卟啉基金属有机框架负载高铁酸钾: 光-化学动力学联合治疗肿瘤性能研究

doi:10.15541/jim20210157

无机材料学报 ›› 2021, Vol. 36 ›› Issue (12): 1305-1315.DOI: 10.15541/jim20210157

所属专题：【生物材料】肿瘤治疗；【能源环境】金属有机框架材料

卟啉基金属有机框架负载高铁酸钾: 光-化学动力学联合治疗肿瘤性能研究

王玉伟¹^,²(), 陈佳杰², 田正芳³, 朱敏¹(), 朱钰方²()

1.上海理工大学材料科学与工程学院, 上海 200093
2.中国科学院上海硅酸盐研究所, 上海200050
3.黄冈师范学院化学化工学院催化材料制备及应用湖北省重点实验室, 黄冈438000

收稿日期:2021-03-12 修回日期:2021-04-15 出版日期:2021-12-20 网络出版日期:2021-06-01
通讯作者: 朱敏, 副教授. E-mail: mzhu@usst.edu.cn;朱钰方, 教授. E-mail: zjf2412@163.com
作者简介:王玉伟(1993-), 女, 硕士研究生. E-mail: 676627664@qq.com
基金资助:
上海理工大学科技发展项目(2018KJFZ016);上海理工大学科技发展项目(2019KJFZ023)

Potassium Ferrate-loaded Porphyrin-based (VI) Metal-organic Frameworks for Combined Photodymanic and Chemodynamic Tumor Therapy

WANG Yuwei¹^,²(), CHEN Jiajie², TIAN Zhengfang³, ZHU Min¹(), ZHU Yufang²()

1. School of Materials Science and Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China
2. Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China
3. Hubei Key Laboratory of Processing and Application of Catalytic Materials, College of Chemical Engineering, Huanggang Normal University, Huanggang 438000, China

Received:2021-03-12 Revised:2021-04-15 Published:2021-12-20 Online:2021-06-01
Contact: ZHU Min, associate professor. E-mail: mzhu@usst.edu.cn;ZHU Yufang, professor. E-mail:zjf2412@163.com
About author:WANG Yuwei (1993-), female, Master candidate. E-mail: 676627664@qq.com
Supported by:
Project of University of Shanghai for Science and Technology(2018KJFZ016);Project of University of Shanghai for Science and Technology(2019KJFZ023)

摘要/Abstract

摘要：

金属有机框架因具有多孔结构、高比表面积、丰富的官能团和金属活性位点以及良好的生物相容性和降解性而被广泛应用于生物医学领域。本研究提出以卟啉基金属有机框架纳米颗粒(PCN-224)为载体负载高化学价态的高铁酸钾氧化剂(K₂FeO₄, Fe(VI)), 经牛血清蛋白(BSA)包覆表面制备多功能复合纳米颗粒(Fe(VI)@PCN@BSA), 用于肿瘤光-化学动力学联合治疗。实验结果表明, PCN-224纳米颗粒粒径约为90 nm, 而Fe(VI)@PCN@BSA纳米颗粒粒径约为100 nm。Fe(VI)@PCN@BSA纳米颗粒在模拟肿瘤微环境条件下能够催化H₂O₂反应, 产生有细胞毒性的•OH而实现化学动力学效应, 同时也能够氧化分解部分H₂O₂产生O₂, 在660 nm激光照射下提高单线态氧(¹O₂)产生量, 增强光动力学效应。进一步细胞实验证实Fe(VI)@PCN@BSA纳米颗粒具有较好的生物相容性, 能够获得增强的光-化学动力学联合治疗肿瘤效果。因此, Fe(VI)@PCN@BSA纳米颗粒在肿瘤治疗方面具有潜在的应用前景。

关键词: 金属有机框架, 高铁酸钾, 肿瘤微环境, 联合治疗

Abstract:

Metal-organic frameworks (MOFs) are widely used in biomedicine due to their porous structure, high specific surface area, abundant functional groups with metal active sites, good biocompatibility, and suitable degradability. In this study, a multifunctional composite nanoparticle (Fe(VI)@PCN@BSA) was prepared for combined photodynamic and chemodynamic therapy of tumors, which was constructed by loading potassium ferrate (K₂FeO₄, Fe(VI)) in porphyrin-based MOFs (PCN-224) and following a surface coating with biocompatible bovine serum albumin (BSA). The results showed that the particle sizes of PCN-224 and Fe(VI)@PCN@BSA nanoparticles were about 90 nm and 100 nm, respectively. Interestingly, Fe(VI)@PCN@BSA nanoparticles could catalyze H₂O₂to produce •OH under a simulating tumor environmental condition. Meanwhile, they catalyzed to decompose H₂O₂ to produce O₂, and thereby increased the production of singlet oxygen (¹O₂) under 660 nm laser irradiation, which enhanced the photodynamic effect. More importantly, in vitro evaluation indicated that Fe(VI)@PCN@BSA nanoparticles were biocompatible, and exhibited enhanced photodynamic and chemodynamic combined therapeutic efficacy against tumor cells. Hence, Fe(VI)@PCN@BSA nanoparticles have a great potential application in tumor therapy.

Key words: metal-organic framework, potassium ferrate, tumor microenvironment, combination therapy

中图分类号:

TQ174

王玉伟, 陈佳杰, 田正芳, 朱敏, 朱钰方. 卟啉基金属有机框架负载高铁酸钾: 光-化学动力学联合治疗肿瘤性能研究[J]. 无机材料学报, 2021, 36(12): 1305-1315.

WANG Yuwei, CHEN Jiajie, TIAN Zhengfang, ZHU Min, ZHU Yufang. Potassium Ferrate-loaded Porphyrin-based (VI) Metal-organic Frameworks for Combined Photodymanic and Chemodynamic Tumor Therapy[J]. Journal of Inorganic Materials, 2021, 36(12): 1305-1315.

图/表 11

图1 (a)PCN-224、(b)Fe(VI)@PCN-224和(c)Fe(VI)@PCN @BSA纳米颗粒的TEM照片及(d)Fe(VI)@PCN@BSA纳米颗粒的元素分布图

Fig. 1 TEM images of (a) PCN-224, (b) Fe(VI)@PCN-224 and (c) Fe(VI)@PCN@BSA nanoparticles, and (d) elemental mapping of Fe(VI)@PCN@BSA nanoparticles

图2 K2FeO4、PCN-224、Fe(VI)@PCN-224和Fe(VI)@PCN @BSA纳米颗粒的XRD图谱

Fig. 2 XRD patterns of K2FeO4, PCN-224, Fe(VI)@PCN-224, and Fe(VI)@PCN@BSA nanoparticles

图3 (a)PCN-224、(b)Fe(VI)@PCN-224和(c)Fe(VI)@PCN@BSA纳米颗粒的DLS粒径分布图以及(d)BSA和PCN-224、Fe(VI)@PCN-224、Fe(VI)@PCN@BSA纳米颗粒的表面Zeta电位

Fig. 3 DLS size distributions of (a) PCN-224, (b) Fe(VI)@PCN-224 and (c) Fe(VI)@PCN@BSA nanoparticles, and (d) Zeta potentials of BSA, PCN-224, Fe(VI)@PCN, and Fe(VI)@PCN@BSA nanoparticles

图4 Fe(VI)@PCN@BSA纳米颗粒在H2O、PBS和DEME培养基中的(a)粒径和(b)Zeta电位的变化图

Fig. 4 Changes of (a) size and (b) Zeta potential of Fe(VI)@PCN@BSA nanoparticles in H2O, PBS and DEME

图5 (a)PCN-224、Fe(VI)@PCN-224和Fe(VI)@PCN@BSA纳米颗粒的紫外-可见光吸收光谱图, 其中插图为纳米颗粒悬浮液的光学照片, 以及(b)BSA、PCN-224、Fe(VI)@PCN-224和Fe(VI)@PCN@BSA纳米颗粒的傅里叶变换红外光谱图

Fig. 5 (a) UV-Vis absorption spectra of PCN-224, Fe(VI)@PCN-224, and Fe(VI)@PCN@BSA suspensions (inset is pictures of the suspensions), and (b) Fourier transform infrared spectra of BSA, PCN-224, Fe(VI)@PCN-224, and Fe(VI)@PCN@BSA nanoparticles

图6 Fe(VI)@PCN@BSA 纳米颗粒的化学动力学性能

Fig. 6 Chemodynamic properties of Fe(VI)@PCN@BSA nanoparticles (a) UV-Vis absorption spectra of TMB solutions under different conditions with inset showing photographs of TMB solutions after reaction for 10 min under different conditions; (b) Absorbance changes of TMB solutions with time after adding Fe(VI)@PCN@BSA nanoparticles (50 µg/mL) into TMB solutions under pH 6.0 with H2O2 (10 mmol/L); (c) Absorbance changes of TMB solutions with time after adding Fe(VI)@PCN@BSA nanoparticles (50 µg/mL) into TMB solutions with pH 6.0; (d) Absorbance changes of TMB solutions with time under pH 6.0 with H2O2 (10 mmol/L); (e) Curves of absorbance at 652 nm versus time for TMB solutions with Fe(VI)@PCN@BSA nanoparticles under acidic (pH 6.0) or neutral (pH 7.4) conditions with or without H2O2; (f) Absorbance changes at 652 nm versus time for TMB solutions under pH 6.0 with different concentrations of H2O2 after adding the same amount of Fe(VI)@PCN@BSA nanoparticles

图7 (a)pH 6.0和(b)pH 7.4, 不同H2O2浓度的乙酸钠测试液中加入Fe(VI)@PCN@BSA纳米颗粒(50 μg/mL)后的溶解氧含量变化图

Fig. 7 Changes of dissolved O2 in NaAc solutions under (a) pH 6.0 and (b) pH 7.4 with different H2O2 concentrations after the addition of Fe(VI)@PCN@BSA nanoparticles (50 μg/mL)

图8 (a~c)加入Fe(VI)@PCN@BSA纳米颗粒(50 μg/mL)的DPBF溶液在不同处理条件下的紫外-可见光吸收光谱图及(d)不同组别的DPBF溶液在439 nm处的特征吸收值变化图

Fig. 8 (a-c) UV-Vis absorbance spectra of the DPBF solutions with Fe(VI)@PCN@BSA nanoparticles (50 μg/mL) and (d) absorbance changes of DPBF solutions at 439 nm for different groups (a) Without 660 nm laser irradiation; (b) With 660 nm laser irradiation; (c) With H2O2 (10 mmol/L) and 660 nm laser irradiation

图9 不同浓度Fe(VI)@PCN@BSA纳米颗粒对MDA-MB- 231 细胞和成纤维细胞作用24 h后的细胞存活率

Fig. 9 Cell viabilities of MDA-MB-231 cells and human dermal fibroblasts after 24 h incubation with Fe(VI)@PCN@BSA nanoparticles at different concentrations

图10 不同条件处理的MDA-MB-231细胞内ROS的荧光显微照片

Fig. 10 Fluorescence images of MDA-MB-231 cells after different treatments for observing intracellular ROS Control: cells were cultured in normal medium; NPs: cells were cultured in normal medium with Fe(VI)@PCN@BSA nanoparticles; H2O2 (pH 6.0): cells were cultured in the medium at pH 6.0 with H2O2 (100 µmol/L); NPs+H2O2 (pH 6.0): cells were cultured in the medium at pH 6.0 with H2O2 (100 µmol/L) and Fe(VI)@PCN@BSA nanoparticles; Laser: 660 nm laser irradiation after cells culture in normal medium; NPs+Laser: 660 nm laser irradiation after cell culture in normal medium with Fe(VI)@PCN@BSA nanoparticles; NPs+H2O2 (pH 6.0)+Laser: 660 nm laser irradiation after cell culture in the medium at pH 6.0 with H2O2 (100 µmol/L) and Fe(VI)@PCN@BSA nanoparticles

图11 Fe(VI)@PCN@BSA纳米颗粒对MDA-MB-231细胞的联合治疗评估(*P < 0.05, **P < 0.01, ***P < 0.001)

Fig. 11 Synergistic therapeutic effect of Fe(VI)@PCN@BSA nanoparticles on MDA-MB-231 cells (*P < 0.05, **P < 0.01, ***P < 0.001)

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卟啉基金属有机框架负载高铁酸钾: 光-化学动力学联合治疗肿瘤性能研究

Potassium Ferrate-loaded Porphyrin-based (VI) Metal-organic Frameworks for Combined Photodymanic and Chemodynamic Tumor Therapy

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