Sulphur Dioxide and Nitrogen Oxides in Industrial Waste Gases: Emission, Legislation and Abatement

280 Pages·1991·10.59 MB·English

by  D. Van Velzen (auth.)

Sulphur Dioxide and Nitrogen Oxides
in Industrial Waste Gases:
Emission, Legislation and Abatement
EURO
C O U R S ES
A series devoted to the publication of courses and educational seminars
organized by the Joint Research Centre Ispra, as part of its education and
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CHEMICAL AND ENVIRONMENTAL SCIENCE
Volume 3
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Sulphur Dioxide
and Nitrogen Oxides
in Industrial Waste Gases:
Emission, Legislation
and Abatement
Edited by
Daniel van Velzen
Commission of the European Communities,
Joint Research Centre,
Environment Institute,
Ispra, Italy
SPRINGER-SCIENCE+BUSINESS MEDIA, B.V.
Based on the lectures given during the Eurocourse on
Sulphur Dioxide and Nitrogen Oxides ni Industrial Waste Gases:
Emission, Legislation and Abatement
held at the Joint Research Centre Ispra, Italy, September 3-7,1990
ISBN 978-94-010-5608-3 ISBN 978-94-011-3624-2 (eBook)
DOI 10.1007/978-94-011-3624-2
Publication arrangements by
Commission of the European Communities
Directorate-General Telecommunications, Information Industries and Innovation,
Scientific and Technical Communication Unit, Luxembourg
EUR 13599
©1991 Springer Science+Business Media Dordrecht
Originally published by Kluwer Academic Publishers in1991
LEGAL NOTICE
Neither the Commission of the European Communities nor any person acting on behalf of the
Commission is responsible for the use which might be made of the following information.
Printed on acid-free paper
All Rights Reserved
No part of the material protected by this copyright notice may be reproduced or
utilized in any form or by any means, electronic ro mechanical,
including photocopying, recording or by any information storage and
retrieval system, without written permission from the copyrigth owner.
CONTENTS
List of Contributors vii
1. PREFACE AND COURSE INTRODUCTION
D. van Velzen
2. EMISSION SOURCES AND QUANTITIES
B. Heinen 9
3. ATMOSPHERIC CHEMISTRY OF SULPHUR DIOXIDE AND NITROGEN OXIDES
G. Reste/li and H. Stangl 23
4. DISPERSION AND TRANSPORT OF ATMOSPHERIC POLLUTANTS
S. Cieslik 47
5. CONTROL OF AIR POLLUTION -THE EUROPEAN COMMUNITY APPROACH
H.P. Stief-Tauch 73
6. DESULPHURIZATION OF FLUE GASES ON THE BASIS OF LIME OR
LIMESTONE SCRUBBING
G. Mittelbach 93
7. THE WELLMAN LORD PROCESS
U. Neumann 111
8. ISPRA MARK 13A DESULPHURIZATION PROCESS
H. Langenkamp 139
9. BF / UHDE / MITSUI-ACTIVE COKE PROCESS FOR SIMULTANEOUS S02-AND
NOx-REMOVAL
E. Richter 157
10. WALTHER PROCESS
W. Schulte 167
11. EBDS-PROCESS
H.-R. Paur 183
12. PRIMARY MEASURES FOR NOx REDUCTION
H.G. Bos 205
13. HIGH AND LOW DUST SCR PROCESSES
E. Weber and D. Schmidt 223
14. COSTS OF DESULPHURIZATION AND DENOXING
D. van Velzen 235
15. SITUATION IN THE UNITED STATES AND JAPAN
G. Caprioglio 263
LIST OF CONTRIBUTORS
H. G. BOS,
Stork Boilers,
P.O. Box 20,
NL-7550 CB Hengelo, THE NETHERLANDS
G. CAPRIOGLIO
Ferlini / General Atomics Development Corporation,
P.O. Box 85608,
San Diego, California, UNITED STATES OF AMERICA
S. CIESLIK
Commission of the European Communities,
Joint Research Centre (JRC), Environment Institute,
1-21020 Ispra, ITALY
B. HEINEN
Energie Consulting Heidelberg,
1m Breitspiel7,
D-6900 Heidelberg, Federal Republic of GERMANY
H. LANGENKAMP
Commission ofthe European Communities,
Joint Research Centre (JRC), Environment Institute,
1-21020 Ispra, ITALY
G. MITIELBACH
Deutsche Babcock Anlagen AG,
Postfach 4 + 6,
D-4150 Krefeld, Federal Republic of GERMANY
U. NEUMANN
Davy McKee AG,
Borsigallee 1 -7,
D-6000 Frankfurt / Main 60, Federal Republic of GERMANY
H.-R. PAUR,
Kernforschungszentrum Karlsruhe GmbH,
Laboratorium fur Aerosolphysik und Filtertechnik I,
Postfach 3640,
D-7500 Karlsruhe 1, Federal Republic of GERMANY
G.RESTELLI
Commission ofthe European Communities,
Joint Research Centre (JRC), Environment Institute -Air Chemistry,
1-21020 Ispra, ITALY
vii
viii
E. RICHTER,
DMT Gesellschaft fur Forschung und Prufung mbH,
Institut fur Warme und Stromerzeugung,
Franz Fischer-Weg 61,
D-4300 Essen 13, Federal Republic of GERMANY
D. SCHMIDT,
Institut fur Umweltsverfahrenstechnik, Universitat Essen,
Leimkugelstrasse 10,
D-4300 Essen 13, Federal Republic of GERMANY
W. SCHULTE,
Krupp Koppers GmbH,
POB102251,
D-4300 Essen 1, Federal Republic of GERMANY
H. STANGL
Commission of the European Communities,
Joint Research Centre (JRC), Environment Institute -Air Chemistry,
1-21020 Ispra, ITALY
H.P. STIEF-TAUCH
Commission ofthe European Communities,
Directorate General XI -B,
Rue de la Loi 200,
B-l049 Brussels, BELGIUM
D. VAN VELZEN
Commission of the European Communities,
Joint Research Centre (JRC), Environment Institute,
1-21020 Ispra, ITALY
E. WEBER
Institut fur Umweltsverfahrenstechnik, Universitat Essen,
Leimkugelstrasse 10,
D-4300 Essen 13, Federal Republic of GERMANY
PREFACE AND COURSE INTRODUCTION
D. VAN VELZEN
Commission of the European Communities,
Joint Research Centre Ispra,
Environment Institute,
1-21020 Ispra (Varese) ITAL Y
1. Introduction
Worldwide, there is an ever increasing interest and concern about the destructive
effects of air pollution on man's ecosystem. The growing awareness of these
effects has revealed the need to take adequate measures to minimize the
emission of air polluting products. The two most important contaminants,
occurring in the largest concentrations and quantities, are sulphur dioxide and
nitrogen oxides. Both pollutants are formed mainly during the combustion of
fossil fuels, particularly by power stations and traffic. The effects of air pollution
caused by these two contaminants have already been studied for several decades
and measures to protect the environment against their adverse effects are now
operative in many countries.
The present volume contains the proceedings of a Eurocourse held in Ispra in
September 1990. The course was meant to give an overview of present
knowledge concerning the emission sources and quantities, to cover features of
present legislation and to give a survey of the most important modern
abatement techniques for S02 and NOx. It was mainly addressed to higher and
medium management in the power, chemical and similar industries, particularly
from those countries where the fight against air pollution is still in its infancy.
Obviously, it was not possible to cover completely the whole range of subjects
during the limited duration of a Eurocourse. For every facet ofthe problem,
choices had to be made. A short justification of these choices is given in the
following paragraphs.
2. Emission and transport
This section consists of a set of three papers. The first one (Heinen) gives a survey
of the sources and quantities of sulphur dioxide and nitrogen oxides emissions.
The chemical processes which take place in the atmosphere and which are
responsable for the conversion of the gaseous products into the acidic
precipitates, causing the destructive effects known as acid rain ", are discussed in
II
the second paper (Restelli and Stangl).
D. van Velzen (ed.).
Sulphur Dioxide and Nitrogen Oxides in Industrial Waste Gases: Emission. Legislation and Abatement, 1-7.
© 1991 ECSC. EEC. EAEC. Brussels and Luxembourg.
2
The third paper (Cieslik) presents the state of the art in atmospheric modelling
used for the prediction of the airborne transport of the contaminants. These
three review papers give together a very satisfactory survey of the present state
of knowledge in the field ofthe emission and transport of air pollutants.
3. Legislation
Limitations of S02 and NOx emissions are imposed by national and international
regulations. Currently there are approximately 20 countries where national
emission standards are operative. Recently important developments in control
regulations took place, both nationally and internationally.
One of the most important international agreements is the United Nations
Economic Commission for Europe (UNECE) Convention on Long-range
Transboundary Air Pollution, signed in 1979 in Geneva by 33 countries. Later, in
1985, this was followed by the adoption of a protocol to the convention which
called for a 30% reduction in total S02 emission by 1993, compared with 1980
levels. This protocol was signed by 21 countries, which have become known as
the "30% club".
The EC Directive on the limitation of emissions of pollutants from large
combustion plants was agreed in 1988 and applies to the twelve member states
of the European Community. The target for existing plants is a 23% reduction in
total EC emissions by 1993 and a 57% reduction by 2003. The baseline figure is,
here also, the emission rate for 1980.
The reduction targets differ from country to country. Less developed countries
like Greece, Portugal and Ireland are even allowed to increase their emissions,
whereas the most stringent targets (70%) are set for Belgium, Germany, France
and the Netherlands.
The background and details of the approach of the European Community in
matters of legislation to prevent air pollution are discussed extensively in the
fourth paper of the course (Stief-Tauch)
4. Sulphur dioxide abatement
The regulations for sulphur dioxide emissions have become considerably more
stringent with time, especially during the 1980s. This has led to the application of
various measures to reduce the emission of S02. There are a number of options to
realize these reductions:
i) - decreasing the sulphur content of the fuel or switching to other fuels;
ii) - the use of processes to decrease emissions during combustion;
iii) - the application of flue gas desulphurisation (FGD) processes.
There are several alternatives in each category, often resulting in different
levels of emission of S02. Particularly in the field of FGD processes, the
alternatives are manifold. It is in this field that rigorous choices had to be made
concerning the contents of this course.
I
4.1 ACTIONS CONCERNING THE FUEL
It is very common practice in countries where regulations for S02 emission are
applied for the first time to switch fuels. For coal fired power stations, the
3
change from high sulphur to low sulphur coal is an obvious one, and also in many
other situations switching from high sulphur fuel oil to natural gas fired furnaces
is applied. Such solutions usually require a limited investment compared to the
installation of bulky FGD equipment and the additional necessary particulate
removal systems. However, availability and price ofthe fuels set a limit to the
applicability of this alternative for the reduction of S02-emissions.
The second alternative in this category is the removal of sulphur from the fuel
before combustion. The desul9hurization of coal has been studied extensively,
but, until now, no practical in ustrial process has been developed. The main
reason is that by washing and/or froth flotation of the coal a certain degree of
sulphur removal can be obtained, but that removal ofthe organically bound
sulphur and pyrites is as yet unpracticable. Studies into the microbiological
desulphurization of coal are at present under way, but are still at the laboratory
stage and the projected process costs seem to be high.
It follows that switching fuels is a rather obvious alternative, whereas the
desulphurization of fuels is as yet not practicable. For these reasons, no paper
dealing with the desulphurization of coal or actions concerning the fuel was
included in the course.
4.2 ACTIONS CONCERNING COMBUSTION
Combustion technologies exist where the control of the emission is an integral
part of the process design. Examples include the fluidised bed combustion of coal
and the application of sorbent injection. In both cases the intrinsically formed
sulphur dioxide reacts with and is bound to an active solid material, usually
calcium or magnesium oxide.
Research on fluidised bed combustion (FBC) for energy production was
started in the early 1960s. In this process, the fuel is burned in a furnace
containing a bed of finely-divided solid particles of high melting point. The
combustion air passes upwards through the bed and causes fluidization of the
particles. The total mass behaves like a boiling fluid. Typically, FBC operates at a
temperature of 850°C, which is several hundred degrees lower than conventional
combustion. With this lower combustion temperature, the formation of nitrogen
oxides is largely avoided. The addition of a calcium or magnesium mineral like
dolomite to the solids can to a certain extent prevent the emission of sulphur
dioxide. The formed S02 is bound to the solids in the form of sulphate or sulphite
and leaves the process together with the spent solids, coal ash and unconverted
sorbent. Most of the early FBC units experienced major mechanical and material
problems, including erosion of the heat exchange tubing and plugging of coal
feed systems. Nowadays most of these problems have been solved and coal fired
FBC boiler systems are fairly widespread in Western Europe and North America,
with over 200 industrial size units in operation in utilities and process industries
with a capacity of up to approximately 100 MWe.
The disadvantages of the method are its high cost, the fact that it is only
applicable to new boilers of relatively small size and the high consumption of
sorbent material needed to achieve at a satisfactory degree of desulphurization.
In our opinion, the contribution of FBC to the solution of the problem of S02
emission is small, so that no detailed specific paper was included in the
Eurocourse.