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DSpace at VNU: Genetic polymorphisms in glutathione S-transferase (GST) superfamily and arsenic metabolism in residents of the Red River Delta, Vietnam

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DSpace at VNU: Genetic polymorphisms in glutathione S-transferase (GST) superfamily and arsenic metabolism in residents...

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Genetic polymorphisms in glutathione S-transferase (GST) superfamily and arsenic metabolism in residents of the Red River Delta, Vietnam

Tetsuro Agusaa,b, Hisato Iwatab,⁎ , Junko Fujiharaa, Takashi Kunitoc, Haruo Takeshitaa, Tu Binh Minhd,

a

Department of Legal Medicine, Shimane University Faculty of Medicine, Enya 89-1, Izumo 693-8501, Japan

b

Center for Marine Environmental Studies (CMES), Ehime University, Bunkyo-cho 2-5, Matsuyama 790-8577, Japan

c

Department of Environmental Sciences, Faculty of Science, Shinshu University, 3-1-1 Asahi, Matsumoto 390-8621, Japan

d

Center for Environmental Technology and Sustainable Development (CETASD), Hanoi University of Science, Vietnam National University, T3 Building, 334 Nguyen Trai Street, Thanh Xuan District, Hanoi, Vietnam

a b s t r a c t

a r t i c l e i n f o

Article history:

Received 14 September 2009

Revised 29 October 2009

Accepted 6 November 2009

Available online 13 November 2009

Keywords:

Arsenic

Glutathione S-transferase ω1 (GSTO1)

GST ω2 (GSTO2)

GST π1 (GSTP1)

GST μ1 (GSTM1)

GST θ1 (GSTT1)

Genetic polymorphism

Vietnam

To elucidate the role of genetic factors in arsenic metabolism, we investigated associations of genetic polymorphisms in the members of glutathione S-transferase (GST) superfamily with the arsenic concentrations in hair and urine, and urinary arsenic profile in residents in the Red River Delta, Vietnam Genotyping was conducted for GST ω1 (GSTO1) Ala140Asp, Glu155del, Glu208Lys, Thr217Asn, and Ala236Val, GSTω2 (GSTO2) Asn142Asp, GST π1 (GSTP1) Ile105Val, GST μ1 (GSTM1) wild/null, and GST θ1 (GSTT1) wild/null There were no mutation alleles for GSTO1 Glu208Lys, Thr217Asn, and Ala236Val in this population GSTO1 Glu155del hetero type showed higher urinary concentration of AsVthan the wild homo type Higher percentage of DMAVin urine of GSTM1 wild type was observed compared with that of the null type Strong correlations between GSTP1 Ile105Val and arsenic exposure level and profile were observed in this study Especially, heterozygote of GSTP1 Ile105Val had a higher metabolic capacity from inorganic arsenic to monomethyl arsenic, while the opposite trend was observed for ability of metabolism from AsVto

AsIII Furthermore, other factors including sex, age, body mass index, arsenic level in drinking water, and genotypes of As (+ 3 oxidation state) methyltransferase (AS3MT) were also significantly co-associated with arsenic level and profile in the Vietnamese To our knowledge, this is the first study indicating the associations of genetic factors of GST superfamily with arsenic metabolism in a Vietnamese population

© 2009 Elsevier Inc All rights reserved

Introduction

Inorganic arsenic (IA) is known to be a carcinogenic chemical in

human Arsenic contamination in groundwater is one of the most serious

where several areas do not have a public water supply system as yet

Since 2001, our research group has investigated arsenic pollution in the

groundwater and residents from Vietnam and Cambodia (Agusa et al.,

1930μg/l) in the groundwater exceeding 10 μg/l of WHO water standard

exposed to high levels of arsenic through the water consumption

In human, IA ingested through the drinking water and food is

metabolized to dimethyl arsenic Two pathways are hypothesized to

account for the metabolism of IA: a classical scheme consists of a

series of reductions and oxidations coupled with methylations

concept, the reductive methylation by interaction with binding proteins (Hayakawa et al., 2005; Naranmandura et al., 2006) In the biotransformation process, two enzymes, arsenic (+ 3 oxidation

(GSTO), are required in a variety of animals including human

detoxify xenobiotics by catalyzing the conjugation with reduced glutathione GST superfamily includes seven classes,α, μ, ω, π, θ, σ,

GST superfamily (Board et al., 2000) Among GSTO isoforms, GSTO1 is involved in the reduction activities of arsenate (AsV), monomethy-larsonic acid (MMAV), and dimethylarsinic acid (DMAV) (Zakharyan

reduction of MMAVand DMAV, but its activity of DMAVreductase was remarkably lower than that of GSTO1 (Schmuck et al., 2005)

It is anticipated that there is a large variation in susceptibility to toxic effect by IA among individuals and ethnics, depending on the difference

in IA metabolism (Vahter, 2000) Polymorphism(s) in the genes that are responsible for the metabolism of arsenic compounds may contribute to

⁎ Corresponding author Fax: +81 89 927 8172.

E-mail address: iwatah@agr.ehime-u.ac.jp (H Iwata).

0041-008X/$ – see front matter © 2009 Elsevier Inc All rights reserved.

Toxicology and Applied Pharmacology

j o u r n a l h o m e p a g e : w w w e l s e v i e r c o m / l o c a t e / y t a a p

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the variability in biotransformation of IA (Loffredo et al., 2003; Vahter,

genotypes and haplotypes in AS3MT, which catalyzes the methylation of

arsenite (AsIII) and monomethylarsonous acid (MMAIII) (Lin et al., 2002;

urinary arsenical profile in a Vietnamese population (Agusa et al., 2008,

polymorphisms in GSTO1 and O2 to arsenic metabolism by in vitro

assays (Tanaka-Kagawa et al., 2003; Whitbread et al., 2003; Schmuck et

with biotransformation of arsenic (Chiou et al., 1997; Kile et al., 2005;

Marcos et al., 2006; Zhong et al., 2006; Lin et al., 2007; McCarty et al.,

distribution of gene polymorphisms in GSTs and their relation to the

arsenic metabolism in Vietnamese In the present study, we investigated

whether genetic polymorphisms in the members of GST superfamily,

GSTO1, GSTO2, GSTM1, GSTP1, and GSTT1, can affect arsenic metabolism

in residents from the Red River Delta, Vietnam The co-influence of

genetic polymorphisms in GSTs and other factors (sex, age, body mass

index (BMI), arsenic level in drinking water, and AS3MT genotypes) on

the accumulation and metabolism of arsenic was also examined

Materials and methods

previous work (Agusa et al., 2009b) Well water (n = 28), human hair

(n = 99), urine (n = 100), and blood (n = 100) samples were

randomly collected in March 2006 from Hoa Hau (HH) and Liem

Thuan (LT) in Ha Nam Province, which is located in the Red River Delta, Vietnam The informed consent was obtained from all the participants, and also this study was approved by the Ethical Committee of Ehime University, Japan Data on concentrations of total arsenic in water and human hair, and arsenic compounds in urine (Agusa et al., 2009b), and cumulative arsenic exposure level are

estimated from the As level in groundwater (mg/L), year of tube-well usage (year), annual ingestion rate of groundwater (182.5 days/year), and daily water consumption (3 L/day) All samples were kept at−25

°C in a freezer of the Environmental Specimen Bank (es-BANK) in Ehime University (Tanabe, 2006) until the following analyses

Analyses of arsenic The analytical method of arsenic was described

in more detail elsewhere (Agusa et al., 2009b) Total arsenic (TA) in water and human hair samples was analyzed with an inductively coupled plasma-mass spectrometer (ICP-MS; HP-4500, Hewlett-Packard, Avondale, PA, USA) using internal calibration method

AsIII, and AsVin urine sample were measured with a high performance liquid chromatograph (HPLC; LC10A Series, Shimadzu, Kyoto, Japan)— ICP-MS To separate each arsenical, a polymer-based anion exchange column (Shodex Asahipak ES-502N 7C) was used with 15 mM citric acid (pH 2.0 with nitric acid) (Agusa et al., 2009b)

In the present study, sum of all arsenic compounds and inorganic arsenic (AsIII+ AsV) detected in urine sample are denoted as SA and

IA, respectively Percentages of AB, AsIII, AsV, MMAV, DMAVand IA to

SA in human urine were denoted as %AB, %AsIII, %AsV, %MMAV, %DMAV and %IA, respectively Urinary creatinine was determined at SRL, Inc (Tokyo, Japan) Concentrations of arsenic compounds in urine were expressed asμg As/g on a creatinine basis Because it is considered

Table 1

Information on water and human samples from Hoa Hau and Liem Thuan in Vietnam.

Groundwater

Used period (years) a

TA (μg/l) b 368 (163–502, and 2120 (an outlier)) 1.4 (0.7–6.8) b0.001 c Filtered water

Drinking water e

Subjects

Residential time (years) a

Cumulative arsenic exposure (mg) b 306 (17.6–12800) 4.8 (1.7–13.4) b0.001 c Hair TA (μg/g) b

0.351 (0.028–2.94) 0.232 (0.068–0.690) b0.001 c Urinary SA (μg/g creatinine) b 92.6 (45.2–365) 97.9 (38.6–397) N0.05 c

Urinary DMA V

Urinary MMA V

Urinary As V

(%) a

Abbreviations: TA, total arsenic; BMI, body mass index (weight (kg)/height (m) 2

); SA, sum of arsenic compounds; AB, arsenobetaine; DMA V

, dimethylarsinic acid; MMA V

, monomethylarsonic acid; As III

, arsenite; As V

, arsenate.

a Arithmetic mean and range.

b Geometric mean and range.

c

t-test.

d

χ 2

test.

e filter, filtered water instead of raw groundwater is assumed to be consumed.

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Table 2

Information on primer sequences, annealing temperatures, restriction enzymes, and fragment sizes of the amplified products and frequencies of allele and genotype of GST superfamily in residents from Hoa Hau and Liem Thuan in Vietnam Gene

symbol

Amino acid

position

rs number a Functional

context

Nucleotide change

Amino acid change

(°C) Restriction enzyme

frequency (%)

Genotype frequency (%)

5′-TGATAGCTAGGAGAAATAATTAC-3′

Ala/Asp: 68, 186, 254 Asp/Asp: 254

Ala: 0.900 Asp: 0.100

Ala/Ala: 0.810 Ala/Asp: 0.180 Asp/Asp: 0.010

5′-GAATTTACCAAGCTAGAGGAGGT-3′

5′-GACCAAGCCAGCATTTTAGG-3′

5′-GCAGGACAGCTTTCTGCTTT-3′

Glu/del: 200, 315, 472 del/del: 315, 472

Glu: 0.955 del: 0.045

Glu/Glu: 0.910 Glu/del: 0.090

5′-CAAAGCGCTTGGCTGTTGATGTC-3′

Glu/Lys: 154, 266, 420 Lys/Lys: 420

Glu: 1.000 Lys: 0

Glu/Glu: 1.000 Glu/Lys: 0 Lys/Lys: 0

5′-CAAAGCGCTTGGCTGTTGATGTC-3′

Thr/Asn: 114, 221, 335 Asn/Asn: 114, 221

Thr: 1.000 Asn: 0

Thr/Thr: 1.000 Thr/Asn: 0 Asn/Asn: 0

5′-CATGCAACCTGAACCTTGGT-3′

Ala/Asp: 116, 192, 308 Asp/Asp: 308

Ala: 1.000 Asp: 0

Ala/Ala: 1.000 Ala/Asp: 0 Asp/Asp: 0

5′-GAGGGACCCCTTTTTGTACC-3′

Asn/Asp: 63, 122, 185 Asp/Asp: 63, 122

Asn: 0.780 Asp: 0.220

Asn/Asn: 0.610 Asn/Asp: 0.340 Asp/Asp: 0.050

5′-TGAGGGCACAAGAAGCCCCT-3′

Ile/Val: 84, 92, 176 Val/Val: 84, 92

Ile: 0.845 Val: 0.155

Ile/Ile: 0.690 Ile/Val: 0.310 Val/Val: 0

5′-GTTGGGCTCAAATATACGGTGG-3′

multiplex PCR

Wild: 210 Null: 0

Wild: 0.580 Null: 0.420

5′-TCACCGGATCATGGCCAGCA-3′

multiplex PCR

Wild: 473 Null: 0

Wild: 0.700 Null: 0.300

a

Rs numbers were cited from NCBI SNP Database (http://www.ncbi.nlm.nih.gov/projects/SNP/).

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that AsV, IA, and MMAVare metabolized to AsIII, MMA, and DMA,

respectively, in the human body, concentration ratios of AsIII/AsV(III/

used as metabolic index for each arsenical

Genotyping of polymorphisms in GSTO1, GSTO2, GSTP1, GSTM1, and

using a QIAamp DNA mini kit (Qiagen, Chatworth, CA) Reference

sequence of each GST was based on the DNA Data Bank of Japan (DDBJ);

accession numbers of GSTO1, GSTO2, GSTP1, GSTM1, and GSTT1 are

AY817669, AY191318, AY324387, BC024005, and AB057594,

respec-tively DNA was subjected to PCR amplification in 10 μl reaction mixture

containing GoTaq®Green Master Mix (Promega, Madison, WI, USA) and

individual primer pairs corresponding to each mutation of GSTO1

Thr217Asn (threonine to asparagine substitution at amino acid base

217), GSTO1 Ala236Val, GSTP1 Ile105Val, GSTM1 wild/null, and GSTT1

wild/null For the detection of GSTO1 Glu155del and Glu208Lys, the

(15 mM Tris–HCl, 50 mM KCl, pH 8.0), 1.5 mM MgCl2, 0.5μM of each

Applied Biosystems, CA, USA) (Fujihara et al., 2007) A PCR mixture

consisting of PCR buffer, 1.5 mM MgCl2, 0.4μM of each primer, 250 μM

dNTP, and 1 U Takara EX Taq DNA polymerase (Takara, Kyoto, Japan)

was used for genotyping of GSTO1 Ala140Asp and GSTO2 Asn142Asp

Glu208Lys, Thr217Asn, and Ala236Val, GSTO2 Asn142Asp, and GSTP1

Ile105Val were detected by PCR restriction fragment length

polymor-phism (PCR-RFLP) using restriction enzymes Genetic polymorpolymor-phisms in

GSTT1 and M1 (wild or null) were identified by allele specific multiplex

PCR includingβ-globin as a positive control (Sreeja et al., 2005) GSTO1

Glu155del was detected by applying the method of confronting

two-pair primers analysis (CTPP) (Fujihara et al., 2007) The PCR products, which were treated with restriction enzyme or were not treated, were separated in 8% polyacrylamide gel by electrophoresis (300 V, 15 min) and were detected by silver staining The genotyping was carried out in duplicate The representativeness of nucleotide sequences for each

Biosystems Foster, CA, USA) Information on primers, annealing temper-ature, restricted enzyme, and fragment size is presented inTable 2

(ver-sion 5.0, SAS® Institute, Cary, NC, USA), SPSS (ver(ver-sion 12, SPSS, Chicago, IL, USA), and EXCEL Toukei (Version 6.05, Esumi Co., Ltd., Tokyo, Japan) were used for statistical analyses One half of the value

of the respective limits of detection were substituted for those values below the limit of detection and used in statistical analysis Normality

Smirnov's one sample test To adapt parametric analyses, data which showed non-normal distribution was log-transformed Stud-ent's t-test and Tukey–Kramer test were conducted to find differences

in arsenic levels and compositions in the hair and urine among allele

checking sample size distribution in each group category To assess the factors affecting arsenic levels and composition in the urine and hair, and metabolic capacity of arsenic, a stepwise multiple regression analysis was executed Genetic polymorphisms in GST superfamily and cumulative As exposure level as well as SNPs in AS3MT, age, sex,

relationships with arsenic levels and compositions in our previous

analysis as independent variables To apply the regression model, nominal variables (sex and genotypes of GST superfamily and AS3MT)

Fig 1 Frequencies of genotypes of GST superfamily in the Vietnamese and the HapMap populations ( http://www.hapmap.org/index.html.ja ) NA means no available data VN: Vietnamese in this study, CHB (H): Han Chinese in Beijing, China, CHD (D): Chinese in Metropolitan Denver, Colorado, JPT (J): Japanese in Tokyo, Japan, GIH (G): Gujarati Indians in Houston, Texas, MEX (M): Mexican ancestry in Los Angeles, California, CEU (C): Utah residents with Northern and Western European ancestry from the CEPH collection, TSI (T):

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Table 3

Concentrations (geometric mean and range) of arsenic compounds in urine and total arsenic in hair for each genotype of GST superfamily in residents from Hoa Hau and Liem Thuan in Vietnam.

Gene and

genotype

MMA V

As III

As V

GSTO1 Ala140Asp

Ala/Asp +

Asp/Asp

GSTO1 Glu155del

GSTO2 Asn142Asp

Asn/Asp +

Asp/Asp

GSTP1 Ile105Val

GSTM1

GSTT1

Abbreviations: AB, arsenobetaine; DMA V , dimethylarsinic acid; MMA V , monomethylarsonic acid; As III , arsenite; As V , arsenate; IA, inorganic arsenic (As III + As V ); SA, sum of arsenic compounds; TA, total arsenic; NA, not available.

⁎ pb0.05.

⁎⁎⁎ pb0.001.

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were transformed to dummy variables The multicollinearity of independent variables was assessed by calculating the variance

inflation factor (VIF) Linkage disequilibrium and haplotype of SNPs

in GSTO1 were assessed by Haploview (version 4.0, Day Lab at the

indicate statistical significance

Results and discussion Distribution of genetic polymorphisms in GST superfamily Allele and genotype frequencies for each gene are shown in

Thr217Asn, and Ala236Val in this population and thus the data on these mutations were not included for further analysis No mutation homozygotes were found for GSTO1 Glu155del and GSTP1 Ile105Val

significant linkage disequilibrium and haplotype

Genotype frequencies for GST superfamily in this Vietnamese and

GSTO1 Ala140Asp, GSTO1 Glu208Lys, GSTO2 Asn142Asp, and GSTP1 Ile105Val genotypes in the Vietnamese population were similar to those in Asian populations such as CHB (H) (Han Chinese in Beijing, China groups), CHD (D) (Chinese in Metropolitan Denver, Colorado), and JPT (J) (Japanese in Tokyo, Japan) However, even among the Asian populations, frequencies of I/I and I/V genotypes for GSTP1 Ile105Val in the Vietnamese and Chinese (CHB (H) and CHD (D)) were largely different from those in the Japanese (JPT (J)) In addition, although mutant homo types of GSTO1 Glu208Lys and GSTP1 Ile105Val were reported in other populations, no such substitution was detected in the Vietnamese There was no mutation in GSTO1 Ala236Val in the Vietnamese Similarly, low mutation frequencies were reported in other populations except for the Mexican Genotype frequencies of GSTO1 Ala140Asp, Glu155del, and Glu208Lys, and GSTO2 Asn142Asp in the Japanese and Mongolian that have been reported in our previous studies (Fujihara et al., 2007; Takeshita

For GSTO1 Glu155del and Thr217Asn, GSTM1 wild/null, and GSTT1 wild/null, the genotype frequencies of the present study were compared with those in previous studies Ninety-one percent of the Vietnamese analyzed in the present study was the wild type of GSTO1

studies (Whitbread et al., 2003; Fujihara et al., 2007; Paiva et al.,

No mutation allele was detected for GSTO1 Thr217Asn in the present study population (Table 2) Up to date, there is no available information on GSTO1 Thr217Asn mutation in any population, although this type has been registered in NCBI SNP Database as

with the wild type using in vitro assay, although the relevance of this variant in arsenic metabolism is still unclear (Schmuck et al., 2005) Null type frequencies of GSTM1 and T1 in Vietnamese were 42% and 30%, respectively (Table 2) In the review article byMo et al

13.1–54.5% in Caucasians, 46.7% in American-Africans, and 26.9% in Africans for GSTM1 null type and 41.9–52% in Asians, 11.1–28.6% in Caucasians, 26.7% in American-Africans, and 36.6% in Africans for GSTT1 null type Compared with the results in the Asian populations, frequency of GSTT1 deletion in the Vietnamese was lower, while proportion of GSTM1 null type was within the range On the contrary, GSTT1 null type frequency in Taiwanese was 26% (Chiou et al., 1997), which was similar to that in the Vietnamese.Lin et al (2007)found

GSTM1 Wild

GSTT1 Wild

V ,

V ,

III ,

V ,

III +A

V );III/V,

III /As

V ;

V /IA;

V /MMA

V ;

⁎p

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T Agusa et al / Toxicology and Applied Pharmacology 242 (2010) 352–362

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Table 5

Stepwise multiple regression of arsenic concentrations and compositions in urine and hair against sex, age, BMI, TA in drinking water, and polymorphisms in GST superfamily and AS3MT in residents from Hoa Hau and Liem Thuan in Vietnam.

%As III

%As V

GSTP1 Ile105Val (0 = Ile/Ile, 1 = Ile/Val) 0.273 0.002

Abbreviations: AB, arsenobetaine; DMA V

, dimethylarsinic acid; MMA V

, monomethylarsonic acid; As III

, arsenite; As V

, arsenate; IA, inorganic arsenic (As III

+ As V

); III/V, As III

/As V

; M/I, MMA V

/IA; D/M, DMA V

/MMA V

; SA, sum of arsenic compounds; TA, total arsenic; BMI, body mass index (weight (kg)/height (m) 2

).

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that prevalence of GSTM1 and T1 deletion type were 71% and 35%,

respectively, in Hmong in China, and 42% and 47%, respectively, in Han

in China Therefore, there may be large variations in the frequencies of

GSTM1 and T1 null type even in the Asian populations

Potential effects of genetic polymorphisms in GST superfamily on arsenic

concentration and metabolism in Vietnamese

Since the hair can be a good indicator of chronic arsenic exposure

status, while arsenic level and speciation in the urine can represent

recent exposure and metabolism of arsenic in humans, respectively,

we measured arsenic in the hair and urine to examine their

relationships to genetic polymorphisms in GST isoforms Although

arsenic concentration in drinking water as well as cumulative arsenic

relationships between arsenic metabolism and TA in drinking water

or cumulative arsenic exposure (pN0.05) Thus, the data of all donors

were pooled for analysis of the relationship between arsenic and

genotypes of GSTs Concentrations and compositions of urinary

arsenicals and metabolic index for each genotype of GST superfamily

are shown inTables 3 and 4 Because the sample sizes of the mutation

homo types of GSTO1 Ala140Asp (n = 1) and GSTO2 Asn142Asp

(n = 5) were small for the statistical analysis, these mutations were

included in hetero + homo type group for the further discussion

Concentrations of AsV(p = 0.018) and IA (p = 0.050) in the urine of

than those with the wild type (Table 3) Furthermore, urinary %IAs was

also low in hetero type of GSTO1 Glu155del (p = 0.039,Table 4) On the

other hand, higher M/I value of GSTO1 Glu155del heterozygote was

thiol-transferase and GSH conjugation in mutation of GSTO1 Glu155del than

the wild type in an in vitro study Hence, it might be suggested that if

methylation of IA by AS3MT occurs in the form of arsenic-glutathione as

GSTO1 Glu155del mutation protein enhances the methylation of IAs

However, since the difference in M/I value between them was not so

large in the present study and also the association between GSTO1

Glu155del andfirst methylation index was not obvious in the multiple

regression analysis as shown later (Table 5), further studies are needed

to confirm the association.Schmuck et al (2005)reported that GSTO1

Glu155del protein expressed in Escherichia coli exhibited higher MMAV

and DMAVreductase activities than the wild type Because MMAIIIand

DMAIIIwere not analyzed in the urine sample of the present study,

relationship between genetic polymorphisms in GSTO1 and methylated

trivalent arsenicals remains unclear for the subjects In the case of

human studies, there was no relationship between GSTO1 Glu155del

and urinary arsenical in Mexican (Meza et al., 2005) and Chilean (Paiva

substitu-tion in Mexicans (n = 75) who were exposed to arsenic through the

consumption of drinking water showed unusual urinary arsenic profile;

one who has GSTO1 Glu155del and Glu208Lys substitutions had high %

Ala140Asp substitution in addition to these two substitutions displayed

high %AsIIIand low %DMAVin the urine compared to the rest of the study

population In the present study, no such haplotype was found

As for GSTM1, concentration (p = 0.018,Table 3) and composition

(p = 0.028,Table 4) of AB in the null type were significantly greater

than those in the wild type, although the reason was not clear

1989), the relationship for %AB might be partially due to a negative

(p = 0.009) was low in GSTM1 null compared with that in the wild type (Table 4), implying that GSTM1 null may affect %DMAVin the Vietnamese However, the result was not consistent with those in

urinary %IA for the null genotype of GSTM1 in Taiwanese In the workers occupationally exposed to arsenic in Chile (Marcos et al.,

between GSTM1 genotype and methylation ratios in Bangladesh people with skin lesions No relation of GSTM1 genotype to arsenic level in toenail was reported in subjects from arsenic-endemic region

in Bangladesh (Kile et al., 2005), whereas arsenic concentrations in urine and hair were high in GSTM1 null carriers exposed to indoor combustion of high arsenic coal in China (Lin et al., 2007)

We found that GSTP1 Ile105Val homozygote had higher concen-trations of AB, MMAV, AsIII, IA and SA, and %AsIIIand %IA in the urine than the heterozygote, whereas the opposite trend was observed for %

Ile105Val hetero type was significantly higher than that in the wild type (p = 0.002,Table 4) Urinary III/V in the heterozygote of GSTP1 Ile105Val was about half of that in the wild homozygote (p = 0.027,

erythrocyte of GSTP1 Ile105Val wild type was higher than that of the mutation type in the healthy Chinese, but AsVreduction activity

variant homo type showed a slightly (p = 0.085) higher %DMAVin the urine than the wild type in Chileans (Marcos et al., 2006), the GSTP1 Ile105Val variant homo type was not observed in the population of the present study

There were no significant associations of GSTO1 Ala140Asp, GSTO2 Asn142Asp, and GSTT1 wild/null with concentrations and composi-tions of arsenic in the urine and hair (pN0.05,Tables 3 and 4) The result for the polymorphism of GSTO1 Ala140Asp was consistent with the results reported in several in vitro studies; activities of MMAV

activities of thioltransferase and GST conjugation between GSTO1

According to the study ofMukherjee et al (2006), protein expression level of GSTO1 Ala140Asp mutation was similar to that of the wild type, although the activity was not measured In human studies, there was no association of GSTO1 Ala140Asp with arsenic metabolism in the Mexican (Meza et al., 2005), Hungarian, Romanian, and Slovakian

Like GSTO1, GSTO2 has six exons that are separated within 7.5 kb nucleotide length on chromosome 10q24.3 The homology of amino

compared to GSTO1 Furthermore, GSTO2 Asn142Asp polymorphism does not affect those reductase activities This result may support our results on GSTO2 Asn142Asp which showed no association with arsenic metabolism (Tables 3 and 4)

Argentina (Steinmaus et al., 2007), and Chinese (Lin et al., 2007) subjects, GSTT1 wild/null polymorphism had no relevance to urinary arsenic in Vietnamese of the present study (Tables 3 and 4) However,

drinking water, %DMAVin urine of subjects with GSTT1 null type was higher than that in the wild type Also, the interaction between GSTT1 wild type and secondary methylation ratio might increase the risk of

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T Agusa et al / Toxicology and Applied Pharmacology 242 (2010) 352–362

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of As in the nail of GSTT1 null type carriers in Bangladesh.

difference (Table 1, pb0.001) and was positively correlated with TA

cumulative arsenic exposure level (pb0.001) Therefore, the

associ-ation of hair TA level with polymorphisms in GST superfamily was

assessed by ANCOVA, having correction with concentration of TA in

drinking water and cumulative arsenic exposure as covariates, but no

significant results were found (pN0.05,Table 3) Similar to our results,

human hair and toenail and polymorphisms of GSTM1 and T1 in the

contrast,Lin et al (2007) found high concentrations of arsenic in

both hair and urine of GSTM1 null carriers who were exposed to

arsenic from indoor coal combustion in Southwest Guizhou, China,

and arsenic levels in hair and urine

Potential effects of genetic polymorphisms in GST superfamily and AS3MT,

sex, age, BMI, arsenic level in drinking water, and cumulative arsenic

exposure level on arsenic concentration and metabolism in Vietnamese

In the previous study (Agusa et al., 2009b), we investigated the

influence of various factors on arsenical concentration and

composi-tion in the urine and hair in this Vietnamese populacomposi-tion, including age,

sex, BMI, occupation, residential years, alcohol and smoking habits,

and TA level in drinking water, and 13 SNPs in AS3MT such as a4602g

(a to g substitution at nucleotide base 4602), t4740c, t5913c, a6144t,

g7395a, t8979a, g12390c, t12590c, c14215t, t14458c, t35587c,

g35991a, and g37853a, and revealed significant effects of sex, age,

BMI, concentration of TA in drinking water, and several SNPs in

AS3MT Therefore, those factors might co-affect the results on

relationships between arsenic and GST genotypes examined in this

regression analyses was conducted to assess whether the

distribu-tions of urinary arsenic metabolites were dependent on sex, age, BMI,

selenium, and gene polymorphisms of GSTO1, AS3MT, and

methyle-netetrahydrofolate reductase (MTHFR) Here, we attempted to detect

the effects of sex, age, BMI, concentration of arsenic in water,

cumulative arsenic exposure status, and polymorphisms in GST

superfamily and AS3MT on arsenic level and profile in the Vietnamese

using a stepwise multiple regression analysis Prior to the analysis, we

numbers of each sex, age and BMI in each genotype of GST

superfamily (pN0.05) The multicollinearity of independent variables

for multiple regression analysis was examined by calculating the VIF

The result showed that there was no significant multicollinearity (all

VIFs were less than 10)

The result of stepwise multiple regression analysis is shown in

of univariate analysis in the present study (Tables 3 and 4) and our

previous results (Agusa et al., 2009b): associations between GSTO1

Ile105Val and concentrations of AB, MMAV, AsIII, IA and SA, %DMAV,

%AsIII, %IA, III/V and M/I in urine; between GSTM1 wild/null and %DMAV

in urine; between age and M/I; between sex and concentrations of

MMAV, AsIII and IA, %MMAV, %AsIII, %IA and D/M in urine, and

concentration of TA in hair; between BMI and concentrations of

DMAV, AsV, IA and SA in urine, and TA in hair; between concentrations

of TA in drinking water and hair; between AS3MT t4740c and

between AS3MT t14458c and M/I in urine; between AS3MT g35991a

GSTM1 wild/null with D/M in urine; of age with DMAVlevel, SA level and %DMAVin urine, and with TA level in hair; of sex with %AB and M/I in urine; of AS3MT t4740c with AsIIIlevel and M/I in urine; of AS3MT t5913c with AsVlevel and D/M in urine; of AS3MT a6144t with

%MMAVin urine; of AS3MT g7395a with AsVlevel and %AsVin urine;

of AS3MT c14215t with III/V in urine; of AS3MT t35587c with AB and

Factors influencing metabolic capacity of arsenic were also character-ized as follows: lower III/V in c/c homo type of AS3MT c14215t and Ile/Val hetero type of GSTP1 Ile105Val; lower M/I in a/a homo type of AS3MT g35991a, Ile/Ile homo type of GSTP1 Ile105Val, t/t homo type

of AS3MT t5913c, t/t homo type of AS3MT t14558c, male, younger people, and t/t homo type of AS3MT t4740c; and lower D/M in g/g homo type of AS3MT g12390c, male, null type of GSTM1, and c/c + t/

c types of AS3MT t5913c

Although we statistically detected co-effects of genetic polymorph-isms in GST superfamily as well as sex, age, BMI, TA in drinking water and AS3MT genotypes on the arsenic concentration and metabolism, adjusted determination coefficient (Radj2 ) in multiple regression equa-tion was not so high (up to 0.344 for M/I) (Table 5) Thus, it seems possible that there are other significant factors to account for the variation in arsenic level and metabolism Other SNP sites in GSTO1

determined in the present study, might also be involved in the variation.Mukherjee et al (2006)found large variations of protein expression levels of GSTO1 Cys32Tyr and GSTO2 Val41Ile, Cys130Tyr, and L158Ile as well as those investigated in the present study (GSTO1 Ala140Asp, Glu155del, Glu105Lys, and Ala236Val, and GSTO2 Asn142Asp), indicating the possibility of significant variations in the expression levels and catalytic functions among polymorphisms in GSTO1 and GSTO2 Also, recombinant Arg173Trp and Thr306Ile

activity and immunoreactive protein compared to the wild type

quite low (up to 5%) in African-Americans, Caucasian-Americans, Han

relationship among the population at small sample scale Many SNPs

in the intron regions of GSTO1, GSTO2 and AS3MT have been reported

Database, and the linkage between the intronic polymorphisms and metabolism of arsenic is of interest Alternatively, other genetic polymorphisms such as MTHFR Ala222Val and Glu429Ala, which may associate with arsenic metabolism in human (Lindberg et al., 2007;

considered Further studies at larger scale are required to detect more rigid relationships between genetic polymorphisms and arsenic

selenium and vitamins C and E are known to modify toxicity of arsenic

metabolism for residents in developing countries

In summary, we suggest here that genotypes of GSTO1 Glu155del, GSTP1 Ile105Val, and GSTM1 wild/null affect arsenic metabolism in a Vietnamese population Interestingly, GSTP1 Ile105Val polymorphism,

on which there is little information in association with arsenic

with urinary arsenic In addition to the genetic polymorphisms of GST superfamily, sex, age, BMI, TA in the drinking water, and various SNPs

in AS3MT were also related to arsenic level and profile in the

indicating the associations between genetic polymorphisms of GSTs and arsenic metabolism in a Vietnamese population

Trang 10

We wish to thank Dr A Subramanian, CMES, Ehime University,

Japan for critical reading of the manuscript The authors express

thanks to the staff of the CETASD, Hanoi University of Science and Dr

H Sakai, CMES (current affiliation; Laboratory of Structure-Function

Biochemistry, Department of Chemistry, Faculty of Science, Kyushu

University, Japan) for their help in sample collection We also

acknowledge Ms H Touma and Ms N Tsunehiro, staff of the

es-BANK, CMES for their support in sample management and Ms Y Fujii,

Department of Legal Medicine, Shimane University Faculty of

Shimane University Faculty of Medicine, Japan) for her technical

assistant This study was supported by Japan Society for the

Promotion of Science (JSPS) for the cooperative research program

under the Core University Program between JSPS and Vietnamese

Academy of Science and Technology (VAST) Financial support was

also provided by grants from Research Revolution 2002 (RR2002; to

H.I.) Project for Sustainable Coexistence of Human, Nature and the

20221003; to S.T.) and (A) (No 19209025; to H.T.) from JSPS, and

21st Century and Global COE Programs from the Ministry of

Education, Culture, Sports, Science, and Technology (MEXT), Japan

and JSPS The award of the JSPS Post Doctoral Fellowship for

Researchers in Japan to T Agusa (No 207871) is also acknowledged

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