Metal-free antioxidant nanozyme incorporating bioactive hydrogel as an antioxidant scaffold for accelerating bone reconstruction

IF 12.8 1区 医学 Q1 ENGINEERING, BIOMEDICAL
Yang Yang , Qianrui Zeng , Chaoyue Zhao , Jie Shi , Wanmeng Wang , Yunkai Liang , Changyi Li , Qingxin Guan , Bo Chen , Wei Li
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Abstract

Oxidative stress at bone defect sites mediates inflammation and even osteoblast apoptosis, severely hindering the repair process. While current antioxidant bone tissue engineering (BTE) scaffolds lack broad-spectrum reactive oxygen species (ROS) scavenging capability and structure-activity elucidation. Herein, we report a three-dimensional nitrogen-doped carbon antioxidant nanozyme (ZIFC) derived from metal-organic frameworks, which exhibits cascading superoxide dismutase- and catalase-like activities, along with the ability to scavenge other harmful free radicals. Through the experimental studies and theoretical calculations, we reveal that the catalase-like activity arises from the synergistic catalytic interaction between graphitized pyridinic nitrogen and its adjacent carbon atom. Moreover, hybrid double network hydrogel integrated with ZIFC is utilized to construct composite scaffold (Gel/ZIFC) by 3D printing. In vivo transcriptome analysis confirms that Gel/ZIFC can rapidly activate antioxidant defense system and suppress local inflammation under oxidative stress microenvironment, thereby protecting cells from oxidative damage. Subsequently, owing to the unique osteoinductive property of carbon nanomaterials and the osteoconductive property of 3D-printed scaffold, Gel/ZIFC composite scaffold exhibits desirable bone repair efficacy. The elucidation of structure-activity relationship and therapeutic mechanism provides new insights and guidance for devising antioxidant BTE scaffolds, and demonstrates their feasibility for clinical application.

Abstract Image

含生物活性水凝胶的无金属抗氧化纳米酶作为加速骨重建的抗氧化支架
骨缺损部位的氧化应激介导炎症甚至成骨细胞凋亡,严重阻碍修复过程。而目前的抗氧化骨组织工程(BTE)支架缺乏广谱活性氧(ROS)清除能力和结构活性鉴定。在此,我们报道了一种由金属-有机框架衍生的三维氮掺杂碳抗氧化纳米酶(ZIFC),它具有级联超氧化物歧化酶和过氧化氢酶样活性,以及清除其他有害自由基的能力。通过实验研究和理论计算,我们揭示了过氧化氢酶的活性是由石墨化吡啶氮与其相邻碳原子之间的协同催化作用产生的。利用与ZIFC集成的杂化双网水凝胶,通过3D打印构建复合支架(Gel/ZIFC)。体内转录组分析证实,Gel/ZIFC可以在氧化应激微环境下快速激活抗氧化防御系统,抑制局部炎症,从而保护细胞免受氧化损伤。随后,由于碳纳米材料独特的骨诱导性能和3d打印支架的骨导电性,Gel/ZIFC复合支架表现出理想的骨修复效果。对其构效关系和治疗机制的阐明,为设计抗氧化BTE支架提供了新的见解和指导,并论证了其临床应用的可行性。
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来源期刊
Biomaterials
Biomaterials 工程技术-材料科学:生物材料
CiteScore
26.00
自引率
2.90%
发文量
565
审稿时长
46 days
期刊介绍: Biomaterials is an international journal covering the science and clinical application of biomaterials. A biomaterial is now defined as a substance that has been engineered to take a form which, alone or as part of a complex system, is used to direct, by control of interactions with components of living systems, the course of any therapeutic or diagnostic procedure. It is the aim of the journal to provide a peer-reviewed forum for the publication of original papers and authoritative review and opinion papers dealing with the most important issues facing the use of biomaterials in clinical practice. The scope of the journal covers the wide range of physical, biological and chemical sciences that underpin the design of biomaterials and the clinical disciplines in which they are used. These sciences include polymer synthesis and characterization, drug and gene vector design, the biology of the host response, immunology and toxicology and self assembly at the nanoscale. Clinical applications include the therapies of medical technology and regenerative medicine in all clinical disciplines, and diagnostic systems that reply on innovative contrast and sensing agents. The journal is relevant to areas such as cancer diagnosis and therapy, implantable devices, drug delivery systems, gene vectors, bionanotechnology and tissue engineering.
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