Vol. 45 Supp.

SCIENCE IN CHINA (Series B) December 2002

Radioactive contamination of the environment as a result of

uranium production: a case study at the abandoned Lincang
uranium mine, Yunnan Province, China
XU Lechang (徐乐昌)1, 2, WANG Yanxin (王焰新)1, LÜ Junwen (吕俊文)2,
LU Xueshi (卢学实)3, LIU Yaochi (刘耀驰)2 & LIU Xiaoyang (刘晓阳)1
1. Department of Environmental Engineering, China University of Geosciences, Wuhan 430074, China;
2. Research Institute of Uranium Mining, China National Nuclear Corporation, P.O. Box 48, Hengyang 421001, China;
3. Research Center of Environmental Science and Technology, Zhuzhou Institute of Technology, Zhuzhou 412008,
China
Correspondence should be addressed to Xu Lechang (email: xu_lechang@hotmail.com)

Received June 20, 2002

Abstract The distribution of radioactive pollutants, such as 222Rn, U, Th and 226Ra in the air, sur-
face waters, soils and crops around the Lincang uranium mine, Yunnan Province, China, is studied.
The mechanical, geochemical and biogeochemical processes responsible for the transport and
fate of the radioactive elements are discussed based on the monitoring data. The pollutants con-
centrations of effluents from the mine tunnels were dependent on pH and which were con-
trolled by biochemical oxidation of sulfide in the ore/host rocks. Radon anomalies in air reached 4
km from the tailings pile depending on radon release from the site, topography and climate. 238U
and 226Ra abnormities in stream sediments and soil were 40—90 cm deep and 790—800 m away
downstream. Anomalies of radioactive contaminants of surface watercourses extended 7.5—13
km from the discharge of effluents of the site mainly depending on mechanical and chemical proc-
esses. There were about 2.86 ha rice fields and 1.59 km stream sediments contaminated. Erosion
of tailings and mining debris with little or no containment or control accelerated the contamination
processes.
Keywords: radioactive contamination, uranium production, air, surface water, soil, crop.

In recent years, environmental issues on uranium mining and milling have become increas-
ingly important. A lot of uranium production facilities have been abandoned; new facilities have
been imposed on stricter environmental requirements in many countries; and remediation actions
are being considered for many abandoned sites. Uranium production facilities produce wastes (e.g.
mill tailings) containing long-lived radionuclides. These radioactive wastes may have impacts on
living organisms including human, water, soil and air, and must therefore be collected and con-
tained in engineered containments or controlled areas. However, in the past some operators dis-
posed of these wastes with little or no control, resulting in some environmental, especially, radio-
active contamination.
Radon, uranium, 226Ra and thorium are ones of the important radioactive contaminants in
uranium production. Raised radon levels are a health hazard and can even cause lung cancer[1].
Radon in homes causes some 2500 lung cancer deaths each year in the UK. The US Environ-
 12 SCIENCE IN CHINA (Series B) Vol. 45

mental Protection Agency (EPA) has estimated that 20000 lung cancer deaths each year in the US
can be linked to radon. It is suggested that action level is 200 Bq/m3 in homes and 400 Bq/m3 (Bq,
the unit of radioactivity, 1 Bq = s−1) in the workplace in the UK. China prescribes that action level
is 200 Bq/m3 in built homes and Radon in building homes shall not exceed 100 Bq/m3 (all in av-
erage equilibrium equivalent radon concentrations)[2]. Above these levels action should be under-
taken to remediate. Uranium as a heavy metal causes kidney diseases and is — if ingested—much
more toxic than as a radionuclides[3]. The World Health Organization (WHO) has established a
Tolerable Daily Intake (TDI) for uranium of 0.6 μg/kg body weight and day. Uranium concentra-
tion of surface water is limited not to exceed 0.05 mg/L in China[4]. The average concentration of
226
Ra in land over any area of 100 m2 shall not exceed the background level by more than 0.18
Bq/g over the first 15 cm and 0.56 Bq/g over the second 15 cm of the soil below the surface in
remedial actions in US and China[4, 5]. Regulatory limit of annual average individual effective dose
over the lifetime of general public from remedied uranium mine/mill in China does not exceed
0.25 mSv/a (Sv, the unit of equivalent dose or effective equivalent dose, 1 Sv = 1 J/kg)[4].
This paper reports a case study at the Lincang abandoned uranium mine, Yunnan Province,
China, where radioactive contaminations of the environment resulted from uranium mining and
milling.

1 Site characterization

The Lincang uranium mine is a small mine/mill complex situated at about 12 km southwest
of Lincang County, Yunnan Province, China. It began production in 1970 and was closed in 1994.
During the production period the final product is (NH4)4UO2(CO3)3. The ores were mined by
conventional open pit and underground methods. The mill process adopted filtration leaching of
non-crashed ore by H2SO4 and MnO2, and extraction of settled leachate by organic phase. Lincang
uranium mine extracted ores of Nos. II, III, V, VI and VIII mining areas (fig. 1) containing pyrite.
The streams and rice fields nearby accumulated
some mill tailings and mining debris resulted
from erosion.
The mining areas and tailings are located
in the NE-SW orientated Mengtuo Basin. The
basin has two river systems, one in the north
and the other in the south. The tailings pile is at
the watershed. Overflowing waters consist of
the tailings pile and mining tunnels (II 1925 of
No. II mining area, III 1925 and III 1942 of No.
III mining area and V 1850 of No. V/VI mining
Fig. 1. Distribution of tailings pile, mining areas, and water- area). Overflowing waters from tailings pile
courses and their sample points in Lincang uranium mine. and II 1925, III 1925 and III 1942 mining tun-
 Supp. RADIOCONTAMINATION FROM URANIUM PRODUCTION 13

nels flow into the northern river system and V 1850 mining tunnel into southern.

2 Methods

2.1 Sampling
Radioactive airborne effluents from uranium production may include dust and radon gas
( Rn, the first daughter nuclide of 226Ra decay); tailings may be the continuing sources of radon
222

and radioactive dust after mining and milling operation are stopped[6]. Since the granularity of the
tailings and debris is large, 62% of tailings and 46% of debris are bigger than 0.9 mm and only
10% of tailings and 15% of debris are less than 0.2 mm[7], radioactive dust is therefore neglected
and only radon is investigated in the air in this study. Radon monitoring points in the air are set up
over the tailings pile and debris piles and outdoors of some representative resident villages in the
basin.
Soil/stream sediment samples consisted of the tailings, mining debris, stream sedi-
ments/alluvial soils and rice fields. All types of surface soils/stream sediments were sampled.
Stream sediments/alluvial soils and rice fields soils were collected from the streams and rice fields
receiving tailings/mining debris alluvium and wastewater. Stream sediments/alluvial soils down-
stream from the tailings and the soils under the base of Nos. II and III mining debris were sampled
in different depths to understand the vertical mobility of the radioactive contaminants.
Soil/sediment samples were air dried, crashed and sieved to 80 mesh (0.18 mm) before analysis.
Water samples were collected down the both river systems and in the overflowing water from
mine tunnels and the tailings pile (fig. 1). Water samples were immediately acidified in the field to
pH < 2 by adding HNO3 after pH measured. Overflowing water were sampled monthly from April
1995 to March 1996 except that the overflowing water of V mining area was sampled monthly
from April 1995 to September 1995 because of its flooding in October 1995. Water samples of the
river systems were collected once in November 1994.
Crop samples comprised rough rice of the contaminated rice fields. Prior to analysis, the
samples were air dried, charred on an electric cooker and then incinerated in a muffle. Samples
must avoid burning during the above pro-processing. Charred samples were incinerated for about
2 h at 200—300℃ and then continued at 400—500℃ until the samples turn into fluffer with
white or hoariness.

2.2 Analytical methods

Radon in the air was monitored with the balloon method developed in China. Its mechanism
is similar to the Thomas method[8]. The balloon method consists of input filter, flow meter, air
pump and balloon connected in order with pipe. Input filter is used to filter existing radon’s
daughter in air during charging air into the balloon. Charged air stays for several minutes in the
balloon and then is deflated through the output filter collected to the balloon. The radon’s daughter
activity attached on the output filter from the radon in the balloon is counted with FJ-13 α radioac-
tive detector. The balloon method has advantages of simple, rapidness and high sensitivity. The
 14 SCIENCE IN CHINA (Series B) Vol. 45

sensitivity mainly depends on the balloon’s volume. Lower limit is 1.8 Bq/m3 for 200 L balloon if
the time of charge, stay, deflation and count is 5, 5, 4 and 10 min, respectively. The method is cali-
brated before monitoring.
238
U, 226Ra and 232Th in soils/sediments were determined by γ spectrometric method with
multi-channel γ spectrometer 918MCD. The lower limit is 0.18 Bq/kg for 238U, 0.03 Bq/kg for
226
Ra and 0.01 Bq/kg for 232Th.
Uranium in water was measured by TRPO extraction-spectrophotometry technique using 721
spectrophotometer. 226Ra was determined by Ba(Ra)SO4 co-precipitation method in which the α
activity of the precipitate was measured with the silver activated zinc sulphide alpha scintillator.
Thorium in water was measured by N235 extraction-spectrophotometry technique using 721
spectrophotometer. Lower limit of U, 226Ra and Th is 1.3 μg/L, 2.0 Bq/m3 and 0.1 μg/L.
Ash samples of crops was melted into liquid and then analyzed for U, 226Ra and Th as water
analysis method mentioned above. Lower limit of U, 226Ra and Th in ash samples of crops is 0.18
mg/kg, 3.0 Bq/kg and 0.14 mg/kg.

3 Radioactive contamination

3.1 Air
Ambient radon concentration depends on topography, climate and source of radon released
from uranium production facilities, especially tailings. Annual amount of radon emanated from the
tailings pile and all the debris is 11.01 TBq/a, 84.0% of which is from the tailings at Lincang ura-
nium mine[4]. Most of the local residents are
around the south of the tailings. So radon moni-
toring points are mainly set up in villages or
towns at the south of the tailings pile. The re-
sults are given in fig. 2.
All monitored radon concentrations are
over the background (13—30 Bq/L)[7], except
Fig. 2. Radon distribution in the air around the Lincang Mengtuo at 8 km SSE, Boshang at 15 km SSE
uranium mine.
and Lincang at 12 km ENE of the tailings pile. It
is evident that the amount of radon released from land is the key factor affecting radon in air. The
radon concentrations in the air over the tailings and the Nos. II, III and V/VI mining areas are 173,
55, 47 and 64 Bq/m3, respectively (fig. 2), and corresponding radon release is 9.254, 0.167, 0.633
and 0.955 TBq/a[4], respectively. Radon concentration in the air over the No. III mining area is
lower than that over the No. II mining area due to disperse distribution of mining debris piles in
the former area. Radon obviously disperses down the basin and prevailing wind direction and
reaches 4 km south of the tailings pile.

3.2 Soils
Erosion of tailings and mining debris is intensive because of flood and the lack of contain-
 Supp. RADIOCONTAMINATION FROM URANIUM PRODUCTION 15

ments. It is investigated that rice fields of about 2.86 ha and streams sediments of 1.59 km are all
contaminated[4]. The rice fields close to the tailings pile, Nos. III and VIII mining areas are 2.51,
0.12 and 0.23 ha, respectively; and the stream sediments close to the tailings pile and No. III min-
ing areas are 0.79 and 0.80 km, respectively. 238U, 226Ra and 232Th concentrations of the tailings,
mining debris, stream sediments/alluvial soils and rice fields were measured (table 1). In order to
understand the mobility of radioactive elements in sediments/soils, the spatial distributions of
these elements were investigated (figs. 3—6).

Table 1 Average contents of radionuclides of the tailings/mining debris and contaminated rice fields and stream sedi-
ments/alluvial soils (< 30 cm depth) of Lincang uranium mine
Tailings/mining debris Rice field Sediment/soil
Parameters
tailings II III V/VI VIII tailings III VIII tailings III
238
U/Bq·g−1 4.94 1.06 1.84 2.23 1.41 0.38 1.08 0.56 0.58 1.19
226
Ra/Bq·g−1 15.0 2.22 2.71 3.71 1.90 2.58 0.94 0.74 5.01 0.89
232
Th/mBq·g−1 86.1 65.5 70.4 71.6 55.2 98.9 65.5 114 87.6 62.9

Fig. 3. 238
U concentration of sediment/alluvial soil as a Fig. 4. 226Ra concentration of sediment/alluvial soil as a
function of distance and depth downstream from the tailings. function of distance and depth downstream from the tailings.

Fig. 5. 232Th concentration of sediment/alluvial soil as a Fig. 6. Concentrations of radionuclides of the soil under the
function of distance and depth downstream from the tailings. base of Nos. II and III mining debris as a function of depth.

238
U and 226Ra are anomalous in the mining debris, sediments, soils and tailings, as compared
with the background (238U 6.84—306.5, 226Ra 7.84—421.8, 232Th 8.23—205.98 Bq/kg in soils of
Yunnan Province)[9]. The spatial distribution of 238U and 226Ra in the neighboring stream sedi-
ments and soils is evident. The anomalies are as deep as 90 cm in the stream sediment and 40 cm
deep in the soil under the base of the mining debris. The anomalies in downstream sediments be-
 16 SCIENCE IN CHINA (Series B) Vol. 45

come weaker away from the source. The only weak anomalies of the stream sediments occur at
the surface at the distance of 790 m from the tailings pile. The anomalies suggest the existence of
superimposed mechanical and chemical processes. Mechanical process in the stream sediment is
the key factor resulting in the anomalies. Geochemical process is important in the soil under the
debris. A large amount of tailings were washed and deposited into the stream since the mine was
established, especially in the early production period when primitive operation method generated
very low uranium recovery of the ores (50%—70%), resulting in intensive abnormality of ra-
dionuclides in deep stream sediments (figs. 3 and 4).

3.3 Surface water

Water is one of the principal pathways by which contamination may be dispersed into the en-
vironment from uranium mining and milling operation[10]. Contaminated water may occur as a
consequence of the dewatering of underground water and open pit, surface water runoff from, and
seepage through, the waste rock piles, tailings piles and stockpiles, and is drained from tailings
during their settling process[6, 10].
Results of investigation suggest that north and south surface watercourses are contaminated
with radioactive elements to some extent (table 2). Locations of sample points are shown in fig. 1.
Thorium in surface water is as in normal concentration as mentioned in the tailings, debris and soil;
however, anomalies of U and 226Ra occur compared with the water which does not receive waste-
water from the mine (W5, W9, W11 and W15). Radioactive anomaly reaches up to 13 km in the
north watercourse and 7.5 km in the south watercourse. The north watercourse contaminated by U
is up to 3 km away from the tailings as compared with the regulatory limits (0.05 mg/L). Distinct
abnormality happens within 0.80 km of the north watercourse. This is produced by the superim-
posed mechanical and chemical processes, i.e. dewatering of seepage from the tailings pile and
acid water leaching of the stream sediment mainly made up of tailings.
Table 2 Contents of radionuclides of surface watercourses around Lincang mine
North watercourse South watercourse
Parameters
W1 W2 W3 W4 W5 W6 W9 W10 W11 W12 W13 W14 W15 W16
Distancea)/km 0.05 0.8 2.5 3 13 19 2 7.5 14 20
U/μg·L−1 456 200 88 78 4.0 19 4.0 4.0 3.0 10 12 4.0 6.0 3.0
226
Ra/mBq·L−1 337 224 89 90 5.0 9.8 33 5.6 7.6 46 8.9 6.1 6.1 9.9
Th/μg·L−1 0.72 0.22 0.42 0.44 0.25 0.61 1.11 1.11 0.22 0.36 0.56 0.42 0.40 0.81
pH 3.65 4.35 4.65 4.90 7.10 6.90 7.00 7.20 6.40 6.90 7.20 7.60 7.40 7.50
a) Distance from the discharge of overflowing water of the tailings pile in north watercourse and V/VI mining area in
south watercourse, respectively.
In order to better understand the observed anomalies, quality of overflowing water from mine
tunnels and the tailings pile is measured (fig. 7). Contents of radioactive elements in wastewater
depend on pH and SO 24− concentration. U and Th increase with reducing pH. 226Ra concentration

decreases when SO 24− is higher under lower pH. Variations of U and Ra as functions of pH and

SO 24− are given in figs. 8—10.

 Supp. RADIOCONTAMINATION FROM URANIUM PRODUCTION 17

226
Fig. 7. Average concentrations of radioactive elements of Fig. 8. Ra concentration as the function of pH.
effluents in Lincang uranium mine.

226
Fig. 9. Ra concentration as the function of Fig. 10. U concentration as the function of pH.

Variation of 226Ra with pH and SO 24− is similar to the result that Levins et al.[11] described:
the effect of pH and leaching solution on the leachability of 226Ra from mill tailings. Leaching
solution is demineralized with added acid or hydroxide (liquid/solid ratio, 30 L/kg; contact time,
1.5 h; and temperature, 25℃). 226Ra leached increases when pH > 3 and decreases when pH < 3 as
pH decrease using H2SO4 leaching, and increases with reducing pH (pH < 11) using HCl, HNO3,
NaOH leaching solution.
Apparently, acid may dissolve the radionuclides and increase their mobility (table 2 and fig.
7). Acid generation derives from the oxidation of sulfide, especially, pyrite. Acid in the seepage
from the tailings also stems from sulphuric acid and the oxidation of sulfide by oxidant (MnO2)
added during milling. This explains why SO 24− concentration in the seepage from the tailings is
much higher.
Natural leaching of radionuclides such as uranium interlinks biogeochemical processes and
involves the following major reactions[10, 12]: the bacterial oxidation of pyrite, the chemical oxida-
tion of pyrite by ferric sulfate, the chemical oxidation and dissolution of uranium by ferric sulfate,
and the bacterial reduction of ferrous sulfate.
UO2SO4 may hydrolyze and produce UO2(OH)2 precipitate as pH is increased (typically > 4
depending on the uranium concentration in water), resulting in the reduction of uranium concen-
 18 SCIENCE IN CHINA (Series B) Vol. 45

tration in water; Radium in water may be co-precipitate with or adsorbed by CaSO4, BaSO4,
PbSO4, Fe(OH)3, and therefore reduced as SO 24− concentration (if more than a certain concentra-
tion) and/or pH are/is enhanced. So radium concentrations of effluents from No. II mining area
and tailings pile are instead less in fig. 7. Additionally, decrease of U and 226Ra in north water-
course indicates the role of the reactions mentioned above (table 2).
Effluents rates are smaller (fig. 7); however, flow rates upstream, 0.05—0.42 m3/s in the
north watercourse and 0.10—1.65 m3/s in the south watercourse[7], are also lower. So, the dilution
of effluents is not very intensive and the anomalies occur for a longer distance.

3.4 Crops
Radioactive elements of rough rice cultivated in the contaminated rice fields are investigated
to understand the transformation of radioactive elements into food chain (table 3).
Table 3 Contents of radioactive elements of fresh rough rice from contaminated rice fields around the Lincang uranium mine
Sample
Content
III mining area VIII mining area tailings pile check point
U/mg·kg−1 0.015 0.006 0.009 0.09
226
Ra/Bq·kg−1 0.48 0.31 0.47 0.30
Th/mg·kg−1 0.38 0.04 0.08 -

Results show only weak abnormalities due to the shorter growth period. The transformation
of radioactive elements is weak. The anomalies are from the alluvial tailings and mining debris
depositing on and the wastewater flowing through rice fields.
Accumulation of radioactive elements in vegetation depends on vegetation species, forms
and behaviors of radionuclides in soils and solutions, transport and precipitation conditions,
chemical compositions of waters, the contact time of vegetation with water/soil, and the ability of
biochemical cycle. Accumulation is mainly encountered in branches and roots. It is reported that
10—15 a old firtrees growing on uranium dump accumulated up to 2500 and 300 mg/kg U in
branches in areas with 800 and 90 mg/kg U, respectively[13].

3.5 Radiological impacts

Radioactive contaminants released into the environment from uranium production facilities
may result in some radiological impact on workers, the general public and the environment. Ra-
diological impacts on humans in the nuclear cycle are stated in terms of dose. Doses to the public
may be determined using a method known as pathway analysis. Atmospheric, aquatic and terres-
trial pathways are typical pathways. It was estimated that the individual effective dose of the
critical group resulting from Lichang uranium mine was 0.24 mSv/a, which is close to the regula-
tory limit. However, the potential individual effective dose was as high as 0.64 mSv/a, which ex-
ceeds the regulatory limit[4].
4 Conclusions
(i) Uranium production resulted in the radiological contamination of the environment and
radioactive anomalies in airs, soils, water and crops to the greater or less extent.
 Supp. RADIOCONTAMINATION FROM URANIUM PRODUCTION 19

dioactive anomalies in airs, soils, water and crops to the greater or less extent.
(ii) Transport and fate of radioactive elements are controlled by mechanical, geochemical and
biogeochemical processes. Rigorous weather and primitive operation accelerate these processes.
Dissolution, transportation, precipitation and assimilation of radioactive elements occur in these
processes.
(iii) Radioactive contaminants released to the environment may cause exposure to humans
through atmospheric, terrestrial and aquatic pathways by external radiation, inhalation of radon
and its daughters or airborne radioactive particles, and ingestion of contaminated water, food-
stuff/food or fish and other aquatic biota[14]. It is necessary that the remediation of abandoned ura-
nium production facilities be conducted as soon as possible to limit exposure to humans.
Acknowledgements This work was supported by the National Natural Science Foundation of China (Grant No.
49832005) and the Teaching and Research Award Program for Outstanding Young Teachers in Higher Education Institutions of
Ministry of Education, China.

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