As an emerging clinical modality for cancer treatment, photodynamic therapy (PDT) takes advantage of the cytotoxic activity of reactive oxygen species (ROS) that are generated by light irradiating photosensitizers (PSs) in the presence of oxygen (O2 ). However, further advancements including tumor selectivity and ROS generation efficiency are still required. Substantial efforts are devoted to design and synthesize smart PSs with optimized properties for achieving a desirable therapeutic efficacy. This review summarizes the recent progress in developing intelligent PSs for efficient PDT, ranging from single molecules to delicate nanomaterials. The strategies to improve ROS generation through optimizing photoinduced electron transfer and energy transfer processes of PSs are highlighted. Moreover, the approaches that combine PDT with other therapeutics (e.g., chemotherapy, photothermal therapy, and radiotherapy) and the targeted delivery in cancer cells or tumor tissue are introduced. The main challenges for the clinical application of PSs are also discussed.

Photosensitizers for Photodynamic Therapy

There is great need for stand-alone luminescence-based chemosensors that exemplify selectivity, sensitivity, and applicability and that overcome the challenges that arise from complex, real-world media. Discussed herein are recent developments toward these goals in the field of supramolecular luminescent chemosensors, including macrocycles, polymers, and nanomaterials. Specific focus is placed on the development of new macrocycle hosts since 2010, coupled with considerations of the underlying principles of supramolecular chemistry as well as analytes of interest and common luminophores. State-of-the-art developments in the fields of polymer and nanomaterial sensors are also examined, and some remaining unsolved challenges in the area of chemosensors are discussed.

/pdf/supramolecular-luminescent-sensors-1rs45r4um4.pdf

Supramolecular Luminescent Sensors

Photo-responsive chitosan/Ag/MoS2 for rapid bacteria-killing.

Herein, a core-shell dual metal-organic framework (MOF) heterointerface is synthesized. The Prussian blue (PB) MOF acts as a core for the growth of a porphyrin-doped MOF which is named PB@MOF. Porphyrins can significantly enhance the transfer of photoinspired electrons from PB and suppress the recombination of electrons and holes, thus enhancing the photocatalytic properties and consequently promoting the yields of singlet oxygen rapidly under 660 nm illumination. PB@MOF can exhibit a better photothermal conversion efficiency up to 29.9% under 808 nm near-infrared irradiation (NIR). The PB@MOF heterointerface can possess excellent antibacterial efficacies of 99.31% and 98.68% opposed to Staphylococcus aureus and Escherichia coli, separately, under the dual light illumination of 808 nm NIR and 660 nm red light for 10 min. Furthermore, the trace amount of Fe and Zr ions can trigger the immune system to favor wound healing, promising that PB@MOF achieves the rapid therapy of bacterial infected wounds and environmental disinfection.

Dual Metal–Organic Framework Heterointerface

Simultaneous photothermal therapy (PTT) and photodynamic therapy (PDT) is beneficial for enhanced cancer therapy due to the synergistic effect. Conventional materials developed for synergistic PTT/PDT are generally multicomponent agents that need complicated preparation procedures and be activated by multiple laser sources. The emerging monocomponent diketopyrrolopyrrole (DPP)-based conjugated small molecular agents enable dual PTT/PDT under a single laser irradiation, but suffer from low singlet oxygen quantum yield, which severely restricts the therapeutic efficacy. Herein, we report acceptor-oriented molecular design of a donor–acceptor–donor (D–A–D) conjugated small molecule (IID-ThTPA)-based phototheranostic agent, with isoindigo (IID) as selective acceptor and triphenylamine (TPA) as donor. The strong D–A strength and narrow singlet–triplet energy gap endow IID-ThTPA nanoparticles (IID-ThTPA NPs) high mass extinction coefficient (18.2 L g−1 cm−1), competitive photothermal conversion efficiency (35.4%), and a dramatically enhanced singlet oxygen quantum yield (84.0%) comparing with previously reported monocomponent PTT/PDT agents. Such a high PTT/PDT performance of IID-ThTPA NPs achieved superior tumor cooperative eradicating capability in vitro and in vivo.

/pdf/molecular-design-of-conjugated-small-molecule-nanoparticles-2qu69paycd.pdf

Molecular Design of Conjugated Small Molecule Nanoparticles for Synergistically Enhanced PTT/PDT

The combination of photodynamic therapy (PDT) and photothermal therapy (PTT) is highly desired to improve the cancer phototherapeutic effect. However, most reported multicomponent therapeutic agents need complex preparation processes and must be excited by using multiple light sources. Herein, triphenylamine flanked furan-diketopyrrolopyrrole (FDPP-TPA) with a donor–acceptor–donor structure has been synthesized and used as a sole-component agent for fluorescence, photoacoustic and photothermal imaging guided photodynamic and photothermal synergistic therapy. FDPP-TPA nanoparticles (NPs) obtained by re-precipitation exhibit a high molar extinction coefficient (e = 2.13 (±0.2) × 104 M−1 cm−1), excellent photothermal conversion efficiency (η = 47%) and favorable singlet oxygen quantum yield (ΦΔ(X) = 40%). In vitro, the half-maximal inhibitory concentration (IC50) is 13 μg mL−1 determined by cytotoxicity assay. And the apoptosis rate is 67.3% according to flow cytometry analysis. In vivo, the tumor can be completely ablated without recurrence, which suggests that FDPP-TPA NPs can generate considerable poisonous singlet oxygen and hyperthermia for tumor treatment.

Triphenylamine flanked furan-diketopyrrolopyrrole for multi-imaging guided photothermal/photodynamic cancer therapy.

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Triphenylamine flanked furan-diketopyrrolopyrrole for multi-imaging guided photothermal/photodynamic cancer therapy.