CN105228696A - 用于光疗法的量子点发光二极管 - Google Patents
用于光疗法的量子点发光二极管 Download PDFInfo
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- CN105228696A CN105228696A CN201480015971.1A CN201480015971A CN105228696A CN 105228696 A CN105228696 A CN 105228696A CN 201480015971 A CN201480015971 A CN 201480015971A CN 105228696 A CN105228696 A CN 105228696A
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Abstract
在本文中所公开的是用于在使用量子点(QD)的光疗法中使用的制品。一个实施方案是具有闭塞层和半透明层的医用敷料。量子点发光二极管芯片被配置在闭塞层内以提供用于在光疗法中使用的特定波长的光。另一个实施方案是具有闭塞层和半透明层的医用敷料,其中量子点材料埋入或浸于一个或二个层内。
Description
背景
光疗法(phototherapy),也被称为日光疗法(heliotherapy),是利用光来治疗医学病症。当前的光疗法由NielsFinsen首创,他因其利用集中的光辐射来治疗疾病的工作而被授予1903年诺贝尔生理和医学奖。Finsen的最初工作包括使用石英晶体分离紫外(UV)射线,其成功用于治疗寻常狼疮(lupusvulgaris)。Finsen还发现可以使用红光降低天花中的疤痕形成。
从那时起,光疗法已经用于治疗大范围的病况,包括皮肤病症、昼夜节律和季节性情绪失调(circadianrhythmandseasonalaffectivedisorder)、新生儿黄疸(neonataljaundice)和肿瘤。
使用光疗法治疗皮肤病况,例如银屑病(psoriasis)、湿疹(eczema)、皮炎(dermatitis)、寻常痤疮(acnevulgaris)主要依赖于UV区中的辐射,然而红光到红外(IR)光可以用于促进伤口愈合。
高胆红素血症(hyperbilirubinaemia),较佳地被称为新生儿黄疸,是常见的病况,通常影响超过50%的新出生的婴儿。黄疸因肝脏不能分解胆红素使其在血液中积聚而引起。光疗法可以用于将反式胆红素光氧化为水溶性的顺式异构体,其之后可以更容易被肝脏分解并且从血液中移除。根据由英国国家卫生与临床优化研究所(NationalInstituteofHealthandClinicalExcellence,NICE)提出的2010指南,新生儿黄疸的治疗取决于血清胆红素的水平。在妊娠37周时或之后出生的婴儿的一线治疗应当是常规的“蓝光”光疗法,而对于早产婴儿来说,可以首先使用光纤或“biliblanket”。尽管研究表明绿光可以恰好为有效的,但是选择蓝光以匹配胆红素的分解(其在458nm最佳),从而提供危害稍微较小的备选方案[H.Ayyash等人,ArchivesofDiseaseinChildhood(儿童疾病档案),1987,62,843]。这表明,因为绿光比蓝光更具穿透性,这补偿了其与胆红素的吸收光谱的较差的匹配,[H.J.Vreman等人,PediatricResearch(儿科研究),1998,44,804]其峰在约458nm。
光疗法已经显示出了一些在肿瘤治疗中的效果。当他注意到光和吖啶的结合对草履虫(paramecium)原生动物有毒时,首先由OscarRaab在20世纪之交观察到了光对光敏分子的作用而产生毒性[O.Raab,dieWirkungFluoreszierenderStoffeaufInfusorienZ.Biol.,1900,39,524]。在已经在美国由食品药品管理局(FDA)批准用于肺癌治疗的光动力学疗法(PDT)中,使用光对光活性分子的作用来促进体内肿瘤坏死。除了肿瘤治疗之外,在英国NICE已经实施了在癌前病况如巴雷特食管(Barrett’soesophagus)以及包括湿性年龄相关黄斑变性(wetage-relatedmaculardegeneration)在内的良性病况的治疗中使用PDT的指导。
因为癌组织比健康组织更易响应光敏剂的吸收,该方法可以用于选择性地靶向癌细胞。选择性的光敏剂吸收依赖于健康组织和肿瘤组织之间的化学组成的差异,其包括低密度脂蛋白受体的数量、组织pH和水含量。适合的光活性药物可以包括卟啉系分子,其吸收640nm以下的红光,用于治疗恰好在皮肤或器官内膜的表面下的肿瘤。为了更深的穿透,需要IR光吸收剂。组织内的发色团,即血红蛋白、黑色素和水,还将会吸收任何进入的光。因此,在血红蛋白的吸收光谱以上并且在水的吸收光谱以下,存在600-1300nm之间的“光学窗口”,其对于PDT来说是理想的。850nm以上的光子吸收通常能量不足以产生单线态氧(singletoxygen)(对于作用机制来说,参见图1),因此在600-850nm范围内强烈吸收的光敏剂最适用于光疗法。同样地,需要在这个区域中发光的光源。
在静脉内(IV)施用光活性物质之后,使用内窥镜或光纤导管来传输光。单线态氧产生的机制概述于错误!未发现引用来源;在光子吸收时,光敏剂由基态激发至激发单线态。在系间窜越(intersystemcrossing)至激发三线态之后,能量从光敏剂转移至身体中氧的激发单线态。单线态氧与癌生物分子反应,导致细胞死亡。
一种用于肿瘤光疗法的第一代光敏剂是血卟啉衍生物(HpD),其具有在400-410nm、500-505nm、535-540nm、565-575nm和620-635nm的五个吸收带。因为穿透深度随着减小的波长而降低,通常用发射630nm的染料激光器来进行光活化。研究表明,绿光可以更有效用于治疗恰好在皮肤或组织表面下方的肿瘤[J.C.vanGemert等人,Br.J.Cancer,1985,52,43]。第二和第三代光敏剂在650-850nm范围内更强烈地吸收。
用于PDT的光源包括激光器、放电和荧光灯以及发光二极管(LED)。光源的选择取决于病变(legion)的深度、光敏剂的吸收光谱和光源本身的属性(可靠性、维护的容易性、成本和尺寸)。以超过150mWcm-2的照射率,通常引起体温过高,其可能会导致氧消耗。因此,较低的频率通常是优选的。尤其应当在皮肤中避免体温过高,因为其引起增加的疼痛。因此高功率激光输出并非总是有利的。此外,归因于热效应和控制光剂量的难度,宽谱光源,如卤素和金属卤化物灯,也可能是不利的。因此,需要在600-850nm区域中发光的窄谱光源,其功率输出可以容易地控制。
白光光疗法常用于昼夜节律失调和季节性情绪失调(SAD)的治疗。据信,在具有较少日光时间的冬季月份期间,清晨的白光疗法可以有助于调节昼夜节律和治疗季节性抑郁症状。目前,荧光盒是最常用的,其结合滤光器以阻挡有害的UV射线。
最近光对皮肤的治疗效果已经扩展至化妆品用途。也许最众所周知的实例是日光浴床。因为使用UV射线刺激皮肤中的黑色素产生因增加皮肤癌的风险而不再受欢迎,正在引入其他化妆品光疗法来恢复皮肤。
尤其是,红光和IR光已经用于化妆品光疗法以改善细纹、皱纹和肤色的出现。对于伤口愈合光疗法来说,据信红光到IR光刺激胶原蛋白产生和重建,得到具有更均匀肤色的更光滑的皮肤。
关于这样的多种用途,光疗法依赖于宽波长范围以针对特定的病况。目前的灯根据所需的发射波长依赖于不同的光源,将它们的使用限定于非常特定的用途。因此,需要容易获得的转换一次光源的发射波长以在遍及整个可见光谱以及到IR中的任何给定的波长处发光的方法。
概述
在本文中所公开的是用于在使用量子点(QD)的光疗法中使用的制品。一个实施方案是具有闭塞层和半透明层的医用敷料。量子点发光二极管芯片被配置在闭塞层内以提供用于在光疗法中使用的特定波长的光。另一个实施方案是具有闭塞层和半透明层的医用敷料,其中量子点材料埋入或浸于一个或二个层内。
附图简述
错误!未发现引用来源。示出了光动力学疗法的能级图。在光子吸收时,光敏剂由基态(S0)激发至单线态(S1)。在系间窜越(isc)至光敏剂的激发三线态(T1)之后,能量转移至激发单线态氧(1O2)。单线态氧与癌生物分子反应,导致细胞死亡。
错误!未发现引用来源。是胆红素的吸收光谱,示出了宽的蓝光-绿光吸收。
图3是多层敷料的图,其包括嵌入在闭塞敷料中、被半透明敷料层覆盖的QDLED芯片阵列(和电路),所述多层敷料用于向伤口施用光疗法。
图4是用于治疗昼夜节律失调的白光疗法灯的图,其包括一次光源和包括QD的透明或半透明灯罩。
图5示出了在CommissionInternationaledel’Eclairage(国际照明委员会)1931颜色空间中的由白色LED以及红色和绿色QD产生的白光的颜色坐标。相关色温(CCT)是5,536K并且白点位于普朗克轨迹(Planckianlocus)附近。
图6示出了包括蓝色固态LED背光和在625nm发光的红色QD磷光体的LED芯片的发射光谱。可以通过改变QD浓度来调节相对峰强度。
图7示出了包括蓝色固态LED背光和在653nm发光的红色QD磷光体的LED芯片的发射光谱。可以通过改变QD浓度来调节相对峰强度。
描述
在本文中所公开的是用于在结合了量子点(QD)的光疗法中使用的制品。调节由QD发射的光的波长用于特定的光疗法。
在申请人的美国专利号7,803,423、7,985,466、8,062,703、7,588,828和7,867,556中提供了QD和制备QD材料的方法的实例,其通过引用结合在本文中。可以简单地通过改变粒径以在遍及整个可见光谱以及到IR处调节QD的发射。来自QD的高量子产率和窄带发射导致来自固态背光的具有低能量损失的高颜色纯度。可调节性和颜色质量二者以及可使用QD获得的光的强度使得QD材料成为用于在光疗法中使用的有前景的材料。
在本文中所描述的具体实施方案使用QD以调节或“降频变换(downconvert)”来自LED光源的光以提供特定光疗法所需的光的波长。发射UV或蓝光的固态LED可以是适合的,然而,由于UV辐射对皮肤的有害作用,可以优选使用蓝色LED。在一个实施方案中,将QD结合至具有固态LED背光的LED芯片封装件中。在申请人的共同拥有的美国专利申请公开号2010/1023155(2010年5月20日公布)和2013/0140600(2013年6月6日公布)中描述了结合QD的LED芯片封装件的制备,其通过整体引用结合于此。可以将这种LED芯片封装件结合至用于如以下所述的在特定形式的光疗法中使用的制品中。
备选地,可以制造远程QD磷光体用于与固态LED背光一起使用。在申请人的共同待审的英国申请号1116517.2(2011年9月23日)中描述了远程QD磷光体的制备,其通过整体引用结合于此。在远程磷光体构造中,QD磷光体可以采取与人组织如皮肤紧密靠近或直接接触的制品的形式。基于远程磷光体的***具有一个远程磷光体可以被具有不同发光颜色的另一个远程磷光体代替的优点,因此单一LED背光***可以通过简单地换出远程磷光体而用于治疗多种不同的病况。
在本文中所描述的制品的一个实例是结合QD的医用敷料。如在本文中所使用的,术语“敷料”可以是指施用至身体以辅助光疗法的任何制品,但是通常是指织物或纺织制品,如绷带、毯子、服装制品、海绵、敷布、包裹物等。敷料可以结合如上所述的LED、远程磷光体,或者可以用QD材料浸渍、涂布或处理。以下在特定光疗法的上下文中更详细地讨论了这些实施方案中的每一个。
在本文中描述的制品可以包括根据用途在一个或多个波长发光的QD。可以在使用前将QD任选地结合至珠中,以提高其稳定性。装置可以使用含重金属(Cd、As或Pb)或不含重金属的QD如III-V和I-III-VI2半导体QD,并且包括掺杂的物种及其合金。可以通过用一个或多个宽带隙材料的壳层包覆QD“核”以形成核/(多)壳QD来提高纳米粒子的光致发光量子产率(QY)。在设备制造过程中使用的玻璃熔接(beading)和/或封装技术明显地降低了暴露于来自QD的有毒重金属的风险,然而对其使用的法律限制可以使不含重金属的QD成为优选的,尤其是对于其中将QD结合至与人组织接触的制品中的实施方案来说。
高胆红素血症的治疗
错误!未发现引用来源中示出了胆红素的吸收光谱。利用具有蓝色固态LED背光的发绿光的QD材料,可以将发光调节为用于新生儿黄疸的安全和有效治疗的EM波谱的蓝色-绿色区。如在本文中所使用的,术语“绿色QD”是指当激发时在可见光谱的绿色区中发光的QD。同样地,“红色QD”是指发红光的QD,依此类推。在某些实施方案中,将QD材料结合至用于外部一次光源的降频变换的二次材料或制品中。
在一个这种实例中,将绿色QD结合至染料中以将半透明或疏松编织的纺织材料染色,其用于制造基底或顶罩,当通过蓝色固态LED灯照射时,所述基底或顶罩发出蓝-绿光的。QD染料通过以下方式制备:通过将QD与适合的溶剂以及任选的添加剂结合,以改变例如染料的涂布性能和/或其对纺织物的粘着性。QD染料通过任何适合的沉积方法涂覆至纺织材料,包括但不限于,将材料浸于染料溶液中、滴落涂布(dropcasting)或喷墨印刷。在将染料涂覆至材料之后,任选借助应用温和的热使材料干燥,以将溶剂蒸发。不同于对于其来说吸收不需要的波长的滤色器,QD磷光体吸收高能量辐射并且以相对少的能量损失在较长波长发光,这是由纳米粒子的光致发光QY决定的。在核/(多)壳QD的现有技术中详细地记载了大于80%的QY。
在备选的实施方案中,将绿色QD结合至使用蓝色固态LED灯远程照射的温育器组件中。可以通过将QD结合至构成其的塑料中来制造温育器组件。例如,申请人的美国专利号8,168,457描述了模制的含QD的塑料材料的制备,其通过引用结合在本文中。备选地,可以将QD作为涂层涂覆至预制的温育器的外表面和/或内表面。
可以合成包括掺杂的物种及其合金的CdSe系和InP系QD以提供蓝色至绿色的发光。在申请人的美国专利号7,803,423、7,985,466、8,062,703、7,588,828和7,867,556中提供了制备这种QD材料的方法的实例。然而,应该理解的是,在本文中所描述的实施方案不限于通过任何特定方法制备的QD。
光动力学疗法
利用QD,可以调节固态LED的发射以匹配用于***和良性病况如湿性年龄相关黄斑变性的光敏化分子的吸收光谱中的峰波长和相对强度(通过改变每种颜色的QD的相对浓度)。利用QD,对于PDT,600-850nm“光学窗口”下的发光是可能的。利用QD,还可以实现来自单一光源的多色发光;通过包括较高活性但是较低穿透性的波长,即蓝色-绿色发光,这可以提高组织表面附近的肿瘤坏死,而仍然可以向组织中较深的靶标细胞发射较高穿透性的波长,即红色-IR。
PDT***可以采用光纤导管以将特定波长的光引导至身体中的靶标组织。在欧洲专利申请EP0783784中教导了填充有分散在液体支持介质中的QD的光纤。通过将固态光源如LED或激光与在用于PDT的光学窗口内的特定波长处发光的QD结合,这种光纤设备可以用于PDT用途。
红色和IR光疗法
可以将发红光和/或IR的QD结合至可以应用于皮肤的装置以在伤口愈合和化妆品光疗法中使用。使用蓝色固态LED作为一次光源,红色和/或IRQD磷光体可以用于使发光降频变换以刺激胶原蛋白产生和重建。
对于促进伤口愈合来说,可以将QD结合至随后用于将无菌纱布或疏松编织的外科手术敷料染色的染料中,使得来自一次光源(根据厚度,位于敷料附近或在敷料中)的光激发与皮肤接触的敷料中的QD。
备选地,如图3中所示,可以组装多层敷料,其包括嵌入在闭塞敷料层中、被半透明敷料层覆盖的QDLED芯片阵列(和电路)。由QDLED芯片发出的光经过半透明敷料层到达伤口。通过将QDLED芯片嵌入至闭塞敷料中,该设备实现了向绝不能暴露于空气(例如,防止感染)的伤口施用光疗法。
在备选的实施方案中,如在申请人的美国专利号8,168,457中描述的,可以将QD结合至透明或半透明的成形制品中。可以在要向其施用的病人身体部分的石膏中将成形制品成型。例如,对于面部组织的恢复来说,可以制造QD面膜形式的成形制品并且将其涂覆至脸上。之后通过一次光源如蓝色LED灯照射QD面膜。在照射时,面膜中的QD将一部分光降频变换以在促进皮肤恢复的波长处发光。
白光光疗法
可以使用QD制造发射具有可调整的相关色温(CCT)的白光的LED,其可以用于治疗昼夜节律和季节性情绪失调。CCT量化所发射的白光的“色度(shade)”,其可以被调节以用于治疗目的。例如,接近自然日光(约5,500-6,500K)的CCT可以有益于昼夜节律失调如季节性情绪失调的治疗。
在一些实施方案中,如在图4中所示,制造发白光的光疗法灯,其包括一次光源和包括QD的灯罩。如美国专利号8,168,457中描述的,可以通过将QD结合至透明或半透明的成形制品中来制备灯罩。QD吸收一部分一次光以产生具有所需色温的白光。在一个实施方案中,光疗法灯包含与包括红色和绿色QD的灯罩组合的蓝色LED一次光源以产生具有在5,500-6,500K范围内的CCT的冷白光,从而模拟自然日光以用于季节性情绪失调的治疗。图5中示出了包括蓝色LED背光和红色和绿色QD、具有5,536K的CCT的白色照明设备的实例。白点位于普朗克轨迹(黑体辐射源在色度空间中随色温变化而将采取的路径)附近,表明所发出的光与在相同色温下太阳所发处的光接近。可以通过改变QD的发射波长和/或蓝光:绿色QD:红色QD的比率来调节CCT。发红光和绿光的纳米粒子的适合的实例包括,但不限于,CdSe和InP,并且包括掺杂物种及其合金。
实施例
在以下实施例中说明了用于特定光疗法用途的QDLED的发射光谱的调节。
实施例1:在光动力学疗法窗口内发光的QDLED
使用通过在446nm发光的蓝色固态LED背光照射的CdSe/CdS/CdZnS/ZnS核-多壳QD制造包括蓝色固态LED作为一次光源和红色量子点硅氧烷树脂的、具有在用于PDT的光学窗口下的红色发光的QDLED芯片。625nm的QD光致发光最大值(PLmax)在HpD的红色吸收带(620-635nm)内,具有35nm的窄FWHM。因此,其可以适用于利用衍生自卟啉的光敏剂作为二极管激光灯的备选方案的PDT。可以通过改变QD浓度来调节相对的蓝色和红色峰强度。
发射光谱在图6中示出。
实施例2具有深红色发光以促进伤口愈合的QDLED
根据以下步骤制造包括蓝色固态LED作为一次光源和红色量子点硅氧烷树脂的QDLED芯片:
将硅氧烷树脂与少量Pt催化剂混合,之后加入红色InP/ZnSQD珠(20个OD/10mmol甲苯中的溶液)并且将混合物转移至LED盒中。将LED在氮气氛下固化。
通过22mW蓝色固态LED照射QDLED。看到在大约442nm的来自固态LED的蓝色发光。红色QD材料以PLmax=653nm和FWHM=60nm发光。这种深红色发光可以适用于伤口愈合或化妆品光疗法。蓝色(LED)相对红色(QD磷光体)光的相对强度为1:1.34,但是可以通过改变QD浓度来调节。发射光谱在图7中示出。
已经参照特定的非限制性实施方案在本文中描述了本发明。应该理解的是,在不背离本发明的范围的情况下,许多修改和排列是可能的。
Claims (6)
1.一种用于光疗法的医用敷料,所述敷料包括:
配置在闭塞层中并且被半透明层覆盖的量子点发光二极管芯片。
2.如权利要求1中所述的装置,其中所述量子点发光二极管芯片包括发射红光或红外线的量子点。
3.如权利要求1中所述的装置,其中所述量子点发光二极管芯片包括包含CdSe、InP、CdTe、PbSe、InAs或Cu(In、Ga)(S、Se)2或它们的掺杂或合金衍生物的量子点。
4.一种用于光疗法的医用敷料,所述敷料包括:
闭塞层和半透明层,以及
浸于所述闭塞层或所述半透明层之一或二者中的量子点。
5.如权利要求4中所述的装置,其中所述量子点包括发射红光或红外线的量子点。
6.如权利要求4中所述的装置,其中所述量子点包含CdSe、InP、CdTe、PbSe、InAs或Cu(In、Ga)(S、Se)2或它们的掺杂或合金衍生物。
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