations above 0.80 pH units.

When the ECE programme started it was important to find test sites with different concentrations of SO2, NO2 and H+ (pH). The figures show that we have been reasonably successful in selecting sites. The yearly mean concentrations for SO2

ranges from I µg/m ³ to 80 µg/m ³ with the majority of sites reporting values below

30 µg/m ^3• For NO2 the distribution is even better with yearly mean concentrations

ranging from 4 to 80 µg/m ³ plus one site (Milan) with more than 100 µg/m ^3•

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The pH was between 3.9 and 6.2 and TOW between 1 800 and 6 000 hours per year. Th ere are also fairly large observed variations for the other precipitation parameters at the different sites. Bilbao (SPA32) has had the highest concentra- tions of ions of all sites. Many of the test sites closer to the Atlantic ocean are more or less affected by marine aerosols contribution. Th is is particularly the case for the sites in the United Kingdom, Lisbon, two Norwegian sites and the sites in the Netherlands. In addition high chloride concentrations are observed at the Italian and Spanish sites.

8 Characterization of the air quality data

In report no. 9 Environmental data report September 1989 to August 1990 (Henriksen, 1992) an extensive statistical evaluation of the results for gas concen- trations was carried out. The main conclusions drawn in this report are still valid and can be summarized as follows:

Mean, median and 90-percentile characteristics of the annual data series were in most cases in good agreement, however, when the data have a distribution that is far from symmetry, their differences may be substantial.

Little difference in the distribution of daily concentrations was found between the three yearly series. Most of the observed differences were due to unequal patterns of missing data. This indicates good quality of the daily reported data.

The three-year and one-year series of gaseous compounds were found to mostly obey log-normal law of distribution, however, the data did not fit either normal or log-normal distribution in more cases than what would be expected by chance. It may therefore be necessary to establish other models. It is reasonable to assume that the deviations from the distribution are to some extent due to seasonal vari- ations, but this hypothesis was not tested.

When calculating annual means of concentrations, the seasonal differences are of most importance; therefore it may be reasonable to construct a rule based on sea- sonal availability of the data rather than on annual availability. Missing of two months in a season may probably be acceptable. However, as illustrated for 03 site 17 four months of missing data will give a biased mean value.

When calculating monthly means, the rules for accepting the mean based on amount of available data were found reasonable. However, if we exclude daily data for calculation of annual means for other reasons than erroneous results, we are loosing information. Therefore we have chosen to use all available daily values for this calculation.

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9 References

Henriksen, J.F., Arnesen, K. and Rode, A. (1991) Environmental data report, September 1987 to August 1989. Lillestrøm, Norwegian Institute for Air Research (UN/ECE international co-operative programme on effects on materials, including historic and cultural monuments. Report No. 3).

Henriksen, J.F., Bartonova, A., Arnesen, K. and Rode, A. (1992) Environmental data report, September 1989 to August 1990. Lillestrøm, Norwegian Institute for Air Research (UN/ECE international co-operative programme on effects on materials, including historic and cultural monuments. Report No. 9) (NILU OR 7/92).

The Swedish Corrosion Institute (1989) Description of test sites. Stockholm (UN/ECE international co-operative programme on effects on materials, including historic and cultural monuments. Report no. 2).

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Tables and Figures

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