Aerosol Science and Technology: History and Reviews

Aerosol Science and Technology: History and Reviews Edited by David S. Ensor RTI Press

2011 Research Triangle Institute. RTI International is a trade name of Research Triangle Institute. All rights reserved. Please note that this document is copyrighted and credit must be provided to the authors and source of the document when you quote from it. You must not sell the document or make a profit from reproducing it. Library of Congress Control Number: 2011936936 ISBN: 978-1-934831-01-4 doi:10.3768/rtipress.2011.bk.0003.1109 www.rti.org/rtipress About the Cover The cover depicts an important episode in aerosol history the Pasadena experiment and ACHEX. It includes a photograph of three of the key organizers and an illustration of a major concept of atmospheric aerosol particle size distribution. The photograph is from Chapter 8, Figure 1. The front row shows Kenneth Whitby, George Hidy, Sheldon Friedlander, and Peter Mueller; the back row shows Dale Lundgren and Josef Pich. The background figure is from Chapter 9, Figure 13, illustrating the trimodal atmospheric aerosol volume size distribution. This concept has been the basis of atmospheric aerosol research and regulation since the late 1970s. This publication is part of the RTI Press Book series. RTI International 3040 Cornwallis Road, PO Box 12194, Research Triangle Park, NC 27709-2194 USA rtipress@rti.org www.rti.org

Chapter 21 Trends in Airborne Concentrations of Total Suspended Particles, PM 10, SO 2, and NO 2 in Five Chinese Cities Shen Tian, Cliff I. Davidson, and H. Keith Florig Introduction During the past few decades, China s sustained and unprecedented economic growth has been accompanied by persistent urban air pollution problems. Significant sources of urban air pollutants include stationary sources such as coal boilers, industrial furnaces, motor vehicles, construction dust, and crop burning in upwind rural areas. National policies for management of urban air pollution were first promulgated by the National Environmental Protection Agency. Reflecting the growing importance of environmental issues in Chinese domestic policy, this agency was twice elevated once to the State Environmental Protection Administration in 1998 and again to the Ministry of Environmental Protection (MEP) in 2008 (Jaheil, 1998; Sun, 2001). This chapter addresses the historical ambient air pollution records for five Chinese cities, each chosen for its importance as a center of government, commerce, or industry. The cities include China s capital city, Beijing (population 13 million); the country s financial hub, Shanghai (population 20 million); and Taiyuan (5 million), Tianjin (8 million), and Xian (2 million), which are industrial centers in the central, north, and mid-west regions, respectively. China s urban ambient monitoring network was launched in the mid-1980s, initially recording total suspended particles (TSP) and sulfur dioxide (SO 2 ). Nitrogen dioxide (NO 2 ) monitoring was added in the mid- 1990s. PM 10 monitoring was phased in around 2000. Today, carbon monoxide (CO) and ozone (O 3 ) are also frequently monitored. Annual average levels of monitored pollutants for many dozens of selected cities (not always the same cities from year to year) are available in the China Environment Yearbook series, published by the MEP.

552 Part V. Reviews Beginning in 2000, each Chinese city has been required to publish a daily air pollution index. The reported number is actually the greatest of several indices, one each for PM 10, SO 2, and NO x representing the sum of nitric oxide (NO) and NO 2, and sometimes CO and O 3. Each index ranges from 0 500, corresponding to different concentration ranges for each pollutant. The daily reported index consists of both the numeric value of the index and the pollutant on which it is based. For many cities, this pollutant changes over periods of days. Currently, the daily air pollution index for a number of cities is available on the MEP website (http://www.zhb.gov.cn). Beginning in 1982, China established primary and secondary ambient air quality standards for several pollutants. Values of these standards for the pollutants of interest here are presented in Table 1. Primary standards are those designed for national parks and historic sites. Secondary standards are for protection of human health and apply to residential and commercial areas in both cities and rural areas. These standards have been adopted based on criteria similar to standards in other countries, such as the United States. In this chapter, we present airborne concentration data reported by the MEP and discuss data trends in terms of economic development, regulations, and control technologies. Table 1. National primary and secondary ambient air quality standards annual average, micrograms per cubic meter Pollutant Primary Secondary US National Ambient Air Quality Standards: Primary Standard SO 2 20 60 0.03 ppm (80 µg/m 3 ) annual average Total Suspended Particles 80 200 N/A PM 10 40 100 N/A NO 2 40 40 0.053 ppm (100 µg/m 3 ) annual average Source: State Environmental Protection Administration, 1996. Air Pollutant Concentrations in Chinese Cities Figure 1 presents annual average particle concentrations in the five cities over a 20-year period. The secondary ambient air quality standards for TSP and PM 10 are indicated by horizontal broken lines. These data show that

Total Suspended Particle Trends (PM 10, SO 2, NO 2 ) in China 553 particle levels declined in each of the five cities over this period, with the most dramatic declines in the more industrial cities of Taiyuan, Tianjin, and Xian. Despite these improvements, ambient particle concentrations remain above the Chinese standard for residential areas in all cities except Shanghai. Levels in Shanghai may be low due to lesser quantities of heavy industry there. 1000 Concentration, micrograms per cubic meter 700 500 300 200 Beijing Shanghai Taiyuan Tianjin Xian TSP & PM 10 stand 100 1986 1990 1994 1998 2002 2006 Year Figure 1. Average annual TSP (1986 1999) and PM 10 (2001 2006) concentrations in five Chinese cities, showing comparison with the secondary ambient air quality standards for annual average concentration. Around the year 2000, TSP measurements were largely replaced with PM 10 measurements. The horizontal broken lines indicate the secondary standards for TSP and PM 10, where the latter standard is coincident with the x-axis. Source: Ministry of Environmental Protection, various years. Figures 2 and 3 present similar plots for annual average SO 2 and NO x /NO 2 concentrations in the five cities, along with their respective secondary ambient air quality standards. SO 2 levels have declined markedly in many cities over the past 20 years, but concentrations in some cities remain above the secondary ambient air quality standard. In contrast to particle and SO 2 concentrations, NO x and NO 2 concentrations have increased in many cities over the past 20 years, presumably the result of the dramatic increase in motor vehicles in urban areas. Nationwide, from 1989 2006, the number of cars, trucks, and buses in Chinese cities increased from 13 million to 37 million (Fridley & Arden, 2008).

. 554 Part V. Reviews 1000 Concentration, micrograms per cubic meter. 100 Beijing Shanghai Taiyuan Tianjin Xian SO 2 standard 10 1986 1990 1994 1998 2002 2006 Year Figure 2. Average annual SO 2 concentrations in five Chinese cities, showing comparison with the secondary standard for annual average concentration. 1000 Beijing Concentration, micrograms per cubic meter 100 NO x NO 2 Shanghai Taiyuan Tianjin Xian NO 2 standard 10 1986 1990 1994 1998 2002 2006 Year Source: Ministry of Environmental Protection, various years. Figure 3. Average annual NO x (1988 2000) and NO 2 (2001 2006) concentrations in five Chinese cities, showing comparison with the secondary standard for annual average concentration. Source: Ministry of Environmental Protection, various years.

Total Suspended Particle Trends (PM 10, SO 2, NO 2 ) in China 555 Air Pollution Management and Emission Trends The history of air pollution control in China is summarized by Sun (2001). China s first national environmental protection law was implemented on a trial basis in 1979, and China s first air pollution control measures were introduced by local governments in the mid-1980s to address high particle levels. These measures included retrofitting coal boilers with cyclones, substituting coal briquettes and gaseous fuel for raw coal in household stoves used for cooking and heating, and replacing smaller residential heating units with larger centralized heating. These measures were responsible for the dramatic declines in particle levels experienced in the 1980s and 1990s by many northern cities with cold weather and high coal consumption. Since then, both local and national governments have implemented a variety of laws, standards, and regulations to manage air pollution. In addition, each province has passed its own environmental regulations. In the following sections, we describe the progress that the five selected cities in China have made in recent years in pursuing a variety of air pollution control strategies. Other Chinese cities have adopted similar strategies. Air Pollution Management in Beijing In the decade leading up to the 2008 Olympic Games, the Beijing municipal government established an aggressive program of air pollution management, consisting of 11 measures aimed at industry, agriculture, construction, transportation, and residential heating (Chai et al., 2006). The measures included closing or moving large industrial facilities far from the city, installing flue gas desulfurization in power plants, substituting gas for coal in many applications, reformulating gasoline and removing old vehicles from the roadways, and reducing dust from construction sites. These control measures were highly effective in reducing emissions, which, in turn, reduced airborne levels. In China, data on particle and SO 2 emissions are self-reported by every enterprise that operates a boiler or furnace, including industrial, commercial, residential, and government entities. Enterprises estimate their emissions based on regulatory formulas that use the mass of coal burned, coal ash and sulfur content, and the technology for flue gas treatment. Reported emissions of particles and SO 2 by enterprises in Beijing from 1998 to 2005 are shown in Figures 4 and 5. Note that the designation of particles is not necessarily the same as TSP measured in ambient air reported above. TSP is an operational definition referring to all

556 Part V. Reviews particles collected by the samplers used for ambient monitoring, while the particle emissions in Figure 4 are estimates based on the regulatory formulas. Emissions, 1,000 metric tons per year 140 120 Particles, Total Particles Industry 100 80 60 40 20 0 1998 2000 2002 2004 Year Figure 4. Self-reported particle emissions in Beijing from coal combustion by industrial, commercial, residential, and governmental end users. Source: Fridley & Arden, 2008. Emissions, 1,000 metric tons per year 350 300 SO 2, total 250 SO 2, Industry 200 150 100 50 0 1998 2000 2002 2004 Year Figure 5. Self-reported SO 2 emissions in Beijing from coal combustion by industrial, commercial, residential, and governmental end users. Source: Fridley & Arden, 2008. Automobile Emission Control In 1995, Beijing started a pilot inspection/maintenance program. This program, which was upgraded to full-scale operations beginning in 1999, focused on CO. In addition, an acceleration simulation mode testing program was implemented specifically to reduce PM 10 and NO x emissions beginning

Total Suspended Particle Trends (PM 10, SO 2, NO 2 ) in China 557 in 2003. Many older vehicles were required to obtain retrofits to reduce emissions. For example, approximately 190,000 carbureted vehicles registered after 1995 were retrofitted with three-way catalysts between 1998 and 2001. This retrofit reduced CO emissions by 78 90% and reduced hydrocarbon plus NO x emissions by 71 88% immediately after the retrofit (Hao et al., 2006). In 1999, the Beijing municipal government implemented the Euro 1 emission standard, which was then adopted by all of China the following year. In 2003, Beijing also implemented the Euro 2, which was subsequently adopted across China in 2004. The two standards are shown in Table 2. Table 2. Euro 1 and Euro 2 emission standards Maximum Emissions Vehicle type Emission standard CO HC + NO x HC NO x PM Light-duty gasoline automobiles (g/km) Euro 1 3.16 1.13 Euro 2 2.20 0.5 Heavy-duty diesel vehicles (g/kwh) Note: kwh = kilowatt-hours. Source: Hao et al., 2006. Euro 1 4.5 1.1 8 0.36 Euro 2 4.0 1.1 7 0.15 Beijing adopted a law requiring the retirement of older vehicles starting in 2003. All light-duty cars are forced to retire in 15 years, while taxis and buses are forced to retire in 8 years. In 1999, the government increased the taxes on leaded gasoline to discourage its use. Furthermore, a new rule granted a 30% reduction in the excise tax, which is 5% of the vehicle price for a typical car in China, for light-duty vehicles meeting Euro 2 emission standards. This rule went into effect at the end of 2001, prior to the requirement of Euro 2 standards in Beijing in 2003 (Hao et al., 2006). Closing and Relocating Industries Since 2000, the Beijing municipal government has undertaken a major effort to relocate industries with high pollutant emissions. At the end of 2000, the Beijing Steel Alloy Company closed and the Beijing Yanshan Cement Company moved to the city of Tangshan, 200 miles southeast of Beijing. The Beijing Coke Industry, one of the largest pollutant emitters in the city, closed in 2006. The biggest company to relocate thus far is Beijing Capital Steel

558 Part V. Reviews Company. Starting in 2002, with a total steel production of 8 million metric tons per year, this company decreased its operations by 2 million metric tons per year while building a new facility in Hebei province. The company eventually closed a blast furnace, four sinter boilers, one coke plant, and three converters at its Beijing location. By the end of 2007, the company had moved its entire production to the new location, which had state-of-the-art equipment. Changes in Energy Sources Changing furnaces from coal to natural gas or to coal gas can be an effective way to decrease air pollutants, especially SO 2. Coal gas, a synthetic gas made from coal, is composed of hydrogen, carbon monoxide, methane, and volatile hydrocarbons. Natural gas and coal gas have replaced coal for residential heating in Beijing. Coal has also been replaced as a raw material in the chemical industry and in industrial boilers, stoves, and furnaces. From 1990 to 2005, total energy consumption in Beijing more than doubled, from 27 Mtce per year to 55 Mtce per year, where Mtce is million metric tons of coal equivalent (Beijing Municipal Statistics Bureau, 2006). This increase in consumption has been accompanied by a significant change in the sources of energy consumed. In particular, Figure 6 shows that the direct use of coal has been replaced by direct use of natural gas and by the use of electricity. Although electricity in China is largely generated by coal, it is listed as a separate category in the figure because managing the combustion process in large, centralized power generation plants allows more efficient control technology to be used to reduce emissions. Furthermore, the pollutants are emitted at the power plants, which are usually located in less densely populated areas compared with urban residences. The percentage of direct coal use in total energy consumption decreased from 77% in 1990 to 21% in 2005; the percentage of electricity use increased from 9% to 35%; the percentage of natural gas use increased from 1.4% to 8.4%; and the percentage of petroleum (in the form of liquefied petroleum gas and gasoline) increased from 6% to 25%. Much of the reduction in pollutant concentrations summarized in Figures 1 and 2 is the result of these changes in energy sources. Table 3 shows the emission standards for Beijing for TSP, SO 2, NO x, and opacity of the plume based on the Ringelmann number.

Total Suspended Particle Trends (PM 10, SO 2, NO 2 ) in China 559 Fraction of total energy consumption 0.9 0.8 0.7 0.6 0.5 0.4 0.3 0.2 0.1 0 Coal Electricity LGP Coal gas Natural gas Geothermal Gasoline 1990 1995 2000 2005 Year Figure 6. Sources of energy consumed in Beijing from 1990 to 2005. Source: Beijing Municipal Statistics Bureau, 2006. Table 3. Emission standards for boilers in Beijing Power Plant Boiler Industry Boiler TSP (mg/m 3 in the plume) 10 10 SO 2 (mg/m 3 in the plume) 20 20 NO x (mg/m 3 in the plume) 100 150 Ringelmann number 1 1 Source: Beijing Municipal Environmental Protection Bureau, 2007. Construction Site Dust Control Extracted surface soils at construction sites are usually stored on site for 1 or 2 days before being transported. Based on Beijing s Air Pollution Prevention and Control Law (Chai et al., 2006), this soil must be covered, which is often done with plastic canvas. Trucks transporting the soil must also be covered. Similar regulations for construction sites as well as for mobile and stationary sources can be found in the local Air Pollution Prevention and Control Laws for each of the other four cities. Air Pollution Management in Shanghai The Shanghai municipal government began implementing air pollution control measures in 1976. In the first 7 years of its control program, 17 large industrial boilers were renovated, and this decreased self-reported particle emissions by 25,000 metric tons over this period. Between 1982 and 1985, many small industrial boilers were renovated. These measures were largely

560 Part V. Reviews responsible for a 38% decrease in dust fall between 1978 and 1984. From 1986 to 1988, the government passed several particle emission regulations that required industries to install precipitators. The efficiency of these precipitators was required to be 50% after this 2-year period. In 1990, the minimum efficiency was increased to 70%, and in 1992 it was increased to 81%. This last regulation required companies to use multicyclones rather than monocyclones for their precipitators. As a result, the average TSP concentration in plumes emitted from industries in Shanghai decreased from 378 mg/m 3 to 241 mg/m 3 (Li, 1996). Relocation of Industries He Tian is an industrial area of Shanghai with 32 major companies, each having significant emissions. The municipal government began moving these companies out of the city in 1992, and as a result coal consumption in the Shanghai urban area decreased steadily: 5,000 kt in 1993, 4,500 kt in 1994, and 3,900 kt in 1995 (Li, 1996), where kt is a thousand metric tons. Starting in 2000, all electricity generating plants using coal in the city were required to install desulfurization equipment. Changes in Energy Sources With a rapidly increasing population and rapidly increasing energy consumption, Shanghai is the largest city in China. Because of efforts to control escalating coal use, the proportion of energy supplied by coal decreased by 5 8% between the 5-year period beginning in 1995 and the 5-year period beginning in 2000. However, the total amount of coal used in Shanghai increased from 45 million metric tons in 2000 to 53 million metric tons in 2005 (Qian & Wang, 2004). There are other areas of progress. By 2005, nearly 3,300 small and midsized boilers had switched from coal to natural gas, thus decreasing their emissions by 10 kt for PM 10, 57 kt for SO 2, and 15 kt for NO x. To decrease SO 2 emissions from direct coal use in residences, the municipal government encouraged citizens to use coal gas as a substitute. By the end of 2000, 86% of families in the city used coal gas, which decreased SO 2 emissions from direct coal use in residences by about half (Qian & Wang, 2004). The fraction of energy contributed by each source during the period 2001 2005 is shown in Figure 7.

Total Suspended Particle Trends (PM 10, SO 2, NO 2 ) in China 561 Fraction of total energy consumption 0.7 0.6 0.5 0.4 0.3 0.2 0.1 0 0.6 0.06 0.25 0.07 2001 2005 0.015 Coal Electricity Petroleum Natural gas Other Wind Solar 0.003 Figure 7. Sources of energy consumed in Shanghai from 2001 to 2005. Source: Data are from Qian & Wang (2004). Air Pollution Management in Taiyuan Because Taiyuan was one of the most polluted cities in China, the local government passed a series of regulations to control air pollution, including the clean development regulation and particulate control laws (Wang, 2004). Taiyuan has also attempted to decrease industrial emissions. Because small companies emit more pollutants per unit product than larger companies, in 2004 the government closed all the cement factories with a capacity less than 300,000 metric tons per year. The government also closed all paper, steel, and coke plants with annual capacities less than 0.5 million, 0.5 million, and 0.4 million metric tons, respectively. Taiyuan implemented the Kyoto Protocol Clean Development Mechanism by switching from coal to natural gas in 2,000 boilers and closing 600 boilers in a 177 km 2 emission control area within the city. In 2003, every company emitting sulfur in Taiyuan was required to install desulfurization equipment. This measure decreased SO 2 by 2,500 metric tons in that year. Also in 2003, a 21 km 2 clean fuels area and a 3 km 2 coal-free area were established within the city. By building a centralizing heating system, Taiyuan was able to close 718 small boilers, which decreased coal use by 95,000 metric tons per year and reduced annual emissions of TSP and SO 2 by 48,000 metric tons and 38,100 metric tons, respectively.

562 Part V. Reviews Air Pollution Management in Tianjin Tianjin is 200 km southeast of Beijing. Like most cities in northern China, the major air pollutants there were from coal combustion, automobile emissions, and construction sites. To reduce air emissions, the government took similar measures as in Beijing, such as substituting natural gas for coal in boilers. By April 1999, over 19,000 residential boilers and 500 industrial boilers had been converted to natural gas. Based on the Air Pollution Control and Prevention Act for the city of Tianjin, a coal-free area was established, and sources outside this area were required to use low-sulfur coal. Dust from construction sites has also been regulated. Air Pollution Management in Xian The municipal government of Xian made progress in air pollution control beginning in the 1980s. Of the total particle emissions in the city, 40% comes from soil, 27% from coal combustion, and 22% from construction sites. The Xian government has promulgated several laws to restrict air pollutant emissions, such as the Air Pollution Control Act Phase I (City of Xian, 1999), Phase II (City of Xian, 2000), and Phase III (City of Xian, 2001). Xian has also enforced the national standard for air pollutant emissions from boilers (State Environmental Protection Administration, 2002). The following is a summary of some of the most important changes in Xian: Seventy-five percent of the automobiles in Xian are required to pass an emission test, and this is enforced through fines. An area of coal combustion control was established for 92% of the city land area by 2006. (Achieving this required updating boilers and using low-sulfur coal.) Residents were provided with natural gas for domestic use instead of coal. Dust emissions from construction sites were reduced by covering excavated soil. The use of natural gas was especially important: During Air Pollution Control Act Phase III, approximately 40,000 families switched from coal to natural gas. This significantly reduced the amount of coal use in Xian, as shown in Table 4. But economic development and associated emissions from other sources were probably responsible for preventing the airborne SO 2 concentration from decreasing substantially over the longer term, as indicated by Figure 2.

Total Suspended Particle Trends (PM 10, SO 2, NO 2 ) in China 563 Table 4. Residential energy fuel mix in Xian, 1995 2000 Type of Energy 1995 1996 1997 1998 1999 2000 Liquefied Petroleum 29,000 30,300 27,500 26,800 39,200 43,000 Gas (t) Natural Gas (10 4 m 3 ) ~0 ~0 61 1,250 4,050 11,500 Coal (10 4 t) 18,400 8,370 8,230 7,830 3,750 2,160 Note: t = metric tons. Source: Cheng, 2003. Conclusion In recent years, air quality in major Chinese cities has improved. The municipal governments no longer focus only on economic development; they also take steps to improve environmental quality. Particle levels have decreased rapidly in the past 20 years, although PM 10 is still the air pollutant most frequently in violation of ambient standards. As a result of establishing coal-free regions within cities, use of low sulfur coal, and other actions, airborne SO 2 is decreasing in most, but not all, urban areas. Most of these cities also target specific sources for air pollutant regulation, focusing on four strategies. The first is automobile emission control, especially in Beijing where the government is restricting operation of vehicles and establishing laws to reduce emissions. The second is closing, renovating, or relocating industries. The third is changing sources of energy, such as switching from coal to natural gas. The fourth is dust control at urban construction sites. Air pollution levels may continue to decrease in Chinese cities as additional pollutant regulations are established. Despite reduction of emissions in Chinese cities, long-range transport from rural areas can contribute substantially to urban air pollutant concentrations as local emissions in cities are reduced. This has been documented in other countries and has recently been documented in China as well (Streets et al., 2007). Furthermore, improving standards of living are likely to increase energy use, which may counteract pollution reduction efforts. Increasing population levels in these cities will also put upward pressure on pollution levels.

564 Part V. Reviews Acknowledgments The authors wish to thank Dr. Thomas Rawski, Department of Economics, University of Pittsburgh, for his help with this work. References Beijing Municipal Environmental Protection Bureau and the Beijing Quality and Technical Supervision Bureau. (2007). Emission standard of air pollutants for boilers (Report DB11/139-2007, implemented September 1, 2007). Retrieved from http://www.bjepb.gov.cn/bjhb/portals/0/fujian/ zwgk/flfg/20070904.pdf. (in Chinese) Beijing Municipal Statistics Bureau, Industrial Transportation Statistics Office, Industrial Investigative Branch. (2006). Beijing energy and economic development analysis (2006-08-23). Retrieved from http://www.bjstats.gov. cn/ldcxxt/tjfx/tjbg/200609/t20060901_62529.htm. (in Chinese) Chai, F., et al. (2006, July). Analysis of effectiveness of air pollutant emission control in Beijing. Environmental Protection, 49 52. (in Chinese) Cheng, J. (2003, September). Changing from coal to natural gas to improve air quality in the city of Xian, Journal of Changan University Arch. and Envir. Science Edition, 44-47. (in Chinese) City of Xian. (1999). Air Pollution Control Act Phase I, 1999. Retrieved from http://law.lawtime.cn/d456068461162.html. (in Chinese) City of Xian. (2000). Air Pollution Control Act Phase II, 2000. Retrieved from http://law.laweach.com/rule_200367_2.html. (in Chinese) City of Xian. (2001). Air Pollution Control Act Phase III, 2001. Retrieved from http: //www.66law.cn/lawlib/viewlawlib.aspx?id=74159. (in Chinese) Fridley, D., & Arden, N. (Eds.) (2008). China energy databook (7th ed.). Berkeley, CA: Lawrence Berkeley Laboratory. Hao, J., Hu, J., & Fu, L. (2006). Controlling vehicular emissions in Beijing during the last decade. Transportation Research, Part A: Policy and Practice, 40, 639 651. Jaheil, A. R. (1998). The organization of environmental protection in China. The China Quarterly, 156, 757 787. Li, J. (1996). Analysis of countermeasure effects of amelioration on atmospheric quality in Shanghai, Shanghai Environmental Science, 15, 1 3. (in Chinese)

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