All forms of energy follow the law of conservation of energy, by which they can be neither created nor destroyed. Light-to-heat conversion as a traditional yet constantly evolving means of converting light into thermal energy has been of enduring appeal to researchers and the public. With the continuous development of advanced nanotechnologies, a variety of photothermal nanomaterials have been endowed with excellent light harvesting and photothermal conversion capabilities for exploring fascinating and prospective applications. Herein we review the latest progresses on photothermal nanomaterials, with a focus on their underlying mechanisms as powerful light-to-heat converters. We present an extensive catalogue of nanostructured photothermal materials, including metallic/semiconductor structures, carbon materials, organic polymers, and two-dimensional materials. The proper material selection and rational structural design for improving the photothermal performance are then discussed. We also provide a representative overview of the latest techniques for probing photothermally generated heat at the nanoscale. We finally review the recent significant developments of photothermal applications and give a brief outlook on the current challenges and future directions of photothermal nanomaterials.

https://pubs.acs.org/doi/pdf/10.1021/acs.chemrev.3c00159

Photothermal Nanomaterials: A Powerful Light-to-Heat Converter

Single‐atom nanozymes (SAzymes) represent a new research frontier in the biomedical fields. The rational design and controllable synthesis of SAzymes with well‐defined electronic and geometric structures are essential for maximizing their enzyme‐like catalytic activity and therapeutic efficacy but remain challenging. Here, a melamine‐mediated pyrolysis activation strategy is reported for the controllable fabrication of iron‐based SAzyme containing five‐coordinated structure (FeN5), identified by transmission electron microscopy imaging and X‐ray absorption fine structure analyses. The FeN5 SAzyme exhibits superior peroxidase‐like activity owing to the optimized coordination structure, and the corresponding catalytic efficiency of Fe‐species in the FeN5 SAzyme is 7.64 and 3.45 × 105 times higher than those in traditional FeN4 SAzyme and Fe3O4 nanozyme, respectively, demonstrated by steady‐state kinetic assay. In addition, the catalytic mechanism is jointly disclosed by experimental results and density functional theory studies. The as‐synthesized FeN5 SAzyme demonstrates significantly enhanced antitumor effect in vitro and in vivo due to the excellent peroxidase‐like activity under tumor microenvironment.

A Bioinspired Five‐Coordinated Single‐Atom Iron Nanozyme for Tumor Catalytic Therapy

Applying Fenton chemistry in the tumor microenvironment (TME) for cancer therapy is the most significant feature of chemodynamic therapy (CDT). Owing to the mild acid and overexpressed H2O2 in TME, more cytotoxic hydroxyl radicals (·OH) are generated in tumor cells via Fenton and Fenton-like reactions. Without external stimulus and drug resistance generation, reactive oxygen species (ROS)-mediated CDT exhibits a specific and desirable anticancer effect and has been seen as a promising strategy for cancer therapy. However, optimizing the treatment efficiency of CDT in TME is still challenging because of the limited catalytic efficiency of CDT agents and the strong cancer antioxidant capacity in TME. Hence, scientists are trying their best to design and fabricate many more CDT agents with excellent catalytic activity and remodeling TME for optimal CDT. In this perspective, the latest progress of CDT is discussed, with some representative examples presented. Consequently, promising strategies for further optimizing the efficiency of CDT guided by Fenton chemistry are provided. Most importantly, several feasible ways of developing CDT in the future are offered for reference.

Recent Advances of Cancer Chemodynamic Therapy Based on Fenton/Fenton-like Chemistry

Low temperature photothermal therapy: Advances and perspectives

Single‐atom nanozyme (SAzyme) with peroxidase‐like activity can alter cellular redox balance and shows promising potential for tumor therapy. However, the “cold” immune microenvironment and limited amount of hydrogen peroxide (H2O2) in solid tumors severely restrict its efficacy. Herein, a light‐controlled oxidative stress amplifier system is designed by co‐encapsulating Pd‐C SAzymes and camptothecin in agarose hydrogel, which exhibits enhanced synergistic antitumor activity by self‐producing H2O2 and transforming “cold” tumors. In this nanozyme hydrogel system, the Pd‐C SAzyme converts near‐infrared laser into heat, resulting in agarose degradation and consequent camptothecin release. The camptothecin increases H2O2 level in tumors by activating nicotinamide adenine dinucleotide phosphate oxidase, improving the catalytic performance of SAzymes with peroxidase‐like activity. Moreover, the combination of photothermal therapy, chemotherapy, and nanozyme‐based catalytic therapy further facilitates tumor immunogenic death and enhanced antitumor immunity. The results reveal the synergistic antitumor potential of the novel SAzyme/chemotherapeutics‐based hydrogel system.

H2O2 Self‐Producing Single‐Atom Nanozyme Hydrogels as Light‐Controlled Oxidative Stress Amplifier for Enhanced Synergistic Therapy by Transforming “Cold” Tumors

Photothermal therapy (PTT) is an extremely promising tumor therapeutic modality. However, excessive heat inevitably injures normal tissues near tumors, and the damage to cancer cells caused by mild hyperthermia is easily repaired by stress-induced heat shock proteins (HSPs). Thus, maximizing the PTT efficiency and minimizing the damage to healthy tissues simultaneously by adopting appropriate therapeutic temperatures is imperative. Herein, an innovative strategy is reported: ferroptosis-boosted mild PTT based on a single-atom nanozyme (SAzyme). The Pd SAzyme with atom-economical utilization of catalytic centers exhibits peroxidase (POD) and glutathione oxidase (GSHOx) mimicking activities, and photothermal conversion performance, which can result in ferroptosis featuring the up-regulation of lipid peroxides (LPO) and reactive oxygen species (ROS). The accumulation of LPO and ROS provides a powerful approach for cleaving HSPs, which enables Pd SAzyme-mediated mild-temperature PTT.

Single-Atom Pd Nanozyme for Ferroptosis-Boosted Mild-Temperature Photothermal Therapy

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Single-Atom Pd Nanozyme for Ferroptosis-Boosted Mild-Temperature Photothermal Therapy