高效靶向示踪钙钛矿纳米系统光电增效抗肿瘤

doi:10.1016/j.actphy.2024.100042

物理化学学报 >> 2025, Vol. 41 >> Issue (5): 100042.doi: 10.1016/j.actphy.2024.100042

高效靶向示踪钙钛矿纳米系统光电增效抗肿瘤

李坚¹^,²^,³^,†, 张毓²^,†, 闫融融¹^,⁴^,†, 孙开媛⁵, 刘晓晴¹, 梁子尚¹^,⁴, 焦忆楠⁴, 卜晖²^,*(), 陈欣¹^,⁶^,*(), 赵晋津¹^,*(), 施剑林⁷

¹ 河北师范大学化学与材料科学学院, 河北省能量转换材料与器件技术创新中心, 薄膜太阳能电池材料与器件工程研究中心, 河北省无机纳米材料重点实验室, 石家庄 050024
² 河北医科大学第二医院神经内科, 临床神经病学教育部重点实验室, 河北省神经病学重点实验室, 石家庄 050051
³ 衡水市人民医院全科医学科, 河北衡水 053000
⁴ 石家庄铁道大学材料科学与工程学院, 石家庄 050043
⁵ 北京航空航天大学生物与医学工程学院, 北京 100191
⁶ 邢台市人民医院神经内科, 邢台市神经病学重点实验室, 河北邢台 054001
⁷ 中国科学院上海硅酸盐研究所, 上海 200050

收稿日期:2024-10-18 修回日期:2024-11-29 录用日期:2024-11-30 发布日期:2025-04-18
通讯作者: Email: jinjinzhao2012@163.com (赵晋津) Email: jinjinzhao2012@163.com (Jinjin Zhao)26500825@hebmu.edu.cn (卜晖)xinc2019@126.com (陈欣)
作者简介:
^†These authors contributed equally.
基金资助:
国家自然科学基金(U2130128); 河北省自然科学基金-燕赵青年科学家专项(B2023205040); 河北省自然科学基金-京津冀基础研究合作专项(H2022205047); 河北省自然科学基金-京津冀基础研究合作专项(22JCZXJC00060); 河北省自然科学基金-京津冀基础研究合作专项(E3B33911DF); 中央引导地方科技发展资金项目(236Z7753G); 中央引导地方科技发展资金项目(246Z7755G); 河北省高等学校科学研究项目基础研究重点培育专项(JCZX2025007); 河北省科技厅引智与人才培养专项基金; 河北省创新能力提升计划(22567604H); 河北师范大学博士科研启动基金(L2023B18); 大学生创新创业训练计划项目(S202410094046)

Highly Efficient, Targeted, and Traceable Perovskite Nanocrystals for Photoelectrocatalytic Oncotherapy

Jian Li¹^,²^,³, Yu Zhang², Rongrong Yan¹^,⁴, Kaiyuan Sun⁵, Xiaoqing Liu¹, Zishang Liang¹^,⁴, Yinan Jiao⁴, Hui Bu²^,*(), Xin Chen¹^,⁶^,*(), Jinjin Zhao¹^,*(), Jianlin Shi⁷

¹ College of Chemistry and Materials Science, Hebei Technology Innovation Center for Energy Conversion Materials and Devices, Hebei Key Laboratory of Inorganic Nanomaterials, Engineering Research Center of Thin Film Solar Cell Materials and Devices, Hebei Province, Hebei Normal University, Shijiazhuang 050024, China
² Department of Neurology, The Second Hospital of Hebei Medical University, Key Laboratory of Clinical Neurology (Hebei Medical University), Ministry of Education, Neurological Laboratory of Hebei Province, Shijiazhuang 050051, China
³ General Practice Department, Hengshui People's Hospital, Hengshui 053000, Hebei Province, China
⁴ School of Materials Science and Engineering, Shijiazhuang Tiedao University, Shijiazhuang 050043, China
⁵ School of Biological Science and Medical Engineering, Beihang University, Beijing 100191, China
⁶ Department of Neurology, Xingtai People's Hospital, Xingtai Key Laboratory of Neurology, Xingtai 054001, Hebei Province, China
⁷ Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China

Received:2024-10-18 Revised:2024-11-29 Accepted:2024-11-30 Published:2025-04-18
Contact: 26500825@hebmu.edu.cn (Hui Bu)xinc2019@126.com (Xin Chen)
Supported by:
the National Natural Science Foundation of China(U2130128); the Yanzhao Young Scientist Project from Hebei Natural Science Foundation(B2023205040); the Basic Research Cooperation Special Foundation of Beijing-Tianjin-Hebei Region from Hebei Natural Science Foundation(H2022205047); the Basic Research Cooperation Special Foundation of Beijing-Tianjin-Hebei Region from Hebei Natural Science Foundation(22JCZXJC00060); the Basic Research Cooperation Special Foundation of Beijing-Tianjin-Hebei Region from Hebei Natural Science Foundation(E3B33911DF); the Central Government Guiding Local Science and Technology Development Project(236Z7753G); the Central Government Guiding Local Science and Technology Development Project(246Z7755G); Key Cultivation Special Project for Basic Research from Hebei Education Department(JCZX2025007); Introducing Intelligence and Talent Cultivation Special Fundation from Hebei Provincial Department of Science and Technology; the Innovation Capability Improvement Plan Project of Hebei Province(22567604H); the Ph.D Scientific Research Start-up Fund of Hebei Normal University(L2023B18); the College student's innovation and entrepreneurship training plan program(S202410094046)

1. WHXB202410014-SI-4p.pdf(2188KB)

摘要/Abstract

摘要：

金属卤化物钙钛矿由于其多维度的晶体结构和优良的荧光成像/示踪及光电转换性质，使其成为一种非常具有前瞻性的光电增效治疗肿瘤材料。然而，传统卤化物钙钛矿纳米晶的水稳定性问题，限制了其应用于生物成像和光电增效肿瘤治疗的药物递送纳米系统研究。本文将甲氨蝶呤-壳聚糖-叶酸(MTX-CS-FA)成功与钙钛矿纳米晶体CsSn_0.5Pb_0.5Br₃ (PeNCs)铆钉连接，制备出了可以在水中稳定228 d且发绿光的PeNCs@MTX-CS-FA纳米载药体系。在可见光照射下，新型PeNCs@MTX-CS-FA纳米载药体系增效抗肿瘤治疗原理：钙钛矿纳米晶体产生电子和活性氧(ROS)；钙钛矿光生空穴耗竭过表达的谷胱甘肽(GSH)；甲氨蝶呤(MTX)抑制二氢叶酸还原酶(DHFR)活性，导致肿瘤细胞的脂质过氧化，上述三点共同作用抑制肿瘤细胞的增殖、促进肿瘤细胞凋亡。在动物体内实验中，采用小鼠移植肿瘤模型，累积用药量达2.4 mg PeNCs@MTX-CS-FA纳米载药系统时，肿瘤体积减少了约63.68%和肿瘤重量下降了约63.26%。通过生物安全性评估实验证实，在治疗剂量下，小鼠肝、肾等器官功能正常，说明纳米体系具有良好的生物安全性，并且研究发现钙钛矿纳米颗粒经小鼠肠道排出，小鼠粪便呈现出与原始钙钛矿晶体相同的绿色荧光，金属卤化物钙钛矿纳米载药体系在生物成像和光电催化化疗方面呈现优异的增效抗肿瘤治疗效果。

关键词: 肿瘤治疗, 生物成像, 钙钛矿纳米颗粒, 光电催化化疗

Abstract:

Metal halide perovskites have emerged as highly promising materials in optoelectronics, owing to their unique multidimensional crystal structures that impart exceptional optical and electronic properties. These materials exhibit remarkable fluorescence imaging and tracking capabilities, as well as efficient photoelectric conversion, making them suitable for a broad range of applications. Nevertheless, despite their significant potential, their poor water stability has posed a major challenge, particularly in biomedical fields such as drug delivery systems, biological imaging, and photoelectrocatalytic oncotherapy. This limitation has hindered their practical use in medical treatments and diagnostics. In this study, we address the water stability issue by successfully synthesizing CsSn_0.5Pb_0.5Br₃ perovskite nanocrystals (PeNCs) and conjugating them with methotrexate-chitosan-folic acid (MTX-CS-FA), resulting in innovative green light-emitting PeNCs@MTX-CS-FA nanoparticles. These nanoparticles exhibited remarkable water stability, maintaining their structural and functional integrity for up to 228 d, a significant improvement that enables their application in complex biological environments. Under visible light illumination, the nanoparticles demonstrated a dual-action therapeutic mechanism. The perovskites effectively generated electrons and reactive oxygen species (ROS), inducing oxidative stress in tumor cells. At the same time, photogenerated holes oxidized glutathione (GSH), a molecule that is typically overexpressed in tumor cells to protect against oxidative damage. By depleting GSH, the nanoparticles weakened the tumor cells' efense mechanisms, thereby enhancing the oxidative damage caused by ROS. In addition, methotrexate (MTX), a chemotherapeutic agent integrated into the system, inhibited dihydrofolate reductase (DHFR) activity. This inhibition disrupted tumor cell metabolism, particularly nucleotide synthesis, leading to lipid peroxidation and subsequent cell death. Together, these mechanisms generated a potent, synergistic therapeutic effect. The therapeutic efficacy of the PeNCs@MTX-CS-FA nanoparticles was validated through in vivo antitumor experiments in mice. A total dose of 2.4 mg of nanoparticles resulted in a 63.68% reduction in tumor volume and a 63.26% decrease in tumor weight, demonstrating significant tumor growth suppression. Biological safety evaluations further confirmed the nanoparticles' biocompatibility. Notably, they were excreted from the mice in their fluorescent form without decomposition, ensuring minimal long-term toxicity. This safe excretion pathway underscores the feasibility of repeated use of these nanoparticles in clinical applications. Overall, this study highlights the transformative potential of metal halide perovskites in cancer treatment. By overcoming the water stability limitations that have previously constrained their biomedical applications, the PeNCs@MTX-CS-FA nanoparticles exhibited outstanding capabilities in real-time bioimaging and effective photoelectrocatalytic chemotherapy, thus paving the way for future innovations in biomedical science.

Key words: Oncotherapy, Bioimaging, Perovskite nanoparticle, Photoelectrocatalytic chemotherapy

李坚, 张毓, 闫融融, 孙开媛, 刘晓晴, 梁子尚, 焦忆楠, 卜晖, 陈欣, 赵晋津, 施剑林. 高效靶向示踪钙钛矿纳米系统光电增效抗肿瘤[J]. 物理化学学报, 2025, 41(5), 100042. doi: 10.1016/j.actphy.2024.100042

Jian Li, Yu Zhang, Rongrong Yan, Kaiyuan Sun, Xiaoqing Liu, Zishang Liang, Yinan Jiao, Hui Bu, Xin Chen, Jinjin Zhao, Jianlin Shi. Highly Efficient, Targeted, and Traceable Perovskite Nanocrystals for Photoelectrocatalytic Oncotherapy[J]. Acta Phys. -Chim. Sin. 2025, 41(5), 100042. doi: 10.1016/j.actphy.2024.100042

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2024.100042

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I5/100042

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高效靶向示踪钙钛矿纳米系统光电增效抗肿瘤

Highly Efficient, Targeted, and Traceable Perovskite Nanocrystals for Photoelectrocatalytic Oncotherapy

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