Real-Time Monitoring of ATP-Responsive Drug Release Using Mesoporous-Silica-Coated Multicolor Upconversion Nanoparticles.
Real-Time Monitoring of ATP-Responsive Drug Release Using Mesoporous-Silica-Coated Multicolor Upconversion Nanoparticles.
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DOI：
10.1021/acsnano.5b00641
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发表时间：
2015-05-26
期刊：
影响因子：
17.1
通讯作者：
Lee KB
中科院分区：
文献类型：
--
作者：
Lai J;Shah BP;Zhang Y;Yang L;Lee KB
近年来，由于材料科学和纳米医学取得了前所未有的进展，刺激响应型药物递送载体引起了人们的极大兴趣。然而，由于成像方式的限制，具有集成实时监测能力的刺激响应设备的开发仍处于起步阶段。在本文中，我们描述了一种多肽包裹的介孔二氧化硅包覆的上转换纳米颗粒（UCNP@MSN）作为三磷酸腺苷（ATP）响应性药物递送系统（DDS）的长期跟踪和实时监测药物释放的发展。我们的UCNP@MSN在UV-NIR波长范围内具有多个发射峰，在其外表面上用锌-吡啶二甲基胺类似物（TDPA-Zn 2+）官能化，并在内部介孔中负载小分子药物如化疗剂。当纳米颗粒用紧凑的支化多肽聚（Asp-Lys）-b-Asp包裹时，药物保持包埋在UCNP-MSN内，因为多肽中存在的Asp部分与UCNP-MSN表面上存在的TDPA-Zn 2+复合物之间存在多价相互作用。这导致从UCNP到包封的药物的发光共振能量转移（LRET），其通常在UV-可见光范围内具有吸收，最终导致UV-可见光范围内UCNP发射的淬灭，同时保留其强NIR发射。加入ATP导致ATP竞争性置换表面结合的多肽，由于其对TDPA-Zn 2+的更高亲和力，这导致包埋药物的释放和随后的LRET消除。监测这种ATP触发的LRET比率变化，使我们能够实时监测释放的药物。鉴于这些结果，我们设想我们提出的UCNP@ MSN-多肽混合纳米颗粒具有巨大的潜力，用于刺激响应性药物递送以及监测活癌和干细胞中发生的生化变化。
Stimuli-responsive drug delivery vehicles have garnered immense interest in recent years due to unparalleled progress made in material science and nanomedicine. However, the development of stimuli-responsive devices with integrated real-time monitoring capabilities is still in its nascent stage because of the limitations of imaging modalities. In this paper, we describe the development of a polypeptide-wrapped mesoporous-silica-coated multicolor upconversion nanoparticle (UCNP@MSN) as an adenosine triphosphate (ATP)-responsive drug delivery system (DDS) for long-term tracking and real-time monitoring of drug release. Our UCNP@MSN with multiple emission peaks in UV-NIR wavelength range was functionalized with zinc-dipicolylamine analogue (TDPA-Zn2+) on its exterior surface and loaded with small-molecule drugs like chemotherapeutics in interior mesopores. The drugs remained entrapped within the UCNP-MSNs when the nanoparticles were wrapped with a compact branched polypeptide, poly(Asp-Lys)-b-Asp, because of multivalent interactions between Asp moieties present in the polypeptide and the TDPA-Zn2+ complex present on the surface of UCNP-MSNs. This led to luminescence resonance energy transfer (LRET) from the UCNPs to the entrapped drugs, which typically have absorption in UV–visible range, ultimately resulting in quenching of UCNP emission in UV–visible range while retaining their strong NIR emission. Addition of ATP led to a competitive displacement of the surface bound polypeptide by ATP due to its higher affinity to TDPA-Zn2+, which led to the release of the entrapped drugs and subsequent elimination of LRET. Monitoring of such ATP-triggered ratiometric changes in LRET allowed us to monitor the release of the entrapped drugs in real-time. Given these results, we envision that our proposed UCNP@MSN-polypeptide hybrid nanoparticle has great potential for stimuli-responsive drug delivery as well as for monitoring biochemical changes taking place in live cancer and stem cells.
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