CN113004792A - Bendable hardening dune buggy/automobile PC wind shield and preparation method thereof - Google Patents
Bendable hardening dune buggy/automobile PC wind shield and preparation method thereof Download PDFInfo
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
- C09D183/00—Coating compositions based on macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon, with or without sulfur, nitrogen, oxygen, or carbon only; Coating compositions based on derivatives of such polymers
- C09D183/04—Polysiloxanes
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- C08J7/00—Chemical treatment or coating of shaped articles made of macromolecular substances
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- C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
- C09D7/00—Features of coating compositions, not provided for in group C09D5/00; Processes for incorporating ingredients in coating compositions
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- C08J2483/00—Characterised by the use of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon with or without sulfur, nitrogen, oxygen, or carbon only; Derivatives of such polymers
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- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
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Abstract
The invention relates to a bendable hardening dune buggy/automobile PC wind shield, wherein a PC plate comprises a base body and a hardening layer. The hardening layer is composed of the following raw materials in parts by weight: 25-35 parts of organic silicon resin hardening liquid; 20-30 parts of melamine formaldehyde resin; 5-30 parts of vinyl MQ silicon resin; 3-5 parts of azodiisodiacid butyl methyl ester; 70-80 parts of ethanol. The invention also relates to a preparation method of the PC board. The bending-hardening PC wind deflector prepared by the invention has the advantages of high toughness, high surface hardness and good ageing resistance.
Description
Technical Field
The invention belongs to the technical field of PC (polycarbonate) plate materials, and particularly relates to a bendable hardened PC wind shield and a preparation method thereof.
Background
The PC board is also called a polycarbonate board, and is often used for a wind shield of a beach vehicle due to its excellent rigidity and toughness balance, ultra-high transparency, good dimensional stability, and the like. However, the polycarbonate has low surface hardness, the measured pencil hardness is generally 3B-2B, the wear resistance is low, and the polycarbonate cannot be applied to the environment with large wind sand in outdoor sand beach.
In the prior art, the surface hardness of the PC board is improved by coating a UV curing agent on the surface of the PC board of the dune buggy, but after the PC board is cured by adopting the UV curing liquid, the transparency and the toughness of the PC board are reduced to some extent, so that the PC board is not beneficial to bending processing; moreover, the hardness of the PC board after UV curing can only reach HB, and the application of the PC board in outdoor wind and sand environments is still difficult to meet.
The invention aims to overcome the defects of the prior art and develops a bendable hardening PC wind shield, and the PC wind shield has good toughness, high surface hardness and good light transmission and ageing resistance. In addition, the invention also provides a preparation method of the material.
Disclosure of Invention
In order to overcome the defects in the prior art, the first object of the invention is to provide a bendable hardening PC wind screen, wherein the PC board comprises a substrate and hardening layers, the hardening layers are distributed on the upper surface and the lower surface of the substrate, and the hardening layers are composed of the following components in parts by weight:
the organic silicon resin hardening liquid comprises the following components in parts by weight:
the silicon-titanium dispersion liquid comprises the following components in parts by weight:
3-10 parts of nano silicon dioxide;
0.5-1 part by weight of nano titanium dioxide;
10-15 parts of ethanol.
Preferably, the particle size of the nano silicon dioxide is 30-50nm, and the particle size of the nano titanium dioxide is 40-60 nm.
The invention also provides a preparation method of the bendable hardening PC wind shield, which comprises the following steps:
s1, preparing the components of the hardened layer according to the weight parts, and mixing and stirring for 1-2h to obtain hardened layer hardening liquid;
and S2, spraying the hardening liquid obtained in the step S1 on the upper surface and the lower surface of the PC board matrix, and naturally drying to form the PC board hardening layer on the upper surface and the lower surface of the PC board matrix, thereby finally obtaining the PC wind shield.
The silicone resin hardening liquid in the hardened layer may be prepared by:
mixing 15-20 parts by weight of silicon-titanium dispersion liquid, 3-8 parts by weight of acrylic acid, 3-8 parts by weight of tricarboxymethylpropane triacrylate and 1-5 parts by weight of deionized water, stirring for 30-40min at 70-80 ℃, adding 0.1-0.3 part by weight of hydroxypropyl methyl cellulose, and continuously stirring for 6.5-7.5h to obtain the organic silicon resin hardening liquid.
The silicon-titanium dispersion liquid in the silicone resin hardening liquid can be prepared by the following method:
mixing 3-10 parts by weight of nano silicon dioxide, 0.5-1 part by weight of nano titanium dioxide and 10-15 parts by weight of ethanol, stirring at 70 ℃ for 25min to obtain nano silicon dioxide dispersion, adding 0.2-0.5 part by weight of organosilane coupling agent, carrying out ultrasonic treatment for 25-30min, and cooling to obtain silicon-titanium dispersion.
Preferably, the organosilane coupling agent in the preparation method of the silicon-titanium dispersion liquid is one or more of vinyltrimethoxysilane, vinyltriethoxysilane and vinyltris (beta-methoxyethoxy) silane.
Preferably, the stirring speed of step S1 is 600-700r/min, and the stirring temperature is 25-35 ℃.
Preferably, the spraying temperature of the step S2 is 25-50 ℃.
Preferably, the step S2 can be repeated 1-2 times to form 1-3 hardened layers on the surface of the PC board substrate, so as to increase the hardness of the PC board.
Preferably, the drying manner in step S2 further includes low-temperature hot air drying, wherein the drying temperature is 40-50 ℃.
Compared with the prior art, the invention has the beneficial effects that:
the PC wind shield capable of being bent and hardened formed by the method has good toughness and stronger notch impact strength; the surface hardness is high, and the pencil hardness is HB-H; the light transmittance is good, and the visible light transmittance reaches more than 90%; easy to process and is suitable for manufacturing the wind shield of sightseeing vehicles and dune buggy.
The foregoing description is only an overview of the technical solutions of the present invention, and in order to make the technical solutions of the present invention more clearly understood and to implement them in accordance with the contents of the description, the following detailed description is given with reference to the preferred embodiments of the present invention and the accompanying drawings. Specific embodiments of the present invention are given in detail by the following examples.
Drawings
The accompanying drawings, which are included to provide a further understanding of the invention and are incorporated in and constitute a part of this application, illustrate embodiment(s) of the invention and together with the description serve to explain the invention without limiting the invention. In the drawings:
fig. 1 is a schematic diagram of the basic structure of the present invention.
FIG. 2 is a schematic structural diagram of the present invention, in which 2 hardened layers are formed on the upper and lower surfaces, respectively, and then the PC board is bent.
Detailed Description
In order to facilitate understanding of the present invention, the following further description is provided with reference to the accompanying drawings and embodiments, and it is to be noted that any combination of the embodiments or technical features described below can form a new embodiment without conflict.
A bendable PC board, as shown in FIG. 1, the PC board 100 comprises a substrate 10 and a hardened layer 11, wherein the substrate 10 is made of the following components in parts by weight:
80-120 parts by weight of polycarbonate;
3-10 parts of a toughening agent;
0.5 to 2 weight portions of antioxidant.
The hardened layer 11 consists of the following components in parts by weight:
the silicone resin hardening liquid in the hardened layer 11 can be prepared by the following steps:
mixing 15-20 parts by weight of silicon-titanium dispersion liquid, 3-8 parts by weight of acrylic acid, 3-8 parts by weight of tricarboxymethylpropane triacrylate and 1-5 parts by weight of deionized water, stirring for 30-40min at 70-80 ℃, adding 0.1-0.3 part by weight of hydroxypropyl methyl cellulose, and continuously stirring for 6.5-7.5h to obtain the organic silicon resin hardening liquid.
The silicon-titanium dispersion liquid in the silicone resin hardening liquid can be prepared by the following method:
mixing 3-10 parts by weight of nano silicon dioxide, 0.5-1 part by weight of nano titanium dioxide and 10-15 parts by weight of ethanol, stirring at 70 ℃ for 25min to obtain nano silicon dioxide dispersion, adding 0.2-0.5 part by weight of vinyl trimethoxy silane, performing ultrasonic treatment for 25-30min, and cooling to obtain silicon-titanium dispersion. The flame retardance of the PC board is improved by adding the melamine formaldehyde resin into the hardened layer of the PC board.
In some embodiments, the vinyltrimethylsilane in the silicon titanium dispersion is replaced with one or more of vinyltriethoxysilane or vinyltris (. beta. -methoxyethoxy) silane.
According to the invention, the vinyl MQ silicon resin and the azodiisodiacid butyl methyl ester are added into the PC plate hardened layer 11, and the vinyl MQ silicon resin and the azodiisodiacid butyl methyl ester have synergistic effect, so that the viscosity of the hardened layer can be effectively improved, and the adhesive force of the hardened layer on the PC plate is improved.
The dibutyltin dilaurate is added into the PC board hardened layer 11, so that the drying temperature can be effectively reduced, the PC hardened layer is dried under normal-temperature or low-temperature hot air, and the energy consumption is reduced; meanwhile, the dibutyltin dilaurate can improve the thermal stability of the PC board.
By adding the nano titanium dioxide into the PC board hardened layer 11, ultraviolet light is effectively absorbed, the anti-aging capability of the PC board is improved, the PC board is prevented from yellowing, and the service life of the PC board is prolonged.
By adding the nano titanium dioxide and the silicon dioxide with the same particle size, the reduction of transparency in the hardening process of the PC board can be effectively avoided. The nanometer silicon dioxide and the titanium dioxide are matched, and can be uniformly dispersed in the hardened layer, so that the appearance visual effect and the hardness of the hardened layer are improved. The nano titanium dioxide has large specific surface area and good dispersibility in an organic phase system, can effectively scatter and absorb ultraviolet light, improves the ageing resistance of the PC board in severe environment, and simultaneously, the titanium dioxide and the silicon dioxide with the same particle size cause low visible light scattering degree and avoid the reduction of the transparency of the PC board.
A preparation method of a bendable hardening PC wind shield comprises the following steps:
s1, preparing the components of the hardened layer 11 according to the parts by weight, and mixing and stirring for 1-2 h; the stirring speed is 600-700r/min, the stirring temperature is 25-35 ℃, and the hardening layer hardening liquid is prepared.
And S2, spraying the hardening liquid obtained in the step S1 on the upper surface and the lower surface of the PC board matrix 10, wherein the spraying temperature is 25-50 ℃, and naturally drying or drying by low-temperature hot air at 40-50 ℃ to coat the surface of the PC board to form a PC board hardening layer, so that the PC wind shield is finally prepared.
The invention adopts the spraying method to form the hardened layers on the upper surface and the lower surface of the matrix, has simple operation and high efficiency and is suitable for mass production. By controlling the spraying temperature, the formation of a uniform hardened layer is ensured, and the hardness of the hardened layer is also ensured.
Step S2 is performed by low-temperature hot air, which can significantly increase the drying speed and is less restricted by external conditions than natural drying.
In some embodiments, step S2 is repeated 1-2 times and different spraying temperatures are used to form 1-2 layers of different thicknesses of hardened layers on the surface of the PC board substrate. Compare with forming one deck sclerosis layer, the sclerosis layer that two-layer thickness differs can guarantee that the PC board has good toughness, is favorable to processing, is favorable to promoting the surface hardness of PC board again. Taking the case of forming two hardened layers on the upper and lower surfaces, as shown in fig. 2, after bending the PC board 100, the hardened layers 11 and 12 are formed on the upper surface of the PC board 100, wherein the hardened layers are gradually thinned from the inner layer close to the substrate to the outer layer, and the thickness of the hardened layer 11 is greater than that of the hardened layer 12, which is achieved by changing the spraying temperature, i.e., when step S2 is performed and repeated, the spraying temperature is sequentially increased, resulting in the thickness of the hardened layer being gradually decreased. In contrast, the lower surface of the PC board forms a hardened layer gradually thickened from the inner layer close to the substrate to the outer layer, i.e., the hardened layer 13 of the lower surface of the PC board has a smaller thickness than the hardened layer 14. Through the thickness that changes the sclerosis layer, be favorable to changing the toughness on every layer of sclerosis layer, promptly in the PC board, the more big sclerosis layer of stress that receives in the bending process, thickness is thinner more, and toughness is better, is favorable to processing more. In addition, compare in different hardened layer of different material formation, adopt the same material of component to form the hardened layer that toughness is different, van der waals' force between every layer of hardened layer is bigger, is favorable to adhering to each other between every layer of hardened layer, and the in-process of bending is difficult to form the interlayer between the layer and slides.
Example one
A PC wind shield capable of being bent and hardened comprises a base body and is composed of the following components in parts by weight:
80 parts by weight of polycarbonate;
3 parts of a toughening agent;
0.5 part of antioxidant.
The hardening layer consists of the following components in parts by weight:
the silicone resin hardening liquid in the hardened layer may be prepared by:
mixing 15 parts by weight of silicon-titanium dispersion liquid, 3 parts by weight of acrylic acid, 3 parts by weight of tricarboxymethylpropane triacrylate and 1 part by weight of deionized water, stirring for 30min at 70 ℃, adding 0.1 part by weight of hydroxypropyl methylcellulose, and continuously stirring for 6.5h to obtain the organic silicon resin hardening liquid.
The silicon-titanium dispersion liquid in the silicone resin hardening liquid can be prepared by the following method:
mixing 3 parts by weight of nano silicon dioxide, 0.5 part by weight of nano titanium dioxide and 10 parts by weight of ethanol, stirring at 70 ℃ for 25min to obtain nano silicon dioxide dispersion, adding 0.5 part by weight of vinyl trimethoxy silane, carrying out ultrasonic treatment for 30min, and cooling to obtain silicon-titanium dispersion.
A preparation method of a bendable hardening PC wind shield comprises the following steps:
s1, preparing raw materials of the hardened layer according to the weight parts, and mixing and stirring for 1 hour; stirring at 600r/min and 25 deg.C to obtain hardened layer hardening liquid.
And S2, spraying the hardening liquid obtained in the step S1 on the upper surface and the lower surface of the PC board substrate 10, wherein the spraying temperature of the upper surface and the spraying temperature of the lower surface are both 25 ℃, and naturally drying to coat the surface of the PC board to form a PC board hardening layer, thereby finally obtaining the PC wind shield.
Example two
A PC wind shield capable of being bent and hardened comprises a base body and is composed of the following components in parts by weight:
120 parts by weight of polycarbonate;
10 parts of a toughening agent;
and 2 parts of antioxidant.
The hardening layer consists of the following components in parts by weight:
the silicone resin hardening liquid in the hardened layer may be prepared by:
mixing 18 parts by weight of silicon-titanium dispersion liquid, 5 parts by weight of acrylic acid, 5 parts by weight of tricarboxymethylpropane triacrylate and 3 parts by weight of deionized water, stirring for 35min at 75 ℃, adding 0.3 part by weight of hydroxypropyl methylcellulose, and continuously stirring for 7h to obtain the organic silicon resin hardening liquid.
The silicon-titanium dispersion liquid in the silicone resin hardening liquid can be prepared by the following method:
mixing 10 parts by weight of nano silicon dioxide, 1 part by weight of nano titanium dioxide and 15 parts by weight of ethanol, stirring at 70 ℃ for 25min to obtain nano silicon dioxide dispersion, adding 0.5 part by weight of vinyl triethoxysilane, performing ultrasonic treatment for 30min, and cooling to obtain silicon-titanium dispersion.
A preparation method of a bendable hardening PC wind shield comprises the following steps:
s1, preparing the components of the hardened layer according to the parts by weight, and mixing and stirring for 2 hours; stirring speed is 700r/min, stirring temperature is 35 ℃, and hardening layer hardening liquid is prepared.
And S2, spraying the hardening liquid obtained in the step S1 on the upper surface and the lower surface of the PC board substrate 10, wherein the spraying temperature of the upper surface is 30 ℃, the spraying temperature of the lower surface is 40 ℃, and the PC board hardening layer is formed by coating the surface of the PC board after low-temperature hot air drying at 40 ℃.
In this embodiment, step S2 is repeated 1 time to form 2 hardened layers on the surface of the PC board substrate. Unlike the first step S2, in the second spraying, the upper surface spraying temperature was 40 ℃ and the lower surface spraying temperature was 30 ℃.
EXAMPLE III
A PC wind shield capable of being bent and hardened comprises a base body and is composed of the following components in parts by weight:
100 parts by weight of polycarbonate;
5 parts of a toughening agent;
1 part of antioxidant.
The hardening layer consists of the following components in parts by weight:
the silicone resin hardening liquid in the hardened layer may be prepared by:
mixing 18 parts by weight of silicon-titanium dispersion liquid, 4 parts by weight of acrylic acid, 3 parts by weight of tricarboxymethylpropane triacrylate and 3 parts by weight of deionized water, stirring for 35min at 75 ℃, adding 0.2 part by weight of hydroxypropyl methylcellulose, and continuously stirring for 7.5h to obtain the organic silicon resin hardening liquid.
The silicon-titanium dispersion liquid in the silicone resin hardening liquid can be prepared by the following method:
mixing 7 parts by weight of nano silicon dioxide, 0.8 part by weight of nano titanium dioxide and 13 parts by weight of ethanol, stirring at 70 ℃ for 25min to obtain nano silicon dioxide dispersion, simultaneously adding 0.2 part by weight of vinyltrimethoxysilane and 0.2 part by weight of vinyltris (beta-methoxyethoxy) silane, carrying out ultrasonic treatment for 28min, and cooling to obtain silicon-titanium dispersion.
A preparation method of a bendable hardening PC wind shield comprises the following steps:
s1, preparing raw materials of the hardened layer according to the weight parts, and mixing and stirring for 1.5 h; stirring at 650r/min and 30 deg.C to obtain hardened layer hardening liquid.
And S2, spraying the hardening liquid obtained in the step S1 on the upper surface and the lower surface of the PC board substrate 10, wherein the spraying temperature of the upper surface is 25 ℃, the spraying temperature of the lower surface is 30 ℃, and the PC board hardening layer is formed by coating the surface of the PC board after low-temperature hot air drying at 50 ℃.
Comparative example 1
In contrast to example one, the PC board prepared in comparative example one has only a substrate and no hardened layer.
Comparative example No. two
3 parts by weight of acrylic acid was reduced based on example one.
Comparative example No. three
3 parts by weight of methyl azodiisodicarboxylate were reduced on the basis of example one.
Comparative example No. four
15 parts by weight of the silicon-titanium dispersion was reduced based on example one.
Comparative example five
0.5 weight part of nano titanium dioxide is reduced on the basis of the first embodiment.
Comparative example six
Compared with the first embodiment, the sixth embodiment adopts the prior art to improve the surface hardness of the PC board, that is, the surface of the PC board substrate is coated with the UV curing liquid thiol curing agent for curing so as to improve the surface hardness of the PC board.
Comparative example seven
Compared with the second example, the seventh comparative example adopts a spraying method to form a PC board hardened layer, and the thickness of the formed hardened layer is consistent with that of the two hardened layers formed in the second example.
The test result method comprises the following steps:
1. and (3) testing pencil hardness: a pencil hardness tester is adopted to test according to ASTM D3363, and the weight is 500 g;
IZOD notched impact strength test: 3.2mm thick specimens according to ASTM D256.
3. And (3) transparency test: testing by adopting a light transmission tester according to ASTM D1003, wherein the thickness of the sample is 4 mm;
4. aging resistance: and (5) directly irradiating the surface of the product by using strong ultraviolet rays, and observing the yellowing degree of the product.
And (3) testing results:
by comparing the first to third examples with the first comparative example, the surface hardness and the ultraviolet resistance of the PC board are improved by coating the hardened layer on the substrate; by comparing the first to third embodiments with the second embodiment, it can be seen that the bending strength of the PC board is ensured by adding the acrylic acid, and the PC board has good toughness; by comparing the first to third examples and the third comparative example, it can be known that the adhesion degree of the hardening liquid on the substrate is improved under the synergistic effect of the vinyl MQ silicon resin and the azodiisodiacid butyl methyl ester; by comparing the first to third examples and the fourth to fifth examples, it can be seen that the hardened layer has higher hardness, light transmittance and ultraviolet resistance intensity by adding the nano titanium dioxide and the nano silicon dioxide; by comparing the first to third examples and the sixth example, it can be seen that the present invention can effectively improve the surface hardness of the PC board compared to the prior art. By comparing the second and seventh examples, it can be seen that the invention adopts a two-time coating method to form two hardened layers on the surface of the substrate, which can effectively improve the surface hardness of the PC board on the premise of ensuring the toughness of the PC board.
The foregoing is merely a preferred embodiment of the invention and is not intended to limit the invention in any manner; those skilled in the art can easily practice the present invention in light of the foregoing description and accompanying drawings; however, those skilled in the art should appreciate that they can readily use the disclosed conception and specific embodiments as a basis for designing or modifying other structures for carrying out the same purposes of the present invention without departing from the scope of the invention as defined by the appended claims; meanwhile, any changes, modifications, and evolutions of the equivalent changes of the above embodiments according to the actual techniques of the present invention are still within the protection scope of the technical solution of the present invention.
Claims (10)
1. A PC wind screen capable of bending and hardening is characterized in that: the PC board includes base member and sclerosis layer, the sclerosis layer distribute in surface about the base member, the sclerosis layer comprises the component of following parts by weight:
2. a flexurally stiff PC wind deflector as claimed in claim 1, wherein: the organic silicon resin hardening liquid comprises the following components in parts by weight:
3. a flexurally stiff PC wind deflector as claimed in claim 2, wherein: the silicon-titanium dispersion liquid comprises the following components in parts by weight:
3-10 parts of nano silicon dioxide;
0.5-1 part by weight of nano titanium dioxide;
10-15 parts of ethanol.
4. A flexurally stiff PC wind deflector as claimed in claim 3, wherein: the particle size of the nano silicon dioxide is 30-50 nm.
5. A flexurally stiff PC wind deflector as claimed in claim 3, wherein: the particle size of the nano titanium dioxide is 40-60 nm.
6. A method of making a flexurally hardened PC wind deflector as claimed in claim 1, comprising the steps of:
s1, preparing the components of the hardened layer according to the weight parts, and mixing and stirring for 1-2h to obtain hardened layer hardening liquid;
and S2, spraying the hardening liquid obtained in the step S1 on the upper surface and the lower surface of the PC board matrix, and naturally drying to form the PC board hardening layer on the upper surface and the lower surface of the PC board matrix, thereby finally obtaining the PC wind shield.
7. A method of making a flexurally rigid PC wind deflector as claimed in claim 6, wherein the method comprises the steps of: the stirring speed in the step S1 is 600-700r/min, and the stirring temperature is 25-35 ℃.
8. A method of making a flexurally hardened PC wind deflector according to claim 6, wherein: step S2 is repeated for 1-2 times to form 1-2 hardened layers on the surface of the PC board substrate.
9. A method of making a flexurally hardened PC wind deflector according to claim 6, wherein: the temperature of the spraying in step S2 is 25-40 ℃.
10. A method of making a flexurally hardened PC wind deflector according to claim 6, wherein: the drying method in step S2 further includes low-temperature hot air drying at 40-50 ℃.
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| CN109355968A (en) * | 2018-10-11 | 2019-02-19 | 广东福美新材料科技有限公司 | A kind of wearable environment protection type impregnated paper and preparation method thereof |
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2021
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| WO2015186717A1 (en) * | 2014-06-02 | 2015-12-10 | Jnc株式会社 | Hard coating agent, cured film, molded object |
| CN107188828A (en) * | 2017-05-19 | 2017-09-22 | 黄叶芳 | A kind of preparation method of azo-bis-isobutyrate |
| CN109355968A (en) * | 2018-10-11 | 2019-02-19 | 广东福美新材料科技有限公司 | A kind of wearable environment protection type impregnated paper and preparation method thereof |
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