Photodynamic therapy is arising as a noninvasive treatment modality for cancer and other diseases. One of the key factors to determine the therapeutic function is the efficiency of photosensitizers (PSs). Opposed to traditional PSs, which show quenched fluorescence and reduced singlet oxygen production in the aggregate state, PSs with aggregation-induced emission (AIE) exhibit enhanced fluorescence and strong photosensitization ability in nanoparticles. Here, the design principles of AIE PSs and their biomedical applications are discussed in detail, starting with a summary of traditional PSs, followed by a comparison between traditional and AIE PSs to highlight the various design strategies and unique features of the latter. Subsequently, the applications of AIE PSs in photodynamic cancer cell ablation, bacteria killing, and image-guided therapy are discussed using charged AIE PSs, AIE PS molecular probes, and AIE PS nanoparticles as examples. These studies have demonstrated the great potential of AIE PSs as effective theranostic agents to treat tumor or bacterial infection. This review hopefully will spur more research interest in AIE PSs for future translational research.

Photosensitizers with Aggregation-Induced Emission: Materials and Biomedical Applications

Light is a particularly appealing tool for on-demand drug delivery due to its noninvasive nature, ease of application and exquisite temporal and spatial control. Great progress has been achieved in the development of novel light-driven drug delivery strategies with both breadth and depth. Light-controlled drug delivery platforms can be generally categorized into three groups: photochemical, photothermal, and photoisomerization-mediated therapies. Various advanced materials, such as metal nanoparticles, metal sulfides and oxides, metal-organic frameworks, carbon nanomaterials, upconversion nanoparticles, semiconductor nanoparticles, stimuli-responsive micelles, polymer- and liposome-based nanoparticles have been applied for light-stimulated drug delivery. In view of the increasing interest in on-demand targeted drug delivery, we review the development of light-responsive systems with a focus on recent advances, key limitations, and future directions.

Light: A Magical Tool for Controlled Drug Delivery.

Multifunctional TiO2/C nanosheets derived from 3D metal-organic frameworks for mild-temperature-photothermal-sonodynamic-chemodynamic therapy under photoacoustic image guidance.

Cancer immunotherapy effect can be greatly enhanced by other methods to induce immunogenic cell death (ICD), which has profoundly affected immunotherapy as a highly efficient paradigm. However, these treatments have significant limitations, either by causing damage of the immune system or limited to superficial tumors. Sonodynamic therapy (SDT) can induce ICD to promote immunotherapy without affecting the immune system because of its excellent spatiotemporal selectivity and low side effects. Nevertheless, SDT is still limited by low reactive oxygen species yield and the complex tumor microenvironment. Recently, some emerging SDT‐based nanomedicines have made numerous attractive and encouraging achievements in the field of cancer immunotherapy due to high immunotherapeutic efficiency. However, this cross‐cutting field of research is still far from being widely explored due to huge professional barriers. Herein, the characteristics of the tumor immune microenvironment and the mechanisms of ICD are firstly systematically summarized. Subsequently, the therapeutic mechanism of SDT is fully summarized, and the advantages and limitations of SDT are discussed. The representative advances of SDT‐based nanomedicines for cancer immunotherapy are further highlighted. Finally, the application prospects and challenges of SDT‐based immunotherapy in future clinical translation are discussed.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202204365

Emerging Sonodynamic Therapy‐Based Nanomedicines for Cancer Immunotherapy

Immunogenic cell death (ICD) has aroused widespread attention because it can reconstruct a tumor microenvironment and activate antitumor immunity. This study proposes a two‐way enhancement of ICD based on a CaO2@CuS–MnO2@HA (CCMH) nanocomposite to overcome the insufficient damage‐associated molecular patterns (DAMPs) of conventional ICD‐inducers. The near‐infrared (NIR) irradiation (1064 nm) of CuS nanoparticles generates 1O2 through photodynamic therapy (PDT) to trigger ICD, and it also damages the Ca2+ buffer function of mitochondria. Additionally, CaO2 nanoparticles react with H2O to produce a large amount of O2 and Ca2+, which respectively lead to enhanced PDT and Ca2+ overload during mitochondrial damage, thereby triggering a robust ICD activation. Moreover, oxidative‐damaged mitochondrial DNA, induced by PDT and released from tumor cells, reprograms the immunosuppressive tumor microenvironment by transforming tumor‐associated macrophages to the M1 subphenotype. This study shows that CCMH with NIR‐II irradiation can elicit adequate DAMPs and an active tumor‐immune microenvironment for both 4T1 and CT26 tumor models. Combining this method with an immune checkpoint blockade can realize an improved immunotherapy efficacy and long‐term protection effect for body.

Synergistic Reinforcing of Immunogenic Cell Death and Transforming Tumor‐Associated Macrophages Via a Multifunctional Cascade Bioreactor for Optimizing Cancer Immunotherapy

Engineering oxygen-deficient ZrO2-x nanoplatform as therapy-activated “immunogenic cell death (ICD)” inducer to synergize photothermal-augmented sonodynamic tumor elimination in NIR-II biological window

Theranostic nanoplatforms that integrate therapy and diagnosis in a single composite have become increasingly attractive in the field of precise and efficient tumor treatment. Herein, a novel oxygen-deficient zirconia (ZrO2-x) nanosystem based on the conjugation of thiol-polyethylene glycol-amine (SH-PEG-NH2) and chlorin e6 (Ce6) was elaborately designed and established for efficacious photothermal/photodynamic therapy (PTT/PDT) and fluorescence/photoacoustic (FL/PA) bimodal imaging for the first time. The crystalline-disordered, PEGylated ZrO2-x nanoparticles (ZP NPs) displayed strong optical absorption in the near-infrared (NIR) window and were featured with significant photothermal conversion capacity. The ZP NPs were further covalently conjugated with Ce6 to form ZrO2-x@PEG/Ce6 (ZPC) NPs, which displayed a long circulatory half-life, efficient tumor accumulation, and outstanding FL/PA imaging performance. Moreover, the nanocomposites effectively generated cytotoxic intracellular reactive oxygen species (ROS) responsive to laser activation. Both cell studies and animal experiments explicitly demonstrated that ZPC NPs mediated remarkable tumor ablation with minimal systemic toxicity thanks to their tumor-specific PTT/PDT effect. Collectively, these findings may open up new avenues to broaden the application of oxygen-deficient ZrO2-x nanostructures as high-performance photothermal agents in tumor theranostics through rational design and accurate control of their physiochemical properties.

Novel Oxygen-Deficient Zirconia (ZrO2-x) for Fluorescence/Photoacoustic Imaging-Guided Photothermal/Photodynamic Therapy for Cancer.

Oxygen deficient TiO2-x nanoparticles (NPs) have been recognized as a category of new-fashioned photothermal agents to offer safer PTT. However, the surface of TiO2-x NPs is deficient in free active groups or radicals to conjugate functional therapeutic molecules, which seriously impedes their in-depth development for versatile medical applications. In this study, surface activation of TiO2-x NPs was realized by the facile conjugation of (3-aminopropyl)triethoxysilane (APTES) through the formation of a stable Si-O-Ti bond, and photosensitizer chlorin e6 (Ce6) was successfully modified onto the TiO2-x NP surface and with a considerably high loading content. The resultant TiO2-x@APTES/Ce6 (TAC) NPs displayed decent biosafety, rapid tumor enrichment and outstanding performance in photoacoustic (PA) imaging. Taking advantage of the intense photo-absorption in the near-infrared (NIR) region and high dose of conjugated Ce6, a powerful antitumor effect was realized based on the combination of hyperthermia-induced cell ablation and cytotoxic reactive oxygen species (ROS)-triggered apoptosis both in vitro and in vivo. Moreover, PA imaging guidance was exceptionally useful for locating the tumor position and optimizing the treatment regimens. Apart from Ce6, this elaborate modification strategy for TiO2-x is believed to be universal for steadily binding more versatile therapeutic agents, which would definitely favor the development of multifunctional TiO2-x-based nanocomplexes for enhanced tumor treatment.

Rational design of oxygen deficient TiO2-x nanoparticles conjugated with chlorin e6 (Ce6) for photoacoustic imaging-guided photothermal/photodynamic dual therapy of cancer.

The invention discloses a novel nanoparticle material based on medicinal chemistry. The special excellent properties of the novel nanoparticle material are used for tumor imaging and treatment. A particle synthesis method mainly includes the following processes: preparation of black nanometer titanium dioxide, modification with an amino group, and connection with a photosensitizer Ce6 to finally form the novel nanoparticle complex. The preparation method of the nanoparticle concretely comprises the following steps: 1) preparing black anoxic nanometer titanium dioxide by high temperature reduction; 2) reacting the black anoxic nanometer titanium dioxide with 3-aminopropyltriethoxysilane (APTES) to modify the surface of the black anoxic nanometer titanium dioxide with the amino group; and 3)connecting the photosensitizer Ce6 with the modified black titanium dioxide nanoparticle by covalent bonds. The obtained nanoparticle complex has the advantages of good biocompatibility, good biosafety, good bioimaging effect and good tumor treatment effect.

Method for preparing Ce6-connected hypoxic black titanium dioxide nanoparticle

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Engineering oxygen-deficient ZrO2-x nanoplatform as therapy-activated “immunogenic cell death (ICD)” inducer to synergize photothermal-augmented sonodynamic tumor elimination in NIR-II biological window

Novel Oxygen-Deficient Zirconia (ZrO2-x) for Fluorescence/Photoacoustic Imaging-Guided Photothermal/Photodynamic Therapy for Cancer.

Rational design of oxygen deficient TiO2-x nanoparticles conjugated with chlorin e6 (Ce6) for photoacoustic imaging-guided photothermal/photodynamic dual therapy of cancer.

Method for preparing Ce6-connected hypoxic black titanium dioxide nanoparticle