Journal of Environmental Radioactivity 102 (2011) 400e406

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Journal of Environmental Radioactivity

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Contribution of 222Rn-bearing water to indoor radon and indoor air quality assessment in hot spring hotels of Guangdong, China
Gang Song a, *, Xinming Wang b, Diyun Chen a, Yongheng Chen a
a b

School of Environmental Science & Engineering, Guangzhou University, Guangzhou 510006, PR China Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, PR China

a r t i c l e i n f o
Article history: Received 7 October 2010 Received in revised form 13 February 2011 Accepted 13 February 2011 Available online 5 March 2011 Keywords: Hot spring hotel Water 222 Rn PM2.5 and PM10 CO2 Indoor air quality

a b s t r a c t
This study investigates the contribution of radon (222Rn)-bearing water to indoor 222Rn in thermal baths. The 222Rn concentrations in air were monitored in the bathroom and the bedroom. Particulate matter (PM, both PM10 and PM2.5) and carbon dioxide (CO2) were also monitored with portable analyzers. The bathrooms were supplied with hot spring water containing 66e260 kBq m3 of 222Rn. The results show that the spray of hot spring water from the bath spouts is the dominant mechanism by which 222Rn is released into the air of the bathroom, and then it diffuses into the bedroom. Average 222Rn level was 110e410% higher in the bedrooms and 510e1200% higher in the bathrooms compared to the corresponding average levels when there was no use of hot spring water. The indoor 222Rn levels were inuenced by the 222Rn concentrations in the hot spring water and the bathing times. The average 222Rn transfer coefcients from water to air were 6.2 104e4.1 103. The 24-h average levels of CO2 and PM10 in the hotel rooms were 89% and 22% higher than the present Indoor Air Quality (IAQ) standard of China. The main particle pollutant in the hotel rooms was PM2.5. Radon and PM10 levels in some hotel rooms were at much higher concentrations than guideline levels, and thus the potential health risks to tourists and especially to the hotel workers should be of great concern, and measures should be taken to lower inhalation exposure to these air pollutants. 2011 Elsevier Ltd. All rights reserved.

1. Introduction Most people stay much longer indoors than outdoors and as a result often have much higher exposure to hazardous air pollutants; therefore health risks due to poor indoor air quality (IAQ) are still of great concern to the academic, the public and the regulatory bodies. Many studies have been conducted on indoor air pollutants including indoor radon (222Rn) (Denman et al., 2007; Espinosa et al., 2008; Tuia and Kanevski, 2008; Vinson et al., 2008; Ciolini and Mazed, 2010; Yoon et al., 2010), particulate matter and CO2 (Jones et al., 2000; Korhonen et al., 2000; Isbell et al., 2002; Lee et al., 2002a; Michielsena and Tymen, 2007; Shao et al., 2007; Perrier and Richon, 2010; Wang et al., 2010). Recently, the Chinese Government has recognized the potential risks and problems related to indoor air pollution, and it has established the new IAQ standard (GB/T18883-2002, China). The IAQ inside restaurants and hotels is an interesting issue in China, but only a few studies were available in restaurants (Lee et al., 2001, 2002b; Liu et al., 2004) and hotels (Feng et al., 2004; Song et al., 2005).

* Corresponding author. Tel.: 86 20 36180459; fax: 86 20 39366946. E-mail address: songg2005@126.com (G. Song). 0265-931X/$ e see front matter 2011 Elsevier Ltd. All rights reserved. doi:10.1016/j.jenvrad.2011.02.010

Of all the radioisotopes that contribute to natural background radiation, 222Rn presents the largest risk to human health (Hopke et al., 2000). Because 222Rn is relatively insoluble in water, 222Rn is a signicant component of the groundwater (Zhuo et al., 2001; Galn Lpez and Martn Snchez, 2008; Vesterbacka et al., 2010) that discharges in the springs (Horvth et al., 2000; Wilkes et al., 2005; Nikolopoulos and Vogiannis, 2007; Prasad et al., 2009; Chaudhuri et al., 2010). Guangdong is one of the provinces in China that has many hot springs. Many hotels have been set up near hot springs. In these so-called spa hotels, hot spring water is distributed to the bath inside each hotel room, and hot spring bathing has become a key point of business development to attract tourists. Radon in spring water has been regarded as a component benecial to health (Zhou, 1987; Feng et al., 1994; Meng and Qin, 1994). Waters with higher 222 Rn levels are used in some health resorts for therapeutic purposes (Lettner et al., 1996; Nikolopoulos et al., 2010) on the theory of radiation hormesis, which refers to a curative effect of small doses of radiation. However, 222Rn in hot spring water has also attracted attention for its potential health risks, since 222Rn transferred from spring water to indoor air may bring about extra exposure to 222Rn via inhalation (Horvth et al., 2000; Vinson et al., 2008), and the health risks of indoor elevated levels of 222Rn have been well documented in a great many studies worldwide (Evans et al., 1981;

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Spengler and Sexton, 1983; Nero et al., 1986; ICRP, 1987, 1993; Clarke and Southwood, 1989; Yu et al., 1994, 2001; Vogiannis et al., 2004; Vinson et al., 2008; Ouabi, 2009; Koz1owska et al., 2010). The 222Rn concentration of hot spring water may lead to health risks from occupational (hot spring hotel workers) and occasional (tourists) exposure. In addition, indoor particulate concentrations are reported for Asian countries higher than Western countries (Salmon et al., 1994; Phillips et al., 1998, 1999; Jones et al., 2000; Chao and Wong, 2002; Xu et al., 2002). This phenomenon is perhaps due to the transport of polluted air from outdoor to indoor environment. This is particularly true for those buildings (houses, restaurant, hotel, et al.) that are located close to heavy trafc. Massey et al. (2009) reported the indoor average concentrations recorded for particulate matter <2.5 mm diameter (PM2.5) were maximum for the rural homes (173 mg m3) followed by roadside homes (138 mg m3) and then by urban homes (136 mg m3). Different living habits among people in Asian and Western countries are another factor that leads to higher indoor particulate levels in homes (WHO, 1999). Also in the hotel rooms there might be elevated indoor CO2 due to the human activities and insufcient ventilation, and indoor CO2 levels in excess of 1000 ppm (0.1%) are closely related to occupant complaints of sickbuilding syndrome (SBS) in WHO (1999) and Li et al. (2001). It was only presented that some hot spring hotel rooms had higher 222Rn levels and thus might have potential health risks through inhalation in Song et al. (2005). Other indoor pollutants need to be investigated because more and more people stay or work at the hot spring hotels. Radon decay products are highly particle-reactive; a signicant health risk could come from 222Rn decay products attached to PM (especially the inhalable particles, IP, both PM10 and PM2.5). Thus, rooms that have both exceeded 222 Rn and PM might have more signicant negative health effects. So we decide to investigate 222Rn and PM levels and there relations in the hot spring hotel rooms. Indoor CO2 is widely used as an indicator of ventilation effectiveness in an enclosed space. In order to study the 222Rn concentration changed with indoor ventilation, and the human activities inuence on indoor 222Rn and CO2, the indoor CO2 is measured in our study. So this study not only assesses the inuence of hot spring water use on indoor air quality in the hot spring hotels, but also a primary screening of indoor air pollutants such as PM and CO2. 2. Materials and methods 2.1. Description of the hotels Four hot spring hotels (S1, S2, S3 and S4) were selected in Guangdong and their locations were shown in Fig. 1. The S2 hotel is a ten-story building in the center of a county town; the other hotels are all four-story buildings in the suburb or rural areas, but S4 is near the Guang-Shao expressway with heavy trafc. All the hotels had central air-conditioning. More detail description of the hotels is given in Table 1. 2.2. Field work In each hotel, measurements were performed in hotel rooms both on the ground oor and on non-ground oors, except for S2 with guest rooms only above the second oor. Fig. 2 shows the generalized layouts of the hotel rooms and the indoor sampling sites. Prior to the bathing of the selected rooms, 222Rn in these rooms was also measured with all the windows and doors closed from 22:00 to 7:00, the time interval that tourists most possibly rest inside. Tourists who occupied the selected hotel rooms were asked to be volunteers and to document their activities in detail, especially their use of the spring

Fig. 1. Locations of sampling sites in Guangdong, China (in right corner of the lower part: location of Guangdong in China).

water. They were voluntarily to have totally more than one and a half hours of spring water bathing in the bathrooms during the three-day consecutive monitoring. They were free to go outside and to open windows in the hotel rooms if they wanted, just like tourists. Smoking at the selected rooms was not allowed in this study. Measurements were conducted indoors and outdoors at each hotel for three consecutive days. Measurements outdoors were performed with fastening the potable analyzers on the windowsills. The pollutants studied were 222Rn, PM10, PM2.5 and CO2. Radon was measured by a RAD7 (Niton Corporation, Bedford, MA, USA) and NR-667A () monitor (Song et al., 2005), PM10 and PM2.5 were analyzed by portable Dust-Trak monitors (Model 8520, TSI Inc., USA) and CO2 by portable Q-Trak monitors (model 8551, TSI Inc., USA; Zhao et al., 2004). The probes or air intakes of the air monitors were placed approximately 1.5 m above the oor and kept away from any source of targeted pollutants. The 222Rn detectors were set for a two-day consecutive monitoring with a cycle time of 30 min. The portable Q-Trak and Dust-Trak monitors only measured 30 min at every 2 h with a frequency of 4 readings per minute. Radon in the spring water used in the bath was also measured during the periods. The test water was directly taken from the bathing tap opened for 20 min. Water samples were collected in glass containers tted with rubber-Teon gaskets to prevent the escape of 222Rn gas, and headspace and air bubbles were avoided. The 222Rn concentration was determined by a scintillation cell method (Zhuo et al., 2001; Papastefanou, 2002; Zhuo and Tokonami, 2005): the air was passed through the sample in a bubbler ask to purge out the dissolved 222Rn by a gas-recirculating system, and then the released 222Rn was then transferred into an evacuated scintillation cell, which had a quartz window and was lined with ZnS (Ag) phosphor. After the transfer of 222Rn to the scintillation cell, the sample was stored at lease 3 h to allow equilibrium to be reached between 222Rn and its short-lived progeny. Then the cell was directly placed in an FD-125 scalar for a-particle counting. To analyze the air sample, the window end of the cell was placed on a photomultiplier tube to count the scintillations produced when alpha particles from 222 Rn decay struck the ZnS coating on the inside of the cell. A calculation was made to convert the counts to 222Rn concentrations. 2.3. Quality control and assurance The 222Rn monitors were calibrated every six months by University of South China. Pre-and post-zero check of Dust-Trak and Q-Trak monitors were performed. Before sampling, the Q-Trak was

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Table 1 Description of the four hot spring hotels selected in Guangdong, China. Hotel Location Background Floor Room dimension Indoor decoration S1 Hillside, Conghua Famous health resort in suburb of Guangzhou, more tourists and trafc 1st, 2nd 2.8 m high; 25 m2in area With wallpaper, oor carpeted S2 County town, Fengshun Downtown, densely populated area with heavy trafc 3rd, 5th, 6th 2.5 m high; 20 m2 in area With wallpaper, oor carpeted S3 Hillside, Huizhou Rural, less tourists and much less trafc inuence 1st, 2nd 2.6 m high, 23 m2 in area Plastering wall and tile oor (1st), wallpaper and carpeted oor (2nd) Tiled oor and wall Central air-conditioned, occupants may sometimes open the window S4 Roadside, Shaoguan Near industrial park, heavy trafc nearby 1st, 2nd 2.5m high, 18 m2in area Plastering wall and tile oor (1st), wallpaper and carpeted oor (2nd) Tiled oor and wall Central air-conditioned, occupants may sometimes open the window

Bath Ventilation condition

Tiled oor and wall Central air-conditioned, occupants may sometimes open the window

Tiled oor and wall Central air-conditioned, occupants may sometimes open the window

calibrated with standard CO2 gas at a known concentration. The Q-Trak was also sent back to and calibrated by the manufacturer annually. The Dust-Trak monitor cannot directly give the mass concentration of airborne particles, and a separate calibration was done to convert the results given by the Dust-Trak monitors into corresponding concentrations obtained by gravimetric methods, the details for calibration can be found in previous papers (Li et al., 2001; Lee et al., 2002a,b). In this study, the results were calibrated by the following equations (Li et al., 2005):

3. Results and discussion 3.1. Concentrations of

222

Rn

  To PM10 : M 0:485 MDT R2 0:92   To PM2:5 : M 0:525 MDT R2 0:96

where M is the calibration results, MD-T is the data of the Dust-Trak monitor measured, in mg m3, respectively.

Fig. 2. Layout of the hotel room and sampling sites (The part in dark is the bathroom) 1. Door; 2. Table; 3. Bath; 4. Window; 5. Bed; 6. Bedroom. :Indoor sampling sites.

The average 222Rn concentrations recorded at the selected four hotel rooms are shown in Table 2. Some of the average air 222Rn levels in the bedroom were lower than the guideline levels of USA (148 Bq m3) and WHO (200 Bq m3), and all of them lower than the IAQ standard of China (400 Bq m3). On the contrary, the average air 222 Rn in the bathrooms were all higher than 200 Bq m3 when bathing with hot spring water, the maximum average value was 720 Bq m3. The indoor 222Rn concentrations changed with the bathing time (Table 2). Higher indoor 222Rn levels were found in the bathrooms when the tourists were bathing as opposed to other activities, especially at S3, where the 222Rn level was up to 1100 Bq m3 during 45 min of bathing with hot spring water. The measured indoor 222Rn concentrations were lower than published data for other spas, for example the average 222Rn levels ranged from 850 Bq m3 to 3300 Bq m3 in the 222Rn treatment facilities studied by Lettner et al. (1996), and 3560 Bq m3e6650 Bq m3 at the various points in the baths studied by Soto et al. (1995). But in our study, when there was spring water bathing, the average increase in air 222Rn levels detected in the bedroom were 110 40% (20e170%, S1), 300 120% (100e470%, S2), 410 270% (170e830%, S3) and 220 160% (30e500%, S4) higher than the averaged levels when there was no bathing with spring water. In the baths, average air 222 Rn levels during bathing were 510 360% (140e1100%, S1), 720 380% (350e1300%, S2), 1200 320% (680e1600%, S3) and 650 320% (230e1100%, S4) higher than those levels in non-bathing times. The results indicated that there is a correlation between indoor 222Rn concentrations and hot spring water 222Rn levels. There are higher 222Rn levels in hot spring water, and there will have higher indoor 222Rn concentrations in different bath times. Short-term diurnal variations of 222Rn concentrations are demonstrated by continuous measurements. Two days variations of 222 Rn concentrations in bathroom and bedroom with different bath times at the S2 hotel are shown in Fig. 3. The results indicated that the 222Rn concentrations in bathroom were signicantly impacted on the bath times and ventilation conditions. The 222Rn concentrations when closed the door and the window were higher than enhancing ventilation with opened the door and the window. The 222 Rn concentrations in bedroom were slightly changed with the bath times. It shows that the indoor 222Rn concentrations are impacted on the bath times and ventilation conditions. The spring water is one of the main sources of the indoor 222Rn. At the S1, S2, S3 and S4 springs, the test water samples were directly taken from the bathing tap in the bathroom. In each hotel, we had one water sample to determine the 222Rn extraction efciencies by multiple degasications. The extraction efciencies

G. Song et al. / Journal of Environmental Radioactivity 102 (2011) 400e406 The average values of radon concentrations for different bathing time excluding for non-bathing time (0 min). Radon transfer coefcients, DCa CN C0, CN is the radon concentrations for different bathing times (15 min, 30 min, 45 min and 60 min, respectively); C0 is the background radon concentration in hotel room; Cw is the radon concentration in tap hot water of bathroom. c The average transfer coefcients at different bathing times.

403

45 min

130 130 170 150 270 130 70 90

were all over 92% in our tests. The 222Rn concentrations and temperatures measured in the tap hot spring water are also shown in Table 2. The measured 222Rn concentrations only at the S3 hotel exceeded the U.S. EPA alternative maximum contaminant level (148 kBq m3). But S1 and S4 did not exceed that of several European countries (Sweden, Finland etc.) where this limit is 100 kBq m3 for municipal waters (Horvth et al., 2000). The measured 222Rn concentrations were similar to the published data or lower those data studied by Horvth et al. (242e576 kBq m3, 2000), Soto et al. (342e840 kBq m3, 1995) and Lettner et al. (20e4400 kBq m3, 1996). The fraction of the initial average 222Rn concentration in water that is contributed to the indoor-airborne 222Rn concentration can be indicated by transfer coefcients, dened as

DCa/Cw (104)
Average 60 min

10 10 50 20 50 10 4 4

160 130 140 110 280 170 120 150

20 30 20 10 20 30 20 2

120 130 130 110 200 140 70 90

40 10 40 30 90 30 30 50

2.2e12.4 9.9e12.0 3.6e9.4 3.2e8.7 2.7e12.7 2.7e5.0 3.0e11.6 1.1e15.7

(7.4) (11.1) (6.7) (5.9) (8.6) (3.8) (5.9) (7.5)

Transfer coefficient DCa =Cw

where DCa is the average increment added to the indoor air 222Rn concentration and Cw is the average concentration of 222Rn in water. The calculated transfer coefcients are shown in Table 2. The transfer coefcients were 4.1 103 (S1), 2.0 103 (S2), 2.3 103 (S3) and 3.1 103 (S4), respectively. The total average transfer coefcient in the bathrooms was (2.9 0.9) 103. Similarly, the values in the bedrooms were 9.2 104 (S1), 6.3 104 (S2), 6.2 104 (S3) and 6.7 104 (S4) respectively, the total average transfer coefcient was (7.1 1.4) 104. Song et al. (2005) reported transfer coefcients of 5.7 104, 5.0 104, 3.9 104 and 1.6 104 for other hot spring hotel bedrooms. The bedroom values in this study seem similar. The 222Rn transfer coefcient is valid for the time and spatial scale at which it is measured. The bedroom transfer coefcients varied because of large variations in room volume, construction methods, and ventilation. Gesell and Prichard (1980) rst estimated a 222Rn transfer coefcient of 104, and NRC (1999) also recommended the best central estimate of 1.0 104 from multi-day tests in houses during normal occupancy. Recently, Vinson et al. (2008) calculated a transfer coefcient of 1.65 103 in bathrooms during water use on short time scales. Our study found higher transfer coefcients in the hotel bathrooms due to the hot spring water use on multi-day measurements. The 222 Rn concentrations in our study are not higher than the other published studies e actually they are similar. Compared with tap water, hot spring water can create higher 222Rn activities and temperature (up to 45  C), both of which might contribute to the higher transfer coefcients in the bathrooms. Also these higher transfer coefcients are the result of high airborne 222Rn, small spatial scale and short temporal scale. 3.2. Carbon dioxide concentrations Radon and CO2 concentrations can change with the indoor ventilation rate and the human activities. The average CO2 concentrations recorded at the bedroom of four selected hot spring hotels are shown in Fig. 4. The average indoor CO2 levels in central air-conditioned bedroom were all higher than the 24-h average value of 1000 ppm stated in the IAQ standard of China. In 89% of the investigated rooms, CO2 levels were higher than 1000 ppm. When the window was opened, the average indoor CO2 levels in central air-conditioned bedroom were quickly lower than 1000 ppm. Carbon dioxide concentration is widely used as an indicator of ventilation effectiveness in an enclosed space (Li et al., 2001). Compared to the other indoor environments, the hotels or restaurants had higher and more variable indoor CO2 levels (Lee et al., 2002b; Li et al., 2001). The tourists occupancy and activities could lead to the high and changeable CO2 levels in the hotel

Table 2 Average radon concentrations measured in different bath times, radon concentrations and temperatures in tap hot spring water and the calculated transfer coefcients.

30 min 15 min 0 min Average 60 min 45 min 30 min 15 min 0 min

a

Rn in bedroom (Bq m3)

222

DCa/Cwb (103)
Rn in bathroom (Bq m3)
222

48 2

42 2

38 2 S3

Tap hot spring water

Rn(kBq m

Floor

Site

S1

S2

S4

1st 2nd 3rd 6th 1st 2nd 1st 2nd

83 66 156 135 201 260 84 75

10 8 11 15 19 20 14 5

45 2

T/ C

100 40 40 40 40 50 40 40

20 10 20 20 10 30 20 20

240 100 190 180 310 520 320 170

10 10 80 40 130 210 180 70

510 300 180 220 410 730 350 130

180 120 40 40 140 210 70 20

390 430 390 410 520 830 360 160

20 40 140 110 130 140 70 20

470 470 480 550 470 790 470 410

100 30 200 140 70 280 150 240

400 330 310 340 430 720 380 220

120 170 150 170 90 140 70 130

1.7e5.0 1.0e6.6 0.9e2.8 1.0e3.8 1.4e2.4 1.8e3.1 3.3e5.1 1.2e4.9

(3.7c) (4.4) (1.7) (2.2) (1.9) (2.6) (3.9) (2.4)

60 60 30 30 30 40 20 30

30 20 10 10 10 20 10 10

74 120 80 70 80 110 50 40

4 50 30 3 10 20 3 10

110 140 130 100 170 130 50 60

20 30 30 30 50 30 10 10

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G. Song et al. / Journal of Environmental Radioactivity 102 (2011) 400e406

800 bath 60min Bathroom Rad o n co n cen tratio n (Bq /m ) 600 bath 45min Enhancing vetilation when bathing with different times 400 bath bath 15min 30min 200 bath 45min bath bath 30min 15min
3

bedroom

0 11:10

17:10

23:10

5:10

Time

11:10

17:10

23:10

5:10

Fig. 3. Two days variations of radon concentrations in bathroom and bedroom with different bath times at the S2 hotel.

3.3. Concentrations of PM10 and PM2.5 Table 3 shows that the range and average indoor PM10 and PM2.5 concentrations at the selected hotel rooms, and includes the mean values of the indoor to outdoor ratio (I/O) and measured relative humidity. The average PM10 and PM2.5 levels at the selected hotel rooms ranged from 35 21 to 158 60 mg m3 and 33 24 to 143 66 mg m3, respectively. The average PM10 concentrations at S1 and S4 were higher than the values of S2 and S3, but all lower than the limit of 150 mg m3 in IAQ standard of China except for S4 hotel rooms. In the all investigated hotel rooms, 22% of them had higher PM10 concentrations than 150 mg m3. From the published data, 57% of the restaurants surveyed in Beijing had higher PM10 level than 150 mg m3 (Liu et al., 2004). The USEPA revised the primary (health-based) particulate matter standards by adding new annual and 24-h PM2.5 standards at 15 and 65 mg m3, respectively (Liu et al., 2004). The average PM2.5 concentrations in the investigated rooms were higher than the 24-h standard of 65 mg m3 except for the S3 hotel rooms. Indoor and outdoor PM2.5, were the important pollutants with relatively higher levels in S1 and S4 than in S2 and S3. It was also found that indoor levels of PM10 and PM2.5 were usually higher than the respective outdoor levels (Li et al., 2001, 2002b), except for the S3 hotel that was sited at the hillside rural area of Huizhou, where there were fewer tourists and much less vehicle trafc. The elevated indoor PM10 and PM2.5 levels were probably due to the higher outdoor levels, especially at S1 and S4. The ndings also showed that there were other sources to the indoor levels of PM10 and PM2.5. Especially the occupants activities could lead to resuspension of the airborne particles settling from the surfaces of the indoor furnishing (Miguel et al., 1995; Lee et al., 2002a), there

Fig. 4. Indoor and outdoor average concentrations of CO2 in selected hotel rooms (the dashed is the standard value line of 1000 ppm).

rooms. Since the hotel rooms were small in size, the guests occupancy on CO2 levels become more signicant. In comparison, average levels of CO2 were about two times higher indoors than outdoors. Also the hot spring water may contain naturally occurring CO2, because the hydrochemical type is HCO3eNaeK for much spring waters in Guangdong province. The highest 222Rn concentrations were measured in hot spring water and indoor air at the S3 hotel, and the indoor CO2 concentrations was also the highest at the S3 hotel of the four hotels. So 222Rn and CO2 maybe have a similar source in the hot spring water. But in this study, we think the tourists occupancy and activities are one of the main sources of indoor higher CO2 concentration. We need to measure the CO2 concentration in hot spring water in a later study.

Table 3 Range and average indoor/outdoor PM10 and PM2.5 concentrations (mg m3) at four hotel rooms, including the mean values of indoor to outdoor ratio (I/O) and measured relative humidity. Site Rooms number Indoor R.Ha.% Outdoor R.H.% Indoor PM2.5 Range S1 S2 S3 S4
a b c

Outdoor PM2.5
b

I/Oc

Indoor PM10 Range Mean S.D. 108 76 35 158 24 58 21 60

Outdoor PM10 Range 80e127 19e101 12e173 66e389 Mean S.D. 102 52 51 147 15 29 48 91

I/O

Mean S.D. 133 73 33 143 24 62 24 66

Range 77e135 16e99 5e133 64e378

Mean S.D. 108 47 42 140 22 29 40 91 1.23 1.55 0.79 1.02

8 6 6 5

66.5 56.3 59.8 64.5

4.8 4.1 8.2 5.3

62.5 68.0 67.8 56.0

2.1 5.2 12.0 6.6

107e200 14e270 10e84 79e395

59e170 16e255 14e83 84e367

1.06 1.46 0.69 1.07

Relative Humidity. Standard Deviation. Indoor/outdoor ratio.

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405

were higher indoor levels of PM10 and PM2.5 at that time of the airborne particles re-suspended. The hotel rooms had carpeted oors, including the corridors, and these were not always cleaned daily. The maximum PM10 and PM2.5 levels reached 367 and 395 mg m3, respectively. The elevated outdoor levels of PM10 and PM2.5 at S4 were probably related to the location of the spring hotel near heavy trafc roads. Except for the outdoor sources, the occupants activities and inadequate ventilation were the main factors of the elevated indoor PM10 and PM2.5 concentrations. The I/O ratios for PM10 and PM2.5 also indicated that indoor sources were the main pollutants sources. The natural generation of 222Rn is considered as the main source for the indoor 222Rn environmental level (BEIR, 1999). Its high mobility and the decay products make the inhalation of 222Rn and 222 Rn daughters (RD) to be one of the important environmental factors associated with the risk of lung cancer for the general public. Nevertheless current information about lung cancer etiology indicates that exposure to suspended particulate matter (SPM) and tobacco smoking must be taken in consideration (Espinosa et al., 2009). The hot spring hotel rooms had carpeted oors, the airborne particles settling on the surfaces of the indoor furnishing, and these were not always cleaned daily. Most of the hot spring hotels are near heavy trafc roads. These lead to higher indoor PM levels. In particular, the danger of the particles to the human body was reported to be related to the existence of PM2.5, compared with PM10 (Anderson et al., 1996; Espinosa et al., 2009). The 222Rn daughters can be adhered easily to the SPM; these radioactive carriers are dangerous due to their high mobility therefore to enter through the nasal fosses into the respiratory system till the alveolus. These particles with the RD associated are trapped in the alveoli, consequently high probability to induce damage exists and therefore cellular transformation in the respiratory tract may result. Therefore there is a correlation between the SPM diffusion and RD concentration (Espinosa et al., 2009). The results also show that some hotel rooms have both higher 222 Rn and higher PM10 and PM2.5 concentrations, e.g. at S1 and S4. It might have more signicant negative health effects to the hotel workers and the tourists. Technical or management measures (such as enhancing ventilation, cleaning the surface of indoor furnishing) should be taken to lower exposure to these air pollutants through inhalation. 3.4. The relationship of PM10 and PM2.5 The correlation analysis of indoor PM10 and PM2.5 with linear regression shows Fig. 5. The linear regression equation as below:

PM2.5/PM10 can reect the content of ne particles in PM10, the mean ratio was 0.91 (0.52e1.19) in this study. The result indicated that PM2.5 was the main particle pollutant in the hotel rooms. 4. Conclusions (1) The present study showed that hot spring water sprayed from spouts during bathing was the dominant mechanism by which 222 Rn was released into the air of the bathroom, and then the 222 Rn diffused into the bedroom. Higher indoor 222Rn concentrations were found in air-conditioned hot spring hotel rooms, especially in the bathrooms. The results showed that the indoor 222Rn was mostly inuenced by 222Rn content in hot spring water, the bathing time and the ventilation status. Also the 222Rn transfer coefcients in this study were consistent with some of the published data. (2) The indoor air quality in the four hot spring hotels was characterized. 89% of the investigated rooms had higher CO2 levels than 1000 ppm. It was probably due to the tourists activities and insufcient ventilation. (3) The 24-h average PM10 and PM2.5 levels were usually higher indoors than outdoors in this study. The highest indoor PM10 and PM2.5 levels were 367 mg m3 and 395 mg m3, respectively, and 22% of the investigated rooms had higher PM10 concentrations than 150 mg m3. The average PM2.5 concentrations in the investigated rooms were all higher than the 24-h standard of 65 mg m3. Except for the outdoor sources, the occupants activities and inadequate ventilation were the main factors of the elevated indoor PM10 and PM2.5 concentrations. The result also indicated that PM2.5 was the main particle pollutant in the hotel rooms. (4) It is recommended that hot spring hotels should regularly inspect the IAQ of the hotel rooms in order to provide and maintain a healthy and comfortable environment. The exceeded indoor 222Rn, PM and CO2 concentrations are the most signicant contaminants for human health, especially to the hotel workers. Technical or management measures (such as enhancing ventilation, keeping the surface of indoor furnishing clean) should be taken to avoid the accumulation of indoor air pollutants to higher levels in these hot spring resorts. Acknowledgments Authors would like to thank Dr. Qiusheng He, Taiyuan University of Science and Technology, for helping to measure in the eld. This work is supported by NSFC with project number 40930743, 40872201 and 40502030. References

  PM2:5 1:0372 PM10 0:007 R2 0:99

0.5
PM 2 .5 co n cen t rat i o n s (mg m )
-3

0.4 0.3 0.2 0.1 0 0

y = 1.0372x - 0.007 R = 0.9891

2

0.1 0.2 0.3 -3 PM 10 concentrations (mg m )

0.4

Fig. 5. Linear correlation relationship of PM2.5 and PM10.

Anderson, H.R., De-Leon, E.S., Bland, J.M., Bower, J.S., Strachan, D.P., 1996. Air pollution and daily mortality in London, 1987e92. J. Epidemiol. Community Health 312, 665e669. BEIR, V.I., 1999. Biological Effects of Ionizing Radiation (BEIR) VI Report: The Health Effects of Exposure to Indoor Radon. National Academy of Sciences, Washington, D.C. Chao, C.Y., Wong, K.K., 2002. Residential indoor PM10 and PM2.5 in Hong Kong and the elemental composition. Atmos. Environ. 36, 265e277. Chaudhuri, H., Das, N.K., Bhandari, R.K., Sen, P., Sinha, B., 2010. Radon activity measurements around Bakreswar thermal springs. Radiat. Meas. 45, 143e146. Ciolini, R., Mazed, D., 2010. Indoor radon concentration in geothermal areas of central Italy. J. Environ. Radioact. 101, 712e716. Clarke, R.H., Southwood, T.R.E., 1989. Risk from ionizing radiation. Nature 338, 197e198. Denman, A.R., Groves-Kirkby, N.P., Groves-Kirkby, C.J., Crockett, R.G.M., Phillips, P.S., Woolridge, A.C., 2007. Health implications of radon distribution in living rooms and bedrooms in U.K. dwellingsda case study in Northamptonshire. Environ. Int. 33, 999e1011.

406

G. Song et al. / Journal of Environmental Radioactivity 102 (2011) 400e406 Nikolopoulos, D., Vogiannis, E., 2007. Modelling radon progeny concentration variations in thermal spas. Sci. Total Environ. 373, 82e93. Nikolopoulos, D., Vogiannis, E., Petraki, E., Zisos, A., Louizi, A., 2010. Investigation of the exposure to radon and progeny in the thermal spas of Loutraki (Attica-Greece): results from measurements and modeling. Sci. Total Environ. 408, 495e504. NRC, 1999. Risk Assessment of Exposure to Radon in Drinking Water. National Academy Press, Washington DC. Ouabi, H., 2009. Modeling of radon and its short-lived decay products emanating from tap water used inside a house: dose to adult members of the public. Appl. Radiat. Isot. 67, 115e121. Papastefanou, C., 2002. An overview of instrumentantion for measuring radon in soil gas and groundwaters. J. Environ. Radioact. 63, 271e283. Perrier, F., Richon, P., 2010. Spatiotemporal variation of radon and carbon dioxide concentrations in an underground quarry: coupled processes of natural ventilation, barometric pumping and internal mixing. J. Environ. Radioact.101, 279e296. Phillips, K., Howard, D.A., Bentley, M.C., Alvan, G., 1998. Assessment of environmental tobacco smoke and respirable suspended particle exposures for nonsmokers in Hong Kong using personal monitoring. Environ. Int. 24, 851e870. Phillips, K., Howard, D.A., Bentley, M.C., Alvan, G., 1999. Assessment of environmental tobacco smoke and respirable suspended particle exposures for nonsmokers in Basel by personal monitoring. Atmos. Environ. 33, 1889e1904. Prasad, Y., Prasad, G., Choubey, V.M., Ramola, R.C., 2009. Geohydrological control on radon availability in groundwater. Radiat. Meas. 44, 122e126. Salmon, L.G., Christoforou, C.S., Cass, G.R., 1994. Air pollutants in the buddhist cave temples at the Yungang Grottoes, China. Environ. Sci. Technol. 28, 805e811. Shao, L.Y., Li, J.J., Zhao, H.Y., Yang, S.S., Li, H., Li, W.J., Jones, T., Sexton, K., BruB, K., 2007. Associations between particle physicochemical characteristics and oxidative capacity: an indoor PM10 study in Beijing, China. Atmos. Environ. 41, 5316e5326. Song, G., Zhang, B.Y., Wang, X.M., Gong, J.P., Chan, D., Bernett, J., Lee, S.C., 2005. Indoor radon levels in selected hot spring hotels in Guangdong, China. Sci. Total Environ. 339, 63e70. Soto, J., Fernandez, P.L., Quindos, L.S., Gomez-Arozamena, J., 1995. Radioactivity in Spanish spas. Sci. Total Environ. 162, 187e192. Spengler, J.D., Sexton, K., 1983. Indoor air pollution: a public health perspective. Science 221, 9e17. Tuia, D., Kanevski, M., 2008. Indoor radon distribution in Switzerland: lognormality and extreme value theory. J. Environ. Radioact. 99, 649e657. Vesterbacka, P., Pettersson, H., Hanste, U.-M., Jakobson, E., Kolstad, T., Roos, P., stergren, I., 2010. Intercomparison of Rn-222 determination from groundwater. Appl. Radiat. Isot. 68, 214e218. Vinson, D.S., Campbell, T.R., Vengosh, A., 2008. Radon transfer from groundwater used in showers to indoor air. Appl. Geochem. 23, 2676e2685. Vogiannis, E., Niaounakis, M., Halvadakis, C.P., 2004. Contribution of 222Rn-bearing water to the occupational exposure in thermal baths. Environ. Int. 30 (5), 621e629. Wang, S.X., Wei, W., Li, D., Aunan, K., Hao, J.M., 2010. Air pollutants in rural homes in Guizhou, China e concentrations, speciation, and size distribution. Atmos. Environ. 44, 4575e4581. WHO, 1999. Guidelines for Air Quality. United Nations Environment Programme. International Labour Organisation and World Health Organization, Geneva. Wilkes, C.R., Mason, A.D., Hern, S.C., 2005. Probability distributions for showering and bathing water-use behavior for various US subpopulations. Risk Anal. 25, 317e337. Xu, J., Bergin, M.H., Yu, X., Liu, G., Zhao, J., Carrico, C.M., Baumann, K., 2002. Measurement of aerosol chemical, physical and radiative properties in the Yangtze delta region of China. Atmos. Environ. 36, 161e173. Yoon, S., Chang, B.U., Kim, Y., Byun, J.I., Yun, J.Y., 2010. Indoor radon distribution of subway stations in a Korean major city. J. Environ. Radioact 101, 304e308. Yu, K.N., Guan, Z.J., Stokes, M.J., Young, E.C.M., 1994. A preliminary study on the radon concentrations in water in Hong Kong and the associated health effects. Appl. Radiat. Isot. 45, 809e810. Yu, K.N., Lau, B.M.F., Guan, Z.J., Lo, T.Y., Young, E.C.M., 2001. Bronchial Rn dose survey for residences. J. Environ. Radioact. 54 (2), 221e229. Zhao, L.R., Wang, X.M., He, Q.S., Wang, H., Sheng, G.Y., Chan, L.Y., Fu, J.M., Blake, D.R., 2004. Exposure to hazardous volatile organic compounds, PM10 and CO while walking along streets in urban Guangzhou, China. Atmos. Environ. 38, 6177e6184. Zhou, R.X., 1987. Book of Practicality Recuperates. Liaoning People Publishing Company, Shenyang (in Chinese). Zhuo, W.H., Iida, T.K., Yang, X.T., 2001. Occurrence of 222Rn, 226Ra, 228Ra and U in groundwater in Fujian province, China. J. Environ. Radioact. 53, 111e120. Zhuo, W.H., Tokonami, S., 2005. Convenient methods for evaluation of indoor thoron progeny concentrations. Int. Congress Ser. 1276, 219e220.

Espinosa, G., Golzarri, J.I., Bogard, J., Gaso, I., Ponciano, G., Mena, M., Segovia, N., 2008. Indoor radon measurements in Mexico City. Radiat. Meas. 43, S431eS434. Espinosa, G., Golzarri, J.I., Ponciano-Rodriguez, G., Gaso, M.I., Mena, M., Segovia, N., Vazquez-Lopez, C., Sajo-Bohus, L., 2009. Population vulnerability due to the exposure to radon and airborne particulate matter (PM10), in Mexico City. Radiat. Meas. 44, 1028e1031. Evans, R.D., Harley, J.H., Jacobi, W., Mclean, A.S., Mills, W.A., Stewart, C.G., 1981. Estimation of risk from environmental exposure to Radone222 and its decay products. Nature 290, 98e100. Feng, Y.L., Wen, S., Wang, X.M., Sheng, G.Y., He, Q.S., Tang, J.H., Fu, J.M., 2004. Indoor and outdoor carbonyl compounds in the hotel ballrooms in Guangzhou, China. Atmos. Environ. 38, 103e112. Feng, Y.S., Meng, W.B., Qin, C.Z., 1994. Radon concentrations measurement in hot spring sanatorium of Liaoning province. Chinese J. Radiological Med. Prot. 14 (3), 182e185 (in Chinese). Galn Lpez, M., Martn Snchez, A., 2008. Present status of 222Rn in groundwater in Extremadura. J. Environ. Radioact. 99, 1539e1543. GB/T 18883-2002, 2002. Standards of Indoor Air Quality. China (in Chinese). Gesell, T.F., Prichard, H.M., 1980. The contribution of radon in tap water to indoor radon concentrations. In: Proceedings of Natural Radiation in the Environment. NTIS, Springeld, VA, pp. 1347e1363. Hopke, P.K., Borak, T.B., Doull, J., Cleaver, J.E., Eckerman, K.F., Gundersen, L.C.S., Harley, N.H., Hess, C.T., Kinner, N.E., Kopecky, K.J., Mckone, T.E., Sexton, R.G., Simon, S.L., 2000. Health risks due to radon in drinking water. Environ. Sci. Technol. 34, 921e926. Horvth, , Bohus, L.O., Urbani, F., Marx, G., Pirth, A., Greaves, E.D., 2000. Radon concentrations in hot spring waters in northern Venezuela. J. Environ. Radioact 47, 127e133. ICRP, 1987. ICRP Publication 50: lung cancer risk from indoor exposures to radon daughters. Ann. ICRP 17 (1), 29e37. ICRP, 1993. ICRP Publication 65: Protection against Radon-222 at Home and at Work. Ann. ICRP 23 (2) Pergamon Press, Oxford. Isbell, M., Gordian, M.E., Duffy, L., 2002. Winter indoor air pollution in Alaska: identifying a myth. Environ. Pollut. 117, 69e75. Jones, N.C., Thornton, C.A., Mark, D., Harrison, R.M., 2000. Indoor/outdoor relationships of particulate matter in domestic homes with roadside, urban and rural locations. Atmos. Environ. 34, 2603e2612. Korhonen, P., Kokotti, H., Kalliokoski, P., 2000. Behaviour of radon, radon progenies and particle levels during room depressurization. Atmos. Environ. 34, 2373e2378. Koz1owska, B., Walencik, A., Dorda, J., Zipper, W., 2010. Radon in groundwater and dose estimation for inhabitants in Spas of the Sudety Mountain area. Poland. Appl. Radiat. Isot. 68, 854e857. Lee, S.C., Li, W.M., Chan, L.Y., 2001. Indoor air quality at restaurants with different styles of cooking in metropolitan Hong Kong. Sci. Total Environ. 279, 181e193. Lee, S.C., Li, W.M., Ao, C.H., 2002a. Investigation of indoor air quality at residential homes in Hong Kongecase study. Atmos. Environ. 36, 225e237. Lee, S.C., Guo, H., Li, W.M., Chan, L.Y., 2002b. Inter-comparison of air pollutant concentrations in different indoor environments in Hong Kong. Atmos. Environ. 36, 1929e1940. Lettner, H., Hubmer, R.R., Steinhusler, F., 1996. Occupational exposure to radon in treatment facilities of the radon-spa Badgastein, Austria. Environ. Int. 22 (Suppl.1), s399e407. Li, L.F., Wang, X.M., Zhao, L.R., He, Q.S., Sheng, G.Y., Fu, J.M., 2005. Variations of PM10 and PM2. 5 levels in street microenvironment in Guangzhou. Earth Environ. 33 (2), 57e60 (in Chinese). Li, W.M., Lee, S.C., Chan, L.Y., 2001. Indoor air quality of nine shopping malls in. Hong Kong. Sci. Total Environ. 273, 27e40. Liu, Y.S., Chen, R., Shen, X.X., Mao, X.L., 2004. Wintertime indoor air levels of PM10, PM2.5 and PM1 at public places and their contributions to TSP. Environ. Int. 30, 189e197. Massey, D., Masih, J., Kulshrestha, A., Habil, M., Taneja, A., 2009. Indoor/outdoor relationship of ne particles less than 2.5 mm (PM2.5) in residential homes locations in central Indian region. Build. Environ. 44, 2037e2045. Meng, W.B., Qin, C.Z., 1994. Radioactivity levels in geothermic spring water. Ind. Health Occup. Dis. 20 (6), 380e382 (in Chinese). Michielsena, N., Tymen, G., 2007. Semi-continuous measurement of the unattached radon decay products size distributions from 0.5 to 5 nm by an array of annular diffusion channels. J. Aerosol Sci. 38, 1129e1139. Miguel, A.H., NetoDe.A., F.R., Cardoso, J.N., Vasconcellos, P.D.C., Pereira, A.S., Marquez, K.S.G., 1995. Characterization of indoor air quality in the cities of Sao Paulo and Rio de Janeiro, Brazil. Environ. Sci. Technol. 29, 338e345. Nero, A.V., Schwehr, M.B., Nazaroff, R.D., Revzan, K.L., 1986. Distribution of airborne radon-222 concentrations in US homes. Science 234, 992e997.