JP4653644B2 - Method for producing aluminum electrode foil for electrolytic capacitor - Google Patents

Method for producing aluminum electrode foil for electrolytic capacitor Download PDF

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JP4653644B2
JP4653644B2 JP2005338836A JP2005338836A JP4653644B2 JP 4653644 B2 JP4653644 B2 JP 4653644B2 JP 2005338836 A JP2005338836 A JP 2005338836A JP 2005338836 A JP2005338836 A JP 2005338836A JP 4653644 B2 JP4653644 B2 JP 4653644B2
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etching
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茂直 新田
清志 成沢
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Nichicon Corp
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本発明は、電解コンデンサ用アルミニウム電極箔の製造方法に関するものである。さらに詳しくは、交流エッチングを用いたアルミニウム箔に対するエッチング技術に関するものである。   The present invention relates to a method for producing an aluminum electrode foil for electrolytic capacitors. More specifically, the present invention relates to an etching technique for aluminum foil using AC etching.

電子機器の小形化に伴い、電解コンデンサの小形化が望まれており、このような要求に対応するには、電解コンデンサ用アルミニウム電極箔の単位面積当たりの静電容量を高める必要がある。
このような電解コンデンサ用アルミニウム電極箔は、アルミニウム箔に交流エッチングを施して表面を粗面化してなるものであり、かかる交流エッチングについては、従来より、原料となるアルミニウム箔の組成、エッチング液の組成、中間処理等が検討されている。
また、交流エッチングに用いる交流電流の波形についても、初期において電流を最大電流値まで急峻に立ち上げる等の提案がなされている（例えば、特許文献１参照）。
特公昭６２−２１０７９公報 With downsizing of electronic devices, downsizing of electrolytic capacitors is desired, and in order to meet such demands, it is necessary to increase the capacitance per unit area of the aluminum electrode foil for electrolytic capacitors.
Such an aluminum electrode foil for an electrolytic capacitor is formed by subjecting an aluminum foil to AC etching to roughen the surface, and for such AC etching, the composition of an aluminum foil as a raw material and the etching solution have been conventionally used. Composition, intermediate treatment, etc. are being studied.
In addition, with regard to the waveform of the alternating current used for alternating current etching, proposals have been made such as steeply raising the current to the maximum current value in the initial stage (for example, see Patent Document 1).
Japanese Examined Patent Publication No. 62-21079

しかしながら、上記特許文献１に開示の技術のように、初期において電流を最大電流値まで急峻に立ち上げると、化学溶解性が低い状態にあるにもかかわらず、大きな電流が流れるため、箔表面の全体が溶解してしまい、静電容量を十分に高めることができないという問題がある。
また、アルミニウム箔に注入した電気量を増やしても、アルミニウム溶解量が多い割には静電容量が伸びないという問題がある。 However, as in the technique disclosed in Patent Document 1 described above, when the current is steeply raised to the maximum current value at the initial stage, a large current flows even though the chemical solubility is low. The whole melt | dissolves and there exists a problem that an electrostatic capacitance cannot fully be raised.
Further, there is a problem that even if the amount of electricity injected into the aluminum foil is increased, the capacitance does not increase for a large amount of aluminum dissolved.

以上の問題点に鑑みて、本発明の課題は、エッチングの際の交流波形を最適化することにより、静電容量をさらに向上することのできる電解コンデンサ用アルミニウム電極箔の製造方法を提供することにある。   In view of the above problems, an object of the present invention is to provide a method for producing an aluminum electrode foil for an electrolytic capacitor that can further improve the capacitance by optimizing the AC waveform during etching. It is in.

上記課題を解決するために、本発明では、エッチング液中でアルミニウム箔に交流電流を印加して表面を粗面化する電解コンデンサ用アルミニウム電極箔の製造方法において、前記交流電流は、初期において電流値が一定の第１の期間と、該第１の期間に続き、最大電流値が出現する第２の期間とを備えた電流波形を備え、前記電流波形における第１の期間の時間は１０ｍｓ以内であり、第１の期間における電流値は、前記最大電流値の０.１〜０．９倍であることを特徴とする電解コンデンサ用アルミニウム電極箔の製造方法である。   In order to solve the above-mentioned problems, in the present invention, in the method for producing an aluminum electrode foil for an electrolytic capacitor in which an alternating current is applied to an aluminum foil in an etching solution to roughen the surface, the alternating current is initially a current. A current waveform having a first period in which the value is constant and a second period in which the maximum current value appears following the first period, and the time of the first period in the current waveform is within 10 ms The current value in the first period is 0.1 to 0.9 times the maximum current value, and is a method for producing an aluminum electrode foil for electrolytic capacitors.

本発明において、前記第２の期間の電流波形が、最大電流値が出現する部分と、該部分に続く、電流値が一定または緩徐にゼロまで低下する部分とからなることを特徴とする電解コンデンサ用アルミニウム電極箔の製造方法である。   In the present invention, the current waveform in the second period includes a portion where the maximum current value appears, and a portion following the portion where the current value is constant or slowly decreases to zero. It is a manufacturing method of the aluminum electrode foil for water.

本発明において、前記エッチング液は、塩素イオンを含む水溶液であって、さらにリン酸イオン、硝酸イオン、硫酸イオンまたはシュウ酸イオンのうちの少なくとも１種を含んでいることが好ましい。   In the present invention, the etching solution is an aqueous solution containing chlorine ions, and preferably further contains at least one of phosphate ions, nitrate ions, sulfate ions, or oxalate ions.

本発明によれば、電流波形の初期には、所定期間、最大電流値より低い電流値でのエッチングが行われるため、電解エッチング（電気化学的な溶解）と、化学的な溶解とのバランスが改善され、高容量のエッチング箔を製造することができる。   According to the present invention, in the initial stage of the current waveform, etching is performed at a current value lower than the maximum current value for a predetermined period, so that the balance between electrolytic etching (electrochemical dissolution) and chemical dissolution is balanced. An improved and high capacity etching foil can be produced.

本発明に係る電解コンデンサ用アルミニウム電極箔の製造方法は、低圧用電極箔または陰極箔の製造に適したエッチング方法であり、エッチング液中でアルミニウム箔に交流電流を印加して表面を粗面化する。   The method for producing an aluminum electrode foil for an electrolytic capacitor according to the present invention is an etching method suitable for producing a low-voltage electrode foil or a cathode foil, and an AC current is applied to the aluminum foil in an etching solution to roughen the surface. To do.

本形態において、交流電流は、初期において電流値が一定の第１の期間と、この第１の期間に続き、最大電流値が出現する第２の期間とを備えた電流波形を備えており、電流波形における第１の期間の時間は１〜１０ｍｓであり、第１の期間における電流値は、前記最大電流値の０．１〜０．９倍である。
さらに、第２の期間の電流波形は、最大電流値が出現する部分と、該部分に続く、電流値が一定または緩徐に低下する部分とからなることが好ましい。
また、本形態において、エッチング液としては、塩素イオンを含む水溶液が用いられ、さらにリン酸イオン、硝酸イオン、硫酸イオンまたはシュウ酸イオンのうちの少なくとも１種を含んでいることが好ましい。 In the present embodiment, the alternating current has a current waveform having a first period in which the current value is constant in the initial stage and a second period in which the maximum current value appears following the first period, The time of the first period in the current waveform is 1 to 10 ms, and the current value in the first period is 0.1 to 0.9 times the maximum current value.
Furthermore, the current waveform in the second period preferably includes a portion where the maximum current value appears and a portion following the portion where the current value decreases constant or slowly.
In this embodiment, an aqueous solution containing chlorine ions is used as the etching solution, and it is preferable that the etching solution further contains at least one of phosphate ions, nitrate ions, sulfate ions, or oxalate ions.

また、電流波形において、そのもとになる波形については特に限定されず、三角波、方形波、台形波等から選ばれる。   In addition, the current waveform is not particularly limited, and is selected from a triangular wave, a square wave, a trapezoidal wave, and the like.

このように構成した製造方法によれば、電流波形の初期（第１の期間）には、所定期間、最大電流値より低い電流値でのエッチングが行われるため、第２の期間において最大電流値が流れる際、アルミニウム箔の表面近傍に塩素イオンが十分、濃縮された状態にある。このため、最大電流を印加した際に、アルミニウム箔は効率的に電解エッチングされるので、高容量のエッチング箔を製造することができる。   According to the manufacturing method configured as described above, the etching is performed at a current value lower than the maximum current value for a predetermined period at the initial stage (first period) of the current waveform. Is flowing, the chlorine ions are sufficiently concentrated near the surface of the aluminum foil. For this reason, when the maximum current is applied, the aluminum foil is efficiently electrolytically etched, so that a high-capacity etching foil can be manufactured.

以下、実施例に基づいて本発明をより詳細に説明する。図１〜４、図６は、本発明の実施例に係る交流電流の波形図を、図５、７は比較例に係る交流電流の波形図を示す。なお、図１〜７には、１波長分の波形を示してあり、横軸が時間で縦軸が電流値である。   Hereinafter, the present invention will be described in more detail based on examples. 1-4 and 6 show waveform diagrams of alternating current according to an embodiment of the present invention, and FIGS. 5 and 7 show waveform diagrams of alternating current according to a comparative example. 1 to 7 show waveforms for one wavelength, with the horizontal axis representing time and the vertical axis representing the current value.

また、以下に説明する実施例または比較例に係る製造方法に用いた交流電流の波形図番号、波形パラメータについて表１に示す。また、表１には、以下に説明する実施例および比較例に係る製造方法でエッチングして得た電解コンデンサ用アルミニウム電極箔を、耐電圧が２２Ｖとなる条件で化成した後の静電容量の測定結果も示してある。
なお、化成を行うにあたっては、エッチング後、純水で洗浄し、乾燥した。そして、リン酸水溶液で皮膜中の塩素を除去した後、リン酸アンモニウム水溶液にて化成を行った。 Table 1 shows the waveform diagram numbers and waveform parameters of the alternating current used in the manufacturing methods according to Examples and Comparative Examples described below. Table 1 shows the capacitance of the aluminum electrode foil for an electrolytic capacitor obtained by etching with the manufacturing methods according to the examples and comparative examples described below after the formation under the condition that the withstand voltage is 22V. The measurement results are also shown.
In addition, in performing chemical conversion, it wash | cleaned and dried with the pure water after the etching. And after removing the chlorine in a film | membrane with phosphoric acid aqueous solution, it formed with ammonium phosphate aqueous solution.

Figure 0004653644
Figure 0004653644

Figure 0004653644
Figure 0004653644

［実施例１−１〜１−１２］
本例では、純度９９．９％、厚さ１１０μｍのアルミニウム箔の硬質材を用い、塩酸１５ｗｔ％に硝酸を０．５ｗｔ％含むエッチング液（液温３０℃）で、平均電流密度０．１Ａ／ｃｍ２、電気量４０Ｃ／ｃｍ２でエッチングした。
交流電流の波形は、図１に示すように、三角波の波形になっており、初期において電流値が一定の第１の期間と、この第１の期間に続き、最大電流値が出現する第２の期間とを備えている（半周期１１〜２１０ｍｓ）。本例において、第１の期間の時間Ｔ、電流比Ｄ１／Ｄ２（Ｄ１＝第１の期間における電流値、Ｄ２＝最大電流値）については、表１に示すように、Ｔ＝１．０〜１０．０ｍｓ、Ｄ１／Ｄ２＝０．１〜０．９の範囲で複数の条件を設定し、エッチング箔を作製した。 [Examples 1-1 to 1-12]
In this example, an aluminum foil hard material having a purity of 99.9% and a thickness of 110 μm is used, and an etching solution (liquid temperature 30 ° C.) containing 15 wt% hydrochloric acid and 0.5 wt% nitric acid is used. Etching was performed with cm 2 and an electric quantity of 40 C / cm 2 .
As shown in FIG. 1, the waveform of the alternating current is a triangular waveform. The first period in which the current value is constant in the initial stage, and the second period in which the maximum current value appears following the first period. (Half period 11 to 210 ms). In this example, as shown in Table 1, the time T in the first period T and the current ratio D1 / D2 (D1 = current value in the first period, D2 = maximum current value) A plurality of conditions were set in a range of 10.0 ms and D1 / D2 = 0.1 to 0.9 to produce an etching foil.

（比較例１−１〜１−４）
Ｔ＝０．５、５．０、１５．０、Ｄ１／Ｄ２＝０．０５（比較例１−２）とした以外は、実施例１−１と同様のアルミニウム箔を用い、同様の条件でエッチングを行い、エッチング箔を作製した（比較例１−１、２、４）。また、比較例１−３として最大電流値が出現しないものについても、エッチング箔を作製した。 (Comparative Examples 1-1 to 1-4)
Except for T = 0.5, 5.0, 15.0, D1 / D2 = 0.05 (Comparative Example 1-2), the same aluminum foil as in Example 1-1 was used and under the same conditions. Etching was performed to produce an etching foil (Comparative Examples 1-1, 2, and 4). Moreover, the etching foil was produced also about the thing where the maximum electric current value does not appear as Comparative Example 1-3.

［実施例２−１〜２−１２］
交流電流の波形を、図２に示すように、方形波とした以外は、実施例１−１と同様のアルミニウム箔を用い、同様の条件でエッチングを行い、エッチング箔を作製した。 [Examples 2-1 to 2-12]
As shown in FIG. 2, except that the waveform of the alternating current was a square wave, the same aluminum foil as in Example 1-1 was used, and etching was performed under the same conditions to produce an etching foil.

（比較例２−１〜２−４）
Ｔ＝０．５、５．０、１５．０、Ｄ１／Ｄ２＝０．０５（比較例２−２）とした以外は実施例２−１と同様のアルミニウム箔を用い、同様の条件でエッチングを行い、エッチング箔を作製した。また、比較例２−３として最大電流値が出現しないものについても、エッチング箔を作製した。 (Comparative Examples 2-1 to 2-4)
Etching under the same conditions using the same aluminum foil as in Example 2-1, except that T = 0.5, 5.0, 15.0, D1 / D2 = 0.05 (Comparative Example 2-2) The etching foil was produced. Moreover, the etching foil was produced also about the thing which does not appear the maximum electric current value as Comparative Example 2-3.

［実施例３−１〜３−１２］
交流電流の波形を、図３に示すように、台形波とした以外は、実施例１−１と同様のアルミニウム箔を用い、同様の条件でエッチングを行い、エッチング箔を作製した。 [Examples 3-1 to 3-12]
As shown in FIG. 3, except that the waveform of the alternating current was a trapezoidal wave, the same aluminum foil as in Example 1-1 was used, and etching was performed under the same conditions to produce an etching foil.

（比較例３−１〜３−４）
Ｔ＝０．５、５．０、１５．０、Ｄ１／Ｄ２＝０．０５（比較例３−２）とした以外は実施例３−１と同様のアルミニウム箔を用い、同様の条件でエッチングを行い、エッチング箔を作製した。また、比較例３−３として最大電流値が出現しないものについても、エッチング箔を作製した。 (Comparative Examples 3-1 to 3-4)
Etching under the same conditions using the same aluminum foil as in Example 3-1, except that T = 0.5, 5.0, 15.0, D1 / D2 = 0.05 (Comparative Example 3-2) The etching foil was produced. Moreover, the etching foil was produced also about the thing which does not appear the maximum electric current value as Comparative Example 3-3.

［実施例４−１〜４−１２］
交流電流の波形は、図４に示すように、電流値が一定の第１の期間と、この第１の期間に続き、最大電流が出現する方形波部分および該部分に続く、電流値一定の方形波部分からなる第２の期間とした以外は、実施例１−１と同様のアルミニウム箔を用い、同様の条件でエッチングを行い、エッチング箔を作製した。 [Examples 4-1 to 4-12]
As shown in FIG. 4, the waveform of the alternating current includes a first period in which the current value is constant, a square wave portion in which the maximum current appears following the first period, and a constant current value that follows the part. Except for the second period consisting of a square wave portion, the same aluminum foil as in Example 1-1 was used, and etching was performed under the same conditions to produce an etching foil.

（比較例４−１〜４−４）
Ｔ＝０．５、５．０、１５．０、Ｄ１／Ｄ２＝０．０５（比較例４−２）とした以外は実施例４−１と同様のアルミニウム箔を用い、同様の条件でエッチングを行い、エッチング箔を作製した。また、比較例４−３として最大電流値が出現しないもの（図５）の条件についても、エッチング箔を作製した。 (Comparative Examples 4-1 to 4-4)
Etching under the same conditions as in Example 4-1, except that T = 0.5, 5.0, 15.0, D1 / D2 = 0.05 (Comparative Example 4-2) The etching foil was produced. Moreover, the etching foil was produced also about the conditions (FIG. 5) in which the maximum electric current value does not appear as Comparative Example 4-3.

［実施例５−１〜５−１２］
交流電流の波形は、図６に示すように、初期において電流値が一定の第１の期間と、この第１の期間に続き、最大電流が出現する方形波部分および該部分に続く、電流値が緩徐にゼロまで低下する部分からなる第２の期間とした以外は、実施例１−１と同様のアルミニウム箔を用い、同様の条件でエッチングを行い、エッチング箔を作製した。 [Examples 5-1 to 5-12]
As shown in FIG. 6, the waveform of the alternating current includes a first period in which the current value is constant in the initial stage, a square wave portion in which the maximum current appears following the first period, and a current value following the part. Etching was carried out under the same conditions using the same aluminum foil as in Example 1-1 except that the second period was composed of a portion that gradually decreased to zero.

（比較例５−１〜５−４）
Ｔ＝０．５、５．０、１５．０、Ｄ１／Ｄ２＝０．０５（比較例５−２）とした以外は、実施例５−１と同様のアルミニウム箔を用い、同様の条件でエッチングを行い、エッチング箔を作製した。また、比較例５−３として最大電流値が出現しないもの（図７）の条件についても、エッチング箔を作製した。 (Comparative Examples 5-1 to 5-4)
Except for T = 0.5, 5.0, 15.0, D1 / D2 = 0.05 (Comparative Example 5-2), the same aluminum foil as in Example 5-1 was used, under the same conditions. Etching was performed to produce an etching foil. Moreover, the etching foil was produced also about the conditions (FIG. 7) in which the maximum electric current value does not appear as Comparative Example 5-3.

［評価結果］
表１に示す結果から分かるように、エッチングに用いた交流電流において、本形態では、初期において電流値が一定の第１の期間と、該第１の期間に続き、最大電流値が出現する第２の期間とを備えた電流波形を備えたため、比較例に比較して静電容量が高い。
また、電流波形における第１の期間の時間は１０ｍｓ以内であり、当該第１の期間における電流値は、前記最大電流値の０．１〜０．９倍であれば、静電容量の改善効果がみられた。 [Evaluation results]
As can be seen from the results shown in Table 1, in the AC current used for etching, in the present embodiment, the first period in which the current value is constant in the initial stage and the maximum current value appears following the first period. Since the current waveform having the period of 2 is provided, the capacitance is higher than that of the comparative example.
In addition, if the time of the first period in the current waveform is within 10 ms and the current value in the first period is 0.1 to 0.9 times the maximum current value, the capacitance improving effect Was seen.

なお、上記実施例では、エッチング液に塩酸、硝酸を含む水溶液を用いたが、これに限定されるものではなく、これらに硫酸、シュウ酸を加えたもの、またはこれらの１種以上を含むもの等適宜用いることができる。   In the above embodiment, an aqueous solution containing hydrochloric acid and nitric acid was used as the etching solution, but the present invention is not limited to this, and those containing sulfuric acid and oxalic acid added thereto, or those containing one or more of these. Etc. can be used as appropriate.

本発明の実施例１−１〜１−１２に係る電解コンデンサ用アルミニウム電極箔のエッチングに用いた交流電流の波形図である。It is a wave form diagram of the alternating current used for the etching of the aluminum electrode foil for electrolytic capacitors which concerns on Examples 1-1 to 1-12 of this invention. 本発明の実施例２−１〜２−１２に係る電解コンデンサ用アルミニウム電極箔のエッチングに用いた交流電流の波形図である。It is a wave form diagram of the alternating current used for the etching of the aluminum electrode foil for electrolytic capacitors which concerns on Examples 2-1 to 2-12 of this invention. 本発明の実施例３−１〜３−１２に係る電解コンデンサ用アルミニウム電極箔のエッチングに用いた交流電流の波形図である。It is a wave form diagram of the alternating current used for the etching of the aluminum electrode foil for electrolytic capacitors which concerns on Examples 3-1 to 3-12 of this invention. 本発明の実施例４−１〜４−１２に係る電解コンデンサ用アルミニウム電極箔のエッチングに用いた交流電流の波形図である。It is a wave form diagram of the alternating current used for the etching of the aluminum electrode foil for electrolytic capacitors which concerns on Examples 4-1 to 4-12 of this invention. 本発明の比較例４−０に係る電解コンデンサ用アルミニウム電極箔のエッチングに用いた交流電流の波形図である。It is a wave form diagram of the alternating current used for the etching of the aluminum electrode foil for electrolytic capacitors which concerns on the comparative example 4-0 of this invention. 本発明の実施例５−１〜５−１２に係る電解コンデンサ用アルミニウム電極箔のエッチングに用いた交流電流の波形図である。It is a wave form diagram of the alternating current used for the etching of the aluminum electrode foil for electrolytic capacitors which concerns on Examples 5-1 to 5-12 of this invention. 本発明の比較例５−０に係る電解コンデンサ用アルミニウム電極箔のエッチングに用いた交流電流の波形図である。It is a wave form diagram of the alternating current used for the etching of the aluminum electrode foil for electrolytic capacitors which concerns on Comparative Example 5-0 of this invention.

符号の説明Explanation of symbols

Ｔ 第１の期間の時間
Ｄ１ 第１の期間の電流値
Ｄ２ 最大電流値 T First period time D1 First period current value D2 Maximum current value

Claims (3)

エッチング液中でアルミニウム箔に交流電流を印加して表面を粗面化する電解コンデンサ用アルミニウム電極箔の製造方法において、
前記交流電流は、初期において電流値が一定の第１の期間と、該第１の期間に続き、最大電流値が出現する第２の期間とを備えた電流波形を備え、
前記電流波形における第１の期間の時間は１〜１０ｍｓであり、当該第１の期間における電流値は、前記最大電流値の０．１〜０．９倍であることを特徴とする電解コンデンサ用アルミニウム電極箔の製造方法。 In the method for producing an aluminum electrode foil for an electrolytic capacitor in which an alternating current is applied to the aluminum foil in an etching solution to roughen the surface,
The alternating current includes a current waveform having a first period in which an initial current value is constant and a second period in which a maximum current value appears following the first period,
The time period of the first period in the current waveform is 1 to 10 ms, and the current value in the first period is 0.1 to 0.9 times the maximum current value. Manufacturing method of aluminum electrode foil. 前記第２の期間の電流波形が、最大電流値が出現する部分と、該部分に続く、電流値が一定または緩徐にゼロまで低下する部分とからなることを特徴とする請求項１に記載の電解コンデンサ用アルミニウム電極箔の製造方法。   2. The current waveform of the second period includes a portion where a maximum current value appears and a portion following the portion where the current value decreases constantly or slowly to zero. Manufacturing method of aluminum electrode foil for electrolytic capacitors. 前記エッチング液は、塩素イオンを含む水溶液であって、さらにリン酸イオン、硝酸イオン、硫酸イオンまたはシュウ酸イオンのうちの少なくとも１種を含んでいることを特徴とする請求項１に記載の電解コンデンサ用アルミニウム電極箔の製造方法。   The electrolytic solution according to claim 1, wherein the etching solution is an aqueous solution containing chlorine ions, and further contains at least one of phosphate ions, nitrate ions, sulfate ions, or oxalate ions. A method for producing an aluminum electrode foil for a capacitor.
JP2005338836A 2005-11-24 2005-11-24 Method for producing aluminum electrode foil for electrolytic capacitor Expired - Fee Related JP4653644B2 (en)

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JPH04305911A (en) * 1990-03-01 1992-10-28 Nippon Light Metal Co Ltd Manufacture of aluminum foil for electrolytic capacitor
JPH07235456A (en) * 1993-12-28 1995-09-05 Nippon Chikudenki Kogyo Kk Etching method of aluminum foil for electrolytic capacitor
JPH11208138A (en) * 1998-01-28 1999-08-03 Konica Corp Manufacture of support for lithographic printing plate, support for lithographic printing plate, and photosensitive lithographic printing plate

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Publication number Priority date Publication date Assignee Title
JPH04305911A (en) * 1990-03-01 1992-10-28 Nippon Light Metal Co Ltd Manufacture of aluminum foil for electrolytic capacitor
JPH07235456A (en) * 1993-12-28 1995-09-05 Nippon Chikudenki Kogyo Kk Etching method of aluminum foil for electrolytic capacitor
JPH11208138A (en) * 1998-01-28 1999-08-03 Konica Corp Manufacture of support for lithographic printing plate, support for lithographic printing plate, and photosensitive lithographic printing plate

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