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. 2013 Dec 23;52(52):13958-13964.
doi: 10.1002/anie.201308986. Epub 2013 Dec 6.

Biodegradable gold nanovesicles with an ultrastrong plasmonic coupling effect for photoacoustic imaging and photothermal therapy

Peng Huang #  1 , Jing Lin #  2 , Wanwan Li  1 , Pengfei Rong  1 , Zhe Wang  1 , Shouju Wang  1 , Xiaoping Wang  1 , Xiaolian Sun  1 , Maria Aronova  3 , Gang Niu  1 , Richard D Leapman  3 , Zhihong Nie  2 , Xiaoyuan Chen  1
Affiliations

Biodegradable gold nanovesicles with an ultrastrong plasmonic coupling effect for photoacoustic imaging and photothermal therapy

Peng Huang et al. Angew Chem Int Ed Engl. .

Abstract

The hierarchical assembly of gold nanoparticles (GNPs) allows the localized surface plasmon resonance peaks to be engineered to the near-infrared (NIR) region for enhanced photothermal therapy (PTT). Herein we report a novel theranostic platform based on biodegradable plasmonic gold nanovesicles for photoacoustic (PA) imaging and PTT. The disulfide bond at the terminus of a PEG-b-PCL block-copolymer graft enables dense packing of GNPs during the assembly process and induces ultrastrong plasmonic coupling between adjacent GNPs. The strong NIR absorption induced by plasmon coupling and very high photothermal conversion efficiency (η=37%) enable simultaneous thermal/PA imaging and enhanced PTT efficacy with improved clearance of the dissociated particles after the completion of PTT. The assembly of various nanocrystals with tailored optical, magnetic, and electronic properties into vesicle architectures opens new possibilities for the construction of multifunctional biodegradable platforms for biomedical applications.

Keywords: biodegradable block copolymers; gold nanovesicles; photoacoustic imaging; photothermal therapy; plasmonic coupling.

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Figures

Figure 1
Figure 1
Plasmonic BGVs self-assembled from GNPs (26.2 ± 1.45 nm). (a) SEM (Inset: 3-D electron density mapping of a broken BGV) and (b) TEM images (Inset: individual BGV). (c) SEM images of GV, BGV1, BGV2, and BGV3. (d) UV-vis-NIR spectra of GNPs, PEG-b-PS tethered gold vesicles (GVs), and block co-polymer (BCP)-tethered biodegradable gold vesicles produced by dialysis of 100, 150, and 250 100 μg/mL THF solution of GNPs. The LSPR peaks of BGVs can be tuned by varying the GNP concentration.
Figure 2
Figure 2
(a) Temperature elevation of the aqueous solutions of GNPs, GNRs, GVs and BGVs exposed to laser (1 W/cm2) as a function of irradiation time. GNPs (same Au concentration with BGVs, λex= 808 nm). GNRs (OD@808 nm=1, λex= 808 nm). GVs (OD@671 nm=1, λex= 671 nm).BGVs (OD@808 nm=1, λex= 808 nm). The irradiation lasted for 5 min, and then the laser was turned off. Pure water was used as a negative control. (b) Photothermal conversion efficiencies of BGVs, GVs, GNRs and GNSs. (c) TEM images of BGVs after being treated at different temperatures for 10 min.
Figure 3
Figure 3
(a) Thermal images of MDA-MB-435 tumor-bearing mice exposed to 808 nm laser for 5 min at post-injection of PBS or BGVs. (b) Heating curves of tumors upon laser irradiation as a function of irradiation time. (c) PA signals of BGVs and GNRs as a function of optical density. (d) In vivo 2D and 3D ultrasonic (US) and photoacoustic (PA) images of tumor tissues at pre-injection and post-injection of BGVs. Arrows indicate the location of BGVs. (e) PA intensities of tumor tissues with intratumoral administration of the same amount of GVs or BGVs.
Figure 4
Figure 4
(a) Tumor growth curves of different groups of MDA-MB-435 tumor-bearing mice after treatment. Tumor volumes were normalized to their initial sizes. Error bars represent the standard deviations of 5-7 mice per group. Asterisk indicates P < 0.01. (b) The photographs of MDA-MB-435 tumor-bearing mice at different days after BGV treatment. (c) Survival curves of tumor-bearing mice after various treatments. BGVs injected mice after PTT treatment showed 100% survival over 30 days. (d) Pharmacokinetics of BGVs after intratumoral injection of 50 μL of BGVs (400 μg/mL). Inductively coupled plasma mass spectrometry (ICP-MS) analysis of Au in different organs at 1, 2 and 8 days post-injection (n = 3/group). (e) H&E staining of tumor sections collected from different groups of mice after laser irradiation.
Scheme 1
Scheme 1
Self-assembly of biodegradable gold vesicles (BGVs) composed of poly(ethylene glycol)-b-poly(ε-caprolactone) (PEG-b-PCL) tethered GNPs via dot-line-plane-vesicle mode during the dialysis process. BGVs with ultra-strong plasmonic coupling effect are superior photoacoustic (PA) imaging and photothermal therapy (PTT) agents with improved clearance after the dissociation of assemblies. PA signal and PTT efficiency of BGVs are increased with the decrease of d (distance between adjacent GNPs).
See this image and copyright information in PMC

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