JP2000214610A - Single layer type electrophotographic photoreceptor - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a single type electrophotographic photoreceptor free from the change of the appearance of the photoreceptor surface even if immersed in Isoper(R) without applying an over coat, remarkably small in the elution of a charge transport agent to the Isoper(R) and having practical sensitivity. SOLUTION: The photographic photoreceptor is constituted so as to form a photosensitive layer constituted at least of a charge generating agent, a hole transport agent, an electron transport agent and a binder resin on a conductive substrate and to satisfy equation I: 0.6<=WHTM/WETM<=1.0 and equation II: 0.6<=(WHTM+WETM)/100<=1.0 in the relation between a hole transport agent content WHTM (wt.%) and an electron transport agent content WETW (wt.%) per the binder resin in the photosensitive layer. As a result, the single type electrophotographic photoreceptor is free from the change of the appearance of the photoreceptor surface even if immersed in the Isoper(R) without being coated with the over coat layer and remarkably small in the elution of the charge transport agent into the Isoper(R) and then is inexpensively obtained and applied to an image forming device using wet developing system.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to an electrophotographic photosensitive member used for an image forming apparatus such as an electrophotographic copying machine, a facsimile, and a laser beam printer.

[0002]

2. Description of the Related Art Electrophotographic developing systems utilizing the Carlson process are broadly classified into dry developing systems and wet developing systems. An image forming apparatus using a dry developing method is widely and generally used at present, such as a copying machine and a printer.However, although an image forming apparatus using a wet developing method has been developed for a long time, At present, it is used only in special fields.

[0003] However, in an image forming apparatus using a wet developing method, a toner is generally dispersed in a hydrocarbon-based solvent called isoper, and the toner particle diameter is 1 μm.
m, the resulting image has very high image quality. For this reason, with the recent expansion of the market of full-color printers that require high image quality, they have been spotlighted again.

An image forming apparatus using a wet developing method is
As described above, since a solvent called isoper is used as a developer, all or a part of the photosensitive drum is immersed in the solvent. For this reason, an inorganic photoreceptor such as selenium or amorphous silicon, which does not elute the photoreceptor component in the isopar, is generally used.

On the other hand, the organic photoreceptor is easier to manufacture and lower in cost than the conventional inorganic photoreceptor, and has a charge transport agent,
In recent years, photoreceptor materials such as a charge generating agent and a binder resin are widely used because they have various options and a high degree of freedom in functional design.

[0006] The organic photoreceptor includes a single-layer type photoreceptor in which a charge transporting agent (hole transporting agent, electron transporting agent) is dispersed in the same photosensitive layer together with a charge generating agent, and a charge generating agent containing a charge generating agent. There is a laminated photoconductor in which a layer and a charge transport layer containing a charge transport agent are laminated.

In particular, a single-layer type photoreceptor is extremely difficult to use because it has a simple structure and is easy to manufacture, can suppress film defects when forming layers, has few interfaces between layers, and can improve optical characteristics. In the limelight. The single-layer type photoreceptor can be used for both positive and negative charging types, but generally, the positive charging type is currently the mainstream due to the characteristics of the photoreceptor constituent materials.

[0008]

However, when a general organic photoreceptor is used in an image forming apparatus using a wet developing method, as described above, all or a part of the photoreceptor drum is immersed in the isoper. As a result, appearance changes such as cracks occur on the surface of the photoreceptor, and low molecular weight substances such as charge transporting agents (hole transporting agents and electron transporting agents) are eluted into the isopers, leading to a decrease in charge or a decrease in sensitivity. A phenomenon such as deterioration occurs, and it becomes difficult to obtain a good image.

Therefore, isoper resistance is exhibited by using an organic photoreceptor in which the surface of the organic photoreceptor is further overcoated (surface protective layer) with a thermosetting resin such as a silicone resin, a melamine resin, or an epoxy resin. However, it has been proposed to prevent the elution of the charge transport agent. However, the application of the overcoat causes a serious problem that the sensitivity is remarkably deteriorated and the production cost is increased.

On the other hand, as a method of not applying an overcoat, a charge transporting ability is imparted to the binder resin itself (CT polymer), and the content of the charge transporting agent is reduced to zero or reduced, thereby exhibiting the isopar resistance. However, the molecular design of the CT polymer is very difficult, and is far from practical sensitivity as an electrophotographic photoreceptor.

Therefore, an object of the present invention is to provide a photoreceptor which has no change in appearance even when immersed in isoper without overcoating and has excellent isoper resistance (very little elution of the charge transport agent into isoper). It is another object of the present invention to provide a single-layer electrophotographic photosensitive member having practical sensitivity.

[0012]

Means for Solving the Problems As a result of intensive studies, the present inventors have found that in order to achieve the above object, at least a charge generating agent, a hole transporting agent, an electron transporting agent and a binder resin are formed on a conductive substrate. And a hole transporting agent content [W _HTM (wt%)] and an electron transporting agent content [W based on the weight of the binder resin in the photosensitive layer.
_ETM (wt%)] is a single-layer type electrophotographic photoreceptor satisfying the relationship of the formula (A) and the formula (B), and has a high sensitivity, extremely high isoper resistance, and a contained hole transport agent. It was found that the electron transport agent was extremely difficult to elute into Isopar.

Formula (A): 0.6 ≦ W _HTM / W _ETM ≦ 1.0 Formula (B): 0.6 ≦ (W _HTM + W _ETM ) /100≦1.0

Further, a stilbene derivative represented by the general formula (1) or (2) as a hole transporting agent (Claim 2),
Alternatively, a naphthoquinone derivative represented by the general formula (3) as an electron transporting agent (Claim 3), or a polyester resin represented by a general formula (4), (5) or (6) as a binder resin (Claim 4) The fact that sensitivity and isopar resistance are further improved by containing is found, and the present invention has been completed.

[0015]

DESCRIPTION OF THE PREFERRED EMBODIMENTS Electrophotographic photoreceptors are classified into a single-layer type and a laminated type as described above, and the single-layer type includes a positively-charged type and a negatively-charged type. The electrophotographic photoreceptor of the present invention relates to a single-layer type electrophotographic photoreceptor, and is particularly excellent in isoper resistance, so that it can be used in an image forming apparatus using the above-mentioned wet developing method.

The single-layer type electrophotographic photoreceptor has a single photosensitive layer provided on a conductive substrate. This photosensitive layer is formed by dissolving or dispersing a charge generating agent, a hole transporting agent, an electron transporting agent, a binder resin, and the like in an appropriate solvent, applying the obtained coating solution on a conductive substrate, and drying. You.

Next, various materials used for the single-layer type electrophotographic photosensitive member of the present invention will be described in detail.

<Charge Generating Agent> Examples of the charge generating agent used in the single-layer type electrophotographic photoreceptor of the present invention include various phthalocyanine pigments such as X-type metal-free phthalocyanine and oxotitanyl phthalocyanine, and polycyclic naphthoquinone pigments.
Azo pigments, perylene pigments, indigo pigments, quinacridone pigments, azurenium salt pigments, squarylium pigments, cyanine pigments, pyrylium dyes, thiopyrylium dyes, xanthene dyes, naphthoquinone immun dyes, triphenylmethane dyes, styryl dyes, selenium, tellurium, amorphous silicon, Cadmium sulfide and the like can be mentioned, and they can be used alone or as a blend of two or more.

The charge generating agent is used in an amount of 0.1 to 50% by weight, and more preferably 0.5 to 30% by weight, based on the weight of the binder resin.
It is preferable to include them.

<Hole transport agent> The hole transport agent used in the single-layer type electrophotographic photosensitive member of the present invention includes, for example, 2,5.
Oxadiazole compounds such as -di (4-methylaminophenyl) -1,3,4-oxadiazole, styryl compounds such as 9-4 (-diethylaminostyryl) anthracene, carbazole compounds such as polyvinylcarbazole , Organic polysilane compounds, pyrazoline compounds such as 1-phenyl-3 (p-dimethylaminophenyl) pyrazoline, hydrazone compounds, triphenylamine compounds, indole compounds, oxazole compounds, isoxazole compounds, thiazole compounds And nitrogen-containing cyclic compounds such as thiadiazole-based compounds, imidazole-based compounds, pyrazole-based compounds, and triazole-based compounds. These can be used alone or as a blend of two or more.

However, the total content of the hole transporting agent used in the single-layer type electrophotographic photoreceptor of the present invention must satisfy the formulas (A) and (B) of claim 1 in order to satisfy the isoper resistance. ) Must be satisfied.

Formula (A): 0.6 ≦ W _HTM / W _ETM ≦ 1.0 Formula (B): 0.6 ≦ (W _HTM + W _ETM ) /100≦1.0 (W _HTM : Contains hole transport agent) Amount, W _ETM : electron transport agent content)

It is not clear why the formulas (A) and (B) satisfy the requirements of the isoper resistance, but the interaction between the hole transporting agent and the electron transporting agent and the total content are large in the isoper resistance. It is presumed to have an effect.

In order to further improve the isoper resistance and photosensitivity of the single-layer type electrophotographic photoreceptor of the present invention, the solubility of the hole transporting agent itself in isoper is small, and the hole transporting agent has a high content with a small content. Is preferred. As the hole transporting agent satisfying this condition, a stilbene derivative represented by the general formula (1) or (2) is particularly preferably used.

When the stilbene derivative is used as a hole transport agent, at least one stilbene derivative may be contained. That is, the hole transporting agent of the above example may be contained together with the stilbene derivative.

<Electron Transport Agent> Examples of the electron transport agent used in the single-layer type electrophotographic photoreceptor of the present invention include a paradiphenonaphthoquinone derivative, a benzonaphthoquinone derivative,
Naphthonaphthoquinone derivatives, tetracyanoethyl, tetracyanoquinodimethane, chloranil, bromoanil,
2,4,7-trinitro-9-fluorenone, 2,4,5,
7-tetranitro-9-fluorenone, 2,4,7-trinitro-9-dicyanomethylene fluorenone, 2,4,
Electron-withdrawing substances such as 5,7-tetranitroxanthone and 2,4,8-trinitrothioxanthone, or those obtained by polymerizing these electron-withdrawing substances, etc., may be used alone or by blending two or more kinds. Can be used.

However, the total content of the above-mentioned electron transporting agent used in the single-layer type electrophotographic photoreceptor of the present invention, as in the case of the hole transporting agent content, satisfies isoper resistance. It is necessary to satisfy the expressions (A) and (B) in the item 1.

In order to further improve the isoper resistance and photosensitivity of the single-layer type electrophotographic photoreceptor of the present invention, the solubility of the electron transporting agent itself in the isopar is small and small, as in the case of the hole transporting agent. It is preferable that the electron transport property is high in the content. As the electron transporting agent satisfying this condition, a naphthoquinone derivative represented by the general formula (3) of claim 3 is particularly preferably used.

When the naphthoquinone derivative is used as an electron transporting agent, it may be contained in at least one kind. That is, the electron transporting agent of the above example may be contained together with the naphthoquinone derivative.

The reason that the above-mentioned isoper resistance is further improved is that the charge transporting agent represented by the general formulas (1), (2) and (3) itself has low solubility in isoper.
In addition to having a high charge transporting property, the photosensitivity of the photoreceptor can be sufficiently ensured with a small content, and also a hole transporting agent represented by the general formula (1) or (2) and a general formula (3) The electron transport agent is a charge transport complex between both (CT co
plex), which may be difficult to elute into the isopar.

<Binder Resin> As the binder resin for dispersing the above components, various resins conventionally used in the photosensitive layer can be used. For example, styrene-butadiene copolymer, styrene-acrylonitrile copolymer, styrene-maleic acid copolymer, acrylic copolymer, styrene-acrylic acid copolymer, polyethylene, ethylene-vinyl acetate copolymer, chlorinated polyethylene , Polyvinyl chloride, polypropylene, ionomer, vinyl chloride-vinyl acetate copolymer, polyester, alkyd resin, polyamide, polyurethane, polycarbonate, polyarylate, polysulfone, diallyl phthalate resin, ketone resin, polyvinyl butyral resin, polyether resin, etc. Thermoplastic resins, silicone resins, epoxy resins, phenolic resins, urea resins, melamine resins, other cross-linkable thermosetting resins, resins such as epoxy acrylate, urethane-acrylate, and other photo-curable resins can be used. It is.

In order to further improve the isoper resistance of the single-layer type electrophotographic photoreceptor of the present invention, it is preferable that the polarity of the binder resin in which the charge transporting agent is molecularly dispersed is high. It is considered that since the polarity of the isoper is low, the higher the polarity of the binder resin is, the smaller the interaction between the photoreceptor surface and the isoper is, and the better the isoper resistance is. The binder resin that satisfies this condition is, in particular, a substantially linear polymer using at least one of the dihydroxy compounds represented by the general formula (4), (5) or (6) of claim 4. Certain polyester resins are preferably used.

When the above-mentioned polyester resin is used as the binder resin, it may be contained in at least one kind. That is, the binder resin of the above example may be contained together with the polyester resin by blending, copolymerization, or the like.

The weight of a polyester resin which is a substantially linear polymer using at least one of the dihydroxy compounds represented by the general formulas (4), (5) and (6), and the weight of the binder resin of the above example The average molecular weight is 5000-2
00000, more preferably 15,000 to 100,000. The higher the molecular weight, the lower the photoconductor production efficiency, and the lower the molecular weight, the lower the isopar resistance.

The electrophotographic photoreceptor of the present invention may contain, in addition to the above-mentioned components, various conventionally known additives such as an antioxidant, a radical scavenger, a single-sided additive as long as the electrophotographic properties are not adversely affected. Term quencher, deterioration inhibitor such as ultraviolet absorber, softener, plasticizer, surface modifier, extender, thickener,
A dispersion stabilizer, a wax, an acceptor, a donor and the like can be blended. Further, in order to improve the sensitivity of the photosensitive layer, a known sensitizer such as terphenyl, halonaphthonaphthoquinones, acenaphthylene and the like may be used in combination with the charge generator.

The thickness of the photosensitive layer in the single-layer type electrophotographic photosensitive member is 5 to 100 μm, preferably 10 to 50 μm.

In a single-layer type electrophotographic photosensitive member, a barrier layer may be formed between the conductive substrate and the photosensitive layer within a range that does not impair the characteristics of the photosensitive member.

As the conductive substrate on which the photosensitive layer is formed, various materials having conductive properties can be used.
For example, simple metals such as iron, aluminum, copper, tin, platinum, silver, vanadium, molybdenum, chromium, cadmium, titanium, nickel, palladium, indium, stainless steel, and brass, and plastic materials on which the above metals are deposited or laminated , Aluminum iodide, tin oxide,
Glass coated with indium oxide or the like can be given.

The conductive substrate may be in the form of a sheet, a drum, or the like, depending on the structure of the image forming apparatus to be used. The substrate itself has conductivity, or the surface of the substrate has a conductive wire. What is necessary is just to have the property. The conductive substrate preferably has a sufficient mechanical strength when used.

When the photosensitive layer is formed by a coating method, a hole transporting agent, a charge generating agent, an electron acceptor, a binder resin and the like described above together with a suitable solvent may be used in a known method.
For example, a dispersion may be prepared by dispersing and mixing using a roll mill, a ball mill, an attritor, a paint shaker, an ultrasonic disperser, or the like, and the dispersion may be applied by a known means and dried.

As the solvent for preparing the dispersion, various organic solvents can be used, for example, alcohols such as methanol, ethanol, isopropanol and butanol, and aliphatic solvents such as n-hexane, octane and cyclohexane. Hydrocarbons, aromatic hydrocarbons such as benzene, toluene, and xylene; halogenated hydrocarbons such as dichloromethane, dichloroethane, chloroform, carbon tetrachloride, and chlorobenzene; dimethyl ether, diethyl ether, tetrahydrofuran, ethylene glycol dimethyl ether, and diethylene glycol dimethyl ether. Ethers, ketones such as acetone, methyl ethyl ketone and cyclohexanone, esters such as ethyl acetate and methyl acetate, dimethylformaldehyde, dimethylformamide, dimethyls Rufoxide and the like. These solvents are used alone or in combination of two or more.

Further, in order to improve the dispersibility of the hole transporting agent, the charge generating agent, the electron acceptor, and the smoothness of the photosensitive layer surface,
Surfactants, leveling agents and the like may be used.

[0043]

The present invention will be described below with reference to examples and comparative examples. Note that the following embodiments are merely examples embodying the present invention, and do not limit the technical scope of the present invention.

Examples 1 to 7, Comparative Examples 1 to 21

X-type metal-free phthalocyanine (CGM) 4 parts by weight as a charge generating material, a hole transporting agent (HTM1) represented by the general formula (1), an electron transporting agent (ETM1) represented by the general formula (3), and A polyester resin having a weight average molecular weight of 20,000 containing a dihydroxy compound represented by the general formula (5) as a binder resin (1,1-bis [4
-(2-Hydroxyethoxy) phenyl] -cyclohexane and 2,6-naphthalenedicarboxylic acid copolymer, mol
A copolymerization ratio of 1: 1, 100 parts by weight of Resin 1) and 800 parts by weight of tetrahydrofuran were mixed in a ball mill for 24 hours.
After dispersing or dissolving for a time, a coating solution for a single-layer type photosensitive layer was prepared. Then, this coating solution is applied on an aluminum tube as a support by a dip coating method.
Drying with hot air at 30 ° C. for 30 minutes was performed to produce a single-layer type photoreceptor having a single photosensitive layer having a thickness of 25 μm.

The content of the hole transport agent (HTM1) and the electron transport agent (ETM) in Examples 1 to 7 and Comparative Examples 1 to 21 were measured.
The M1) content is shown in Table 1. At the same time, the calculated values of the equations (A) and (B) are also shown.

[0047]

Embedded image (CGM)

[0048]

Embedded image (HTM1)

[0049]

Embedded image (ETM1)

[0050]

Embedded image (Resin1)

The characteristics of the electrophotographic photoreceptors of the above Examples and Comparative Examples were evaluated by performing the following tests.
Table 1 shows the evaluation results.

<Initial sensitivity test>
Using a drum sensitivity tester (trade name: Gentec Cynthia 30M) manufactured by E.C.), an applied voltage was applied to the electrophotographic photosensitive members of each of the examples and comparative examples, and the surfaces thereof were charged to +700 V.

Next, monochromatic light (half-width 20 nm, light intensity 20 μW) having a wavelength of 780 nm extracted from white light of a halogen lamp, which is an exposure light source of the tester, using a band-pass filter is applied to the charged photosensitive member. Was exposed (exposure time: 100 msec).

Then, 500 msec from the start of exposure.
The surface potential at the time when the elapsed time was measured as the post-exposure potential VL (V). That is, the smaller the potential after exposure, the higher the sensitivity of the photoconductor.

<Isopar Resistance Test> A single-layer type photoreceptor having a thickness of 25 μm was prepared on an aluminum vapor-deposited sheet in the same manner as described above using the above coating solution to obtain a test piece of 5 cm × 5 cm.

Next, the test piece was immersed in 100 g of Isopar G in a closed system at 25 ° C. for one week in a dark place. On the other hand, the hole transporting agent and the electron transporting agent in the UV measurement were forcibly dissolved in Isopar G at a predetermined concentration to prepare a concentration-absorbance calibration curve at each peak wavelength.

Then, UV measurement was performed on Isopar G in which the test piece was immersed, and the elution amount was calculated from the absorbance at the peak wavelength of the hole transporting agent and the electron transporting agent using the above calibration curve. The smaller the elution amount, the higher the isopar resistance of the photoconductor.

The appearance change of the photoreceptor surface was visually observed after drying of Isopar G.

[0059]

[Table 1]

From the results shown in Table 1, the HTM1 content and ET
When the M2 content satisfied the relations of the formulas (A) and (B), there was no change in the appearance of the surface of the photoreceptor, and the amount of the charge transport agent eluted was extremely small.

Examples 8 to 12

A stilbene derivative (HTM2, HTM3) represented by the general formula (1) or a stilbene derivative (HTM4, HTM) represented by the general formula (2) is used as a hole transporting agent.
A single-layer type photoreceptor was produced in the same manner as in Example 5, except that TM5 and HTM6) were used.

Comparative Examples 22 to 24 Single-layer type photoconductors were prepared in the same manner as in Example 5, except that HTM7, HTM8 and HTM9 were used as hole transporting agents.

Example 13 A single-layer type photoreceptor was produced in the same manner as in Example 5, except that a naphthoquinone derivative (ETM2) represented by the general formula (3) was used as an electron transporting agent.

Comparative Examples 25 to 27 Single-layer photoreceptors were prepared in the same manner as in Example 5, except that ETM3, ETM4 and ETM5 were used as electron transporting agents.

Comparative Examples 28 to 30 As the binder resin, a polycarbonate resin having a weight average molecular weight of 20,000 (Resin 2, Resin 3, R
A single-layer type photoreceptor was prepared in the same manner as in Example 5, except that esin4) was used alone.

[0067]

Embedded image (HTM2)

[0068]

Embedded image (HTM3)

[0069]

Embedded image (HTM4)

[0070]

Embedded image (HTM5)

[0071]

Embedded image (HTM6)

[0072]

Embedded image (HTM7)

[0073]

Embedded image (HTM8)

[0074]

Embedded image (HTM9)

[0075]

Embedded image (ETM2)

[0076]

Embedded image (ETM3)

[0077]

Embedded image (ETM4)

[0078]

Embedded image (ETM5)

[0079]

Embedded image (Resin2)

[0080]

Embedded image (Resin3)

[0081]

Embedded image (Resin4)

With respect to the electrophotographic photoreceptors of the above Examples and Comparative Examples, the above-described tests were performed to evaluate the characteristics.
Table 2 shows the evaluation results.

[0083]

[Table 2]

From the results shown in Table 2, the stilbene derivative represented by the general formula (1) or (2) as the hole transporting agent, the naphthoquinone derivative represented by the general formula (3) as the electron transporting agent, and the general formula (5) as the binder resin The use of a polyester resin containing a dihydroxy compound represented by the formula (1) further improved the isopar resistance.

[0085]

The single-layer type electrophotographic photoreceptor of the present invention does not undergo overcoating, has no change in the appearance of the photoreceptor surface even when immersed in an isoper, and has excellent isoper resistance (to the isopar of the charge transport agent). Is extremely low), so that the cost is low and application to an image forming apparatus using a wet development method is possible.

Claims (4)

[Claims] 1. A photosensitive layer comprising at least a charge generating agent, a hole transporting agent, an electron transporting agent and a binder resin is formed on a conductive substrate, and the content of the hole transporting agent is based on the weight of the binder resin in the photosensitive layer. [W _HTM (wt%)]
And a single-layer electrophotographic photoreceptor having an electron transporting agent content [W _ETM (wt%)] satisfying the relationship of the formulas (A) and (B). Formula (A): 0.6 ≦ W _HTM / W _ETM ≦ 1.0 Formula (B): 0.6 ≦ (W _HTM + W _ETM) /100≦1.0 2. A stilbene derivative represented by the general formula (1) or (2) as a hole transporting agent.
The single-layer type electrophotographic photoreceptor according to the above. General formula (1): General formula (2): (In the general formulas (1) and (2), R ¹ and R ³ are the same or different and each may represent an alkyl group which may have a substituent, an aryl group which may have a substituent, Represents an aralkyl group or an alkoxy group which may have R ² and R ⁴ are the same or different and each represents a hydrogen atom or an alkyl group or an alkoxy group which may have a substituent, provided that R ² and When the substitution position of R ⁴ is para, R ² and R ⁴ are hydrogen atoms.) 3. The single-layer type electrophotographic photoreceptor according to claim 1, which contains a naphthoquinone derivative represented by the general formula (3) as an electron transporting agent. General formula (3): (In the general formula (3), R ⁵ represents a halogen atom, an optionally substituted alkyl group or an aryl group, R ⁶ represents an optionally substituted alkyl group or an aryl group,
Or a group: -OR ^6a . R ^6a represents an alkyl group or an aryl group which may have a substituent. ) 4. A binder resin having the general formula (4):
The single-layer type electrophotographic photoreceptor according to claim 1, comprising a polyester resin which is a substantially linear polymer using at least one of the dihydroxy compounds represented by (5) or (6). General formula (4): General formula (5): General formula (6): (In general formulas (4), (5) and (6), R ⁷
Is an alkylene group having 2 to 4 carbon atoms, R ⁸ , R ⁹ , R ¹⁰ and R
¹¹ is the same or different and represents a hydrogen atom, an alkyl group having 1 to 4 carbon atoms, an aryl group or an aralkyl group. In the general formula (5), n is an integer of 2 or more. In the general formula (6), R ¹² and R ¹³ are the same or different and represent an alkyl group having 1 to 10 carbon atoms. )