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Interaction of the GTS1 gene product with glyceraldehyde-3-phosphate dehydrogenase 1 required for the maintenance Weidong Liu, Jinqing Wang, Kazuhiro Mitsui, Hua Shen and Kunio Tsurugi D

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Interaction of the GTS1 gene product with

glyceraldehyde-3-phosphate dehydrogenase 1 required for the maintenance

Weidong Liu, Jinqing Wang, Kazuhiro Mitsui, Hua Shen and Kunio Tsurugi

Department of Biochemistry, Yamanashi Medical University, Japan

We previously reported that GTS1 is involved in regulating

ultradian oscillations of the glycolytic pathway induced by

cyanide in cell suspensions as well as oscillations of energy

metabolism in aerobic continuous cultures Here, we

screened a yeast cDNA library for proteins that bind to

Gts1p using the yeast two-hybrid system and cloned multiple

TDH cDNAs encoding the glycolytic enzyme

glyceralde-hyde-3-phosphate dehydrogenase (GAPDH) We found

that the zinc-finger and dimerization sites of Gts1p were

required for full ability to bind GAPDH, and Gts1ps

mutated at these sites lost the ability to regulate both aerobic

and unaerobic ultradian oscillations of energy metabolism

Of the three TDH genes, only TDH1 fluctuated at the mRNA level in continuous culture and its deletion resulted

in the disappearance of the oscillation without any affect on growth rate This loss of biological rhythms in the TDH1-deleted mutant was rescued by the expression of TDH1 but not of TDH2 or TDH3 under the control of the TDH1 promoter Thus, we hypothesized that Gts1p plays a role in the regulation of metabolic oscillation by interacting with the TDH1product, GAPDH1, in yeast

Keywords: continuous culture; glyceraldehyde-3-phosphate dehydrogenase; Gts1p; metabolic oscillation; yeast

Ultradian (cycles with a period shorter than 24 h)

oscilla-tions of the glycolytic pathway were induced after addition

of glucose by inhibiting mitochondrial respiration with

cyanide in cell suspensions [1–3] or cell extracts [4] of yeast

with a periodicity of 1–2 min as monitored by measuring

the level of NAD(P)H (reviewed in [5]) The glycolytic

pathway has been shown to be an autogenous oscillator

under extreme nonequilibrium conditions of energy in

dissipative structures, which theoretically include all living

organisms [5–7] The pathway oscillates under the primary

control of phosphofructokinase [8,9], transferring energy

from glucose to NADH, which acts as the feed-forward

activator, and then from NADH to ATP, which acts as the

feedback inhibitor After ATP as an inhibitor has been

consumed, glucose again begins to enter the glycolytic

pathway Yeast cells also exhibit sustained ultradian

oscil-lations of energy metabolism, with a periodicity of 4 h in

continuous (chemostat) culture under aerobic conditions in

an open system using a bioreactor [10–13] (Hereafter,

aerobic oscillation will be referred to as energy metabolism

or metabolic oscillation in distinction from cyanide-induced

glycolytic oscillation.) Energy-metabolism oscillations,

which arise spontaneously under conditions of high cell

density ( 5 · 108cellsÆmL)1) [14], are detectable as a

periodic change in the factors involved in energy

metabo-lism such as dissolved oxygen (DO) levels, CO2production, glucose and ethanol concentrations, and amounts of storage carbohydrates [10–13] DO oscillation is caused by the periodic change between respiratory and respiratory-fer-mentative phases, in which oxygen demands are relatively high and low, respectively Although the mechanism of energy-metabolism oscillation has not been elucidated, we assume that it is similar to that of glycolytic oscillation except for the involvement of mitochondria in ATP production as the NAD(P)H level is increased during the respiratory-fermentative phase [14] and the ATP level is increased in the early respiratory phase (J Wang &

K Tsurugi, unpublished data) The energy-metabolism oscillation is coupled to oscillations of cell division [12,13,15] and cellular responses to various stress conditions, such as heat, oxidative agents and cytotoxic compounds [14,16] (In this report, the term coupling is used to refer to a state in which multiple oscillators fluctuate with the same periodic-ity irrespective of phase.) It should be added that a cell-cycle-independent oscillation of energy metabolism with a short periodicity (20 min to 1 h) was observed under particular conditions in continuous cultures [17]

The gene GTS1 was originally isolated from a yeast cDNA library with oligonucleotides encoding three Gly-Thr repeats which had been found in the clock-related gene period[18] and was thus named GTS1 [19] We subsequently found that the repeat was translated as an Ala-Gln repeat

in the GTS1 product Gts1p [20], which is similar to the Gln-rich domain found in the clock-related protein Clock [21] Although the structural basis of Gts1p as a clock-related protein is obscure, mutations of GTS1 showed pleiotropic effects on yeast in a gene-dosage-dependent manner; these effects included the timing of budding and sporulation and the capacity for heat tolerance [19,22], all of which are known to be clock-related in other organisms

Correspondence to K Tsurugi, Department of Biochemistry 2,

Yamanashi Medical University, 1110 Shimokato, Tamaho,

Nakakoma, Yamanashi 409-3898, Japan.

Fax: + 55 273 6784, Tel.: + 55 273 6784,

E-mail: ktsurugi@res.yamanashi-med.ac.jp

Abbreviations: DO, dissolved oxygen; GAPDH,

glyceraldehyde-3-phosphate dehydrogenase; ABC, ATP-binding cassette.

(Received 4 April 2002, revised 4 June 2002, accepted 12 June 2002)

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(reviewed in [23,24]) Further, we found that the amplitudes

and durations of the cyanide-induced ultradian oscillation

changed significantly as a function of the GTS1 gene

dosage, whereas the frequencies of oscillation did not vary

very much among the stains tested [25] We then reported

that ultradian oscillation of energy metabolism and

coup-ling of oscillations of cell division and stress responses in

continuous culture were disrupted by inactivation of the

GTS1 gene [16] We recently presented evidence that the

metabolic oscillator drives the heat resistance oscillator

composed of machinery involved in the synthesis of

trehalose [26] We hypothesized that the synthesis of

trehalose parallels activation of the glycolytic pathway,

and trehalose is degraded by trehalase activated by cAMP

coupled to the metabolic oscillation Deletion of GTS1

resulted in the loss of the fluctuations in the synthesis of

trehalose and cAMP [26], leading to the disappearance of

the oscillations These results suggested that Gts1p plays

some role in the coupling of these oscillators Furthermore,

we suggested that the rhythmic expression of Gts1p is more

important than the protein level for maintenance of

ultradian rhythms, as the constitutive expression of GTS1

under the control of the TPI promoter resulted in the

disappearance of ultradian rhythms [16] More recently, we

reported that, when GTS1 was expressed under the control

of a short (183-bp) promoter in the GTS1-disrupted mutant,

the amplitude of Gts1p fluctuations was restricted, leading

to attenuation of the metabolic oscillation and the

uncoup-ling of stress-resistance oscillations [27] Thus, we suggested

that, for stress-resistance oscillations to occur, full

fluctu-ation in the level of Gts1p is required We are now studying

the molecular mechanism by which Gts1p functions in the

coupling of ultradian oscillations This study of ultradian

oscillation in yeast should contribute to our understanding

of the biological rhythms in other organisms, as the energy

metabolism pathway is an autogenous oscillator in all living

organisms [5–7], although there may be various

modifica-tions

Gts1p contains a zinc-finger motif similar to that of

GATA-transcription factors [28] in the N-terminal region

and a glutamine-rich strand in the C-terminal region and

thus Gts1p has been conventionally classified as a

tran-scription factor in the yeast genome database [29] However,

it is unlikely that Gts1p is a DNA-binding protein because it

binds to neither oligomers containing the GATA motifs nor

Sau3AI fragments derived from the yeast genome in gel

mobility-shift assays (

1 S Yaguchi & K Tsurugi, unpublished

data) Now, the zinc finger is shown to be similar to that

contained in GTPase-activating proteins of

ADP-ribosyla-tion factors, which are considered to play a role in protein

interaction rather than DNA binding [30,31] In addition,

Gts1p has a dimerization site in an 18-amino-acid region of

the C-terminal portion, which plays a role in the formation

of a homodimer and heterodimer with the homologous

cytoplasmic domain of some ATP-binding cassette (ABC)

transporters [32] The sequence was characterized by a few

acidic amino-acid residues preceded by hydrophobic amino

acids The presence of these sequences suggested that Gts1p

interacts with various proteins to show pleiotropic effects on

yeast

In this study of how Gts1p functions, we searched for

proteins that interact with Gts1p using the yeast two-hybrid

system We found that GAPDH binds to Gts1p and that

both the zinc-finger and the dimerization sites of Gts1p were involved We showed that mutations of Gts1p that removed the zinc finger or dimerization region affected the mainten-ance of ultradian oscillations of energy metabolism in yeast Further, we present evidence that, of the three GAPDH species in yeast, GAPDH1 is involved in the appearance and maintenance of metabolic oscillations via interaction with Gts1p

M A T E R I A L S A N D M E T H O D S

Yeast strains and culture conditions

A haploid strain of the yeast S cerevisiae, W303, was used for cyanide-induced glycolytic oscillation in cell suspensions [25] Cells were cultured in medium containing 10 gÆL)1 glucose, 6.7 gÆL)1yeast nitrogen base without amino acids (Difco Laboratory, Detroit, MI, USA), and 100 mM potassium phosphate at pH 5.0 supplemented with

40 lgÆmL)1adenine sulfate and essential amino acids The cells harvested 1–2 h after the glucose in the medium had been exhausted [25] were washed and resuspended in

100 mM potassium phosphate, pH 6.8, to a concentration

of 4 mg proteinÆmL)1before being starved for 3 h at 30C Oscillations were induced by adding 20 mMglucose to the starved cells and then after 4 min, 5 mMpotassium cyanide The oscillations were monitored by NADH fluorescence using a spectrofluorimeter (Hitachi F-4500) in a stirred and thermostatically regulated cuvette

Another haploid strain of the yeast S cerevisiae, S288C, was used for the continuous cultures [14] The cells were cultured at 30C in a synthetic medium containing 1% glucose as defined elsewhere [10] using a modified bench-top fermenter, MDL-6C (Marubishi Bioengineering, Tokyo, Japan) with a constant volume of 500 mL The batch and successive continuous cultures were performed as described previously [14,16], and the periodic change in respiratory-fermentative metabolism was monitored by measuring the level of DO with an oxygen electrode

Construction ofGTS1 mutants for the two-hybrid assay N-Terminal and C-terminal truncated mutants of GTS1 were constructed from the wild-type GTS1 as described previously [32] The GTS1 mutant with the KpnI–NcoI fragment deleted (for a physical map of GTS1, see Fig 1A), named GTS1[KN], which corresponds to the dimerization site covering 18 amino-acid residues from 296 to 313, was constructed as described previously [32] and named GTS1[DKN] To replace the cysteine residue at position

53 in the putative zinc finger with tyrosine, site-directed mutagenesis was performed according to the protocol of the kit In vitro Mutagenesis Primers (Takara, Tokyo, Japan) using primers 1 and 2 (Table 1) as 5¢ primers for the first and second PCR, respectively The 2.4-kbp SphI–SpeI fragment thus obtained containing nucleotides)1572 to +1513, with respect to the first residue A of GTS1, named GTS1[C53Y], was inserted into pAUR112 The mutation was con-firmed by determining the nucleotide sequence of the PCR-amplified EcoRI–SalI fragment directed on the recombinant plasmid The EcoRI–SalI fragment was inser-ted into the plasmid (pGBT9) of the two-hybrid system GTS1[C53Y] with the dimerization site deleted [32], named

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GTS1{[DKN] + [C53Y]}, was obtained by removing the

KpnI–NcoI fragment from GTS1[C53Y] GTS1[DC] was

constructed by deleting the ClaI-ClaI fragment from GTS1

GTS1{[DC] + [DNS]} and GTS1{[DC] + [DKS]} were

obtained by deleting the NcoI–SalI and KpnI–SalI

frag-ments, respectively, from GTS1[DC]

The yeast two-hybrid system

The two-hybrid assay was performed using the

Matchma-ker Two-hybrid System (Clontech) as described previously

[32] To screen for Gts1p-interacting proteins, a yeast

cDNA library prepared using a cDNA synthesis kit

(Amersham Pharmacia Biotech) was inserted into the plasmid pGAD424 (LEU2 Ampr) downstream of the activation domain of GAL4 The recombinant plasmids were transformed together with the recombinant plasmid pGBT9 (TRP1 Ampr) carrying GTS1 in-frame downstream

of the DNA-binding domain of GAL4 To determine the binding site of Gts1p and GAPDH, the wild-type and mutant GTS1 genes were inserted into pGBT9, and the cloned cDNA encoding the C-terminal 97 amino-acid residues of GAPDH3 (GAPDH3-C97) was inserted into pGAD424 The interactions between the prey and bait hybrid proteins were determined as activation of the lacZ reporter gene by measuring the b-galactosidase activity of the cells using either or both the colony lift assay and liquid culture assay for b-galactosidase as described previously [32] The protein levels of the Gts1p mutants were examined

by Western blotting using antibody to Gts1p as described previously [10]

Transformation with a chimeric plasmid harboringGTS1 The GTS1-deleted mutant gts1D(W303) was produced using the strain W303 as described previously [22,25] To transform gts1D(W303) with GTS1, GTS1[DKN] and GTS1[C53Y], the constructs were inserted into the vector pYX222 at the multicloning site These transformants were named pYXGTS1/gts1D(W303), pYXGTS1[DKN]/gts1D (W303) and pYXGTS1[C53Y]/gts1D(W303), respectively The GTS1-deleted mutant gts1D was produced using strain S288C as described previously [14,16] GTS1[DKN] and GTS1[C53Y] inserted into pAUR112 were transformed into gts1D and the transformants were named pACGTS1 [DKN]/gts1D and pACGTS1[C53Y]/gts1D, respectively Preparation ofTDH-deleted mutants

TDH1, TDH2 and TDH3 encoding GAPDH1, GAPDH2 and GAPDH3, respectively [33,34], were cloned by PCR directed against yeast genomic DNA from S288C Synthetic oligonucleotides for 5¢ and 3¢ primers, 3 and 4 for TDH1,

Table 1 List of synthetic oligonucleotides used for primers (1–13) or probes (14,15) in this experiment.

No Sequence (5¢-3¢)

1 5¢-CCCGAAGCATGCTGTGCCTAC-3¢

2 5¢-CCCGAAGCATGCTGTGCTCAC-3¢

3 5¢-GGAGAATTCGTTGGGCTGAGCTTCTGATCC-3¢

4 5¢-TTGGGATCCTTAAGCCTTGGCAACATATTC-3¢

5 5¢-CTTTGAATTCTGCTGTAACCCGTACATGCC-3¢

6 5¢-ATTAGAATTCGCGGCTAAAGTTAAGCATGC-3¢

7 5¢-GAAAACTGGATCCGACTTGTATGCTAAAGG-3¢

8 5¢-TTGGGATCCTTAAGCCTTGGCAACATATTC-3¢

9 5¢-GAAAACTGGATCCGACTTGTATGCTAAAGG-3¢

10 5¢-TAATAGGAATTCTGATCATTTTGTTTTGTG-3¢

11 5¢-AACAAGAATTCATGGTTAGAGTTGC-3¢

12 5¢-AGGAGCTCGAGTTAAGCCTTGGCAAC-3¢

13 5¢-AACTAACTAGTACTTGTATGCTAAAGG-3¢

AAGTTCTTGATGAATTTC-3¢

15 5¢-GTGTATTTTTCTTCGTTAACACCCATGACGAA

CATTGGGGCGGTG-3¢

Fig 1 Determination of the binding site of Gts1p in the 97 C-terminal

residues of GAPDH3 (GAPDH3-C97) using N-terminal and C-terminal

deletion mutants (A),and mutants with modifications in the zinc finger

and/or dimerization site of GTS1 (B) in the two-hybrid system Binding

activity was determined by measuring b-galactosidase activity in

colony lifts and in liquid cultures The activity in liquid cultures is

indicated by A 420 due to decomposition of o-nitrophenyl b- D

-galacto-pyranoside (NpGal) as a substrate after incubation for 1 h at 30 C in

a cell suspension containing 106cells [32] Bait genes indicate DNAs

inserted in-frame downstream of the DNA-binding domain of GAL4.

For prey, a cDNA encoding GAPDH3-C97 inserted downstream of

the activation domain of GAL4 was used Open boxes and solid lines

indicate open reading frames and deleted regions, respectively

Lateral-striped and vertical-Lateral-striped boxes indicate approximate positions of a

zinc finger and the dimerization site, respectively In (B), black boxes

indicate approximate positions of the disrupted zinc finger.

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5 and 4 for TDH2, and 6 and 4 (Table 1) for TDH3,

respectively, were used The PCR products were inserted

into pUC19 vector, and the resulting plasmids, named

pUCTDH1, pUCTDH2 and pUCTDH3, were digested to

remove the promoters and 5¢ halves of the TDH genes The

remaining fragments containing the 3¢ halves of the TDH

genes were ligated with fragments from the plasmid

ASAJ2682 containing the kan gene as a selective marker

[35] The fragments containing mutated TDH genes

(TDH1::kan, TDH2::kan, and TDH3::kan) were purified

from the plasmids and transformed into S288C The

TDH-deleted mutants were identified by determining physical

maps of products of PCR directed against genomic DNA

fragments from each mutant In addition, the

TDH1-deleted mutant (tdh1D) was confirmed by analyzing the

length of TDH1 mRNA by Northern blotting, and

TDH2-deleted and TDH3-TDH2-deleted mutants (tdh2D and tdh3D,

respectively) by analyzing the length of the gene loci by

Southern blotting

For the experiment to rescue tdh1D, the 1811-bp BamHI–

BamHI fragment carrying the TDH1 ORF and its 804-bp 5¢

upstream sequence was PCR-amplified on genomic DNA

using oligonucleotides 7 and 8 (Table 1) as 3¢ and 5¢ primers,

respectively The fragment was inserted into the SmaI site of

pAUR112 and transformed into tdh1D To construct TDH3

under the control of the promoter of TDH1, the 804-bp

BamHI–EcoRI fragment was PCR-amplified on genomic

DNA using oligonucleotides 9 and 10 (Table 1) for 3¢ and 5¢

primers, respectively The BamHI–EcoRI fragment ligated

to the EcoRI–BamHI fragment from pUCTDH3 was

inserted into the SmaI site of pAUR112 To construct

TDH2 under the control of the promoter of TDH1, the

TDH2ORF was amplified by PCR using oligonucleotides

11 and 12 (Table 1) for 5¢ and 3¢ primers, respectively, and,

after digestion with EcoRI, the PCR product was ligated

with the 804-bp BamHI–EcoRI fragment The ligated

fragment was amplified by PCR using oligonucleotides 13

and 12 (Table 1) as 5¢ and 3¢ primers, respectively The PCR

product was digested with SpeI and XhoI and inserted into

the cognate sites of pRSA103 The recombinant plasmid

carrying TDH2 and TSH3 under the control of the TDH1

promoter was transformed into tdh1D

Northern and Southern blotting

For Southern-blot analysis of TDH2 and TDH3, the

EcoRI–SnaBI fragment from pUCTDH2 encoding the

5¢-upstream sequence between)649 and )204, with respect

to the first nucleotide A of TDH2, and the EcoRI–NspV

fragment from pUCTDH3 encoding the 5¢-upstream

sequence between)572 and )25, with respect to the first

nucleotide A of TDH3, were used for probes of TDH2 and

TDH3, respectively The probes were labeled using the kit

PCR DIG-Labeling Mix (Roche Diagnostics, Mannheim,

Germany) The HindIII and HpaI fragments of genomic

DNAs of tdh2D and tdh3D, respectively, were

Southern-blotted and visualized using these probes

For Northern blotting, TDH1 mRNA was detected using

the synthetic oligonucleotide 14 (Table 1), which is

comple-mentary to the 5¢ end extension specific for TDH1 mRNA

spanning nucleotide positions )91 to )46 from the first

nucleotide A of TDH1 [33] TDH2 and TDH3 mRNAs

were detected together using oligonucleotide 15 (Table 1),

which is identical with the complementary sequence between + 371 and + 435, with respect to the first nucleotide A of each gene, having 30% dissimilarity from the corresponding region of TDH1 mRNA The probes were labeled with the DIG Oligonucleotide Tailing kit (Roche Diagnostics) and found to have almost the same specific activities Then,

20 lg (for TDH1) and 10 lg (for TDH2 and TDH3) of total RNA extracted from cells using Isogen (Wako, Tokyo, Japan) were electrophoresed in a 1% agarose gel containing 2.2Mformaldehyde, and fluorescence was measured using a fluorimetric image analyzer Fuji LAS-1000 (Fuji-Film Co., Tokyo, Japan) after Northern blotting The relative mRNA level was corrected by total RNA amount based on ethidium bromide staining after agarose gel electrophoresis Western blotting and immunoprecipitation

Western-blot analysis was performed as described previ-ously [16], and immunoprecipitation was performed using anti-(mouse GAPDH) IgG obtained from Funakoshi Co (Tokyo, Japan)

Determination of GAPDH activity GAPDH activity was determined as described previously [34]

R E S U L T S

Interaction between Gts1p and GAPDH in the yeast two-hybrid system

The yeast cDNA library was screened for proteins interact-ing with Gts1p usinteract-ing the yeast two-hybrid system Of eight positive clones, four contained cDNA fragments of TDH3 encoding GAPDH3 and the others contained all different genes As GAPDH is a key enzyme in the energy-metabolism pathway, we decided to study it in detail as a candidate for a Gts1p-binding protein The four fragments

of TDH3 all differed in length, encoding the C-terminal 120,

100, 97, and 76 amino-acid residues of GAPDH3 However,

as the shortest fragment, named GAPDH3-C76, had only weak binding activity in the two-hybrid assay compared with the others (data not shown), the one with the C-terminal 97 residues (GAPDH3-C97) was used to search for binding site(s) of Gts1p The screening of a series of deletion mutants of GTS1 [32] for activity to bind GAP-DH3-C97 in the two-hybrid system revealed that the binding sites were located in both the N-terminal and C-terminal portions of Gts1p, as truncation of either portion resulted in a significant loss of binding activity (Fig 1A) Keeping in mind that Gts1p was characterized structurally by a putative zinc finger and a dimerization site located in the N-terminal and C-terminal portions, respect-ively, we examined the binding sites using a new series of GTS1mutants with modifications at these sites (Fig 1B) The binding activity of Gts1p-DC encoded by GTS1[DC] lacking the ClaI–ClaI region in the middle of Gts1p was even higher than that of wild-type Gts1p Comparing the binding activity of (DC + DKS) with that of (DC + DNS), deletion of the dimerization site from

Gts1p-DC resulted in almost complete loss of the activity (Fig 1B), suggesting that the dimerization site plays an important role

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in the binding to GAPDH However, the finding that Gts1p

lacking only the dimerization region (Gts1p-DKN) still had

some binding activity suggested the presence of other sites

Consistently, the binding activity of Gts1p-C53Y with a

disrupted zinc finger was much weaker than that of

Gts1p-DKN, and Gts1p-(DKN + C53Y) lacking the zinc finger

together with the dimerization site lost all activity (Fig 1B)

Thus, for full activity of Gts1p to bind GAPDH-C97, both

the zinc finger and dimerization site were required

Yeast contains three GAPDH proteins, named

GAP-DH1, GAPDH2, and GAPDH3, which are encoded by

TDH1, TDH2, and TDH3, respectively [33,34] The

amino-acid sequence of GAPDH3 has 90% identity with that of

GAPDH1 and 98% identity with that of GAPDH2 in either

the C-terminal 97 residues or whole sequences As these

proteins are so similar, we examined whether the binding

activity to Gtsp1 is specific for GAPDH3 using whole

lengths of GAPDH proteins as prey in the two-hybrid

system The results showed that there were no differences

among them in terms of their ability to bind Gts1p as bait

(data not shown) Therefore, it is likely that all GAPDH

proteins possess similar binding activity to Gts1p, although

cDNA fragments encoding GAPDH3 were obtained in the

screening assay for Gts1p-binding proteins

Binding of Gts1p to GAPDH in cell lysate

The binding activities of Gts1p-DKN and Gts1p-C53Y to

GAPDH were further tested by the coimmunoprecipitation

assay (Fig 2) Cell lysates expressing the wild-type and

mutant Gts1p proteins were immunoprecipitated with

antibodies to GAPDH, and Western blots of immunopre-cipitates were stained with a labeled anti-Gts1p IgG Consistent with the result from the two-hybrid assay, neither Gts1p-DKN nor Gts1p-C53Y could bind to GAP-DH-C97 (Fig 2) Why Gts1p-C53Y migrated slower than Gts1p on SDS/PAGE is not known

Effect of Gts1p mutants on cyanide-induced glycolytic oscillation

To investigate whether Gts1p interacts with GAPDH to regulate the ultradian oscillations in yeast, GTS1[C53Y] and GTS1[DKN] were transformed into gts1D(W303), and the transformants were subjected to experiments on cyanide-induced glycolytic oscillation We previously reported that the duration of cyanide-induced glycolytic oscillations was lengthened by 27% in the GTS1-deleted mutant and shortened by 20% in the GTS1-overexpressing strain compared with the wild-type cell [25] Similarly the duration

of the oscillations was severely shortened when the wild-type GTS1 was overexpressed in gts1D (pYXGTS1/gts1D) (Fig 3) When gts1D cells overexpressed Gts1p-C53Y or Gts1p-DKN, the duration of the oscillations was lengthened

Fig 2 Determination of binding activity of the dimerization-site-deleted

Gts1p-DKN and zinc-finger-disrupted Gts1p-C53Y for GAPDH in vivo

by coimmunoprecipitation The protein levels of Gts1p in cell lysates

from the GTS1-deleted mutants [gts1D(W303)] expressing the

wild-type (pYXGTS1/gts1D) (lane 1), zinc-finger-disrupted (pYXGTS1

[C53Y]/gts1D) (lane 2) or dimerization-site-deleted (pYXGTS1[DKN]/

gts1D) (lane 3) were determined by Western blotting using antibodies

to Gts1p (upper panel) The cell lysates were immunoprecipitated with

antibodies to GAPDH, and coprecipitated Gts1p was detected by

Western blotting using antibodies to Gts1p (lower panel).

Fig 3 Representative patterns of ultradian oscillation of the NADH fluorescence at 20 °C in cell suspensions of gts1D(W303) (A), gts1D(W303) overexpressing the wild-type (pYXGTS1/gts1D) (B), gts1D(W303) overexpressing the zinc-finger-disrupted Gts1p (pYXGTS1 [C53Y]/gts1D) (C),and gts1D(W303) overexpressing the dimerization site-deleted Gts1p (pYXGTS1[DKN]/gts1D) (D) Cells were harvested about 1.5 h after the diauxic shift Glucose (20 m M final concentra-tion) was added at )5 min and KCN (5 m M ) at time z ero.

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severalfold compared with that of the GTS1-overexpressing

strain (Fig 3) The fact that the oscillation was lengthened

by inactivation of GTS1 [25] suggested that mutant Gts1ps

without the ability to bind GAPDH could not function like

the wild-type Gts1p to regulate cyanide-induced glycolytic

oscillation

Effect of Gts1p mutants on the coupling of biological

rhythms in continuous cultures

As we previously reported [16], the wild-type Gts1p,

expressed with the centromeric recombinant plasmid

carry-ing GTS1 with its upstream region of about 1.0 kbp

(pACGTS1[N-C]) rescued the metabolic oscillations lost in

the GTS1-deleted mutant (gts1D) in continuous culture

(Fig 4A) The energy-metabolism oscillation continued for

about 4 days, although the amplitude of DO oscillation was

about 30% lower than it was in the wild-type cell [16] (also

summarized in Table 2) To investigate whether Gts1p

mutants that had lost the ability to bind GAPDH can rescue

the metabolic oscillations in gts1D, the recombinant

plas-mids carrying GTS1[C53Y] and GTS1[DKN] in

centro-mere-based plasmids, named pACGTS1[DKN]/gts1D and

pACGTS1[DKN]/gts1D were transformed into gts1D, and

the transformants subjected to continuous culture

Although the cells grew normally reaching a critical density

at the beginning of the culture, oscillations of energy

metabolism did not appear in either transformant (Fig 4

and Table 2) This suggested that Gts1p–GAPDH

interac-tion was required for metabolic oscillainterac-tion

Changes in theTDH mRNA levels during the

energy-metabolism oscillation in continuous cultures

GAPDH is generally considered to be a constitutively

expressed protein However, the finding suggesting that

GAPDH is involved in the regulation of metabolic

oscilla-tion raised the possibility that at least one component of

GAPDH fluctuates at the protein level to function in the

metabolic oscillation We examined the activity and protein

concentration of GAPDH as a whole during metabolic

oscillation in continuous culture, but found no apparent

fluctuations (data not shown) Thus it is possible that only a

particular GAPDH species was oscillating

It has been reported that TDH2 and TDH3 were

expressed predominantly in exponentially growing cells,

whereas the expression of TDH1 was increased in the

stationary phase and under conditions of stress [36,37]

Consistent with such reports, we found that the mRNA

level of TDH2/TDH3 [determined together, as their

nuc-leotide sequences are too similar (93% identity) to

discrimi-nate between them by Northern-blot analysis] in the

stationary-phase cells was decreased by about 20% and

that the TDH1 mRNA was increased by 50%, occupying

about 20% of total TDH mRNA, compared with the case

in exponentially growing cells (data not shown) The

mRNA levels of TDH1 and TDH2/TDH3 were determined

during continuous culture in wild-type cells (Fig 5) The

TDH1mRNA level fluctuated with the same periodicity as

energy metabolism, whereas the level of TDH2/TDH3

mRNAs did not fluctuate The result suggested that the

expression of TDH1 apparently fluctuated in concert with

metabolic oscillation, although it remains possible that the

expression of TDH2 and TDH3 fluctuated, with opposite phases canceling out the oscillations of each other

Effect ofTDH gene disruption on energy-metabolism oscillation in continuous cultures

2

To further investigate which TDH genes participate in the regulation of the ultradian oscillations in yeast, we constructed deletion mutants of each gene and subjected them to continuous culture As the deletion of TDH genes reportedly inhibits the growth of yeast to varying degrees

Fig 4 Representative patterns of the DO oscillation in a continuous culture of gts1D expressing the wild-type Gts1p (pACGTS1[N-C]/gts1D)

as a control (A), gts1D expressing the dimerization-site-deleted Gts1p (pACGTS1[DKN]/gts1D) (B), and gts1D expressing the zinc-finger-dis-rupted Gts1p (pACGTS1[C53Y]/gts1D) (C) Continuous culture was started at time zero and continued at a dilution rate of 0.1 h)1with a synthetic medium containing 1% glucose at 30 C The energy meta-bolism oscillation was monitored by measuring the level of dissolved oxygen (DO).

Trang 7

[34], we determined the cell densities at the beginning of the

continuous culture and thereafter The tdh1D mutant grew

as fast as the wild-type cell, reaching a critical cell density

(Table 2), and DO oscillations disappeared within a day

(Fig 6A) similar to the case of gts1D [16] The growth of

tdh2D was disturbed, but the cell density reached 90% of

that of the wild-type at the beginning of the continuous

culture (Table 2) The culture showed a DO oscillation

with wavelength and amplitude similar to those of the

wild-type (Fig 7A and Table 2), but it disappeared in

2 days because eof disturbance of cell growth, as the cell

density decreased to 4.14· 108mL)1 at the end of the

oscillation During the transient oscillation, the TDH1

mRNA level oscillated, whereas that of TDH3 did not

(Fig 7B) The result confirmed the fluctuation of the TDH1mRNA level and eliminated the possibility that the expressions of TDH2 and TDH3 fluctuated with opposite

Table 2 Cell densities and durations and amplitudes of the DO oscillations in continuous cultures of the wild-type and GTS1 and TDH mutants.

Strain

Cell density

pACGTS1[DKN]/gts1D 5.08 ± 0.23 (3) (No oscillations)

pACGTS1[C53Y]/gts1D 5.03 ± 0.15 (3) (No or short oscillations (<12 h))

pACTDH1pr.TDH2/tdh1D 3.40 ± 0.40 (2) (No continuous cultures)

pACTDH1pr.TDH3/tdh1D 2.45 ± 0.35 (2) (No continuous cultures)

a Cell density at the beginning of continuous culture b The amplitude was estimated by subtracting the DO concentration (%) of the valley from that of the peak of the next wave c The number of experiments used for statistical analysis d Continuous cultures could not be started because of the disturbance of cell growth.

Fig 5 Changes in the TDH mRNA levels during the DO oscillation in a

continuous culture of the wild-type S288C Cell samples were harvested

on the second day of the DO oscillation TDH1 (s) and TDH2/TDH3

mRNA levels (d) were determined by Northern-blotting analysis.

Total RNA stained with ethidium bromide was conventionally used

for the quantitative control for applied RNA amounts.

Fig 6 Representative patterns of the DO oscillation in continuous cul-tures of TDH1-deleted mutant (tdh1D) (A) and cells transformed with TDH1 under the control of its own promoter (B) Continuous culture was started at time zero and continued at a dilution rate of 0.1 h)1with

a synthetic medium containing 1% glucose at 30 C.

Trang 8

phases (Fig 6) The growth of tdh3D was most disturbed

among the three TDH mutants as reported in the previous

report [34] without reaching the cell density or showing the

appearance of DO oscillations (Table 2) These results

suggested that the TDH1 gene is the most likely one

required for metabolic oscillation, while the others are

predominantly engaged in the growth of cells

Effect ofTDH gene expression on the rescue

of the metabolic oscillations intdh1D

To examine the possibility that TDH1 is involved in the

regulation of metabolic oscillations, we examined whether

the expression of the TDH1 gene in tdh1D can rescue the

disappearance of biological rhythms by transforming the

centromeric recombinant plasmid carrying TDH1 with its

upstream region of about 0.8 kbp The energy-metabolism

oscillation appeared and continued for about 4 days

(Fig 6B), although the wavelength of the oscillation was

about 35% shorter and the amplitude about 30% lower

than in the wild-type cell (Table 2) In contrast, when TDH2

or TDH3 was expressed in tdh1D under the control of the promoter of TDH1, the cell growth of either transformant was even more disturbed than that of the parental tdh1D, and thus continuous cultures could not be started (Table 2) Thus, GAPDH2 and GAPDH3 could not replace GAP-DH1 to rescue the DO oscillation in tdh1D

D I S C U S S I O N

Using the two-hybrid system to search for Gts1p-binding proteins with a yeast cDNA library, only TDH3 cDNAs encoding GAPDH3 were cloned However, three other results in this report suggested that GAPDH1 interacts with Gts1p to regulate ultradian oscillations in yeast First, the mRNA level of GAPDH1 fluctuated in concert with energy metabolism whereas those of GAPDH2 and GAPDH3 were constant Secondly, inactivation of TDH1 caused the disappearance of the metabolic oscillation without affecting growth of the yeast, whereas inactivation of either TDH2 or TDH3was considered to primarily cause disturbance of cell growth Thirdly, disappearance of metabolic oscillation in tdh1D was rescued by transformation of TDH1 but not by transformation of the other genes This discrepancy is probably explained by the difference in mRNA abundance

in the cDNA library, with TDH3 mRNA being the most and TDH1 mRNA the least abundant (< 10%) in vegetatively growing cells [36] Although there are several substitutions of amino acids in the C-terminal 97 residues between GAPDH1 and the others, they are all very homologous Furthermore, GAPDH1 and GAPDH3 did not show any differences in terms of ability to bind Gts1p in the two-hybrid assay This lack of difference suggested that the C-terminal region of GAPDH1 possesses the same binding activity as that of GAPDH3 However, the result cannot rule out the possibility that GAPDH1 has a preference for Gts1p, as all GAPDH proteins exist as homotetramers in vivo, whereas they are monomers in the two-hybrid system Alternatively, the subcellular localiza-tion of GAPDH1 may be different from others so that it preferentially associates with Gts1p in vivo

In this report, we suggested that Gts1p interacted with GAPDH via the zinc finger in the N-terminal region and the dimerization site in the C-terminal region However, whether

or not these two regions are located adjoining each other is not known because of lack of knowledge of the 3D structure

In addition, we cannot explain why deletion of the ClaI–ClaI region spanning these structures increased the ability to bind GAPDH in the two-hybrid analysis However, it is pointed out that the binding sites are related, if not directly, to nucleotide binding, as the zinc finger is homologous to that

of GTPase-activating proteins of ADP-ribosylation factors [28,30,31] and the dimerization domain is similar to the sequence downstream of Walker’s motif A of some ABC transporters [32,38] The deletion of the ClaI–ClaI region may facilitate interaction Alternatively, as the ClaI–ClaI region contains a ubiquitin-association domain (residues 193–234) [39], which was found to be involved in a rapid degradation of Gts1p itself (

& K Tsurugi, unpublished results), deletion of the region may stabilize the protein (Gts1p-DC) causing elevation of the protein level In fact, the Gts1p-DC level was elevated in most transformed cells in the experiments of the two-hybrid assay

Fig 7 Representative patterns of the DO oscillation in continuous

cul-tures of TDH2-deleted mutant (tdh2D) (A) and the TDH1 (s) and

TDH3 mRNA levels (d) during the DO oscillation (B) Continuous

culture was started at time zero and continued at a dilution rate of

0.1 h)1 with a synthetic medium containing 1% glucose at 30 C.

In (A), the horizontal bar indicates the time when cell samples for

(B) were collected.

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We previously reported that two acidic amino-acid

residues which are preceded by hydrophobic amino acids

were important for the interaction between the

dimeriza-tion domains of Gts1p and some ABC transporters [32]

In this report, of the four positive clones of GAPDH

genes, the shortest one encoding 76 C-terminal amino-acid

residues had only weak binding activity compared with

the one encoding 97 residues Thus, it is likely that a core

binding site of GAPDH exists 97–76 residues from the

C-terminus The sequence of the region

(237-VDVSVVDLTVKLDKETTYDEI-257) is rich in acidic

amino acids preceded by hydrophobic amino acids,

although the overall homology to the Gts1p dimerization

region is low Possibly, the dimerization domain plays a

role in the interaction with various proteins via as yet

unidentified mechanisms, and so Gts1p can have

pleio-tropic effects on yeast phenotypes

The glycolytic enzyme GAPDH is one of the most

abundant proteins and is generally considered to be

constitutively expressed In higher organisms, one copy of

the gene encoding GAPDH is expressed (reviewed [40]) and

has been reported to have a variety of activities including

apoptosis, nuclear RNA transport, microtubule assembly,

protein kinase reactions, and DNA replication [40]

Fur-thermore, it should be pointed out that the protein level of

GAPDH in Neurospora crassa [41] and that of chloroplast

GAPDH in the dinoflagellate Gonyaulax polyhedra [42]

have been reported to undergo circadian oscillation On the

other hand, yeast contains three members of the GAPDH

family, and GAPDH1 has been suggested to have a unique

function among the GAPDH proteins, as it is

predomin-antly synthesized in stationary phase or stressed cells [36,37]

and alone it cannot support growth [34] Structurally, while

there are no nonhomologous substitutions between

GAPDH2 and GAPDH3, there are seven such substitutions

between GAPDH1 and the others In particular, although

GAPDH1 does not have N-degron

acid of GAPDH1 is isoleucine, which is known as a

destabilizing residue according to the N-end rule [43], and

thus differs from the others, which have the stabilizing

residue valine Thus, from the structural viewpoint, it is

possible that GAPDH1 plays a unique role among the three

GAPDHs Here, we showed that the GAPDH1 level

fluctuated in concert with metabolic oscillation, and that

deletion of the gene resulted in disappearance of the

oscillation Thus, we hypothesized that, in yeast, the

metabolic oscillator drives other oscillators via the

interac-tion of Gts1p and GAPDH1, but the precise molecular

mechanism remains to be clarified In addition, as the

mutations in GAPDH affected cyanide-induced glycolytic

oscillation, which supposedly is not coupled to other

oscillators, it is possible that Gts1p plays some direct

role in the oscillation of the glycolytic pathway

Under-standing the biological rhythms in yeast will contribute to

understanding them in other organisms, as it has been

shown that the energy metabolism pathway is an

autogen-ous oscillation in dissipative structures including all living

organisms [5–7]

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