coOncawe report no.1/82 so, emission trends and control options in western europe Prepared by CONCAWE’s ad hoc group "$0.5 Emissions” Reproduction permitted with due acknowledgement © CONCAWE Den Haag January 1982@ NOTE ‘The disconinuity of the page numbering is due to some blank pages that had been normally numbered in the original hard copy but left out of the scanned file in order to reduce the digital file size Considerable efforts have been made to assure the accuracy and reliability of the information contained in this publication. However, neither CONCAWE — nor any ‘company participating in CONCAWE — can accept liability for any loss, damage or injury whatsoever resulting from the use of this information. This report does not necessarily represent the views of any company participating in CONCAWEconcawe 10. CONTENTS INTRODUCTION EFFECTS OF SULPHUR DIOXIDE EMISSIONS HEALTH EFFECTS ENVIRONMENTAL EFFECTS ‘TRANSBOUNDARY POLLUTION SULPHUR CONTENT OF FUELS/EMISSION RESTRICTIONS AIR QUALITY CRITERIA/STANDARDS FOR S02 AND SPM ) PARTICULATE MATTE ENERGY GROWTH SCENARIOS PETROLEUM PRODUCT DEMAND FORECASTS OF POTENTIAL SULPHUR EMISSIONS DESULPHURIZATION OF PETROLEUM FUELS _ DISTILLATE DESULPHURIZATION RESIDUE DESULPHURIZATION (RDS) CONTROL OPTIONS GENERAL, FLUE GAS DESULPHURIZATION FLUIDIZED BED COMBUSTION (FBC) CONCLUSIONS REFERENCES: Page uw 13 13 15 19 21 23 23 23 27 27 27 28 29 31COncawe Sulphur dioxide pollution resulting from the combustion of fossil fuels has been the centre of attention for many years Ambient levels of SO, in urban areas decreased significantly during the seventies “due to the increased use of low sulphur fuels, particularly natural gas and desulphurized gas oil and the building of tall industrial stacks for better dispersion of flue gases. Many people are convinced that the sulphur problem in Western Europe is now largely under control and that there is no real evidence of risk of damage caused by the current ambient levels, On the other hand, some authorities are tending to create more and larger zones of special protection. The identification of long distance transportation of pollutants by air (transboundary pollution) resulted in requests - mainly from Scandinavian countries - for the development of a common European policy to further reduce sulphur emissions, Some intergovernmental advisory organizations are also supporting suggestions for additional control. CONCAWE has in the past studied and reported on many aspects of the European sulphur problem, Now, in the light of recognizable trends in energy supply and demand and the consequent changes in European refining patterns, CONCAWE has re-examined the industry's view with regard to emission trends and technical/ economic implications of controls which may be applied to sulphur emissions.conca we HEALTH EFFECTS The main problem in attempting to quantify the effects of SO, on health is that of isolating them from the possible effects of other coincident atmospheric pollutants, in particular suspended particulate matter (SPM). The effect of high concentrations of SO, is apparent. After, 30 minutes exposure to ambient concentrations of 14000 ug/m? most individuals will show a pulmonary response. Certain sensitive individuals will already show such response at 3000 g/m level. However, at typical ambient concentrations epidemiological studies have not been able to separate the effect of SO, from that of SPM. Some experts have even concluded that, in the absence of suspended particulates, SO, at these lower concentrations is not a significant health hazard. In the "Environmental Health Criteria" series (No. 8: Sulfur Oxides and Suspended Particulate Matter, 1979)(1) the World Health Organization published the following expected effects of sulphur dioxide/suspended particulates (smoke) on health: Short term exposure: Expected effects — ° SO, ‘Smoke | Excess mortality among elderiy people or patients | 500 500 with pulmonary diseases Worsening of the 1 condition of patients 250 250 with existing respiratory disease | 24 hours mean concentration o/m? Long term exposure: Annual mean concentration g/m? Expected effects SO, ‘Smoke Increased respiratory | | | symptoms among adults and children and in 100 100 | creased frequencies of respiratory linesses among childrenThe absence of a clear correlation between sulphur dioxide levels and health effects has led some experts to suspect that aerosol sulphates, as distinct from S0,, are responsible for causing adverse human health effects. However, the evidence to-date is inconclusive. ENVIRONMENTAL EFFECTS The possibility of reduced crop yield and damage to vegetation caused by chronic exposure to low concentration of SO, (< 50 g/m) is currently attracting attention from farming groups in some countries. Such evidence as there is to-date is inconclusive but research in this respect is continuing. Apart from the interests of the agriculturalists, much of the current environmental concern is directed towards aesthetic effects. This is especially so in the case of sulphur oxides which through the formation of sulphate aerosols have also been linked with impairment of visibility. The Commission of the European Economic Community is currently working on a four-year programme to study the chemistry of pollutants in the atmosphere and this may highlight further aspects of SO, pollution. Acidification of rain or the presence of SO, in humid air can accelerate the deterioration of various matérials; e.g. metals can be affected as well as carbonaceous building materials, fabrics, old stained glass windows and certain paints. There is also concern that sulphur and nitrogen oxides deposited by rain increase the acidity of fresh water but the relation between emissions and ecological damage is still not entirely clear. There are claims that as a result of transboundary pollution and consequent "acid rain" the lakes of southern Scandinavia have become acidic to the extent that fish populations are being severely depleted. It is feared in addition that the soil structure may be adversely affected in the long term. There is, however, also the view that naturally occurring weak acids, together with the poor buffering capacity (calcium deficiency) of the soils in these areas contribute to this acidity.TRANSBOUNDARY POLLUTION Several studies in Europe, U.S.A. and Canada have now confirmed that Sulphur compounds can travel long distances in the atmosphere. Thus a proportion of emissions in one country can be transported to neighbouring countries and consequently influence the air quality and acid deposition there. In north-west Europe a major study of the long-range transport of air pollutants was co-ordinated by the Organization for Economic Co-operation and Development (OECD) over the period 1972-78. The OECD study involved the detailed assessment of measured pollution levels in eleven countries for the year 1974, the compilation of SO, emission inventories for that year and the use of computer models incorporating meteorological data, to estimate the contribution that each country made to the sulphur deposition in other countries. ‘The study concluded that deposition was greatest in the area of the emitting sources and declined with distance. In most parts of Eurone dry deposition exceeded wet deposition except in areas of high precipitation. It was also concluded that during 1974 the Netherlands, Germany and the U.K. were net exporters, whereas Norway was a net importer of airborne sulphur. However, only 1% of the total Western European emissions were found to have been deposited in Norway and 2% in Sweden, Furthermore, the study failed to identify the source of 40% of Norway's total sulphur deposition. It has been suggested that this was due to very long-range transport from sources outside Western Europe, to natural sources, or to local sources not accounted for in the models. Due to limitations and assumptions used in the models, the calculated depositions may only be accurate to a factor of two. In 1978, OECD repeated the calculations with the inclusion of an improved deposition simulating model. The results of this study have not yet been published, but OECD do intend to produce a more refined sulphur pollution map of Europe. In November 1979, thirty-five countries meeting under the auspices of the United Nations Economic Commission for Europe (UN-ECE), signed a convention, committing the member countries to study the problem of trans-boundary pollution. The signatories agreed to set up research programmes for the study of the transport and deposition of sulphur compounds in addition to monitoring the work already accomplished in Europe3.1 Icawe LEGISLATION AN ) REGULATIONS SULPHUR CONTENT OF FUELS/EMISSION RESTRICTIONS Most European countries have legislation with respect to sulphur contents of various petroleum products. ‘The "Sulphur in Gas 0i1" Directive of the Council of European Com- munities (2) has now been ratified by all member states, limiting the sulphur content of gas oils, effective 1.10.1980 to 0.3% wt (for unrestricted use) or to 0.5% wt (for use in zones where ground level concentrations of atmospheric SO, pollution are sufficiently low, or where gas oil accounts fér an insignificant proportion of atmospheric SO, pollution). Sweden has also set the sulphur limit of gas oi18 at 0.3% wt; Greece, Portugal, Spain and Switzerland apply a 0.5% wt restriction, whilst the current limit in Austria, Finland and Norway is 0.8% wt. The sulphur content limits specified for fuel oils vary from country to country. In general the national regulations aim at Protecting specific zones or areas. In Belgium, Germany, France, Norway and Spain the sulphur content specifications are linked to restrictions on SO, emissions. Such restrictions relate to specified zones or aréas and/or to types/sizes of installations burning the fuel. AIR QUALITY CRITERTA/STANDARDS FOR SO, AND SPH ™ Proper definition of air quality criteria/standards is a Prerequisite for the introduction of control measures. There are currently a number of these criteria/standards, confusingly referred to as guidelines, target values, objectives, etc. They vary with regard to time scales of exposure and degree of accounting for suspended particulates. There is a tendency towards legally specified maximum permissible concentrations; however, until now only Germany has adopted a legal standard (140 ‘ug/a3 annual average for S0,). suspended particulate matterIn the "Environmental Health Criteria” series (No. 8: Sulfur Oxides and Suspended Particulate Matter, 1979) the World Health Organization proposed the following "guidelines" for exposure limits consistent with the protection of public health: Concentration g/m? * 80 ‘Smoke 24 hours mean 100 - 150 | 100 - 150 Annual arithmetic mean | 40- 60| 40- 60 * Values for S02 and smoke as measured by OECD or British standard daily smoke/SO2 method, On 15th July 1980 the Council of the European Communities adopted a Directive (80/779/EEC) (3) concerning air quality values for 80,/SPM in the atmosphere. The Directive requires Member States to“install measuring networks, to identify by October 1982 the areas which, by April 1983 will not be in compliance with the Limit values in the following tables, and to submit their plans for achieving compliance in all areas "as soon as possible and by April 1993 at the latest". Limit values specified in Directive 80/779/EEC for, respectively, sulphur dioxide and suspended particulates, are reprinted on the following page (reference Official Journal L.229 of 30.8.80).COncawe Limit values for sulphur dioxide expressed in yig/m? with the associated values for suspended particulates (as measured by the black-smoke method (*)) expressed in g/m? Reference period Limie value for sulphur dioxide smears rata] suspended paruculates 80 40 (median of daily mean values | {median of daily mean values taken throughout the year) taken throughout the year) Year Ro =40 (median of daily mean values | (median of daily mean values taken throughout the year) taken throughout the year) 130 >60 (median of daily mean values | (median of daily mean values ‘taken throughout the winter) taken throughout the winter) ‘Winter (1 October to 31 March) i <0 (median of daily mean values taken throughout the winter) (median of daily mean values taken throughout the winter) Yer (made up of units of measuring periods of 24 hours) (98 percentile of all daily mean values taken throughout the year) (98 percentile of all daily mean values taken throughout the year) 250 @) > 150 (98 percentile of all daily mean ‘values taken throughout the year) 350.) <150 (98 percentile of all daily mean values taken throughout the year) Limit values for suspended particulates (as measured by the black-smoke method (*)) ‘expressed in jig/m? Reference period Year Winter (1 October to 31 March) Year made up of units of measuring periods of 24 hours) ‘value for suspended particulates 80 {median of daily mean values taken throughout the yeat) 130 (median of daily mean values taken throughout the winter) 250.) (28 percentile of all daily mean values taken throughout the year) (0) The results of the measurements of black smoke taken by the OECD method have been converted into gravimetric units as described by ECD. 2) Member States must take all appropriate steps to ensure that this value is not exceeded for more than three consecutive days. Moreover, Member States must endeavour to prevent and to reduce ny such instances in which this value has been exceeded.concaw ENT LEVELS OF SO,/SUSPENDED PARTICULATE ENT LEVELS OF SQ,/SUSPENDED PARTICULAT IN EUROPEAN CITIES Direct comparison of the absolute levels of S0,/SPM between various cities is difficult since analytical methods differ and definition of what constitutes a city varies; some cities’ monitoring systems include peripheral sites, others do not. Even so, what can be demonstrated is that with few exceptions the S0,/SPM pollution levels have been significantly reduced in European cities between the sixties and the seventies. The table below is illustrative and shows annual averages. $0, palm? SPM g/m? ] % % | Fre6er6a | 1976/77 | reduction [1971 [1974/76 | reduction anewerp | 130 | 60 |e =| 18 | 46 | | Hamburg 10 | 75 se} | - | | Lyon 82 70 15 | 68) 47 | 31 | | woseite =| 198 |) 100 ef a] ew | sn wo | m]u | -| - | - | | rowedam | 108 | 56) a 9 27) we | a Lt 1 “The UK tends to publish statistics by regions, but the monitoring stations are generally located in urban situations. N..England includes Teesside, Newcastle, whilst NW.-England includes Manchester and Liverpool. Sulphur dioxide levels vary considerably between summer and winter, winter levels being in general 1.5 or more times the annual mean, Daily concentrations show even greater variation, e.g. against the annual averages quoted above, maximum daily SO, levels during 1977 reached about 500 g/m? and even higher if a number of large European cities. The main causes of the reduction in ground level S0,/SPM concentrations in urban areas are: - the introduction of the use of high stacks in industrial sites for increased dispersion of flue gases; aconcaw - reduction in coal burning for domestic heating; - replacement of light residual fuel oil (3% sulphur) by distillate gas oil for domestic heating; - increased use of natural gas, the share of which in the EEC primary energy balance rose from 1.5% in 1960 to 16% in 1975; - limitations on the sulphur content of heating and diesel oils, and to some extent heavy fuel oils; - energy conservation measures, with a trend in some countries towards district heating. 12ENERGY AND PETROLEUM PRODUCT TRENDS Since, in the field of energy production, fossil fuels (coal and oil) are the primary source of sulphur omissions, it is essential to examine the future use of these fuels to establish whether additional emission controls will be necessary for environmental reasons and to select the most effective methods of control taking account of cost and energy conservation factors. Because implementation of some control options could require five years or more and the necessary equipment would be expected to have an economic life of at least 20 years, energy requirements and usage patterns must be studied for the long term; the year 2000 has been selected as an appropriate future point for which predictions may be made. When considering future energy requirements account must be taken of the effects on economic growth of the squeeze by producing countries on oil supply and the continuing spiral of increased oil prices. These concerns are reflected in European governments’ policies to reduce their dependence on imported oil by - encouraging the more efficient use of energy; - replacing the use of oil by other forms of energy (such as coal/nuclear) where practicable; - reserving oil predominantly for those uses, such as transportation fuels and chemical feedstocks, for which no viable substitutes are available at present. The electricity generating and industrial/commercial heat sectors offer the largest potential for replacing oil by other energy sources and since there is a considerable price differential in favour of coal, there is an economic incentive to do so. Nuclear energy also offers an opportunity for reduced dependence on crude oil, and because of this it is anticipated that power generation from nuclear sources will increase. Since the residual fuel oil used in the electricity and industrial sectors is the predominant source of sulphur emissions from petroleum products, consideration of the future demand and availability of this material will be a central aspect of the following sections. ENERGY GROWTH SCENARIOS There is a general consensus that the rate of progression of the energy growth index experienced in the late 60s will slow down significantly in the 80s. Some authorities consider that current economic circumstances could result in a zero, or even negative growth rate. 13concawe For the purpose of these studies which span a 25-year period between 1975 and 2000, CONCAWE has chosen constant energy growth rates of 1 and 2% per year. Zero or negative growth rates have not been evaluated since the SOz emissions would be less than in the above cases. In developing these scenarios, the following assumptions have been made: - 1975 was chosen as the base year because it reflected the situation after the first oil crisis. - There will be a continuing increase in the demand for natural gas and coal, the rate of increase being greater for the higher energy growth rates. This, in turn, assumes increased production and importation of gas, and possibly coal, by various means into Western Europe. - The projections for crude oil take account of the need for most governments to change their energy base away from imported crude oil for reasons of external balance of payments and the security/continuity of energy supplies. - The growing demand for transportation fuels will be met by increased conversion of residue which will reduce the availability of fuel oil, this deficit in turn being balanced by a reduced demand for fuel oil due to competition from coal and non-fossil energy in the electricity and industrial sectors. = Most of the increase in overall energy consumption will be provided from coal or non-fossil sources. In support of this, reference may be made to the May 1980 TFA Ministers’ meeting offering support to any recommendations for action needed to double coal production and use by 1990, and the work of the IEA Coal Industry Advisory Board to achieve that target and the further objective of tripling coal production/use by 2000. The following table shows the resulting primary energy pattern (in million tonnes fuel oil equivalent) for the EEC Member States: 14concawe Year 1975 | 2000 Eneray growth rate/year | 2% Tose | 2 | 50 Natural gas 142 | 240] 265 Crude oil 496 | 980] 400 | Non-fossi | 48 | 197] 450. (320)" Coal + lignite 198 | 315 | 335. (465)" * In event of short-fall in nuclear programme, These projections would indicate that between 1975 and 2000 oil Consumption would decrease significantly under any realistic scenario, The share of oil in total energy demand would fall from about 55% in 1975 to about 30% in 2000. Farlier forecasts by EEC for the year 2000 indicated a total energy requirement of 1.640 million tonnes/year compared to 1.450 million tonnes/year as the maximum in the CONCAWE cases considered. However, the share of crude oil in the BEC projection is 35% compared to 28% in the CONCAWE case which places a greater emphasis on the need for W. European countries to reduce their dependence on crude oil imports. With respect to the interim period, the Tokyo Agreement limit for oil imports to EEC of 472 million tonnes/year in 1985 and the IEA expectation that the oil share in total energy would decline to about 40% by 1990 indicates that demand for oil may well peak in the interim, between 1975 and 2000, ‘These estimates underline the fact that there is unlikely to be any expansion in European primary oil refining capacity. However, extensive investment for conversion facilities will be required in most of the existing refineries. PETROLEUM PRODUCT DEMAND The assumptions made in developing the total energy scenarios include changes in the usage of oil so that the limited quantities available will be used predominantly for those purposes for which no practical or economic substitute fuel is available e.g. transportation fuels and feedstocks for chemical synthesis. 15con we The following tabulation shows the pattern for petroleum products in 2000 (million tonnes of oil), related to the assumptions and objectives mentioned in the previous section with a comparison to the base case of 1975: 1975 2000 Energy growth rate/year = 1% 2% | LP.Gskerofrefinery gas | 34 6.9) | 3810.0) | 40(10.0) Motor gasoline 76(15.3) | 100(26.3) | 100(25.0) Gas oils 149(30.0) | 1231324) 133(33.3) Non-energetic" bunkers | 67(13.5) | 67(17.6) | 67(16.7) | Fs oils (inland) 170(34.3) | 52(13.7) | 60(15.0) L * including naphthas (Figures in brackets are percentages on crude oil) Total petroleum products | 496( 100) | 380{ 100) | 400{ 100) The products have been grouped in this table in respect of their potential for emitting sulphur into the European atmosphere. For example: - LPG/kerosine/refinery gas and motor gasolines have a negligible sulphur content - Gas oils, although representing a substantial provortion of petroleum fuels in Europe, have a relatively low sulphur content of in general 0.3%. - Non-energetic applications, such as lubricants, bitumens and chemical feedstocks do not emit sulphur compounds to the atmosphere. - Inland fuel oils contain residual components which may have sulphur contents in the range of 1%-4.5% depending on the type of refining operation and the crude oil being processed. - Marine fuels may contain higher proportions of high sulphur residual components than inland fuel oils. However, marine fuels are burnt mainly at sea and are not considered to contribute significantly to European sulphur emissions. Examination of this table indicates that the principal change with respect to sulphur emissions is the reduction in inland residual fuel oil consumption from 170 million tonnes in 1975 1618 COnGée to between 50-60 million tonnes in 2000. This change will result from an alteration in the existing petroleum refining pattern in Europe to increase the proportion of distillate material and to reduce the "residual" products (fuel oil plus marine bunkers and certain non-energetic products) from about 44% of the crude oil barrel to about 25% by 2000. It should be noted that although constant annual rates of increase have been assumed for total energy demand between 1975 and 2000, it should not be assumed that there will be constant rates of change in demand and availability of the various types of energy/fuels over that period. There will be a degree of rigidity in the demand/supply pattern related to ‘the time needed to increase the supply of coal/non-fossil energy and to convert installations from oil to coal firing. 1CONE On the basis of the foregoing energy scenarios and product demani patterns, the combustion of fossil fuels in EEC Member States inthe year 2000 is likely to generate S02 in the quantities shown in the table below. These figures, in million tonnes of sulphur/S0j, have been calculated using the following assumptions concerning the effective sulphur content of the fuels. The coal/lignite value is on a "fuel oil equivalent” basis and allows for 10% of the sulphur being retained in the ash: Sulphur content ~ wt.% Year 1975, 2000 Gas oils 0.5 0.3 Fuel oils 2.5 2.5 Coal + lignite 1.5 1.5 Towne | 80 | ear] €a0) 090] 12.74 | 13.80 | 1780 —— 260 | 27.0 | | i * In event of short-fall in nuclear programme. ** Excluding marine fuels Potential SO emissions | 18.0 % Contribution from oil | 62.0 l 21.0 | The above figures indicate that potential 0, emissions, i.e. the amount corresponding to the effective sufshur content of the fuels prior to any measures to remove 80, either during or post-combustion, is likely to be lower than the 1975 emissions in the 1% and 2% cases chosen. Only in the event of a short-fall in the assumed nuclear vrogramme, or in the extreme case of a 3% growth rate, would the level of 1975 emissions be exceeded. Even more significant is the indication that the contribution from petroleum products will decline drastically, both in absolute terms and as a proportion of total SOg emissions, from 62% in 1975 to about 27% in the year 2000. 19PETROLEUM REFINING PATTERNS Atmospheric distillation, the basic process in all crude oil refineries, separates the crude oil into "fractions" on the basis of their boiling range characteristics. For the purpose of this discussion, three broad fractions will be considered: - light distillate (L.P.G., motor gasoline, naphtha, kerosine) - middle distillate (diesel/gas oils) ~ atmospheric residue (fuel oils, bunkers, lubricants, bitumens) By taking advantage of crude oil characteristics, it is possible to produce a limited range of product patterns direct from a blend of crudes, using a simple "hydroskinming" refinery consisting of atmospheric distillation units, naphtha reformers, hydrotreaters for light distillates, and hydrodesulphurization facilities for the middle distillate fractions. In practice this is no longer sufficient due to the limited and variable availability of appropriate crudes to the refinery and the necessity to adjust production to changing market demand. Therefore there will be a continuing need for refiners to install additional vacuum distillation and conversion capacity such as catalytic cracking, thermal cracking or coking facilities, The application of these processes will have two important consequences with respect to the future control of sulphur emissions from petroleum products: - Firstly, a considerable amount of sulphur will be removed throvgh treating the distillate products of the additional processes and recovering sulphur from the Process gases - Secondly, the reduced quantities of residues resulting from these processes will have characteristics which render them msuitable as feedstocks for currently proven residue desulphurization processes. To illustrate these effects, a simple refinery with only atmospheric distillation and the associated distillate hydrotreating/bydrodesulphuri zation facilities may recover about 17% of the sulphur contained in the crude oil feed and produce atmospheric residue equal to some 42% of the crude input (4). The inclusion of a vacuum distillation unit plus associated catalytic cracking facilities could increase the recovered 21Cone: we sulphur to 42% of that in the crude, eliminate all the atmospheric residue and produce a vacuum residue amounting to less than 20% of the crude oilinput to the refinery. In the extreme case, where a coking unit is installed, the vacuum residue fraction is eliminated and more than 90% of the crude oil sulphur content is recovered in the refinery. Taking account of these trends, it is extremely unlikely that residue desulphurization for the production of low sulphur fuel oil will be a processing option in Zuropean refineries, particularly since the availability of suitable residue feedstocks will decline markedly. 22DISTILLATE DESULPHURIZATION Desulphurization of gas oils and other middle distillates is a widely known process, applied in many European refineries. The process consists of treating distillate fractions with hydrogen under pressure in the presence of a catalyst. The process consumes about 3.5% fuel on intake and cost figures for 1980 are inthe order of $ 14-18 per tonne of feed, depending on size of unit and associated sour gas treating units required. It was calculated (CONCAWE report No. 13/72) (5) that a 0.3 wt % sulphur limit for gas oils shows the optimum cost/benefit relationship for desulphurization. To achieve a gas: oil pool with a sulphur content of less than 0.3 wt %, requires a disproportionate increase in desulphurization costs. This is because the initial reduction to 0.3% is achieved by processing a relatively small volume of high sulphur gas oil To achieve afurther reduction it is necessary to process larger volumes of lower sulphur fractions from which only a small amount of sulphur can be removed. For instance to go from 0.3wt % sulphur to 0.2% requires the desulphurization of a gas 6i1 volume which is twice as great as the volume required to reduce the gas oil pool from 0,5 wt to 0.3 wt % sulphur. RESIDUE DESULPHURIZATION (RDS) The direct desulphurization process operating at high temperature and pressure with hydrogen in the presence of a catalyst can be applied to residues resulting from crude oil distillation. The main problems with residue desulphurization are deactivation of the catalyst, e.g. by metals, and fouling of the reactor. Therefore, the heavier vacuum residues which contain higher concentration of metals, are more difficult to treat. Cracked residues cannot be processed with currently available technology. The theoretical hydrogen consumption would make this option prohibitive. Residue desulphurization is relatively new with only limited commercial experience available. Sulphur removal from atmospheric residue can be as high as 90%, whereas removal from vacuum residue is unlikely to be higher than 80%. Three important facets of residue desulphurization need to be highlighted: 1) The lead-time to design, install and commission any residue desuiphurization plant is certainly not less than five years. It will be expected to operate for at least 15 years, This emphasizes that such a 23con IGaV commercial plant must be viable in the year 2000 as well as in 1985. ii) Considerable energy penalties are incurred by residue desulphurization. Atmospheric residue desulphurization consumes energy equivalent to about 10-12% of the residue based on output, and for vacuum residues this increases to over 16%. (For flue gas desulphurization the energy consumption may be about the same order of magnitude as for atmospheric residue desulphurization and therefore will be considerably less than for vacuum residue desulphurization). iii) The availability of residues suitable for desulphurization will be a key factor in any decision to build an RDS plant. In this respect it should be noted that very Little atmospheric residue is likely to be available after the mid-1980s, Further, the increasing difficulty of guaranteeing a reliable supply of a given crude to a refinery would require careful selection of the residue desulphurization plant to be installed to ensure operating flexibility on a variety of residues. For example, it is most unlikely that a refiner would wish to build a residue desulphurizer specifically for a medium sulphur feedstock. Rather, the unit would be designed for a more severe desulphurization duty. The efficiency of the process and the operating costs would vary significantly when desulphurizing feedstocks with characteristics different to those for which the unit was designed. The large variety of possible feedstocks ~ in terms of difficulty of desulphurization ~ makes it practically impossible to produce typical investment and operating costs. However, to illustrate the above points, CONCAWE has examined the desulphurization of both atmospheric (4% S) and vacuum ©.5% S) residues from Kuwait crude to produce a maximum quantity of 1% S product (6). Kuwait was chosen because it was the only feedstock for which adequate comparative data were readily available to CONCAWE, but it must be stressed that these residues have relatively low metals content and the sulphur is of a type which is relatively easy to remove. They are, therefore, among the easier residues to desulphurize. The losses and energy requirements of desulphurization are substantial. There are three elements to be taken into account when considering the material not appearing in the low sulphur fuel end-product: - firstly, the sulphur; secondly, the carbon lost as COg in the Hg production; thirdly, the energy requirements for the process. 24These losses and energy requirements to produce a 1% S product from Kuwait residues will fall within the ranges given in the following table and are reported as equivalent tonnes of residue feed lost per 100 tonnes of low sulphur end-product. | Equivalent Tonnes Feedstock Consumed/ 100 Tonnes Product Atmospheric residue | Vacuum residue Total loss and energy ‘comprising: 10.6 — 12.2 164-194 — Sulphur removed 31- 34 82-54 Hy Production (C09) 22-27 33-46 | | — Energy requirements B1~ 62 73-94 In terms of 1980 values, the cost for desulphurizing the Kuwait atmospheric residue ranges from $ 40-51 per tonne of 1% S product for atmospheric residue valued at $ 150 per tonne. For Kuwait vacuum residue, the cost for desulphurization ranges from $ 67-88 per tonne of 1% 8 product for vacuum residue valued at $ 125 per tonne. In both cases a yearly capital charge of 25% on investment has been included and a credit of $ 200 per tonne for the recovered sulphur has been taken into account. It is recognised that some light products are produced by these processes and that the resulting 1% S product will have a lover viscosity than the feedstock, but the variations in the circumstances of individual refineries and market conditions make it impracticable to consider the economic implications of this. Any such calculation would be valid only for a specific circumstance and, in particular, dependant on the long-term continuity of those circumstances. Therefore, it is considered that this aspect would not alter the overall conclusions concerning the vibility of RDS units. It should be noted that processing residues from different crude oils which are more wifficult than Kuwait to desulphurize would result in a considerable increase in cost. To illustrate this, a comparison has been made between two residue desulphurization plants producing 1% sulphur fuel oil, one being designed specifically for processing Kuwait vacuum residue and the other being designed specifically for processing Arabian Heavy vacuum residue. ‘The comparison indicated that, in terms of low sulphur product, desulphurization in the Arabian Heavy case compared to the Kuwait case required: - 16% greater hydrogen consumption - a gross energy and loss, in terms of feedstock which 25con we disppears, increased by up to 13% - a capital investment increased in the range 15 - 20% Under these circumstances, the overall effect on desulphurization cost per tonne of low sulphur product will be an increase in the order of 15% for Arabian Heavy versus Kuwait vacuum residue. However, the availability of different crudes is a subject of great uncertainty. The only indication is that the proportion of heavier high sulphur crudes is likely to be greater in the future. For reasons relating to operational flexibility, it is unlikely that the refiner would wish to construct residue desulphurization units which have been designed specifically for feedstocks having lower sulphur content than Kuwait residues and the unit may have to process more difficult feedstocks under certain circumstances The variety of crudes makes it virtually impossible to study all cases and the effect of processing other residues from different crudes can only be indicated in very simple qualitative terns based on the sulphur content and the concentration of complex hydrocarbon and metal compounds. Taking Kuwait residue as reference at 100, other Middle East atmospheric residues may range from 60 to 115 as an indication of the relative ease of desulphurization, e.g. for a residue with high sulphur and metals content and higher proportion of complex hydrocarbons such as Arabian Heavy, the desulphurization capacity for agiven unit designed for Kuwait could be about 60% of the Kuwait feedstock base case, assuming that sufficient hydrogen could be made available. On this basis, a rough estimate for the cost of desulphurizing Arabian Heavy atmospheric residue (4.5% S) and vacuum residue (5.7% S) would be between $ 67-85 and $ 105-140 per tonne of 1% S product respectively For the few residues which are easier to desulphurize than Kuwait the intake of a given unit could be expected to increase by some 15%, and the resulting sulphur content of the product could be less than for Kuwait feedstock. However, the net unit operating costs will be only slightly reduced since the fixed costs of the plant remain unchanged. For example, if feedstocks of lower sulphur content are processed in a unit designed for Kuwait residue, the capacity will be limited by feed punips and reactors will be under-utilized, and with fixed costs of the plant unchanged, the net unit processing cost will only be slightly reduced by the portion related to lower hydrogen consumption. Therefore, it is not possible to interpolate desulphurization costs for feedstocks between 4.0 and 1.0 wt. % sulphur. It should be noted that in the event that residue desulphurization units might be constructed, they would not be operational before about 1985 and the cost data presented above would be subject to adjustments for inflation and increases in crude oil prices which may occur after 1980. 262 GENERAL, The preceding analysis of the energy and petroleum product trends shows that total potential sulphur emissions from fossil fuel combustion in Europe are likely to be lower than, or of the same order of magnitude as, 1975 emissions, and that between now and the year 2000 coal is likely to be the predominant source of S02. Various types of technology are available, or under development, for controlling sulphur emissions before, during, or after fuel combustion. The costs and energy requirements for desulphurizing petroleum fuels have been described in detail in the preceding sections (8.1 and 8.2). Highlights of the technical and economic implications of other major control options such as flue gas desulphurization and fluidized bed combustion are given below. It should be noted that these may be applied to the control of sulphur emissions from both liquid and solid fuels. The development of strategies to control sulphur emissions should consider all available technologies and determine their optimum application, taking into account trends in primary fuel availability in the area concerned, e.g. the declining availability of residual fuel oils and the forecast increase in coal consumption. FLUE GAS DESULPHURIZATION Flue gas desulphurization, also referred to as "stack gas scrubbing" is a process in which SO, is removed from the flue gas by absorption or adsorption. There are non-regenerable systems such as scrubbing with lime or limestone slurry or with alkaline solutions. These may lead to problems in disposal of the resulting calcium sulohite/ sulphate mixtures, In some countries full oxidation to gypsum as a saleable product is favoured. Regenerable systems use magnesium oxide (which reacts with SO to form magnesium sulohite which is then calcined to regenerate the magnesium oxide) or sodium sulphite to obtain bisulphite. Citrate, carbon and conver oxide adsorption are some other potentially available systems. The final product from regenerable processes may be concentrated $0), sulvhuric acid, or elemental sulphur. 27Most processes can achieve up to 90% removal of SO,. Energy consumption is in the order of 10% of fuel burned.”This is about the same as the energy requirements of atmospheric residue desulphurization, but only one half to two-thirds of that required for vacuum residue desulphurization Flue gas desulphurization may be used to control emissions from both coal and oil fired sources, although there are differences with regard to selecting the ovtimum process. The aplication of the technique may be envisaged for sources of large scale continuous emissions. For smaller or seasonal sources the unit investment and operating costs will be significantly higher FLUIDIZED BED COMBUSTION (FBC) Fluidized bed combustion of either liquid or solid fuels is viewed as a potentially energy efficient technology that can also have environmental advantages. The concent is a break with traditional boiler firing. It consists of a combustion chamber, partly containing a bed of crushed particles, measuring 1.5-3 mm diameter, of sand, firebrick or limestone. The particles are set into violent and random flotation by blowing evenly distributed air through the bed. Fuel is then injected into the bed at a rate which vermits total combustion with the fluidizing air. Tubing carrying the heat exchange medium (water) is immersed in the bed The addition of limestone or dolomite to the bed can result in 80-90% of the fuel sulphur being retained. The bed burns at a relatively low temperature of 800°C compared with say 1800°C in conventional firing systems, which reduces the formation of nitrogen oxides. FBC systems operate under either atmospheric or pressurized conditions. Pressurized systems have the advantage in that the hot gases can be used to drive a gas turbine in addition to the steam turbine driven by the steam generated in the tubing immersed in the bed. Disvosal of the solids, including the ash, from FBC systems reoresents a problem. Develovment work in the U.K. and U.S. is currently being directed towards. regeneration of bed particles to reduce the quantity of waste for disposal. FBC is recognized as having the greatest notential application for small scale industrial usage. However, it must be realized that FBC is a new technology which is still in the pilot plant testing phase. Commercial availability of atmospheric systems is expected in the mid-1980s; pressurized systems may not be developed before the end of the decade. 28ne 10. CONCAVE studies on SOj emission trends in Western Europe and on the direct desulphurization of residues (Report No. 5/81) (6) lead to the following conclusions: 1. 5. Within the range of CONCAWE’s assumptions regarding energy growth and petroleum products trends, the potential sulphur emission from fossil fuels burnt in the EEC countries in the year 2000 is likely to fall or in the most extreme conditions cannot be more than 12% above 1975 emissions, The contribution of petrolem products to sulphur emission will drastically decrease while coal is likely to become the major source. ‘The change in petroleum product demand pattern will be accompanied by the increasing application of technology to convert residues into lighter products. The volume of residual fuels as well as their share in the sulphur emissions will thus decrease. The limited amounts of residues from conversion processes will have characteristics which render them difficult as feedstocks for desulphurization and the process would incur heavy energy penalties. Thus the availability of residues suitable for desulphurisation will decrease during the estimated lifetime of 15 years for a commercial unit, e.g. it is likely that very little atmospheric residue will be available after the mid-1980s, Residue desulphurization incurs a high energy penalty equivalent to 10-12% of the residue based on output for atmospheric residue and 16-19% for vacuum residue. Investment and operating costs for residue desulphurization units are high and vary with the type of feedstock. For Kuwait feedstocks, the cost per tonne of 1% sulphur product ranges from $ 40-51 for atmospheric residue and § 67-88 for vacuum residue. For Arabian Heavy feedstocks, which are more difficult to desulphurize due to their higher concentrations of metals and more complex chemical constituents, the cost per tonne of 1% sulphur product produced in a unit designed for Kuwait would be in the order of $ 67-85 for atmospheric residue and $ 105-140 for vacuum residue, It should be noted that in the event that such process units might be constructed, they would not be operational before about 1985 and the cost data presented above would be subject to adjustments for inflation and increases in crude oil prices which may occur after 1980, 2930 Care should be taken in any attempt to apply the above cost data to cases other than those quoted. For example, serious errors could be encouttered in making a simple application of these data to determine the cost of reducing a fuel oil pool from 2% to 1% sulphur when the pool originates from crudes of widely varying characteristics. The development of strategies to control sulphur emissions should consider all available technologies and determine their optimum application, taking into account trends in primary fuel availability in the area concerned, e.g. the declining availability of residual fuel oils and the fore~ cast increase in coal consumption.co Icawe REFERENCES: World Health Organization (1979), Environmental Health Criteria Series, No. 8: Sulfur Oxides and Suspended Particulate Matter, Geneva, WHO. EEC (1975), Council Directive on the Sulphur Content of Fuels (75/716/EEC), Official Journal of the European Communities No. L.307, 27th November 1975. EEC (1980), Council Directive on Air Quality Limit Values and Guide Values for Sulphur Dioxide and Suspended Particulates (80/779/EEC), Official Journal of the European Communities No. L.229/30, 30th July 1980. CONCAWE (1977), Costs of Reducing S02 Emissions and Improving Effluent Water Quality from Refineries, Report No. 5/77, The Hague, CONCAWE. CONCAWE (1972), A Study of the Costs of Residue and Gas Oil Desulphurization for the Commission of the European Communities, Report No. 13/72, The Hague, CONCAW! CONCAWE (1981), Direct Desulphurization of Residual Petroleum 0i1 - Investment and Operating Costs, Report No. 5/81, The Hague, CONCAWE 31