CN1607911A - 烟制品 - Google Patents
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- CN1607911A CN1607911A CNA028262433A CN02826243A CN1607911A CN 1607911 A CN1607911 A CN 1607911A CN A028262433 A CNA028262433 A CN A028262433A CN 02826243 A CN02826243 A CN 02826243A CN 1607911 A CN1607911 A CN 1607911A
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- A—HUMAN NECESSITIES
- A24—TOBACCO; CIGARS; CIGARETTES; SIMULATED SMOKING DEVICES; SMOKERS' REQUISITES
- A24B—MANUFACTURE OR PREPARATION OF TOBACCO FOR SMOKING OR CHEWING; TOBACCO; SNUFF
- A24B15/00—Chemical features or treatment of tobacco; Tobacco substitutes, e.g. in liquid form
- A24B15/10—Chemical features of tobacco products or tobacco substitutes
- A24B15/16—Chemical features of tobacco products or tobacco substitutes of tobacco substitutes
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- A—HUMAN NECESSITIES
- A24—TOBACCO; CIGARS; CIGARETTES; SIMULATED SMOKING DEVICES; SMOKERS' REQUISITES
- A24F—SMOKERS' REQUISITES; MATCH BOXES; SIMULATED SMOKING DEVICES
- A24F42/00—Simulated smoking devices other than electrically operated; Component parts thereof; Manufacture or testing thereof
- A24F42/10—Devices with chemical heating means
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- A—HUMAN NECESSITIES
- A24—TOBACCO; CIGARS; CIGARETTES; SIMULATED SMOKING DEVICES; SMOKERS' REQUISITES
- A24B—MANUFACTURE OR PREPARATION OF TOBACCO FOR SMOKING OR CHEWING; TOBACCO; SNUFF
- A24B15/00—Chemical features or treatment of tobacco; Tobacco substitutes, e.g. in liquid form
- A24B15/10—Chemical features of tobacco products or tobacco substitutes
- A24B15/16—Chemical features of tobacco products or tobacco substitutes of tobacco substitutes
- A24B15/165—Chemical features of tobacco products or tobacco substitutes of tobacco substitutes comprising as heat source a carbon fuel or an oxidized or thermally degraded carbonaceous fuel, e.g. carbohydrates, cellulosic material
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- A—HUMAN NECESSITIES
- A24—TOBACCO; CIGARS; CIGARETTES; SIMULATED SMOKING DEVICES; SMOKERS' REQUISITES
- A24D—CIGARS; CIGARETTES; TOBACCO SMOKE FILTERS; MOUTHPIECES FOR CIGARS OR CIGARETTES; MANUFACTURE OF TOBACCO SMOKE FILTERS OR MOUTHPIECES
- A24D1/00—Cigars; Cigarettes
- A24D1/22—Cigarettes with integrated combustible heat sources, e.g. with carbonaceous heat sources
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- A—HUMAN NECESSITIES
- A24—TOBACCO; CIGARS; CIGARETTES; SIMULATED SMOKING DEVICES; SMOKERS' REQUISITES
- A24D—CIGARS; CIGARETTES; TOBACCO SMOKE FILTERS; MOUTHPIECES FOR CIGARS OR CIGARETTES; MANUFACTURE OF TOBACCO SMOKE FILTERS OR MOUTHPIECES
- A24D3/00—Tobacco smoke filters, e.g. filter-tips, filtering inserts; Filters specially adapted for simulated smoking devices; Mouthpieces for cigars or cigarettes
- A24D3/17—Filters specially adapted for simulated smoking devices
Abstract
本发明的烟制品(10)具有:在前端部安置的散热部(13)、在后端部具有吸口部(17)的筒状体(11);和在该筒状体(11)接近该散热部(13)处安置的香味散发部(15)。该香味散发部(15)多个粒状物(151)分别含有:以干燥质量为基准,实质上非多孔无机填料65~93重量%、粘合剂1~3重量%以及香味物质6~32重量%。
Description
技术领域
本发明涉及烟制品,更具体地说,涉及不伴随燃烧而通过加热产生香味的香味散发部的烟制品。
背景技术
一种不燃烧烟叶而能品味出香烟的香味或烟味的烟制品早已众所周知,并已有各种类型公开。例如,特开昭63-35468号公报、特开平6-46818号公报、特许第1681670号、特许第3012253号公报、特开平2-84164号公报等公开了一种利用安置在前端部的发热部件由此产生的热而产生香味类型的烟制品的典型例子。这些烟制品在发热部和吸口部之间,例如填充粒状或片剂状产生香味的香味散发部,当通过发热部加热香味散发部时,香味成分发生气化·散发。
作为香味散发部,有方案提出不燃性的多孔性物质或烟草原料等各种成型制品。然而,采用多孔性物质时,为了使其内部吸附的香味物质气化或脱吸附,必须要求有过剩的能量,从而导致气化效率降低及香味物质热变性发生变化。另外,在以烟草材料等可燃性物质作为基材时,由于发生实质上燃烧或热解,致使热行为非常不稳定,对散发出的香味量有不良影响之虑。
另外,对这种类型的烟制品来说,香味的散生量易受发热部件的发热状况所左右,这也是个重要问题。对发热部来说,以炭作为主原料形成的燃料元件是最常用的,通常在香烟点着以后至吸烟的前半部分之间,热量达最大值,在此以后,热量逐渐下降,直至熄灭显示不均匀性。因此,经受这种热而产生的香味的量也同样显示这样的变化,与最大量之间,特别是与吸烟过半的量产生明显差异。因此,指出:吸烟者由于在吸烟过程中烟量或烟味的不均匀变化而感到有压力感,满足感减少。
另一方面,特开平5-277191号公报公开了一种,为了散发出一定质量的香味,把燃料部和预先设定的吐烟次数多少的香味散发部制成板状加以粘贴的烟制品的案例。然而,由于把燃料部件和香味散发部或绝缘体加以粘贴,则燃料部件的温度下降、燃烧难以持续、立即熄灭的可能性大,所以,由于经常加热香味散发部,通过不必要的加热作用,易引起质量下降。另外,燃料部件的燃烧速度和吸烟的时间必须吻合,不能根据吸烟者的爱好来选择吸烟间隔,不仅有增大紧迫感,而且结构复杂,制造极为困难。
鉴于上述问题,本发明提供一种结构简单的烟制品,该烟制品使吸烟者在吸烟时,每次吐烟均能散发出稳定量的香味,不会因烟量或烟味的不均匀变化而感到紧迫感,并可品偿到吸烟乐趣。
发明内容
为了解决上述课题,按照本发明提供的烟制品,其中包括:在前端部安置散热部、在后端部具有吸口部的筒状体和;在该筒状体内,在接近该散热部处设置的香味散发部;该香味散发部按照干燥质量标准(即,不含水分时的比例),分别包含实质上非多孔无机填充材料为65~93重量%、粘合剂为1~3重量%以及香味物质为6~32重量%等多个粒状物。
在本发明中,无机填料优选具有3m2/g或3m2/g以下的BET比表面积的无机填料,优选由碳酸钙构成。
粒状物,优选的是以最密的状态填充、在筒状体的轴向上粒状物的填充长度和筒状体的内径之比为2~4、筒状体的内径和粒状物的代表粒径之比为4~15。粒状物的形态可以是颗粒、片剂状或球状。
另外,本发明中的粘合剂,优选含有甲基羟乙基纤维素。
在本发明的优选实施方案中,散热部在常温下显示1.0W/m·K或1.0W/m·K以下的导热率。散热部优选由实质上含多孔无机填料15~65重量%的炭质材料构成,散热部中所含的无机填料优选由具有3m2/g或3m2/g以下的BET比表面积的碳酸钙构成。
在本发明的烟制品中,吸口部可由过滤率在20%或20%以下的过滤嘴或空心过滤嘴构成。
附图说明
图1是表示本发明1个实施方案的烟制品的截面图。
图2A及图2B是采用实质上非多孔无机填料作为无机填料时和,采用多孔无机填料、与香味物质混合时的DSC的分析结果图。
图3是表示即将详述的实施例1中的烟制品,每次吐烟所捕集到的香味物质量的图。
图4是表示即将详述的实施例2中的烟制品,每次吐烟所捕集到的香味物质量的图。
图5是表示在实施例1的烟制品中每次吐烟从炭成型散热部流入香味散发部中的热量的图。
图6是比较例1的烟制品,表示每次吐烟所捕集到的香味物质量的图。
实施具体方案
下面详细说明本发明。
本发明的烟制品,是一种不使香味散发部燃烧的所谓非燃烧型烟制品,包括采用从着火的散热部进行加热而散发出香味成分的香味散发部。香味散发部具有特定的组成,设置在筒状体中。在筒状体的前端部具有散热部,而筒状体的后端部由吸口部构成。
图1是表示构成本发明的烟制品之一的简要剖面图。示于图1的烟制品10具有构成烟制品本体的筒状体11。在筒状体11的前端部,设置散热部13,筒状体11的后端部构成吸口部17。本发明的香味散发部15,其接近散热部13设在筒状体11内。
通常,筒状体11为圆筒形,优选由铝、不锈钢等对热稳定性好的材料形成,另外,为了降低其热容量,厚度要薄,例如优选薄到0.03mm~0.1mm。筒状体11,与普通的香烟一样,可以具有约7mm~8mm内径、约80mm~120mm长。通常,筒状体11,其整个外侧用隔热材料12卷绕,使手持香烟时不会产生障碍。
本发明的烟制品中使用的香味散发部15,以干燥质量为基准,由多个粒状物151构成,其分别含有实质上非多孔无机填料65~93重量%、粘合剂1~3重量%以及香味物质6~32重量%。
香味物质,包含通过着火的散热部的热进行加热而生成气溶胶的物质(醇类、糖类、水)或,仅产生香味的物质(薄荷醇、咖啡碱、天然提取物)、烟草、烟草提取物、它们的混合物等。作为醇类,例如,可以使用甘油或丙二醇及它们的混合物。
香味散发部15的成分之一的即实质上非多孔无机填料优选BET比表面积在3m2/g或3m2/g以下。
活性炭、氧化铝珠或硅石等陶瓷类、分子筛等具有无数精细孔的所谓多孔物质,具有通过吸附或吸收其他物质进入其内部的性质。在如本发明烟制品之类的烟制品中,通过加热可有效释放出香味时,当香味物质进入基材的孔内时,除了香味物质的蒸发所必须的热量,还必须进一步用于从孔内脱出的热能,因而气化效率明显降低,继续在孔内加热则易引起热变性等问题。在本发明中,由于香味物质仅仅是保持在实质上非多孔无机填料构成的基材粒子间隙中,所以,多孔性物质不会产生上述问题而通过加热容易地从香味散发部15中放出。
作为实质上非多孔性的孔性无机填料,特别优选使用BET比表面积在3m2/g或3m2/g以下的碳酸钙粒子。从烟草原料或替代的植物原材料及其提取物等,也可以充分地成型为粒状成型制品,但由于通过加热很少引起燃烧或热分解,所以,通过不稳定的热行为则放出的香味量容易变得不均匀,多孔性物质同样有可能引起香味的热变性问题。
作为本发明的香味散发部中所含的粘合剂,可以使用纤维素或各种纤维素衍生物、藻酸类、愈疮胶或黄原胶、刺槐豆胶等。特别是当采用甲基羟乙基纤维素时,香味物质的持久性增加,可赋予良好的吸烟香味。粘合剂添加量愈多成型物的物理强度增加,操作容易。然而,几乎所有粘合剂在高温加热时,对香味多数有不良影响,所以,为便于操作,少到1~3重量%范围内是优选的。
构成本发明的香味散发部的粒状(成型)物,是把上述实质上非多孔无机填料、粘合剂和香味物质以上述比例混合后,添加用于粘合剂产生粘合力的必要量的水,用挤出成型机或造粒机、制片机等,成型为所希望的大小及形状。因此,粒状物可成型为颗粒物、片剂或球等的形态。
如图1所示,在散热部13和香味散发部15之间,设置金属筛等通气性耐热性部件16a使香味散发部15不直接接触散热部13。
在本发明的烟制品中的筒状体11的前端部设置的散热部13,可通过炭质材料形成。炭质材料可用挤出成型机、制片机等制成所希望的形状。作为炭质成型制品的形状,圆柱状是优选的。这种散热部,通过从吸口部抽吸,从外部通过散热部13把空气导入筒状体11的内部,从散热部13把加过热的导入空气,通入香味散发部15的粒状物151间的空气流路,借品味所产生的香味成分,所以,必须具有空气流通路。该空气流通路,由沿着筒状体11的长轴、在炭质圆柱成型体的外周面内设置的至少有1条沟槽,或沿着筒状体11的长轴、贯穿炭质圆柱成型体的至少1个贯穿孔构成。在图1中,作为这种通路,由贯穿散热部13轴向的中央贯穿孔131及设置在该贯穿孔131周边的多个贯穿孔(在图1中,显示贯穿孔132、133)构成。
在散热部13中,空气通路的形状(沟槽的深度、贯穿孔的直径)或数目,与炭质材料的种类或组成,一起对散热部的着火时间、燃烧速度、燃烧温度、燃烧产物的生成量等燃烧特性产生影响。特别是着火时间特性,使用者要求与普通的香烟着火(约1秒以内)相同的着火时间特性。从本发明可知,约1.5秒以内的炭质成型体着火时间,通过选择炭质材料的组成可以达到,在常温(约22℃)的导热率达到1.0W/m·K或1.0W/m·K以下。另外,从本发明可知,通过采用含实质上非多孔性无机填料15~65重量%的炭质材料组合物(其余为炭)形成散热部,炭质量可得到实质性削减,燃烧产物量,特别是一氧化炭的削减可更加明显,同时,可以降低燃烧量,即吐烟次数,也可以减少燃烧产物总量。作为实质上非多孔无机填料,特别优选使用BET比表面积在3m2/g或3m2/g以下的碳酸钙。散热部13的燃烧产生的热,把与散热部相邻配置的香味散发部15进行加热,使香味气化·散出。
散热部13,通常其外周用耐热性包围材料14包住,并插入·固定在筒状体11内。
在筒状体11内,在香味散发部15的下流侧设置香味补充部18。香味补充部18,除了从香味散发部15生成的香味成分外,还得必须在赋予香味特征的场合或者事先载带最好不曝露在高温下的各种香料,根据目的由烟草、再生烟草构成,或者,用载带有香料的纸、无纺布等载体构成也可。另外,香味补充部18,也可提供含香料的成型物。
吸口部17,通常可以设置该技术领域一般使用的香烟过滤器171。为了有效释放出使用者最终可能吸入的香味量,对香味的生成量,采用具有过滤率20%或20%以下过滤性的过滤器,或空心过滤器。另外,在吸口部17,为了调整吸入量及吸入压力,可根据需要在所希望的位置(通常为吸口部17的圆周方向),分别贯穿隔热材料12及筒状体11形成多个通气孔VH。
在本发明中,香味散发部15和香味补充部18,可以直接接触地配置,如图1所示,在它们之间优选设置空隙部19。通过该空隙部19,有时可以促进香味散发部15生成的气溶胶或香味的冷却,可以降低因在香味补充部18及吸口部17的冷凝所造成的损失。空隙部19的体积,可根据这些目的适当设定。在设置这种空隙部19时,如图1所示,在香味散发部15的下端部,使粒状物151不发生移动并设置与通气性材料16a相同的通气性材料16b。
在本发明中,填充筒11内的粒状物151,优选最紧密的填充。当粒状物151松散地填充时,使用中变成不均匀的填充状态,使粒状物151间形成的流体流路也变成不平衡,使香味散发量的均匀性受损,所以,优选在开始填充时保持最紧密的填充状态。其中,所谓最紧密填充,系指把粒状物通过振动或敲打等达到紧密的填充状态。
由此可见,最紧密填充的粒状物151的填充长度(L)和筒状体11的内径(D),其比(L/D)优选设定在2~4。当该比例小于2时,来自香味散发部15的香味成分的散发行为变得易受散热部13的发热类型的影响,相反,当该比例大于4时,在香味散发部15内由于凝固沉淀,释放出的香味量变得减少,香味释放的均匀性变得降低。因此,筒状体11的内径(D),与一般的香烟同样约为7~8mm时,填充长度(L)优选设定在约14~32mm范围内。另外,粒状物151的大小,其代表粒径(d)和筒状体11的内径(D)之比(D/d)为3.5~16,特别优选设定在4~15。当该比例小于4时,粒状物151一个的热容量增大,所以,开始吸入的释放香味量有减少的倾向,另外,当该比例大于15时,由于吸引阻力增大而变得难以吸入。因此,筒状体11的内径(D)与普通香烟同样,当约为7~8mm时,粒状物151的代表粒径优选设定在约2.0~0.5mm范围内。其中,所谓粒状物的代表粒径,系指轴向或半径方向的最长的径。
下面通过实施例说明本发明,但本发明又不受这些实施例的限定。
实验例1
图2A及图2B,是使用BET比表面积1m2/g的碳酸钙作为非多孔无机填料,在与香味物质混合时的DSC分析结果(图2A);使用比表面积120m2/g的氧化铝作为多孔无机填料,与同样的香味物质和以同样的比例混合时(图2B)的DSC分析结果。如图2A所示,在采用非多孔无机填料时,通过香味物质的气化,吸热峰仅出现1次,而如图2B所示,采用多孔无机填料时,除1个吸热峰(吸热峰(1))外,还在高温区域出现第2次吸热峰(吸热峰(2))。这表示为了使多孔性物质中吸附的香味物质发生气化,必须有更多的能量,所以,使用非多孔性物质是明显有意义的。
实施例1
按下列式样制造图1所示结构的烟制品。
[筒状体]
材质:铝箔层压纸
长度:85mm
内径(D):7.5mm
[香味散发部]
组成:BET比表面积1m2/g的碳酸钙,80重量%
甲基羟乙基纤维素,1重量%
甘油(香味物质),19重量%
形状:球状
代表粒径(d):1.5mm
最密填充长度(L):15mm
L/D=2
D/d=5
[香味补充部]
组成:黄色的烟丝
长度:20mm
[吸口部]
过滤器
长度:20mm
[散热部]
组成:炭85%
BET比表面积1m2/g的碳酸钙15重量%
[空隙部]
长度:15mm
对该烟制品,用自动吸烟仪,以30秒间隔,每次吐烟容量以50mL/2秒进行吸烟,测定每次吐烟捕集的香烟物质的量,结果示于图3。本实施例的烟制品释放出的香味成分的均匀性指数(下述)为0.79。香味物质的总捕集量为约11mg。
实施例2
除构成香味散发部的粒状物最紧密填充长度为30mm(L/D=4,无空隙部),粒状物的代表粒径为1.0mm(D/d=7.5)以外,制成与实施例1同样的烟制品。对该烟制品,用自动吸烟仪,以30秒间隔,每次吐烟容量以50mL/2秒进行吸烟,测定每次捕集的香烟物质量,结果示于图4。本实施例的烟制品的均匀性指数高达0.81,但由于L/D大,与前例相比,香烟物质捕集总量低,约为7mg。
上述实施例中的均匀性指数,使用2~11次吐烟的测定值,按下式进行计算:
均匀性指数=1-(变动系数)
变动系数=(标准偏差)/(平均值)
该均匀性指数接近于1左右,显示均匀性良好。
图5表示在实施例1的烟制品中,每次吐烟绘制的从炭质材料成型散热部流入香味散发部的热量结果图。均匀性指数的评价范围以2~11次吐烟为根据,流入香味散发部的热量以其最大值(约为第5次吐烟)的50%以上为条件。
实施例3
除了散热部中的碳酸钙含量为40重量%以外,制成与实施例1同样的烟制品,进行同样的吸烟操作。结果是,一氧化碳生成量降至实施例1的50%。
比较例1
当香味散发部为不耐热易燃烧的性质或形态时,填充状态因燃烧而变化,由于燃烧热使香味生成量急剧增大,所以,散热部本身的发热行为进一步变得不均匀。特开平6-46818号公报中记载的由纸浆及烟草类材料构成的片剂状烟丝介质中,含香味物质(例如甘油)40重量%的香味散发部填充到约30mm长,制成与实施例2同样的烟制品,测定每次吐烟捕集的香味物质量,结果示于图6。香味物质的总捕集量约13mg,与实施例1之差不大,但均匀性指数非常低,为0.31。另外,当打开吸烟后的烟制品时可以确认,因燃烧造成片剂状烟丝的灰化及烧掉。
实施例4
实施例1及实施例2的烟制品和,比较例1的烟制品,由专门训练的吸烟人员进行实际比较。结果表明,本发明的实施例1及实施例2的烟制品,每次吐烟的香味烟量感稳定,特别是吸到后半部时香味量不下降,所以,即使接着吸烟,得到烟量感持续性很高的评价。另外,比较例1的烟制品,由于吸到后半部的香味散发部燃烧,确认有特殊的吸烟味变化。
如上所述,按照本发明,提供一种结构简单的烟制品、使用者在吸烟时,每次吐烟放出稳定量的香味,不会感到烟量或烟味不均匀变化而带来的压力感,可以感受香烟的乐趣。
Claims (11)
1.一种烟制品,其中包括:在前端部安置散热部、在后端部具有吸口部的筒状体;在该筒状体内接近该散热部处安置的香味散发部;该香味散发部包含多个粒状物,其中该粒状物分别含有:以干燥质量为基准,实质上非多孔无机填料65~93重量%、粘合剂1~3重量%以及香味物质6~32重量%。
2.按照权利要求1所述的烟制品,其中,所述无机填料为具有3m2/g或3m2/g以下的BET比表面积。
3.按照权利要求2所述的烟制品,其中,所述无机填料为碳酸钙。
4.按照权利要求1所述的烟制品,其中,所述粒状物以最紧密的状态填充,在上述筒状体的轴向上,该粒状物的填充长度和上述筒状体的内径之比为2~4,上述筒状体的内径和粒状物的代表粒径之比为4~15。
5.按照权利要求1所述的烟制品,其中,所述粒状物为颗粒状、片剂状、或球状。
6.按照权利要求1所述的烟制品,其特征在于,所述粘合剂含有甲基羟乙基纤维素。
7.按照权利要求1所述的烟制品,其中,所述散热部在常温下显示1.0W/m·K或1.0W/m·K以下的导热率。
8.按照权利要求1所述的烟制品,其中,所述散热部由含有实质上非多孔无机填料15~65重量%的碳质材料组成。
9.按照权利要求1所述的烟制品,其中,所述散热部中所含的无机填料,是由具有3m2/g或3m2/g以下的BET比表面积的碳酸钙构成。
10.按照权利要求1所述的烟制品,其特征在于,所述吸口部是由过滤率为20%或20%以下的过滤器构成。
11.按照权利要求1所述的烟制品,其特征在于,所述吸口部是由空心过滤器构成。
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- 2002-12-18 DK DK02806062T patent/DK1468618T3/da active
- 2002-12-18 CA CA002471732A patent/CA2471732C/en not_active Expired - Fee Related
- 2002-12-18 AT AT02806062T patent/ATE400192T1/de active
- 2002-12-18 WO PCT/JP2002/013232 patent/WO2003056949A1/ja active IP Right Grant
- 2002-12-18 CN CNB028262433A patent/CN1286409C/zh not_active Expired - Fee Related
- 2002-12-18 KR KR1020047009974A patent/KR100587849B1/ko active IP Right Grant
- 2002-12-18 ES ES02806062T patent/ES2305353T3/es not_active Expired - Lifetime
- 2002-12-18 JP JP2003557321A patent/JP3974898B2/ja not_active Expired - Fee Related
- 2002-12-18 DE DE60227562T patent/DE60227562D1/de not_active Expired - Lifetime
- 2002-12-18 RU RU2004123208/12A patent/RU2268631C2/ru not_active IP Right Cessation
- 2002-12-18 EP EP02806062A patent/EP1468618B1/en not_active Expired - Lifetime
- 2002-12-18 PT PT02806062T patent/PT1468618E/pt unknown
- 2002-12-26 TW TW091137424A patent/TWI226821B/zh not_active IP Right Cessation
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Also Published As
Publication number | Publication date |
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CN1286409C (zh) | 2006-11-29 |
KR100587849B1 (ko) | 2006-06-12 |
PT1468618E (pt) | 2008-09-17 |
JPWO2003056949A1 (ja) | 2005-05-12 |
CA2471732C (en) | 2008-11-18 |
ES2305353T3 (es) | 2008-11-01 |
RU2268631C2 (ru) | 2006-01-27 |
DK1468618T3 (da) | 2008-08-11 |
ATE400192T1 (de) | 2008-07-15 |
JP3974898B2 (ja) | 2007-09-12 |
US20040226568A1 (en) | 2004-11-18 |
EP1468618A4 (en) | 2006-12-27 |
TWI226821B (en) | 2005-01-21 |
KR20040066928A (ko) | 2004-07-27 |
TW200301086A (en) | 2003-07-01 |
EP1468618B1 (en) | 2008-07-09 |
RU2004123208A (ru) | 2005-03-10 |
WO2003056949A1 (fr) | 2003-07-17 |
AU2002357599A1 (en) | 2003-07-24 |
EP1468618A1 (en) | 2004-10-20 |
CA2471732A1 (en) | 2003-07-17 |
DE60227562D1 (de) | 2008-08-21 |
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