J Mater Cycles Waste Manag (2009) 11:229–243 DOI 10.1007/s10163-008-0235-z

SPECIAL FEATURE: ORIGINAL ARTICLE

© Springer 2009

The 3rd Expert Meeting in Solid Waste Management in Asia and Pacific Islands

Hideto Yoshida · Kazuaki Takahashi · Nobuo Takeda Shin-ichi Sakai

Japan’s waste management policies for dioxins and polychlorinated biphenyls

Received: April 28, 2008 / Accepted: February 27, 2009

Abstract We summarize the measures taken by the Japanese government to prevent the emission of dioxins and polychlorinated biphenyls (PCBs) into the environment. Because incineration is the main method of waste management in Japan, reducing the amount of dioxins emitted from waste incinerators is an essential aspect of proper waste treatment. Intensive measures to prevent the formation of dioxins at the source have been implemented, with a focus on waste treatment methods and improving comprehensive management. The efforts have been very successful, with a 95% reduction in the amount of dioxins emitted between 1997 and 2003. The toxicity of PCBs has been monitored with keen interest since the Yusho incident. Unfortunately, treatment facilities for PCB wastes were not built until long after PCBs had been removed from use, and PCB wastes remained in storage in an untreated state. The Japanese government has promoted the construction of facilities for treating PCB wastes, and five such facilities have commenced operations. To more completely eradicate dioxins, a future challenge will be to reduce the amount of PCBderived dioxins, which are persistent in the environment and have a long exposure pathway from the environment media to the organism and the human body. H. Yoshida (*) Executive Managing Director, Japan Environmental Sanitation Center, 10-6 Yotsuyakamicho, Kawasaki-ku, Kawasaki 210-0828, Japan Tel. +81-44-288-4937; Fax +81-44-288-5217 e-mail: [email protected] K. Takahashi Industrial Waste Division, Waste Management and Recycling Department of the MOE, Government of Japan, Tokyo, Japan N. Takeda Research Center for Eco-Technology, Ritsumeikan University, Kusatsu, Shiga, Japan S. Sakai Environment Preservation Center, Kyoto University, Kyoto, Japan The views expressed herein are those of the authors and not necessarily the official views of the organizations with which the authors are affiliated.

Key words Dioxins · PCBs · Waste management · Incineration · Control technology

Introduction Dioxins are unintentional byproducts of chemical and thermal reaction processes. Waste incineration has been the predominant source of dioxin formation, and the measures taken to reduce dioxin emissions have evolved along with waste management policies and practices in Japan and other countries. In this article, we examine the political measures used to tackle the dioxin problem that resulted from late twentieth century practices of mass production, mass consumption, and mass disposal. We also evaluate the political measures associated with polychlorinated biphenyl (PCB) issues.

History of dioxin control measures in Japan Japan has a relatively small usable land area, and incineration, a waste-processing method that began in about 1912 and became common in the 1950s, is the most widely used method of waste management.1 In fiscal year (FY) 2003, a total of 54.27 Mtonnes of municipal waste was generated in Japan, 74% of which (40.24 Mtonnes) was incinerated.2 Incineration, if carried out properly, is an effective method of reducing waste while at the same time preserving a clean environment. Prevention of secondary pollution associated with waste management, however, is crucial. In particular, the problems associated with the formation of dioxins as a byproduct of waste incineration have been important political issues, and there has been a recent paradigm shift in waste management. The reduction of dioxin emissions from waste incineration has become an important aspect of general environmental administration. Olie et al.3 first reported that dioxins were present in fly ash from municipal waste incineration in the Netherlands in 1977. Two years later, Eiceman et al.4 detected dioxins in

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fly ash of municipal waste incinerated in Kyoto, and based on this report, Kyoto City undertook measures to reduce the production of dioxins.5 Dioxin pollution, caused by waste landfills and polluted oil in places such as Love Canal and Times Beach (USA), was a serious international social issue in the late 1970s and 1980s.6 However, the first incident to raise social concerns about dioxins in Japan was Tatsukawa et al.’s 1983 report that dioxins were detected in fly ash from municipal waste incineration.7,8 Following the release of this news, the Ministry of Health and Welfare created the Expert Committee on Dioxins Related to Municipal Waste Treatment in 1983.9 More assessments of the presence of dioxins in environmental media and organisms were conducted,10–12 and at the same time, studies on the mechanism of dioxin formation in waste incineration facilities were carried out.13 The 6th International Conference on Dioxins was held in Fukuoka in 1987, and through that and other similar events, knowledge of waste incineration, formation of dioxins, and control of dioxin production were integrated. Based on such integrated knowledge, the Guidelines to Prevent Formation of Dioxins (hereafter, the original guidelines)14 were issued in 1990. In addition, a Japan Broadcasting Corporation (NHK) news program reported that high levels of dioxins had been detected at a municipal solid waste incineration site just before the guidelines were issued,15 and the issue gained increased public attention. The guidelines specified that, to the extent that they were technically possible, measures should be implemented to prevent the formation of dioxins. These included methods for achieving complete combustion and preventing de novo synthesis of dioxins, as well as highly effective methods for removing dioxins after they had been generated. It was expected that the use of such measures could reduce the dioxin concentration contained in exhaust gas from the new continuous incinerators to 0.5 ng-I-TEQ/Nm3 (I-TEQ: international toxicity equivalent), which would be less than one-tenth of the previous levels of formation of dioxins from waste incineration systems in Japan. In particular, emphasis was given to secondary gas combustion conditions (the 3Ts of complete combustion: temperature, time, and turbulence) and to the reduction in dust collector temperatures. The guidelines focused on dioxin emission control measures in waste incineration. It was not enforced by law, however, but it was promoted using government subsidies for building new facilities; the monitoring of emissions was not mandated. As a result, the guideline mainly applied to new facilities. Outside of Japan, Sweden set the first emission criterion at 0.1 ng-TEQ/Nm3 in 1987, and regulations stipulating equivalent levels were established in other Western countries (e.g., the Netherlands and Germany) in the early 1990s, even though there was no proven technology for dioxin reduction at that time. Investigations on emission conditions and risks, the basic information needed for system design for dioxin management, were then conducted, and the tentative value of tolerable daily intake (TDI) of dioxin in Japan was set at 10 pg-I-TEQ/kg/day in 1996.16 This is identical to the value that had been already adopted by the World Health

Organization (WHO) and European countries at that time. Setting the TDI was a significant factor in establishing a system for dioxin reduction measures in waste treatment. After the value was set, the Ministry of Health and Welfare formed a Commission for Dioxin Reduction Measures Relating to Waste Disposal. A survey was then conducted on the actual conditions of dioxin emissions in waste incineration facilities in local governments. Facilities with dioxin emission concentrations exceeding 80 ng-I-TEQ/Nm3, which had been set as the emergency criteria, were identified, and emergency measures, including the shutdown and abandonment of small and obsolete facilities, were requested.17 In 1997, the original guidelines were revised and the Guidelines for Prevention of Dioxin Formation Relating to Waste Treatment (the new guidelines) were proposed.18 The salient features of the new guidelines were the avoidance of environmental accumulation, which necessitated the use of advanced technology; a response by waste treatment systems; and the use of new measures to control residues19 (see Fig. 1). The idea was to reduce dioxin formation as much as possible by introducing the best available technology (BAT). Following the discussions of The Dioxin Risk Assessment Commission, which investigated the issue at the same time, 0.1 ng-I-TEQ/Nm3 was adopted as the permanent emission gas criterion. The idea behind avoiding environmental accumulation is to control the total dioxin release associated with waste incineration, with a special emphasis on fly ash, which contains relatively large amounts of dioxins. In addition to reducing dioxin accumulation in the environment, it was hoped that transformation of incinerated residue into slag would develop a new recycling system and increase of the life of final disposal sites. At the time, it was expected that, if the measures were implemented, the total release of dioxins in the emission gas, fly ash, and bottom ash associated with waste treatment would be 5 μg-WHO-TEQ/waste tonne (WHO-TEQ: toxicity equivalent as set by WHO). Attempts were also made to develop amendments of applicable laws and regulations and to improve financing of the waste treatment system; these measures included expansion of the range of waste treatment facilities for which construction permits were required, banning open burning, and consolidating structural and maintenance criteria.20 In addition, the Air Pollution Control Law was amended to add dioxin emission criteria. An annual average of 0.6 pgTEQ/m3 was set as the tentative environmental management criterion for ambient air. Government subsidies for building and updating municipal waste incineration facilities operated by local municipal governments were increased. A major emphasis was placed on facilities that treated more than 100 tonnes of waste per day, as was supporting, power-generation facilities using refuse-derived fuels (RDF), and aiding renovation projects at facilities that had a high degree of gas emissions.21 Before and after enactment of the new guidelines, public concern about dioxins increased rapidly. There was a good deal of media coverage of cases such as the illegal dumping of industrial wastes (e.g., residues from automobile shred-

231 Fig. 1 Systematic and technical aspects of the measures taken to reduce dioxins formed in the process of waste incineration. 3R, reduce, reuse, recycle; RDF, refuse-derived fuels

ders and waste oils) in Teshima, dioxin contamination in the Tokorozawa area, and the detection of highly concentrated dioxins in the Toyonou Clean Center. The number of dioxin-related articles that appeared in three major newspapers (Asahi, Mainichi, and Yomiuri) increased from about 100 a year before 1995 to nearly 2000 in 1997 and to 3780 in 1998.22 In response to the growing concern about dioxins, the Law Concerning Special Measures Against Dioxins (Dioxin Special Measures Law) was enacted. A feature of the Dioxin Special Measures Law was the adoption of a TDI limit of 4 pg-WHO-TEQ/kg/day,23 including dioxin-like PCBs. Environmental standards were also set for air, water, soil, and sediment quality. In addition, emission standards relating to gas emissions and water discharge were set for designated facilities. Furthermore, standards for final effluent from leachate treatment facilities as a management standard of final disposal sites and for residues at waste incinerators were set. The goal for the emission of dioxins was 843–891 g-WHO-TEQ/year by the end of 2002, which was an approximately 88% reduction from the estimated amount of discharge in 1997.24 The measures taken on the basis of the Waste Management Law and the Dioxin Special Measures Law for reducing dioxin emissions have been quite successful, particularly with respect to waste incineration, which accounts for much of the total discharge of dioxins in Japan. The reduction plan was amended in June 200524 because the original reduction target had been achieved, and a new goal of 315–343 gWHO-TEQ/year by 2010 was set. This value represented a reduction of almost 96% compared with 1998 values and an approximately 15% reduction compared with 2003.

The Stockholm Convention on Persistent Organic Pollutants (POPs convention) was established from the perspective of the precautionary approach raised in Principle 15 of the Rio Declaration. Japan became a member in 2002, and the convention was put into effect in 2004. The convention aims to protect human health and preserve the environment from the effects of POPs. Specifically, the convention pursues the eradication of 12 POPs, including dioxins. In 2005, the Conference of the Parties 1 (COP1) was held in Geneva, and guidelines related to best available techniques (BATs) and best environmental practices (BEPs) have been created regarding dioxins, PCBs, and hexachlorobenzene, which are unintended by products of many processes.

History of PCB control measures in Japan PCBs played an important role in the history of chemical substance management policy in Japan. The PCB issue first became widely known in Japan because of the Yusho incident in 1968. In this industrial accident, PCBs used as a heating medium leaked into rice bran oil during the manufacturing process, and people who consumed the contaminated oil suffered significant health problems. PCBs were identified as the causative agent of these problems in 1972. As a result, its manufacture was discontinued and the collection of waste PCBs was instructed by the government. In 1973, the Law Concerning the Examination and Regulation of Manufacture of Chemical Substances (Chemical Substances Control Law) was established, and a framework was

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created to review and regulate the use of chemical substances. The Chemical Substances Control Law bans the use and manufacture of PCBs and requires the safe storage of PCBs. It is estimated that about 54 ktonnes of PCBs were consumed in Japan from 1954 to 1972, the period in which they were most commonly used.25 Although the manufacture and use of PCBs were banned in the 1970s, the risk of negative environmental consequences continued because many of the products were used in business enterprises and it was difficult to store PCBs safely. In addition, some PCB products were used in open systems. For these reasons, policies mandating the control and management of wastes containing PCBs were needed. In 1972, when the storage of PCB was made substantially obligatory, a tentative allowable limit for PCBs emitted when incinerating carbonless copy paper was fixed at a maximum of 0.25 mg/m3.26 In 1973, handling guidelines for used home appliances containing PCBs were announced.27 In 1976, the landfill of PCBs and disposal into the seas and oceans were banned, and the Waste Management Law was amended to set criteria for the release of PCBs into the environment. Additionally, carbonless copy paper was included as an industrial waste. During this period, used equipment containing PCBs was collected, stored, and managed as directed by the Waste Management Law; however, very little progress was made with regard proper disposal of PCBs. The Kaneka Corporation, Takasago Office, began to conduct experiments on thermal decomposition of liquid waste PCBs. The actual thermal decomposition of the wastes started in 1987, and 5.5 ktonnes were treated by 1989. After 1989, however, the stored PCB wastes were not treated until 2004, except for a few cases in which industries that had a large amount PCB wastes did conduct treatment. The primary reason for the lack of treatment was the difficulty in gaining local consent for locating treatment facilities.28 The Waste Management Law was amended again in 1992, and PCBs were designated as a specially controlled waste; special standards for waste management (e.g., collection, transport, storage, and intermediate treatment) were established, with special attention to the handling of PCB wastes. In 1993, a review of the state of storage and disposal of used PCB-containing equipment was conducted.29 Nearly 7% of the PCB-containing high-pressure transformers and capacitors were either lost from their original locations or their current location was unknown. The main cause was determined to be either the closure or bankruptcy of storage establishments or errors made when stock was handed over when management at the storage facilities changed. Similarly, 4% of the waste carbonless copy paper containing PCBs was either lost from its original location or the current location was unknown. Under such circumstances, the possibility of PCB leakage into the environment caused by long-term storage became clear, and this underlined the urgent necessity for prompt development of a treatment system. Establishment of chemical decomposition methods other than incineration were deemed to be necessary to solve the treatment issue.30

By 1997, an interim report showed that great progress had been made in the proper treatment of PCBs.31 The report, however, expressed concerns over the increased environmental pollution risk associated with long-term PCB storage and emphasized the necessity of prompt PCB treatment at the safest level possible. The report also stated that chemical dechlorination and supercritical water processes could be the basis of feasible treatment technologies. The report fixed 0.5 mg-PCB/kg-oil (ppm) as the treatment target criterion for the chemical treatment of PCBs and the oil containing them. This level meets the strictest criteria32 and was established on the basis of leaving no toxic residue in the treated oil and on the use of BATs, as well as on the existence of proper analytical methods for confirmation. In 1998, the enforcement ordinance of the Waste Management Law was amended and new treatment methods were added. In 1999, the PCB Treatment Technology Information Packet was distributed, and self-treatment by chemical decomposition methods was promoted. As of April 4, 2005, self-treatment of PCB wastes was either planned or implemented in 22 business establishments.33 Even with the advancement in treatment technologies, the lost equipment containing PCBs could not effectively be recovered. Moreover, the situation for smaller businesses having PCB-containing wastes was unchanged because they could not meet the demands of treating the equipment, and it was estimated that such businesses had about 60% of all stored waste containing PCBs.31 Meanwhile, PCB treatment was improving in other countries, including those of the EU, which had adopted the POPs convention in 2001 to eliminate PCBs by 2028, and there was a growing concern that Japan might be lagging behind other developed countries in terms of PCB treatment.34 To promote the proper and reliable treatment of PCB wastes, the Law Concerning Special Measures against PCB Wastes (PCB Special Measures Law) was enacted in 2001. In addition, a financial support system for promoting facility improvement and treatment in medium and small businesses was established. The PCB Special Measures Law stipulated that businesses were obligated to issue a storage/ treatment status report annually and to complete treatment by 2016. The law also established a government-run, widearea treatment system (see Fig. 2). The Japan Environmental Safety Corporation (JESCO), which succeeded the Japan Environment Corporation in undertaking the PCB Waste Treatment Programs in 2004, was responsible for improving the treatment system to meet the time limit set by the PCB Special Measures Law. JESCO was in charge of the development of facilities at five sites in Kitakyusyu, Tokyo, Toyota, Osaka, and Muroran, with the cooperation of local authorities and residents, and all of these sites had opened by the end of May 2008.35 Meanwhile, the Ministry of the Environment (MOE) continues to study technically reliable, cost-efficient disposal methods for electrical machinery containing small amounts (very tiny amounts compared to PCB-used transformers) of PCB-contaminated insulating oil (low-contaminated PCB wastes). Since April 2005, in cooperation with

233 Fig. 2. Systematic and technical aspects of the measures taken to control polychlorinated biphenyls (PCBs.)

prefectural governments and waste management facilities, MOE has been conducting verification tests for the incineration of low-contamination PCB wastes at existing facilities. So far, the results show that the emission levels of PCBs and dioxins in the emission gas and water meet national safety standards; thus, low-contamination PCB wastes can be disposed of safely with minimal impact on the surrounding environment. In addition, more verification tests are planned at other facilities. Studies on safe, reliable, and specialized disposal of lowcontamination PCB wastes are also being conducted by the Experts’ Committee, a committee established by the Central Environmental Council for the treatment of low-contamination heavy electrical machinery. An interim progress report was submitted in September 2008, and MOE will take further action on the basis of the research and decisions by the committee.

Control programs and technologies for dioxins and PCBs Dioxins As a response to the dioxin problem, Japan has significantly changed its waste management policies, adopted improved new programs, and developed advanced treatment technologies (see Fig. 1). A pillar of the dioxin reduction program in waste management policy is waste reduction and the promotion of recycling and wide-area waste treatment. Basic guidelines concerning dioxin measures promo-

tion36 and the target volume of waste reduction37 were established in 1999, and they laid out a national goal for controlling waste generation as well as setting the desired recycling ratio. This goal eventually became the basic guidelines for the Waste Management Law,38 which is a major indicator of waste management policy in Japan. At the same time, laws related to recycling were implemented.39 These laws are based on the philosophy presented in the Basic Law for Establishing Society, which was promulgated in 2000, and they serve as tools for shifting toward a recycling-based society from the 3R viewpoint (reduce, reuse, recycle) of recycling resource management. The purpose of promoting wide-area waste treatment is to combine the small and intermittently operating waste incineration facilities in each city or town into large and continuously running facilities which will work within an energy-efficient combustion scale and reduce dioxin emissions. The policy establishes a wide-area plan in each prefecture,40 and prefectures must follow the plan to receive subsidies to improve waste treatment facilities.41 In addition to the dioxin reduction measures, wide-area waste disposal management is expected to aid in the advanced treatment of incinerated residues, promote material and thermal recycling, help in securing final disposal sites, and reduce the cost of public work projects.40 Development of joint treatment systems on the basis of the wide-area plan became a common development method for waste treatment facilities, especially as local communities suffered from worsening financial conditions and municipalities were allowed to merge based on the Municipal Merger Law, which came to an end in 2004.

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Technology has progressed on advanced flue gas treatment, including combustion control and heat recovery and the proper treatment of incinerated residues. The 3T process is important in combustion control and is a critical aspect of facility design. In the process, an incineration temperature of 850°C or higher must be maintained with a residence time of 2 s or longer, and gas turbulence must be promoted, in addition to ensuring safe combustion by maintaining CO levels below a specified maximum value. In the advanced flue gas treatment process, it is important to have the flue gases rapidly cooled (to approximately 200°C or less) by employing a boiler to avoid the de novo synthesis of dioxins. Rapid cooling is combined with the use of a highly efficient dust collector and other removal and decomposition technologies using agents such as calcium hydroxide, activated charcoal, and an NOx removal catalyst. The incinerated residue is detoxified through processes such as melting or heating followed by dechlorination. Details of the advanced control technology for dioxins are described by Hiraoka,42 Nagata,43 and Hiraoka and Okajima,44 and the details of the incinerator are explained by the Japan Environmental Facilities Manufacturers Association.45,46 A manual for the maintenance of industrial waste incinerators is also available.47 The development of advanced control technology for dioxins also promoted the advancement and reconstruction of the entire system of waste treatment facilities. To promote the development and popularization of new technologies, including advanced dioxin control, the Japanese government established performance guidelines, which were incorporated into the requirements for adoption of government-supported projects.48 Previously, the government had issued only structural guidelines, which had caused new technology to be adopted. Technologies related to the dioxin emission control measures designated in the new guidelines were also effective with respect to emission control for other environmental pollutants, such as particulate matter, hydrogen chloride, nitrogen oxide, and heavy metals, and also exhibited synergistic control.13 Moreover, the technical development of a gasification melting furnace for stabilizing final residues44 and an ash melting furnace contributed greatly to improving recycling by forming residue slag and thereby increasing the lifetime of final disposal sites. At the same time, RDF production technology, which effectively utilizes wastes as a heat source, and RDF power generation technology also became popular.49 The control technology, which at first was limited to incinerators with a capacity of at least 100 tonnes/day, has also been applied to smaller incinerators; small-scale facilities with equivalent performance have begun to be developed.50 In addition to the application of BATs, proper management of the facilities is crucial to the advanced emission control of dioxins. Ishibashi et al.51 suggested that the secondary formation of dioxins occurs in the presence of inorganic salt and fly ash attached to the walls of incinerator stacks; thus, it is essential to establish a total control framework, which also includes maintenance systems.

PCBs The technical development of PCB treatment technologies has been done by the electricity generation and supply companies, which also serve as PCB storage facilities, and by corporations that construct waste treatment facilities pursuing the introduction and practical use of imported technologies. In the past, the former Environmental Agency, former Ministry of International Trade and Industry, and former Ministry of Health and Welfare investigated the improvement of legislation based on the evaluation of new PCB treatment technologies.33,52 Current technologies primarily involve chemical and physical treatment. Before the technologies came into practical use, they were standardized with regard to structure and maintenance in accordance with the newly established treatment standard by the amended Enforcement Order of the Waste Management Law. The descriptions of these new technologies were first introduced in the PCB treatment technology guidebook,52 and the technologies developed afterwards were described in the revised and enlarged guidebook33 to promote their use. Under the Waste Management Law, hydrothermal oxidation, thermochemical and mechanochemical processes and melting are specified for current use. These chemical and physical decomposition technologies are based on the principle of dechlorination of chlorinated compounds. Some of these same technologies are therefore being applied to waste pesticide treatment,53 and they will be added to guidelines for environmentally proper waste treatment specified under the Basel Convention, which seeks international standardization of proper treatment technology for pesticides as POPs.54

Effects of dioxin control measures Advanced control measures of dioxins in Japan were substantially triggered by the new guidelines. Furthermore, under this legal framework, technological development of measures against emission sources as well as development of risk management systems has made rapid progress. In this section, we discuss the extent of dioxin control after the establishment of the new guidelines and the effects of the implementation of the policy. We also examine the prevention of dioxin accumulation in the human body, which is the ultimate purpose of the measures.

Emission control in waste incineration systems The reduction of dioxins during incineration has been accomplished through promotion of waste recycling, aggregation of facilities for continuous operation, and emissions control through the introduction of BATs. The annual total amount of municipal solid waste (MSW) increased rapidly from the late 1980s until it reached about 50 Mtonnes in the 1990s, and afterwards it hovered around that amount. Figure 3 shows the total amount of MSW

235 Fig. 3. The amount of municipal solid waste (MSW) generated and incinerated in Japan, 1997–2004

generated and the amount incinerated from 1997, when the new guidelines were established, to 2004.55 After peaking at 52.36 Mtonnes in 2000, the total amount of MSW generated showed a slight declining trend, and in 2004 it was 50.59 Mtonnes, or 97.9% of the peak amount. Continued observation is required to conclude whether this trend is a result of 3R policies, especially policies that promote recycling, such as the full-fledged implementation of the Container and Packaging Recycling Law that was promulgated in April 2000. Although the amount of wastes treated by incineration also declined from the peak value of 2001, 40.1 Mtonnes of MSW were incinerated in 2004, representing only a slight decline from the peak. The complete ban on open burning and the abolition of self-treatment with simple small incinerators at businesses may have increased the amount of MSW generated and incinerated in each municipality. Figure 4 shows the number, type, and average capacity of waste incinerators from 1997 to 2004.55,56 The number of operating municipal waste incineration facilities (Fig. 4a) decreased from 1997 to 1998 and again from 2001 to 2002. The former decrease occurred at the same time as an urgent response to the new guidelines was required, and some operations were suspended as a response to the urgent criteria. The latter decrease was due to the suspension of operations at some facilities on 1 December 2002, the day the permanent criteria were implemented. As a result, only 76% as many facilities were operating in 2003 as were operating in 1997. Meanwhile, the average treatment capacity per facility and the number of continuously operating facilities increased (Fig. 4a). As a whole, it is clear that the aggregation of facilities has progressed. The reduction in the number of industrial waste incinerators is even greater

(Fig. 4b). A 20% decline was observed from 1997 to 1998, when the urgent measures were carried out, and when the permanent criteria were applied in 2002, another 35% of operations were suspended. From 1997 to 2004, more than 60% of the facilities were either suspended or closed. During the same period, unit treatment capacity rose, indicating an aggregation of facilities. An aim of the new guidelines was to encourage the aggregation of both municipal and industrial waste incineration facilities, and it is clear that this goal is being met. Figure 5 shows the amount of dioxins emitted from waste incineration facilities from 1997 to 2004 and the 2010 target rate.57 The total amount of waste-derived dioxins emitted into the air or water from municipal waste treatment facilities, industrial waste treatment facilities, and small waste incinerators with a treatment capacity of less than 200 kg/h are included in the total. In 1997, when the new guidelines were established, the amount of waste-derived dioxins emitted was 7659 g-WHO-TEQ/year, accounting for 94.1% of the total amount of dioxin emissions from all sources. In 1998, when the urgent measures were implemented, the amount was reduced to 3809 g-WHO-TEQ/year, or by more than 50%. In 2004, after the application of the permanent criteria, the amount was further reduced to 231 gWHO-TEQ/year, or only about 3% of the 1997 amount. The ratio of the incinerator-generated dioxins to the total amount of dioxin emissions from all sources also decreased to 63.7%. It is likely that these reductions were achieved as a result of technical contributions that were promoted in the new guidelines through the introduction of BATs. Aggregation of facilities as a result of the wide-area treatment plans as well the expansion of financial support for improving facili-

236 Fig. 4. The number, type, and operating capacity of municipal waste incinerators (a) and industrial waste incinerators (b) for 1997–2003

Fig. 5. The total amount of emitted dioxins and the ratio of dioxins from waste incineration to total dioxins, 1997–2004. The data for 2010 are the target values for that year. TEQ, toxicity equivalent

ties were also crucial. The use of gasification melting systems (which have been developed as an advanced dioxin control measure) in new incineration facilities increased from less than 10% in 1997 to almost 70% in 2003 (Fig. 6).58 Figure 7 shows the distribution of dioxins from incinerators that began operating in four different periods: before 1990 (when the original guidelines prevailed), 1991–1996 (the period between the guidelines), from 1997 (when the new guidelines prevailed) to November 1999 (when the new measures were established), and after December 1999 (when the new permanent measures were implemented). The relation between the concentration of dioxins in flue gases and incinerator size is also shown. In incinerators that

began operations prior to 1996, the average concentration was 0.38 to 0.60 ng-WHO-TEQ/Nm3, and overall concentrations were found to be broadly distributed. At incinerators that started operating after the establishment of the new guidelines’ urgent measures in 1996 but before the implementation of permanent criteria, the average concentration was 0.33 ng-WHO-TEQ/Nm3, but some incinerators had much lower values. In the facilities that started operating after the implementation of the permanent criteria, the average concentration was 0.05 ng-WHO-TEQ/Nm3, or about one-tenth of the average value for facilities that started operating before the implementation of the permanent criteria. Concentrations particularly decreased in the

237 Fig. 6. The distribution of disposal systems adopted by new municipal incinerators, 1997–2004

Fig. 7. Distribution of the concentration of dioxins emitted during four time periods for municipal waste incineration facilities: a before 1990 (the old guidelines prevailed), b 1991–1996 (between the guidelines),

c from 1996 to November 1999 (the establishment of new measures), and d after December 1999 (implementation of new permanent measures)

middle- and small-sized incinerators, and many of those incinerators have values considerably lower than the guideline criterion. Overall, among waste-derived dioxin sources, emissions from flue-gas-derived sources in municipal waste incineration facilities decreased to 1.3% of 1997 levels by 2004. It is clear that technologies have evolved in accordance with the stages and requirements of regulations, especially for the middle- and small-sized incinerators, and they have successfully reduced the concentration of dioxins in emissions.

After the permanent measures were implemented, the amount of dioxin released from incineration was expected to be 5 μg-WHO-TEQ/waste tonne. This goal was a unique Japanese strategy, and it was cited in the technical guidelines of the Stockholm Convention as an integrated dioxin control strategy aimed at reducing the amount of dioxins in incinerated residue.59 Table 1 shows the amounts of dioxin released for three cases: the estimates under a scenario in the new guidelines (no ash melting); the estimates of Sakai et al.,61 which include the use of BATs such as incinerated

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residue slag production; and estimates based on data from 2003 (the data sources and calculations are further described in Table 1). A total release of 14.57 μg-WHO-TEQ/waste tonne was estimated from 2003 data, which is almost three times the goal of 5 μg-WHO-TEQ/waste tonne in the new guidelines. Reducing the amount of discharge from flue gas is the most important issue because these gases are directly emitted into the environment; however, the amount discharged was estimated to be 1.76 μg-WHO-TEQ/waste tonne, which is approximately three times the new guidelines’ level. The flue gas concentration was roughly estimated to be 0.352 ng-WHO-TEQ/Nm3, more than three times the 0.1 ng-WHO-TEQ/Nm3 of the permanent emission criterion. Many facilities that began to operate before the implementation of the permanent measures remained in operation in 2003, and it is conceivable that these facili-

ties influenced the total amount of release. In the near future, these facilities are expected to be updated to perform as well as the newer facilities. Once these improvements are completed, even if the amount of waste incinerated remains the same, the amount of the emissions derived from flue gas is expected to be 14% (0.050/0.352) of the current amount, which is about 0.2–0.3 μg-WHO-TEQ/waste tonne. The total amount of dioxin in the incinerated bottom ash and fly ash from the 2003 data was estimated to be 12.8 μgWHO-TEQ/waste tonne, which is 3.4 times the level set in the new guidelines. Melting is effective in reducing the amount of dioxins in incinerated residues; however, as of 2003, only 113 facilities could melt the incinerated ash and 66 facilities could melt fly ash (some could do both).63 Further reduction in the amount of dioxins released could be accomplished by improving the capabilities of facilities to reduce the concentration of dioxins in flue gases and by using stabilization treatments on incinerated residue.

Table 1. Dioxin emissions from incinerators per unit weight of waste Estimate

Emission gas

Bottom ash

Fly ash

Total

Dioxin concentrations in air and soil

2.5 0.5 0.55 1.76

3 0.75 0.1 2.07

45 3 0.2 10.74

51 4.25 0.85 14.57

Here we examine the effects of the dioxin control policies on the concentrations of dioxins in air and soil, which serve as indicators of the environmental transport of dioxins,64 as well as exposure pathways to humans. Table 2 shows dioxin concentrations in the air from 1997 to 2004.64 The average concentration was 0.55 pg-WHOTEQ/Nm3 in 1997, and this had decreased by half to 0.23 pgWHO-TEQ/Nm3 in 1998. It then gradually decreased to 0.059 pg-WHO-TEQ/Nm3 in 2004, or about one-tenth of the 1997 level. No differences were found in atmospheric levels of dioxins in the general environment, the surroundings of release sources, and at roadsides. The effect of the urgent measures implemented in 1998 can be seen in the reduction of the dioxin concentrations in the air; no similar change was seen after the implementation of the permanent criteria in 2002. It is likely that because of the lower relative contribution (61%; see Fig. 5) of waste-derived dioxins to the total amount of emissions in 2003, the rate of decrease in the concentration of dioxin in the air was smaller after the permanent measure. The influence of dioxin formation associated with the open burning of material as a result of large-scale disasters (e.g., earthquakes),65 which were not

60

New guideline Without measures With measures Sakai et al.a61 2003 Datab

Data are given in micrograms-WHO-TEQ/tonne of waste (toxicity equivalent as set by the World Health Organization) a This scenario meets the permanent standards of the new guidelines and incinerated residuals can be melted. The emission gas includes the incineration gas and flue gas from the melting furnaces. The bottom ash is molten slag61 b The following data and sources were used to make these estimates. Emission gas: 71 g-WHO-TEQ/year ÷ 40 237 t/year = 1.76 μg-WHOTEQ/t of waste, where 71 g-WHO-TEQ/ year is the amount of dioxins emitted from waste incinerators to the atmosphere in 200357 and 40 237 t/year is the amount of domestic waste incinerated in 2003.55 Incineration ash: 150 kg/waste t × 0.01383 ng-WHO-TEQ/g = 2.07 μgWHO-TEQ/t of waste, where 150 kg/t is the amount of emitted fly ash per unit amount of waste incinerated1 and 0.01383 ng-WHO-TEQ/g is the simple average of TEQ concentrations in bottom ash at 18 incinerators in Tokyo in 200362 (premelting data were used for incinerators that had melting furnaces). Fly ash: 30 kg/waste t × 0.358 ng-WHO-TEQ/g = 10.74 μg-WHO-TEQ/t of waste, where 150 kg/t is the amount of fly ash emitted per unit amount of waste incinerated60 and 0.01383 ngWHO-TEQ/g is the simple average of TEQ concentrations in bottom ash at 18 incinerators in Tokyo in 200362 (premelting data were used for incinerators that had melting furnaces)

Table 2. Dioxin concentrations in the atmosphere, 1997–2004 Year Dioxin concentration in the atmosphere Minimum Average Maximum General environment Average Surroundings of release sources Average Roadside Average (pg-WHO-TEQ/m3)

1997

1998

1999

2000

2001

2002

2003

2004

0.01 0.55 1.40

0.0 0.23 0.96

0.0065 0.18 1.1

0.0073 0.15 1.0

0.0090 0.13 1.7

0.0066 0.093 0.84

0.0066 0.068 0.72

0.0083 0.059 0.55

0.55

0.23

0.18

0.14

0.14

0.093

0.064

0.058

0.58

0.20

0.18

0.15

0.13

0.092

0.078

0.063

0.47

0.19

0.23

0.17

0.16

0.091

0.076

0.055

239

Fig. 8. Dioxin concentrations in the soil, 1998–2004

Fig. 10. Estimated daily human intake of dioxins from preserved tissue samples. The Coplanar-PCB (Co-PCB) ratio is the ratio of Co-PCBs to total TEQ. PCDD/DFs, polychlorinated dibenzodioxins and polychlorinated dibenzo furans

Fig. 9. Estimated daily human intake of dioxins from food, 1997–2004

counted in the inventory, is another probable reason for the decreased rate of reduction. Figure 8 shows dioxin concentrations in soil samples from 1998 to 2004.64 The average values ranged from 3.1 to 6.9 pg-WHO-TEQ/g. Although the average concentration decreased from 2000 to 2004, it increased from 2002 to 2003. The correlation between dioxin concentrations in soil and the effects of the measures remains unclear.

Monitoring human exposure The total amount of daily human exposure to dioxins65 was estimated at 6.08 pg-WHO-TEQ/kg/day in the new guidelines, and the estimation has been conducted continuously since the establishment of the guidelines.18 More than 90% of human exposure to dioxins in Japan is through food.66 In this section, we examine the relationship between the amount of human exposure and the advanced dioxin control measures based on the daily intake of dioxins from food (Fig. 9).67 The average daily intake was estimated to be 2.41 pg-WHO-TEQ/kg/day in 1997. The level in 1998, when the urgent measures were implemented, was 83% of that in 1997, and the level continued to gradually decline over subsequent years. The average intake was 1.41 pg-WHO-TEQ/ kg/day in 2004, or 59% of the 1997 level. A similar trend was also seen for dioxin levels in the soil and water, which indicates that the urgent measures were notably more effective than the other measures. The daily intake of dioxins can also be estimated from preserved food samples.68 According to estimates made from those samples, the daily intake was more than 8 pg-

Fig. 11. Dioxin concentrations in breast milk, 1973–2004

WHO-TEQ/kg/day in 1977, and it rapidly decreased until 1992 and was about 2–3 pg-WHO-TEQ/kg/day in the late 1990s (Fig. 10). The ratio of coplanar PCBs (Co-PCBs) in TEQ exceeded 50% and is slightly increasing. The relationship between the advanced dioxin control measures and dioxin accumulation in the human body can also be examined by looking at dioxin concentrations in breast milk, for which data have been obtained over a long period of time. Figure 11 shows the changes in the concentration of dioxins in breast milk from 1973 to 2004.69 A rapid decrease in Co-PCBs started in 1974 and continued until 1986. The Co-PCBs concentration decreased by 30 pgWHO-TEQ/g-fat over this period. Afterwards, the decreasing trend continued but at a slower rate of 15 pg-WHO-TEQ/g-fat from 1987 to 2004. The first rapid decrease corresponds to the period of PCB regulation that began in 1973, and it also corresponds to the abovedescribed reduction of the daily intake. It is known that 1%–14% of PCBs in industrial products in Japan are CoPCBs.70 It is conceivable that the concentration of Co-PCBs in breast milk rapidly decreased as a result of the rapid decrease in the amount of PCB exposure when PCB production and use were banned in 1973. During the 23 years from 1973 to 1996, the polychlorinated dibenzodioxins and

240

polychlorinated dibenzo furans (PCDD/DFs) level decreased gradually from 30 pg-WHO-TEQ/g-fat to approximately 20 pg-WHO-TEQ/g-fat; however, a more rapid decrease was seen during the 5 years from 1999 to 2004. This second period roughly corresponds to the time when advanced dioxin control measures were implemented. The levels of total dioxins (PCDDs/DFs + Co-PCBs) are also shown in Figure 11. There was a decrease of almost 10 pg-WHO-TEQ/g-fat from 1996 to 1998 and a similar decrease from 2001 to 2004. Thus, it is likely that each of the advanced dioxin control measures had effects on the concentration of dioxins in breast milk. As described above, two major periods are noteworthy for their decreasing concentration of dioxins in breast milk: a period of rapid decrease of Co-PCBs from 1973 to 1986 and a period of rapid decrease of PCDDs/DFs after 1999. We believe that the former decrease resulted from the control measures related to the PCB products, and the latter decrease resulted from the advanced dioxin control measures in waste incineration.

Dioxin transport pathways Figure 12 shows the effects of dioxin reduction policies in various areas from 1997 to 2004 (levels in 1997 = 100%).

The dioxin source is represented by the dioxin concentration in flue gases and the total amount of dioxin emitted, the environment is represented by dioxin concentrations in the air and soil, and the human body is represented by the daily intake and dioxin concentration in breast milk. In this discussion, the general exposure pathway from the source to the human body is assumed to be as follows. Dioxins are transferred from a source into the air through flue gases and are deposited in the soil and on soils and food. The air and vegetables also serve as media that are directly ingested by humans. Some of the dioxins settle in the ocean and other bodies of open water. Soil also flows into the water system via erosion caused by rainfall. The mud deposited in the rivers by surface erosion is moved to the ocean by river flow. Part of the mud settles on the bottom of the ocean, another part is taken into the food chain, and the dioxins are accumulated in fish and seafood. Fish and other seafood are consumed by humans. According to Fukushima et al.,71 wide-area diffusion in the air, erosion of soil by rainfall, and its settlement in bay areas are the major transfer routes of polycyclic aromatic hydrocarbons (PAHs) and dioxins in the environment. The intake pathway from fish and seafood is particularly important in Japan, where the consumption of fish and other seafood is popular. By 2004, the dioxin concentration in flue gas and the amount of dioxin discharged had decreased to 6% and 4%, respectively, of the 1997 levels (Fig. 12). Further decreases are expected as more facilities are updated to meet the permanent measures criteria. The dioxin concentration in the air has decreased to 11% of the 1997 level, and the soil concentration is 48% of the 1997 level. The pattern of decrease is different for the air and soil concentrations. Since soil, unlike air, is a stationary medium and is not able to quickly flow and diffuse, the effect of the measures to reduce contamination is also slower. In addition, soil sampling sites may be contaminated by other dioxin sources such as herbicides.72

PCB reduction

Fig. 12. Effects of dioxin reduction policies on a humans, b the environment, and c emission sources, 1997–2004. Values for 1997 are set as 100%

Because the ratio of Co-PCBs to the total substances contributing to TEQ is high, it is necessary to pay further attention to Co-PCBs for reduction of dioxins in foods. In particular, proper management of PCB wastes that contain a high ratio of Co-PCBs has been identified as a high-priority issue.73 Fish and seafood are preferred foods in the Japanese diet,73 and it is known that fish and seafood contain a higher proportion of Co-PCBs than other foods.74 Iimura et al.75 studied the dioxin distribution in sea water, bottom sediments, and aquatic organisms in Tokyo Bay and found that Co-PCBs account for 90% of dioxin TEQ and that CoPCBs are derived from PCB products. According to a survey on the daily intake of dioxins,67 60%–70% of the TEQ of dioxins contained in fish and seafood is a result of Co-PCBs. Since dairy products are popular in European diets, studies have also been conducted on the dioxins con-

241

tained in milk and dairy products in addition to fish and seafood. A study of daily intake in the UK showed that the Co-PCB TEQ is 60%–70% in fish and about 50% in dairy products.76 In Germany, Co-PCBs in milk (sampled from 2001 to 2004) and butter (sampled in 2002) contributed about 70% of TEQ.77 The EU has determined the upper limit of the dioxin concentration in specific foods,78 but these limits need more attention because Co-PCBs are not included.79 The influence of Co-PCBs on TEQ is also significant from the perspective of dioxins in the human body. In Japan, Co-PCBs account for more than 30% of dioxin TEQ in breast milk (see Fig. 11), and cases as high as about 40% in human blood have been reported.66 In Norway, where the consumption of fish and seafood is high, the contribution of Co-PCBs to dioxin TEQ in breast milk was 49%.80 It has been speculated that the cause of these high values is exposure to PCBs. Recently, there was a report on the relative increase in the proportion of incineration-derived CoPCBs in breast milk in the Osaka region.81 Co-PCBs in the environment can be divided into CoPCBs derived from products containing PCBs (hereafter, PCB products) and unintentionally generated Co-PCBs. The PCB-products-derived Co-PCBs enter the environment from equipment that contains PCBs, as well as from improper storage and illegal dumping of PCB wastes. The unintentional generation of Co-PCBs mainly occurs in association with waste incineration. Comparison of the two types reveals significant differences in isomers and in the congener pattern.70 Co-PCBs widely penetrated into the environment in the period when PCB products were produced and used, and they also accumulated, primarily in marine areas and lakes. When PCB regulation began, the Co-PCB concentration in the environment decreased. Due to this reduction, the proportion of incineration-derived Co-PCBs has increased. The use of advanced dioxin control measures has drastically reduced the amount of incineration-derived Co-PCB formation, but the level of Co-PCBs remains high in fish and seafood. Therefore, control of CoPCBs is considered to be crucial for preventing human exposure to PCBs. PCB-waste-derived Co-PCBs are persistent in the environment; thus, they will be of particular importance in the future. For that reason, further promotion of successful PCB treatment projects and implementation of strict management criteria for stored PCB wastes are needed. In other words, since dioxins have only negative effects on humans, it would be better to have zero formation and zero intake if at all possible. Co-PCBs, which account for most of the TEQ of dioxin intake, are considered to have a long exposure pathway from the environmental media to the organism and the human body, so considerable time will be needed to observe the effect of the preventative measures. The essential viewpoint required in waste management policy today is to prevent shifting the burdens of the present generation to future generations. From this viewpoint, it is obvious that political measures are needed for further, prompt eradication of Co-PCBs.

Conclusion Japan has tackled the challenges of managing dioxins and PCBs by introducing both new policies and new technologies. As a result, a 95% reduction of the amount of dioxins emitted was achieved between 1997 and 2003. Since the Japanese government made efforts to promote the construction of facilities for treating PCB wastes, five facilities have commenced operations. To maintain current successful programs and meet future challenges, it is necessary to continually promote measures to control these substances and to provide information regarding political experiences to the public. Acknowledgment We deeply appreciate the contributions of the late Professor Hiraoka, who had been long engaged in scientific work on dioxins and PCBs.

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