Single Atom Iron‐Doped Graphic‐Phase C₃N₄ Semiconductor Nanosheets for Augmented Sonodynamic Melanoma Therapy Synergy with Endowed Chemodynamic Effect

Abstract

Sonodynamic therapy (SDT) is a non‐invasive therapeutic modality with high tissue‐penetration depth to induce reactive oxygen species (ROS) generation for tumor treatment. However, the clinical translation of SDT is restricted seriously by the lack of high‐performance sonosensitizers. Herein, the distinct single atom iron (Fe)‐doped graphitic‐phase carbon nitride (C3N4) semiconductor nanosheets (Fe‐C3N4 NSs) are designed and engineered as chemoreactive sonosensitizers to effectively separate the electrons (e−) and holes (h+) pairs, achieving high yields of ROS generation against melanoma upon ultrasound (US) activation. Especially, the single atom Fe doping not only substantially elevates the separation efficiency of the e−‐h+ pairs involved in SDT, but also can serve as high‐performance peroxidase mimetic enzyme to catalyze the Fenton reaction for generating abundant hydroxyl radicals, therefore synergistically augmenting the curative effect mediated by SDT. As verified by density functional theory simulation, the doping of Fe atom significantly promotes the charge redistribution in the C3N4‐based NSs, which improves their synergistic SDT/chemodynamic activities. Both the in vitro and in vivo assays demonstrate that Fe‐C3N4 NSs feature an outstanding antitumor effect by aggrandizing the sono‐chemodynamic effect. This work illustrates a unique single‐atom doping strategy for ameliorating the sonosensitizers, and also effectively expands the innovative anticancer‐therapeutic applications of semiconductor‐based inorganic sonosensitizers.

Application of single-atom Ti-doped g-C3N4 in photocatalytic H2O2 production

“…1(d), suggesting that a quantity of single Ti atoms have been embedded in the g-C 3 N 4 matrix. [24][25][26][27] The concentration of Ti of Ti-C 3 N 4 -100 is 0.09%, as determined using inductively coupled plasma (ICP) analysis, as seen in Table S1 (ESI †). The elemental mapping of Ti-C 3 N 4 -100 further illustrates that C, N, Ti atoms are homogeneously distributed in the g-C 3 N 4 nanosheets (Fig.…”

Optimized silicate nanozymes with atomically incorporated iron and manganese for intratumoral coordination-enhanced once-for-all catalytic therapy

“…Recently, researchers have been interested in single-atom nanozymes (SAzymes) as potential anticancer drugs because of their high catalytic activity and maximum atomic utilization efficiency. 18–22 A number of SAzymes with different extremely active metal centers have been developed, in which metal atoms as active sites are monodispersed on supports. 23–28 Compared with single-atom nanozymes, diatomic catalysts possess not only uniform active centers and high atom utilization efficiency but also the possibility for synergistic collaborations between two neighboring metal atoms, which would greatly improve catalytic performance.…”

Single-Atom-Based Nanoenzyme in Tissue Repair

“…Those nanozymes, capable of mimicking oxidoreductases or hydrolases, , exhibit physicochemical properties, making them more versatile than natural enzymes. They are increasingly utilized in areas such as biosensing, and therapies like antitumor treatments, − antibacterial wound treatments, and ischemic brain damage treatments . The effectiveness of nanozymes is primarily influenced by their nanostructure and composition, which also present significant challenges.…”