WO2018218821A1 - Apprêt inorganique aqueux riche en zinc et son procédé de préparation - Google Patents

Apprêt inorganique aqueux riche en zinc et son procédé de préparation Download PDF

Info

Publication number
WO2018218821A1
WO2018218821A1 PCT/CN2017/102677 CN2017102677W WO2018218821A1 WO 2018218821 A1 WO2018218821 A1 WO 2018218821A1 CN 2017102677 W CN2017102677 W CN 2017102677W WO 2018218821 A1 WO2018218821 A1 WO 2018218821A1
Authority
WO
WIPO (PCT)
Prior art keywords
parts
component
aqueous
agent
zinc
Prior art date
Application number
PCT/CN2017/102677
Other languages
English (en)
Chinese (zh)
Inventor
李瑞清
Original Assignee
太仓卡斯特姆新材料有限公司
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by 太仓卡斯特姆新材料有限公司 filed Critical 太仓卡斯特姆新材料有限公司
Publication of WO2018218821A1 publication Critical patent/WO2018218821A1/fr

Links

Classifications

    • 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
    • C09D161/00—Coating compositions based on condensation polymers of aldehydes or ketones; Coating compositions based on derivatives of such polymers
    • C09D161/20—Condensation polymers of aldehydes or ketones with only compounds containing hydrogen attached to nitrogen
    • 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
    • C09D1/00—Coating compositions, e.g. paints, varnishes or lacquers, based on inorganic substances
    • C09D1/02—Coating compositions, e.g. paints, varnishes or lacquers, based on inorganic substances alkali metal silicates
    • C09D1/04—Coating compositions, e.g. paints, varnishes or lacquers, based on inorganic substances alkali metal silicates with organic additives
    • 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
    • C09D5/00—Coating compositions, e.g. paints, varnishes or lacquers, characterised by their physical nature or the effects produced; Filling pastes
    • C09D5/08—Anti-corrosive paints
    • C09D5/10—Anti-corrosive paints containing metal dust
    • C09D5/106—Anti-corrosive paints containing metal dust containing Zn
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/02—Elements
    • C08K3/08—Metals
    • C08K2003/0893—Zinc
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
    • C08K3/20—Oxides; Hydroxides
    • C08K3/22—Oxides; Hydroxides of metals
    • C08K2003/2231—Oxides; Hydroxides of metals of tin
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
    • C08K3/20—Oxides; Hydroxides
    • C08K3/22—Oxides; Hydroxides of metals
    • C08K2003/2237—Oxides; Hydroxides of metals of titanium
    • C08K2003/2241—Titanium dioxide
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K2201/00—Specific properties of additives
    • C08K2201/011—Nanostructured additives

Definitions

  • the invention relates to an aqueous inorganic zinc-rich primer and a preparation method thereof.
  • Zinc-rich coatings are generally classified into two types: organic zinc-rich coatings and inorganic zinc-rich coatings, depending on the film-forming materials.
  • the inorganic zinc-rich coating is an inorganic polymer as a film-forming base liquid, and the zinc powder reacts with it to form a zinc-iron complex on the metal surface, thereby forming a solid protective coating film.
  • This year with the increasing awareness of environmental protection, the restrictions on volatile organic solvents have become more and more strict.
  • Water-based coatings and solvent-free coatings which are called the mainstream of the development of the coatings industry, have received attention.
  • the content of zinc powder in the water-based inorganic zinc-rich coating is high, far exceeds that of CPVC, and the coating film is porous, resulting in poor weather resistance of the coating and poor impact resistance.
  • an object of the present invention is to provide an aqueous inorganic zinc-rich primer and a preparation method thereof.
  • the primer is composed of two components, and the water-based amino resin, the silicon-acrylic emulsion, the alkali metal silicate is the main component of the component A, and the zinc component and the nano-TiO 2 -SnO 2 are used as the main raw material component B.
  • Deionized water is used as solvent, and the adhesion ability is strong, and the production environment is effectively improved.
  • the use process is environmentally friendly and low-toxic; the nano TiO 2 -SnO 2 ultrafine particles are added to the primer to accelerate the curing rate of the primer and dry quickly.
  • the construction efficiency is high, and the density of the primer film formation and the weather resistance of the coating are improved, and the impact resistance and corrosion resistance of the coating are enhanced.
  • An aqueous inorganic zinc-rich primer comprising the following parts by weight:
  • Component A aqueous amino resin: 40-60 parts; silicone-acrylic emulsion: 8-15 parts; alkali metal silicate: 30-45 parts; silicone coupling agent: 3-8 parts; aqueous adhesion promoter : 3-8 parts; anti-sink Agent: 1-3 parts; dispersing agent: 0.5-1.5 parts; defoaming agent: 0.5-1.5 parts; deionized water: 45-65 parts;
  • Component B zinc powder: 30-40 parts; nano TiO 2 -SnO 2 : 1-2 parts; inorganic pigment: 10-20 parts; modified polyamine curing agent: 2.5-5 parts.
  • the primer comprises the following parts by weight:
  • Component A aqueous amino resin: 42-55 parts; silicone-acrylic emulsion: 10-12 parts; alkali metal silicate: 33-40 parts; silicone coupling agent: 5-8 parts; aqueous adhesion promoter : 3-5 parts; anti-settling agent: 1-1.5 parts; dispersing agent: 0.7-1.2 parts; defoaming agent: 0.8-1.2 parts; deionized water: 45-58 parts;
  • Component B zinc powder: 30-36 parts; nano-TiO 2 -SnO 2 : 1.1-1.3 parts; inorganic pigment: 10-15 parts; modified polyamine curing agent: 3.5-5 parts.
  • the primer comprises the following parts by weight:
  • Component A Aqueous amino resin: 47 parts; Silicone-acrylic emulsion: 11 parts; Alkali metal silicate: 36 parts; Silicone coupling agent: 7.5 parts; Aqueous adhesion promoter: 3.5 parts; Anti-settling agent: 1.2 parts; dispersing agent: 0.9 parts; defoaming agent: 1 part; deionized water: 51 parts;
  • Component B zinc powder: 34 parts; nano TiO 2 -SnO 2 : 1.2 parts; inorganic pigment: 13 parts; modified polyamine curing agent: 4 parts.
  • the mass ratio of the A component to the B component is 3-8:1.
  • the zinc powder is scaly zinc powder.
  • alkali metal silicate is one or more selected from the group consisting of potassium silicate, sodium silicate or lithium silicate.
  • the inorganic pigment is one or more of titanium white powder, iron oxide red, mica powder, carbon black or phthalocyanine blue.
  • the primer has a pH of 7.2-8.0 and a particle size of 65-85 ⁇ m.
  • a method for preparing an aqueous inorganic zinc-rich primer comprises the following steps:
  • component B (2) adding zinc powder, nano TiO 2 -SnO 2 , inorganic pigment and modified polyamine curing agent to another mixer, stirring at 200-400r / min for 10-15min, to obtain component B;
  • a component A and a component B are obtained at 1000-1200 r/min to obtain an aqueous inorganic zinc-rich primer.
  • the primer is composed of two components, and the water-based amino resin, the silicon-acrylic emulsion, the alkali metal silicate is the main component of the component A, and the zinc component and the nano-TiO 2 -SnO 2 are used as the main raw material component B.
  • Deionized water is used as solvent, and the adhesion ability is strong, and the production environment is effectively improved.
  • the use process is environmentally friendly and low-toxic; the nano TiO 2 -SnO 2 ultrafine particles are added to the primer to accelerate the curing rate of the primer and dry quickly.
  • the construction efficiency is high, and the density of the primer film formation and the weather resistance of the coating are improved, and the impact resistance and corrosion resistance of the coating are enhanced.
  • the present invention provides an aqueous inorganic zinc-rich primer comprising the following parts by weight:
  • Component A aqueous amino resin: 40-60 parts; silicone-acrylic emulsion: 8-15 parts; alkali metal silicate: 30-45 parts; silicone coupling agent: 3-8 parts; aqueous adhesion promoter : 3-8 parts; anti-settling agent: 1-3 parts; dispersing agent: 0.5-1.5 parts; defoaming agent: 0.5-1.5 parts; deionized water: 45-65 parts;
  • Component B zinc powder: 30-40 parts; nano TiO 2 -SnO 2 : 1-2 parts; inorganic pigment: 10-20 parts; modified polyamine curing agent: 2.5-5 parts.
  • the primer comprises the following parts by weight:
  • Component A aqueous amino resin: 42-55 parts; silicone-acrylic emulsion: 10-12 parts; alkali metal silicate: 33-40 parts; silicone coupling agent: 5-8 parts; aqueous adhesion promoter : 3-5 parts; anti-settling agent: 1-1.5 parts; dispersing agent: 0.7-1.2 parts; defoaming agent: 0.8-1.2 parts; deionized water: 45-58 parts;
  • Component B zinc powder: 30-36 parts; nano-TiO 2 -SnO 2 : 1.1-1.3 parts; inorganic pigment: 10-15 parts; modified polyamine curing agent: 3.5-5 parts.
  • the primer comprises the following parts by weight:
  • Component A Aqueous amino resin: 47 parts; Silicone-acrylic emulsion: 11 parts; Alkali metal silicate: 36 parts; siloxane coupling agent: 7.5 parts; aqueous adhesion promoter: 3.5 parts; anti-settling agent: 1.2 parts; dispersing agent: 0.9 parts; defoaming agent: 1 part; deionized water: 51 parts;
  • Component B zinc powder: 34 parts; nano TiO 2 -SnO 2 : 1.2 parts; inorganic pigment: 13 parts; modified polyamine curing agent: 4 parts.
  • the mass ratio of the A component to the B component is 3-8:1.
  • the zinc powder is scaly zinc powder.
  • alkali metal silicate is one or more selected from the group consisting of potassium silicate, sodium silicate or lithium silicate.
  • the inorganic pigment is one or more of titanium white powder, iron oxide red, mica powder, carbon black or phthalocyanine blue.
  • the primer has a pH of 7.2-8.0 and a particle size of 65-85 ⁇ m.
  • the invention also provides a preparation method of an aqueous inorganic zinc-rich primer, comprising the following steps:
  • component B (2) adding zinc powder, nano TiO 2 -SnO 2 , inorganic pigment and modified polyamine curing agent to another mixer, stirring at 200-400r / min for 10-15min, to obtain component B;
  • a component A and a component B are obtained at 1000-1200 r/min to obtain an aqueous inorganic zinc-rich primer.
  • 1 is a list of ingredients of an aqueous inorganic zinc-rich primer according to various embodiments of the present invention.
  • the invention provides an aqueous inorganic zinc-rich primer provided by the invention, wherein the aqueous amino resin, the silicon-acrylic emulsion and the alkali metal silicate are the main components of the component A, and the zinc powder and the nano TiO 2 -SnO 2 are used as the main raw materials.
  • nano TiO 2 -SnO 2 ultrafine particles are added to the primer to accelerate the primer as a nanocatalyst Curing rate, fast drying, high construction efficiency, improve the density of primer film formation and weather resistance of coating, strong impact strength, adhesion grade 1 grade, 3% NaOH solution, no blistering for 10 days, Rust point phenomenon, seawater resistance, no blistering, rust phenomenon for 30 days, and high temperature resistance. No cracking or discoloration during 500h at 500°C.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Wood Science & Technology (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Paints Or Removers (AREA)

Abstract

L'invention concerne un apprêt aqueux inorganique riche en zinc, comprenant les composantes suivantes en parts massiques : composante A : une résine aminique aqueuse : 40-60 parts; une émulsion silicone-acrylique : 8-15 parts; silicate de métal alcalin : 30-45 parts, un agent de couplage de silicone : 3-8 parts; un promoteur d'adhésion aqueux : 3-8 parts; un agent anti-sédimentation : 1-3 parts; un agent dispersant : 0,5-1,5 part; un agent antimousse : 0,5-1,5 part; de l'eau désionisée : 45-65 parts; et composant B : poudre de zinc : 30-40 parts; du nano TiO2-SnO2 : 1-2 parts; un pigment inorganique : 10-20 parts; un agent de durcissement polyamine modifié : 2,5-5 parts. Le procédé de préparation de l'apprêt consiste à : (1) ajouter proportionnellement une résine aminique aqueuse, une émulsion silicone-acrylique, du silicate de métal alcalin et entre 15 et 22 parts d'eau désionisée dans un mélangeur à une température constante de 50 °C, et agiter à une vitesse de rotation de 600-800 t/min pendant 20 à 30 min, continuer à agiter, et ajouter en continu un agent de couplage de silicone, un promoteur d'adhésion aqueux, un agent anti-sédimentation, un agent dispersant, un agent antimousse et l'eau désionisée restante, puis régler la vitesse de rotation à 1200-1500 t/min et agiter pendant 10 à 20 min pour obtenir le composant A; (2) ajouter de la poudre de zinc, du nano TiO2-SnO2, un pigment inorganique et un agent de durcissement polyamine modifié dans un autre mélangeur, et agiter à une vitesse de rotation de 200-400 t/min pendant 10 à 15 min pour obtenir le composant B; (3) agiter le composant A et le composant B à 1000-1200 t/min pour obtenir l'apprêt inorganique aqueux riche en zinc.
PCT/CN2017/102677 2017-05-27 2017-09-21 Apprêt inorganique aqueux riche en zinc et son procédé de préparation WO2018218821A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
CN201710390979.1A CN107189618A (zh) 2017-05-27 2017-05-27 一种水性无机富锌底漆及其制备方法
CN201710390979.1 2017-05-27

Publications (1)

Publication Number Publication Date
WO2018218821A1 true WO2018218821A1 (fr) 2018-12-06

Family

ID=59874889

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/CN2017/102677 WO2018218821A1 (fr) 2017-05-27 2017-09-21 Apprêt inorganique aqueux riche en zinc et son procédé de préparation

Country Status (2)

Country Link
CN (1) CN107189618A (fr)
WO (1) WO2018218821A1 (fr)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112646447A (zh) * 2020-12-18 2021-04-13 瑞康诺(深圳)创新发展有限公司 一种纳米二氧化钛紫外光催化净化涂层的制备方法
CN115558322A (zh) * 2022-09-26 2023-01-03 中远关西涂料（上海）有限公司 一种快干水性无机富锌车间底漆及其制备方法

Families Citing this family (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108727881B (zh) * 2018-06-15 2020-08-28 武汉工程大学 一种高附着力高柔韧性水性无机富锌涂料的制备方法
CN109181382A (zh) * 2018-09-02 2019-01-11 张家港市五湖新材料技术开发有限公司 一种防腐蚀型富锌底漆的配方
CN109468001A (zh) * 2018-09-19 2019-03-15 惠州市惠阳区嘉泰涂料有限公司 一种水性无机富锌底漆及其制备方法
CN109439201A (zh) * 2018-10-31 2019-03-08 安徽腾龙泵阀制造有限公司 一种用表面活化接枝玻璃鳞片制备水性硅酸盐富锌防锈防腐漆的方法
CN110054957A (zh) * 2018-11-21 2019-07-26 镇江禹亨新材料有限公司 一种双组份水性无机富锌底漆

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101735674A (zh) * 2010-01-07 2010-06-16 中国人民解放军海军后勤技术装备研究所 水性无机富锌涂料及其制备方法
CN102443291A (zh) * 2011-12-08 2012-05-09 上海工程技术大学 一种纳米TiO2-SnO2复合溶胶、涂层及其制备方法
CN105131665A (zh) * 2015-08-03 2015-12-09 宜兴市巨人涂料有限公司 一种水性无机富锌底漆及其制备方法
CN105400244A (zh) * 2015-12-21 2016-03-16 无锡市太湖防腐材料有限公司 一种水性无机富锌底漆及制备方法

Family Cites Families (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN103305041B (zh) * 2013-05-30 2018-01-30 玖青新材料科技（上海）有限公司 改性水性无机富锌涂料及其制备方法
CN104974626B (zh) * 2015-06-25 2017-06-20 武汉铁神化工有限公司 防腐用水性无机富锌底漆及其制备方法和应用
CN106118149B (zh) * 2016-06-30 2018-10-12 无锡华东锌盾科技有限公司 一种水性无机富锌涂料及其制备方法

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101735674A (zh) * 2010-01-07 2010-06-16 中国人民解放军海军后勤技术装备研究所 水性无机富锌涂料及其制备方法
CN102443291A (zh) * 2011-12-08 2012-05-09 上海工程技术大学 一种纳米TiO2-SnO2复合溶胶、涂层及其制备方法
CN105131665A (zh) * 2015-08-03 2015-12-09 宜兴市巨人涂料有限公司 一种水性无机富锌底漆及其制备方法
CN105400244A (zh) * 2015-12-21 2016-03-16 无锡市太湖防腐材料有限公司 一种水性无机富锌底漆及制备方法

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112646447A (zh) * 2020-12-18 2021-04-13 瑞康诺(深圳)创新发展有限公司 一种纳米二氧化钛紫外光催化净化涂层的制备方法
CN115558322A (zh) * 2022-09-26 2023-01-03 中远关西涂料（上海）有限公司 一种快干水性无机富锌车间底漆及其制备方法

Also Published As

Publication number Publication date
CN107189618A (zh) 2017-09-22

Similar Documents

Publication Publication Date Title
WO2018218821A1 (fr) Apprêt inorganique aqueux riche en zinc et son procédé de préparation
CN101633808A (zh) 含不锈钢鳞片的高氯化聚乙烯涂料及其制备方法
CN103756377A (zh) 有机蒙脱土作抗沉分散剂的改性硅酸盐水性富锌防腐涂料
WO2017028373A1 (fr) Apprêt à un seul constituant extrêmement anticorrosion à base d'eau pour surface rouillée, son procédé de préparation et son application
CN108997889A (zh) 一种海洋舰船用石墨烯重防腐底漆及其制备方法
CN110305580B (zh) 一种石墨烯基疏水型防腐蚀涂料及其制备方法和应用
CN106189677A (zh) 一种低表面处理环氧涂料及其制造方法
CN105925178A (zh) 一种水性有机无机杂化防腐涂料组合物及制备方法
CN104927646A (zh) 一种叉车发动机排气管用高致密性复合水性有机硅树脂涂料及其制备方法
CN109181477A (zh) 原油集输管线内壁挤涂无溶剂环氧重防腐涂料及其制备方法
CN105111860A (zh) 一种水性双组分防腐工业涂料及生产方法
CN110845879A (zh) 一种新型环保的水性涂料及其制备方法
CN107841175A (zh) 一种耐摩擦的无铬达克罗涂料
CN104845499A (zh) 水性环氧厚浆漆的制备方法
CN107722682A (zh) 一种钢铁表面防腐蚀纳米陶瓷涂料
WO2022088146A1 (fr) Peinture anti-corrosion en paillettes composite aqueuse de zinc-aluminium, son procédé de préparation et son utilisation
CN104119708A (zh) 一种无机富锌防腐涂料
CN109181466A (zh) 水性防腐底漆及其制备方法
CN105907240A (zh) 一种含有防闪锈剂的水性环氧防腐涂料及其制备方法
WO2017049697A1 (fr) Couche de finition anti-corrosive crue destinée à une canalisation enterrée pour le transport de l'eau du robinet, et son procédé de préparation
CN102408816B (zh) 一种环氧压载舱涂料及其制备方法
CN108641543B (zh) 一种基于液态金属的海洋防腐涂料及其制备方法
CN112608647A (zh) 一种水性无机纳米耐高温陶瓷防腐涂料及其应用方法
CN104140737B (zh) 应用于铁路支座上水性环氧富锌底漆的制备方法
CN112457697A (zh) 一种超细矿渣微粉防锈底漆及其制备方法

Legal Events

Date Code Title Description
121 Ep: the epo has been informed by wipo that ep was designated in this application

Ref document number: 17911869

Country of ref document: EP

Kind code of ref document: A1

NENP Non-entry into the national phase

Ref country code: DE

32PN Ep: public notification in the ep bulletin as address of the adressee cannot be established

Free format text: NOTING OF LOSS OF RIGHTS PURSUANT TO RULE 112(1) EPC (EPO FORM 1205A DATED 29/05/2020)

122 Ep: pct application non-entry in european phase

Ref document number: 17911869

Country of ref document: EP

Kind code of ref document: A1