Food and Chemical Toxicology 39 (2001) 959–962

www.elsevier.com/locate/foodchemtox

Brief Communication

Processing procedures of brick tea and their influence on

fluorine content
Cao Jin*, Zhao Yan, Liu Jianwei
Tea and Health Laboratory, Hunan Medical University, Changsha 410078, Hunan, People’s Republic of China

Accepted 30 March 2001

Abstract
China is the only country that produces brick tea, and more than 90% of the brick tea is consumed in the western minority
nationality regions of China. The high fluorine content of brick tea is possibly associated with the special processing procedures, but
no investigation has been conducted in this field. To explore the characteristic features of brick tea manufacturing and the altera-
tions in fluorine content during the processing procedures, we performed a field survey involving two brick tea factories and the
nearby tea plantations. For the fluorine contents of the initial, intermediate and final processing products, altogether eight types of
specimens were collected and determined by using the ion-selective electrode standard curve technique. It was found that the raw
material tea leaf for brick tea processing was old, coarse and not the tender delicate tea leaf used for ordinary green or black tea
processing. For the fluorine content of the raw material tea leaf, the intermediate and the final products showed that the fresh raw
leaf contained a fluorine content as high as 489.31–512.68 mg/kg. During one fermentation-like processing procedure, the fluorine
content rose by 4.67% and 1.88% in the specimens from the two factories, respectively, which revealed no statistical significance
(P>0.5). These results suggest that the high fluorine content in brick tea might be due to the high content in the raw material and
not related with the processing procedures. # 2001 Elsevier Science Ltd. All rights reserved.
Keywords: Tea; Fluorine

1. Introduction ceae family, Camellia genus, which originated in China

China is the only country that produces brick tea.
Except for a relatively minor population in the Republic
of Mongolia, Republic of Kazakhstan and some other
mid-Asian countries, more than 90% of the brick tea
commodities are consumed in the western minority
nationality regions of China. We had reported (Cao et
al., 1996a, 1997) that the fluorosis found in children of
the Chinese Zang (Tibetan), Mongol, Kasak and Yugu
nationalities resulted from long-term consumption of
large quantities of brick tea in the form of milk tea. It
was reported (Cao et al., 1996b) that the fluorine con-
tent of Chinese brick tea was in the range of 352.2–576.4
mg/kg and even as high as 1175.0 mg/kg in some
regions, while in contrast the fluorine content of con-
ventional Chinese green and black teas were between
2.10 and 123.40 mg/kg (Cao, 1994). The tea tree
(Camellia sinensis L., O. Kuntze) belongs to the Thea-
* Corresponding author. Tel.: +86-731-449-8102; fax: +86-731-
449-8102.
E-mail address: caojin@public.cs.hn.cn (C. Jin).
0278-6915/01/$ - see front matter # 2001 Elsevier Science Ltd. All rights reserved.
PII: S0278-6915(01)00039-4
and distributed around the world 1000 years ago along
with the use of its leaves as a beverage. The tea tree has
been introduced into 57 countries, and some 150 more
countries now consume tea; however, only the minority
nationalities in the western and northern China border
regions consume this high-fluoride content brick tea.
The major brick tea producing factories are located in
Hunan Province, and some in Sichuan, Hubei and
Yunnan. One of the biological characteristics of the tea
tree is that it selectively absorbs fluorine from the earth,
and accumulates it progressively within the leaves. It
was reported (Wei, 1995; Okada and Furuya, 1996) that
the branches which contribute 20% to the brick tea
contain 26.11–134.83 mg/kg fluorine, while the principal
raw material, the rough and old leaves harvested during
July, August and September, contain 431.30–822.47 mg/
kg fluorine. Apparently the tea-leaf fluorine content is
increased as the age of the leaf increases. The brick tea is
processed from the older, coarse and rough leaves.
However, it was also suspected (Wei, 1995) that the high
fluorine content in the brick tea might be associated
with the manufacturing process procedures. Despite
960 C. Jin et al. / Food and Chemical Toxicology 39 (2001) 959–962
recent interest from the medical profession, agriculture
and industry, there have been no studies reported in the
literature. We therefore conducted the present study in
order to clarify whether the high fluorine content of
brick tea is associated with the processing procedure,
since Hunan is the major manufacturing province for
the vast majority of the brick tea commodities.
2. Materials and methods
Factories A and B are the two largest brick tea man-
ufacturing factories in Hunan province. These two fac-
tories and the nearby tea plantations were surveyed.
2.1. Raw materials
The fresh old, coarse rough fresh tea leaves, were
collected. The eight processing procedures that might
affect the physical–chemical properties of the brick tea,
their initial, intermediate and final product samples
were collected from the two factories, respectively.
Sampling of the initial and intermediate products was
performed by a repetitive cross-division into four por-
tions, taking the two contrast parts and discarding the
other two parts until the sampling quantities were
reached. The brick tea products sampling method con-
forms to the PRC National Standard GB8303-87 (Chi-
nese National Standard, 1988), and the preparation of
ground tea sampling and dry constituent content estima-
tion method. Five samples were taken from the surface of
each brick by an electric drill. Five parallel samples were
collected in each processing procedure for estimation.
The samples were dried in an incubator at 50 C for 6 h,
ground, and passed through a 40-mesh sieve.
2.2. Method of preparation
A 2000-mg sample was weighed on a Sartorius elec-
tronic balance (Sartorius, Germany; sensitivity 0.001 g),
and added to 200 ml deionized water, boiled for 15 min,
filtered after cooling to room temperature, thus obtain-
ing the filtrate I. The procedure was repeated four times
and subsequent filtrates II, III and IV were obtained,
respectively. An ion-selective electrode (ORION model
818, USA) measured the fluorine content in the four
filtrates separately with the standard curve method. The
total water-soluble fluorine content of the object sample
was the average of the four measurements.
2.3. Quality control measures in the determination of
fluorine content
The National Standard Material Center provided the
tea standard reference. The determination of fluorine
content of the tea standard was repeated six times, and
the mean value and the coefficient of variation were
obtained. The analytical devices were checked under
normal conditions, and standard material was deter-
mined using the same methods and procedures as used
in the determination of the samples. The results were
compared with the standard material.
3. Results
3.1. Characteristic features of the collection of raw
material for processing of brick tea
It was revealed from the two tea plantations that the
raw material for high quality tea in the Hunan tea-pro-
ducing areas is collected before 20 April, most being the
new buds and the small delicate leaves picked by hand.
After 20 April through 10 May, both machine and hand
collection is employed, and the collected raw materials
consisted of buds and larger but still delicate leaves.
These raw materials are used for the production of the
green and black (red) tea, respectively. However, the
raw material for brick tea production is collected during
the period through July, August and September, which
is late summer in Hunan Province. Collection is per-
formed by machine, and the tea leaves are course and
rough old leaves and branches, not the tender delicate
leaves collected during the spring.
3.2. Processing procedures for brick tea
The brick tea raw material is first processed like green
tea, and then processed by fermentation to a brick-form
intermediate which is called ‘‘black tea’’ in Hunan. This
processing procedure is the so-called ‘‘after-fermenta-
tion’’ technique. The fresh raw leaves and branches are
heated in an iron pot, 80–90 cm in diameter, after the
addition of about 10% water, and stir-fried con-
tinuously with a shovel or mechanically, which is the so-
called ‘‘ShaQing’’, namely the ‘‘deactivation of
enzymes’’ process. The stir-fried hot leaves are then
‘‘rubbed’’ to break the cell walls and to squeeze out the
juice from the tea leaves, which adheres to the surface of
the leaves. The rubbed tea leaf branches are then piled
into 1 m70 cm70 cm piles, and covered with wet
cloths to maintain a temperature of about 25 C and
relative humidity of 85%. During the summer, these
conditions are maintained for 8–12 h or more. This is a
unique fermentation procedure in the processing of
black tea that induces complex chemical reactions,
resulting in the specific color, smell and taste of the
black tea and its final product, brick tea. This is the so-
called ‘‘OuDui’’, namely the ‘‘piling fermentation’’ pro-
cedure. After that, the material is rubbed further and
dried to cure, and the intermediate of brick tea, the
black tea, is obtained.
 C. Jin et al. / Food and Chemical Toxicology 39 (2001) 959–962 961

Table 1 with the fresh leaves the increments were 4.01 and
Alteration in fluorine content during the processing of black tea (mg/kg) 1.76%, respectively. Concerning the rolling processing
n Factory A (xs) n Factory B (x s) procedure, it was found (Wang et al., 1984) that this
procedure, on heating, breaks down the cell walls and
Fresh leaves 5 489.31123.12 5 512.68178.22 decomposes the gelatinous substances, and enhances the
Deactivation of enzymes 5 491.36195.68 5 512.84211.57
Rolling 5 502.31135.54 5 515.22175.33
solubility of the ingredients and also the fluorine ions.
Pile fermentation 5 512.1699.75 5 522.33128.96 There was no generally accepted conclusion concerning
Drying 5 511.54202.35 5 521.97175.36 the actual chemical reactions related to the pile fermen-
tation procedure. It was suspected that there were
enzymic, microbial and wet-heat effects; however, the
Table 2 wet-heat effect was predominant. The increase of fluor-
Alteration in fluorine contents during the modeling of brick tea (mg/kg)
ine content might be because this specific fermentation
n Factory A (x s) n Factory B (x s) modality enhanced the solubility of fluoride within the
Steaming 5 511.32185.86 5 523.12179.23
tea leaves.
Compression 5 510.41179.44 5 522.5498.62 However, statistical analysis showed that the altera-
Drying 5 508.91165.22 5 521.68201.23 tion of fluorine content during the different processing
procedures for brick tea manufacture was non-sig-
nificant. It is evident that the high fluorine content of
At the brick tea factory the purchased black tea is the brick tea is not caused by these processing proce-
placed into a huge sealed container and steam-heated at dures but due to the original high content in the raw
98–102 C for 50 s. The black tea is then wet and soft, material fresh leaves and branches. Taking an adult
and is again piled into 2–3-m3 piles. Three to four h consuming 10 g brick tea per day, the fluorine intake
later, the temperature is gradually reduced to about was 4.89 mg, or 5.13 mg as the fresh tea leaves, and 5.09
80 C, and the height of the piles reduced. The processed or 5.22 mg as the final commodity brick tea from these
black tea is again inflated with steam for 5–6 s and then two factories, respectively.
compressed in a modeling machine under 80 tons of Fluorine appears to be an non-essential nutrient.
pressure into the brick form, and dried thereafter at 26– Intake of excess fluoride causes a harmless mottling of
28 C for 20–22 days to become the final brick tea. the teeth, called fluorosis, and bone pathology. Fur-
thermore, our animal model of brick tea-type fluorosis
3.3. Alteration in fluorine content during the processing demonstrated renal pathology exhibited as inhibited
procedure fluoride excretion and appearance of urinary b-micro-
globulin (Cao et al., 1998).
The semi-final product black tea is produced through The Recommended Dietary Allowance (RDA, 1989;
five steps: the fresh leaves; the deactivation of enzymes Cao et al, 1996a,b, 1997) for fluoride intake for an adult
process; the rolling process; the pile fermentation pro- was suggested as 1.5–4.0 mg, with the upper limit for an
cess; and the drying process. The fluorine content chan- adolescent as 2.5 mg. Our previous survey revealed that
ges in the samples from the two factories are listed in for foodstuffs of the Chinese western minorities, apart
Table 1. from Zamba and milk tea, which are both prepared
After a short period of steaming, the black tea with brick tea water and are high in fluoride, the milk,
becomes wet and soft, which facilitates the model com- flavoured, and others have a low fluoride content. Fur-
pressing procedure. After a further 20 days of drying, thermore, the water sources of Tibet, Qinghai, Gansu
with simple packaging, the commodity is then finally and Sichuan also have a low fluoride content. Our epi-
transported to the Chinese minority nationality regions. demiological survey in these regions indicated that con-
The alterations in fluorine content of the samples from sumption of milk and Zamba teas with added brick tea
the two factories are listed in Table 2. water increased the daily fluorine intake markedly in
excess of the RDA, resulting in endemic fluorosis (Cao
et al., 1996a, 1997, 2000).
4. Discussion Statistical data indicate that the increase in fluoride
content of brick tea after processing compared with that
It is apparent that the fluorine content in the brick tea of the fresh raw material showed no significant differ-
from the two factories showed an increasing trend, ence. The high fluoride of brick tea is not due to the
although the trend is weak and is mainly during the processing procedure. Assuming that an adult consumes
rolling and piling procedures. As compared to the raw 10 g brick tea daily, the fluoride content in the fresh leaf
material fresh tea leaves, the fluorine content from the is 4.89 or 5.13 mg, while in the brick tea it is 5.09 or 5.22
two factories increased 4.67 and 1.88%, respectively, mg, respectively, which is the reason that the Chinese
whereas in the final product brick tea in comparison western minorities suffer from fluorosis.
962 C. Jin et al. / Food and Chemical Toxicology 39 (2001) 959–962
Characteristics in the collecting season of the raw
materials for producing the green, black and brick tea
suggest that this should be shifted to an earlier date, so
that by collecting the more delicate leaves it would be
possible to decrease the fluorine content in brick tea.
Furthermore, use of natural, non-toxic adsorptive
reagents can adsorb a large part of the fluoride in the
tea water and reduce it to a safe level. We researched
such adsorptive additives and produced a low-fluoride
brick tea. Animal experiments demonstrated that this
low-fluoride brick tea did not produce tooth fluorosis in
rats, and population trials are ongoing to confirm whe-
ther it would indeed prevent the occurrence of fluorosis
(Cao et al., 2001) if used instead of ordinary brick tea.
References
Cao, J. 1994. The general review of the research and the development
of the fluoride of tea. In: Proceedings of the XXth Conference of the
International Society for Fluoride Research, China. Beijing: Minis-
try of Health of People’s Republic of China, Beijing, p. 225.
Cao, J., Bai, X.X., Zhao, Y., Liu, J.W., 1996a. The relationship of
fluorosis and brick tea drinking in Chinese Tibetans. Environmental
Health Perspectives 104, 1340–1343.
Cao, J., Bai, X.X., Zhao, Y., Liu, J.W., 1996b. Fluorosis induced by
drinking brick tea. Fluoride 3, 139–143.
Cao, J., Zhao, Y., Liu, J.W., 1997. Brick tea consumption as the cause
of dental fluorosis among children from Mongol, Kazak and Yugo
populations in China. Food and Chemical Toxicology 35, 827–833.
Cao, J., Zhao, Y., Liu, J.W., 1998. Animal model of brick tea type
fluorosis. Journal of Chinese Endemic Disease 23, 257–260.
Cao, J., Zhao, Y., Liu, J.W., et al., 2000. Environment fluoride con-
tent in Tibet. Environmental Research 83, 333–337.
Cao, J., Zhao, Y., Liu, J.W., 3001. Prevention of brick tea fluorosis in
rats with low-fluoride brick tea on laboratory observation. Food
and Chemical Toxicology 39, 615–619.
Chinese National Standard, 1988. GB 8303-87. Tea-preparation of
ground sample and determination of matter content. Tea-test
methods of physical-chemical properties.
RDA, 1989. Recommended Dietary Allowance, 10th Edition.
National Academy Press, Washington, DC.
Wang, J.Q., Guo, J.T., Li, S.L., et al., 1984. Study on the urinary
fluoride excreted law and influence factors for healthy adults. Bul-
letin of the Sichuang Medical Academy 15, 44–48.
Wei, Z.D. (Ed.), 1995. Selected Papers of Chinese Fluorine Research.
Guizhou Science Technic Press, Guiyang. 325–330.