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Engineering of a Multi-Modular dna nanodevice for Spatioselective Imaging and Evaluation of NK Cell-Mediated Cancer Immunotherapy

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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 2025年第2期64卷 e202414064页

作者： Chen, Zhao-Peng Zeng, Wei-Jia Lei, Yan-Mei Liang, Wen-Bin Yang, Xia Yuan, Ruo Yang, Chaoyong Zhuo, Ying Southwest Univ Coll Chem & Chem Engn Key Lab Luminescence Anal & Mol Sensing Southwest Minist Educ Chongqing 400715 Peoples R China Southwest Univ Inst Dev Biol & Regenerat Med Chongqing 400715 Peoples R China Shanghai Jiao Tong Univ Renji Hosp Inst Mol Med Sch Med Shanghai 200127 Peoples R China Xiamen Univ Coll Chem & Chem Engn Dept Chem Biol MOE Key Lab Spectrochem Anal & Instrumentat Xiamen 361005 Peoples R China

Granzyme A (GzmA) secreted by natural killer (NK) cells has garnered considerable interest as a biomarker to evaluate the efficacy of cancer immunotherapy. However, current methodologies to selectively monitor the spatial distribution of GzmA in cancer cells during NK cell-targeted therapy are extremely challenging, primarily due to the existence of diverse cell populations, the low levels of GzmA expression, and the limited availability of GzmA probes. Herein we develop a multi-modular, structurally-ordered dna nanodevice for evaluating NK cell-mediated cancer immunotherapy (MODERN), that permits spatioselective imaging of GzmA in cancer cells through GzmA-induced apurinic/apyrimidinic endonuclease 1 (APE1) inactivation. The MODERN incorporates multiple functional modules, including an APE1-gated recognition module, a photo-activated amplification module, an aptamer-mediated tumor-target module, and a polycatenane dna module, enabling improved sensitivity and specificity towards intracellular GzmA. The MODERN was activated (on) in cancer cells due to the overexpression of APE1, whereas it remained silent (off) in the NK-treated cancer cells owing to the GzmA-induced APE1 inactivation. Furthermore, we demonstrated that GzmA-induced APE1 inactivation blocks the cellular repair of target cells, resulting in efficient cell death. This MODERN that relies on the specific inactivation of APE1 by GzmA should be beneficial for evaluating the efficacy of cancer immunotherapy.

关键词： APE1 dna nanodevice Granzyme A immunotherapy Natural killer cells

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A self-powered theranostic dna nanodevice for amplification of both intracellular microRNA imaging and photodynamic therapy

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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY 2025年 324卷 124987页

作者： Shi, Ming He, Yifang Li, Yuanlin Fan, Mingzhu Huang, Huakui Zhong, Xiaohong Xu, Jiayao Wang, Rong Liu, Yuhui Wang, Shulong Luo, Zhihui Huang, Yong Yulin Normal Univ Coll Chem & Food Sci Guangxi Key Lab Agr Resources Chem & Biotechnol Yulin Peoples R China Guilin Normal Coll Dept Chem & Pharm Guilin Peoples R China Guangxi Normal Univ Sch Chem & Pharmaceut Sci State Key Lab Chem & Mol Engn Med Resources Guilin Peoples R China

While numerous methods exist for diagnosing tumors through the detection of miRNA within tumor cells, few can simultaneously achieve both tumor diagnosis and treatment. In this study, a novel graphene oxide (GO)based dna nanodevice (DND), initiated by miRNA, was developed for fluorescence signal amplification imaging and photodynamic therapy in tumor cells. After entering the cells, tumor-associated miRNA drives DND to Catalyzed hairpin self-assembly (CHA). The CHA reaction generated a multitude of dna Y-type structures, resulting in a substantial amplification of Ce6 fluorescence release and the generation of numerous singlet oxygen (1O2) species induced by laser irradiation, consequently inducing cell apoptosis. In solution, DND exhibited high selectivity and sensitivity to miRNA-21, with a detection limit of 11.47 pM. Furthermore, DND discriminated between normal and tumor cells via fluorescence imaging and specifically generated O21 species in tumor cells upon laser irradiation, resulting in tumor cells apoptosis. The DND offer a new approach for the early diagnosis and timely treatment of malignant tumors.

关键词： dna nanodevice Graphene oxide Signal amplification MiRNA imaging Photodynamic therapy

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An epH-driven dna nanodevice for impeding metastasis in vivo by selectively blocking cell signaling

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NATIONAL SCIENCE REVIEW 2025年第3期12卷 nwae471页

作者： Yuan, Kun Meng, Hong-Min Sun, Hongzhi Qu, Lingbo Li, Zhaohui Tan, Weihong Zhengzhou Univ Inst Analyt Chem Life Sci Coll Chem Zhengzhou 450001 Peoples R China Zhengzhou Univ Affiliated Hosp 1 Zhengzhou 450052 Peoples R China Chinese Acad Sci Zhejiang Canc Hosp Hangzhou Inst Med HIM Hangzhou 310022 Peoples R China Shanghai Jiao Tong Univ Renji Hosp Sch Med Inst Mol Med IMM Shanghai 200240 Peoples R China Shanghai Jiao Tong Univ Coll Chem & Chem Engn Shanghai 200240 Peoples R China

Invasion and metastasis dominate tumor progression, causing a substantial proportion of cancer-related deaths. However, the efficacy of current antimetastatic treatments is hampered by the dearth of targeted therapeutics. Recently developed synthetic-receptor toolkits offer potential for artificially regulating cellular behavior. However, to the best of our knowledge, none has yet successfully suppressed tumor metastasis in vivo. Here, we report the first extracellular pH (epH)-driven dna nanodevice for use in antimetastatic treatment in vivo by manipulating heterogeneous receptors on the tumor cell surface. This dna nanodevice was constructed by partially locking tumorigenic receptor-specific aptamers with two i-motifs. Acidic extracellular pH induced dynamic allosteric reassembly within the nanodevice. The restructured nanodevice enabled oligomerization of c-Met and transferrin receptor, which inhibited tumor metastasis by blocking the hepatic growth factor (HGF)/c-Met signaling pathway. A suppressive efficacy of 86.25% was verified in an early hepatocarcinoma-pulmonary-metastasis mouse model. Such impressive antimetastatic efficacy suggests an efficient paradigm for developing adaptive antimetastatic therapeutics. An extracellular pH-actuated dna nanodevice was developed as an antimetastatic inhibitor to suppress tumor metastasis in vivo by selectively blocking hyperactive receptor signaling.

关键词： antimetastatic therapy cellular signaling blockade dna nanodevice extracellular pH tailored bioregulation

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NIR-II dna nanodevice for Spatiotemporal MicroRNAs Imaging Based on "and" Logic-Gate Strategy

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ADVANCED FUNCTIONAL MATERIALS 2025年

作者： Li, Lei Zhang, Baochun Wang, Yifan Han, Hui Chen, Kai Li, Meixing Fan, Quli Zhang, Hui Shen, Qingming Nanjing Univ Posts & Telecommun Inst Adv Mat IAM State Key Lab Flexible Elect LoFE Nanjing 210023 Peoples R China Nanjing Univ Posts & Telecommun Inst Adv Mat IAM Jiangsu Key Lab Biosensors Nanjing 210023 Peoples R China Nanjing Normal Univ Sch Chem & Mat Sci Jiangsu Key Lab New Power Batteries Nanjing 210023 Peoples R China

The precise detection of multiple microRNAs (miRNAs) is of great significance to the classification of various cell subtypes. However, miRNA detection is hindered by signal leakage, false-positive signals and low expression of miRNAs. Herein, a dna nanodevice in the second near infrared region (NIR-II, 1000-1700 nm) (DND-II) is developed for dual miRNAs bioimaging based on "AND" logic-gate signal amplification strategy. The spatiotemporally controlled logic-gate-based DND-II is fabricated by thermosensitive liposomes integrated with the second near-infrared dna probes. In particular, the "always-on" photoacoustic signal of dna probes provided an additional imaging tool to monitor the distribution of DND-II in vivo. When both miRNAs are present, the dna probes generated a "turn on" fluorescent signal through dna logical analysis and molecular computation, further triggering an entropy-driven dual-cycle fluorescence signal amplification. The spatiotemporal DND-II provides a powerful platform for early diagnosis and photothermal ablation of different subtypes of tumor cells.

关键词： dna nanodevice logic gate circuit microRNAs NIR-II fluorescence imaging spatiotemporal activation

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dna nanodevice as a multi-module co-delivery platform for combination cancer immunotherapy

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JOURNAL OF COLLOID AND INTERFACE SCIENCE 2024年 667卷 1-11页

作者： Nie, Cunpeng Ye, Jingxuan Jiang, Jian-Hui Chu, Xia Hunan Univ Coll Chem & Chem Engn State Key Lab Chemo Biosensing & Chemometr Changsha 410082 Peoples R China

A major challenge in combining cancer immunotherapy is the efficient delivery of multiple types of immunological stimulators to elicit a robust anti -tumor immune response and reprogram the immunosuppressive tumor microenvironment (TME). Here, we developed a dna nanodevice that was generated by precisely assembling three types of immunological stimulators. The doxorubicin (Dox) component induced immunogenic cell death (ICD) in tumor cells and enhanced phagocytosis of antigen -presenting cells (APCs). Exogenous double -stranded dna (dsdna) could act as a molecular adjuvant to activate the stimulator of interferon genes (STING) signaling in APCs by engulfing dying tumor cells. Interleukin (IL) -12 and small hairpin programmed cell death-ligand 1 (shPD-L1) transcription templates were designed to regulate TME. Additionally, for targeted drug delivery, multiple cyclo[Arg-Gly-Asp-( D -Phe)-Cys] (cRGD) peptide units on dna origami were employed. The incorporation of disulfide bonds allowed the release of multiple modules in response to intracellular glutathione (GSH) in tumors. The nanodevice promoted the infiltration of CD8 + and CD4 + cells into the tumor and generated a highly inflamed TME, thereby enhancing the effectiveness of cancer immunotherapy. Our research results indicate that the nanodevice we constructed can effectively inhibit tumor growth and prevent lung metastasis without obvious systemic toxicity, providing a promising strategy for cancer combination treatment.

关键词： dna nanodevice Immunogenic cell death STING pathway Reprogram tumor environment Cancer immunotherapy

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An aptamer-driven dna nanodevice for improved delivery of synthetic immunostimulants

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Nano Research 2024年第10期17卷 9078-9083页

作者： Dejie Lu Zhenghan Di Lele Li Jian Zhao Li Zheng Guangxi Engineering Center in Biomedical Materials for Tissue and Organ Regeneration Collaborative Innovation Centre of Regenerative Medicine and Medical BioResource Development and ApplicationGuangxi Key Laboratory of Regenerative MedicineThe First Affiliated Hospital of Guangxi Medical UniversityGuangxi Medical UniversityNanning 530021China CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety National Center for Nanoscience and TechnologyBeijing 100190China

Efficient delivery of therapeutics to immune cells remains a formidable challenge for cancer *** this work,we demonstrate that an aptamer-driven dna nanodevice,constructed through linkage of a synthetic immunostimulant(Toll-like receptor 9 agonist:CpG motif)to an aptamer,could significantly enhance the immunostimulatory activity by facilitating the uptake and retention of therapeutics in *** administration of the dna nanodevice results in efficient tumor growth inhibition in both breast cancer and melanoma mouse *** studies suggest that the dna nanodevice leads to reeducation of tumor-associated macrophages and ultimately to reversing the tumor immune *** strategy for aptamer-mediated and vehicle-free delivery of immunostimulatory oligonucleotides provides a potential platform for cancer immunotherapy.

关键词： aptamer immunostimulatory oligonucleotides dna nanodevice tumor-associated macrophages cancer therapy

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NIR light-controlled dna nanodevice for amplified mRNA imaging and precise gene therapy

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NANO TODAY 2024年 54卷

作者： Xiang, Miaomiao Jiang, Yuelin Zhou, Jiajia Bao, Guochen Luo, Xianzhu Zhang, Le Jin, Dayong Xian, Yuezhong Zhang, Cuiling East China Normal Univ Shanghai Engn Res Ctr Mol Therapeut & New Drug Dev Sch Chem & Mol Engn Dept Chem Shanghai 200241 Peoples R China Univ Technol Sydney Inst Biomed Mat & Devices IBMD Fac Sci Sydney NSW 2007 Australia

Accurately delivering antisense oligonucleotides (ASOs) to tumor cells for gene therapy poses a significant challenge. To address this issue, we develop a NIR light-activable dna nanodevice to target survivin mRNA and simultaneously release ASOs in tumor cells, which allows high-precision spatiotemporal imaging and efficient gene therapy. The concept is based on upconversion nanoparticles, which can convert NIR light into UV emissions to activate an entropy-driven dna walking system for mRNA recognition in tumor cells. The intramolecular toehold-mediated entropy-driven catalytic reaction generates a large amount of Bcl-2 ASOs, which allows accurate delivery of ASOs for gene therapy due to the specific targeting of mRNA in tumor cells. The results from in vitro and in vivo experiments show that the NIR light-activated dna nanodevice can detect mRNA with high sensitivity by dna walking amplification and high precision in gene delivery. Moreover, the released ASOs from dna walking system down-regulate the expression of Bcl-2 anti-apoptosis protein and induce tumor cell apoptosis, thereby suppressing tumor growth without a transfection reagent. The NIR-light-controlled dna nanodevice holds great potential for precise gene therapy in clinical applications.

关键词： Near -infrared photoactivation dna nanodevice MRNA Bioimaging Gene silencing

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"Sense-and-Treat" dna nanodevice for Synergetic Destruction of Circulating Tumor Cells

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ACS APPLIED MATERIALS & INTERFACES 2016年第40期8卷 26552-26558页

作者： Chen, Nandi Qin, Shiya Yang, Xiaohai Wang, Qing Huang, Jin Wang, Kemin Hunan Univ Coll Chem & Chem Engn Key Lab Bionanotechnol & Mol Engn Hunan Prov State Key Lab Chemo Biosensing & Chemometr Changsha 410082 Hunan Peoples R China

dna nanostrucures are promising materials for biomedical applications. Herein, we established a "sense-and-treat" localized drug delivery system based on a dna nanodevice to specifically destroy circulating tumor cells (CTCs) by synergetic chemotherapy and photodynamic therapy. The dna nanodevices could sense the existence of CTCs and treat CTCs with anticancer agents. Typically, the presence of target cell promoted the formation of hairpin structure of aptamer, and then the aptamer-accompanied dna tetrahedron would release from the supporter. The chemotherapy drugs (doxorubicin, Dox) loaded in dna tetrahedron would destroy the CTCs specifically. Moreover, the photosensitizer labeled on dna tetrahedron would be activated by lights and generated toxic O-1(2), once dna nanodevices bound CTCs flow through the superficial capillary. Unlike the aptamer only labeled with photosensitizer, the dna nanodevice showed the capability to promote cellular internalization of anticancer agents, increase drug loading capacity, and realize synergetic therapy, which enhanced the destructive ability of anticancer agents. As proof of concept, this dna nanodevice has the potential to inhibit metastasis by synergetic destruction of CTCs.

关键词： dna nanodevice circulating tumor cell aptamer photodynamic therapy chemotherapy metastasis

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Sulfonium-Driven Neoantigen-Released dna nanodevice as a Precise Vaccine for Tumor Immunotherapy and Prevention

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ACS NANO 2022年第11期16卷 19509-19522页

作者： Zhang, Yaping Xu, Hongkun Jiang, Leying Liu, Zhaodi Lian, Chenshan Ding, Xiaofeng Wan, Chuan Liu, Na Wang, Yuena Yu, Zhiqiang Zhu, Lizhi Yin, Feng Li, Zigang Pingshan Translat Med Ctr Shenzhen Bay Lab Shenzhen 518055 Peoples R China Peking Univ Sch Chem Biol & Biotechnol State Key Lab Chem Oncogen Shenzhen Grad Sch Shenzhen 518055 Peoples R China Anhui Med Univ Affiliated Hosp 1 Dept Radiat Oncol Hefei 230022 Peoples R China Southern Med Univ Sch Pharmaceut Sci Guangdong Prov Key Lab New Drug Screening Guangzhou 510515 Peoples R China Shenzhen Univ Shenzhen Peoples Hosp 2 Dept Pharm Affiliated Hosp 1Shenzhen Inst Translat Med Shenzhen 518055 Peoples R China

Peptide-based neoantigen vaccines hold tremendous potential for personalized tumor immunotherapy. However, effective delivery and controllable release of antigen peptides remain major challenges in stimulating robust and sustained immune responses. Programmable dna nanodevices provide accurate fixed positions for antigens, which are convenient for the calculation of clinical dosage, and hold great potential as precise carriers. Here, a peptide-nucleic acid conjugate was prepared, which was driven by a propargyl sulfonium-based efficient and reversible bio-orthogonal reaction under weakly alkaline conditions, and folded into regular dna nanodevice vaccines. The well-defined nanoplatform not only exhibits outstanding stability in serum, satisfactory safety, and effective internalization by antigen-presenting cells (RAW264.7 and BMDCs) but also obviously enhances cytokine (TNF-alpha, IL-6, and IL-12) secretion for further immune response. In vivo, the nanovaccine cooperating with OVA model antigens and CpG adjuvants stimulated an antigen-specific CD8(+)T cell response, significantly preventing the lung metastases of melanoma. In the B16-OVA tumor-bearing model, the growth inhibition rate of melanoma reached up to 50%. Similarly, the dna nanodevice with neoantigen induced up to a maximum degree of complete MC-38 tumor regression in 80% of mice, possibly owing to antigen peptide reversible release driven by sulfonium and further cross-presentation. In brief, this study demonstrates that dna nanodevices with sulfonium centers can provide a precise, biocompatible, and effective co-delivery vaccine platform for tumor immunotherapy and prevention.

关键词： dna-peptide conjugation sulfonium dna nanodevice immunotherapy immune prevention

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An AND-Gate dna nanodevice for Dual Protein-Mediated,Tumor-Specific Imaging

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Chinese Journal of Chemistry 2023年第12期41卷 1437-1442页

作者： Zetan Fan Fangzhi Yu Mingming Yu Lele Li CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety National Center for Nanoscience and Technology Beijing 100190 China Beijing Municipal Pollution Source Management Center Beijing 100089 China Green Catalysis Center and College of Chemistry Zhengzhou University Zhengzhou Henan 450001 China

Sensitive and specific imaging of tumor-associated biomarkers offers an effective way for cancer ***,most of the reported imaging probes are limited to the targeting of a single biomarker,which may impair imaging ***,we report an aptamer-based,AND-gate dna nanodevice that relies on the sequential processing of two tumor-associated proteins to produce a specific fluorescent signal for precise tumor *** dna nanodevice integrates an AS1411 aptamer to bind cell surface nucleolin for tumor targeting and a dna sensor to respond to intracellular apurinic/apyrimidinic endonuclease 1 for activatable *** evaluated the performance of the system in both living cells and a tumor-bearing mouse model,and demonstrated its capability in tumor cell-specific *** anticipate that this strategy will accelerate the design of multivariate protein-stimulated probes for tumor diagnosis.

关键词： Aptamer dna nanodevice Protein Sensor Bioimaging

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