Chemodynamic therapy (CDT), a novel cancer therapeutic strategy defined as the treatment using Fenton or Fenton-like reaction to produce •OH in the tumor region, was first proposed by Bu, Shi, and co-workers in 2016. Recently, with the rapid development of Fenton and Fenton-like nanomaterials, CDT has attracted tremendous attention because of its unique advantages: 1) It is tumor-selective with low side effects; 2) the CDT process does not depend on external field stimulation; 3) it can modulate the hypoxic and immunosuppressive tumor microenvironment; 4) the treatment cost of CDT is low. In addition to the Fe-involved CDT strategies, the Fenton-like reaction-mediated CDT strategies have also been proposed, which are based on many other metal elements including copper, manganese, cobalt, titanium, vanadium, palladium, silver, molybdenum, ruthenium, tungsten, cerium, and zinc. Moreover, CDT has been combined with other therapies like chemotherapy, radiotherapy, phototherapy, sonodynamic therapy, and immunotherapy for achieving enhanced anticancer effects. Besides, there have also been studies that extend the application of CDT to the antibacterial field. This review introduces the latest advancements in the nanomaterials-involved CDT from 2018 to the present and proposes the current limitations as well as future research directions in the related field.

Chemodynamic Therapy via Fenton and Fenton-Like Nanomaterials: Strategies and Recent Advances.

Recent trends of mesoporous silica-based nanoplatforms for nanodynamic therapies

It is an urgent need that defect repair can develop from simple device fixation to living tissue reconstruction, from short life function replacement to permanent regeneration repair. At present, bone transplantation has become the second largest transplantation surgery after blood transfusion, and artificial bone transplantation generates great hope for the repair and treatment of bone defect. In order to repair bone defect, artificial bone must have good biological properties and sufficient mechanical properties, and it should also have the shape matching to bone defect site and the connected porous structure. For structures and properties requirements of artificial bone, in this review three major challenges faced by artificial bone transplantation are systemtically analyzed and current methods and strategies to address these issues are discussed: 1) the need for developing a type of bone scaffold material with both biological and mechanical properties, 2) the need for realizing the controllable fabrication of individual shape and multistage pore structure of bone scaffold, 3) the need for realizing the transformation from man‐made structure to biological structure. Besides, it summarizes the advantages and disadvantages of these methods and discusses the potential future directions of structural and functional adaptive artificial bone for bone defect regeneration.

Structural and Functional Adaptive Artificial Bone: Materials, Fabrications, and Properties

Microchannel networks within engineered 3D scaffold can allow nutrient exchange and rapid blood vessels formation. However, fabrication of a bone microenvironment‐mimicking scaffold with hierarchical micro/nanofibrous and microchannel structures is still a challenge. Herein, inspired by structural and functional cues of bone remodeling, a microchannel networks‐enriched nanofibrous scaffold by using 3D printing and thermally induced phase separation techniques, which can facilitate cells migration and nutrients transportation, is developed. The customizable vascular‐like structure of polycaprolactone within the nanofibrous gelatin‐silica scaffold is fabricated using 3D‐printed sacrificial templates, while dimethyloxalylglycine (DMOG)‐loaded mesoporous silica nanoparticles (MSNs) located on the scaffold surface and bone forming peptide‐1 (BFP)‐loaded MSNs embedded in the scaffold are implemented for sequential release of DMOG and BFP. The cell experiments show that dual‐drug delivery scaffold (DBM/GP) promotes angiogenesis by stimulating migration, tube formation, and angiogenesis‐related genes/protein expression of endothelial cells, and osteogenesis by promoting osteo‐related genes expression and mineral deposition of osteoblasts. Additionally, DBM/GP scaffold facilitates the angiogenic activity of osteoblasts by activating phosphatidylinositol 3‐kinase/protein kinase B/hypoxia inducible factor‐1α pathway. Furthermore, enhanced vascularization and bone regeneration of DBM/GP scaffold are demonstrated via subcutaneous and skull defect models. Overall, this study reveals that the bone microenvironment‐mimetic dual‐drug delivery scaffold provides a promising strategy for bone defects treatment.

Bone Microenvironment‐Mimetic Scaffolds with Hierarchical Microstructure for Enhanced Vascularization and Bone Regeneration

The favorable microstructure and bioactivity of tissue-engineered bone scaffolds are closely associated with the regenerative efficacy of bone defects. For the treatment of large bone defects, however, most of them fail to meet requirements such as adequate mechanical strength, highly porous structure, and excellent angiogenic and osteogenic activities. Herein, inspired by the characteristics of a "flowerbed", we construct a short nanofiber aggregates-enriched dual-factor delivery scaffold via 3D printing and electrospinning techniques for guiding vascularized bone regeneration. By the assembly of short nanofibers containing dimethyloxalylglycine (DMOG)-loaded mesoporous silica nanoparticles with a 3D printed strontium-contained hydroxyapatite/polycaprolactone (SrHA@PCL) scaffold, an adjustable porous structure can be easily realized by changing the density of nanofibers, while strong compressive strength will be acquired due to the framework role of SrHA@PCL. Owing to the different degradation performance between electrospun nanofibers and 3D printed microfilaments, a sequential release behavior of DMOG and Sr ions is achieved. Both in vivo and in vitro results demonstrate that the dual-factor delivery scaffold has excellent biocompatibility, significantly promotes angiogenesis and osteogenesis by stimulating endothelial cells and osteoblasts, and effectively accelerates tissue ingrowth and vascularized bone regeneration through activating the hypoxia inducible factor-1α pathway and immunoregulatory effect. Overall, this study has provided a promising strategy for constructing a bone microenvironment-matched biomimetic scaffold for bone regeneration.

Flowerbed-Inspired Biomimetic Scaffold with Rapid Internal Tissue Infiltration and Vascularization Capacity for Bone Repair.

Three-dimensional (3D) printed scaffolds provide a promising prospective for application in bone tissue engineering. 3D printed scaffolds with micro- and nano-fibrous structures that facilitate cell adhesion and migration, and combined vascularization and osteoinduction bioactivity will be ideal implants for bone defect repair. Here, we fabricated a 3D printed biodegradable poly (glycerol-co-sebacic acid-co-l-lactic acid-co-polyethylene glycol) (PGSLP)-based scaffold that was internally filled with gelatin nanofibers and allowed the local release of deferoxamine (DFO), which is essential for angiogenesis and osteogenesis in bone regeneration. The nanofibrous structured gelatin/PGSLP (NGP) scaffold was fabricated using a thermally induced phase separation (TIPS) technique, and the macroporous structured gelatin/PGSLP (MGP) scaffold was prepared by directly freeze-drying. The in vitro experiments demonstrated that both DFO-loaded NGP and DFO-loaded MGP scaffolds can promote the migration and tubular formation of human umbilical vein endothelial cells (HUVECs), and enhance the mineralized nodule formation and osteogenic-related gene expression during osteogenic differentiation of bone marrow-derived mesenchymal stem cells (BMSCs). In a rat critical-sized calvarial defect model, the results suggested that the scaffolds with DFO loading significantly promote the vascular formation and accelerate bone regeneration, while the enhancement of vascularization and osteogenesis in vivo in DFO-loaded NGP scaffold was better than that in DFO-loaded MGP scaffold. Therefore, the constructed PGLSP-based scaffolds with micro- and nano-fibrous structures would be promising candidates to match the structural and functional requirements for vascularized bone regeneration.

Construction of a nanofiber network within 3D printed scaffolds for vascularized bone regeneration

Construction of nanofibrous scaffolds with interconnected perfusable microchannel networks for engineering of vascularized bone tissue

In this study, an effective and facile strategy is reported to construct a multifunctional nanoplatform by in situ doping metal manganese on gold core mesoporous silica nanoparticles (Au@MMSN). After further modification of alendronate (Ald) on Au@MMSN, the obtained Au@MMSN-Ald efficiently integrates bone targeted chemo-chemodynamic combination therapy and dual-modality computed tomography/magnetic resonance (CT/MR) imaging into a single platform. In particular, Au@MMSN-Ald exhibits excellent tumor microenvironment responsive drug release efficiency. The doxorubicin hydrochloride (DOX) loaded Au@MMSN-Ald (DOX@Au@MMSN-Ald) is demonstrated with excellent targeted ability toward osteosarcoma. Accordingly, in a specific tumor microenvironment, DOX@Au@MMSN-Ald also displays outstanding combined efficiency for killing cancer cells in vitro and suppressing the osteosarcoma growth in vivo. Benefiting from the Au nanoparticles confined in the core and manganese ions released from the shell, CT and MR dual-modality imaging were performed to verify the effective accumulation of Au@MMSN-Ald at the tumor site. Overall, the constructed DOX@Au@MMSN-Ald nanoparticles integrated imaging guide, responsive drug release and combination therapy, which may provide some insight for further biomedical applications in efficient osteosarcoma therapy.

Manganese-doped gold core mesoporous silica particles as a nanoplatform for dual-modality imaging and chemo-chemodynamic combination osteosarcoma therapy.

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Construction of a nanofiber network within 3D printed scaffolds for vascularized bone regeneration

Construction of nanofibrous scaffolds with interconnected perfusable microchannel networks for engineering of vascularized bone tissue

Manganese-doped gold core mesoporous silica particles as a nanoplatform for dual-modality imaging and chemo-chemodynamic combination osteosarcoma therapy.