氯掺杂增强四氧化三钴类过氧化物酶活性机制研究及应用
Mechanism of Chloride Doping to Enhance Peroxidase Activity of Co3O4 Nanocrystals and Its Application
任亚丽 1梁书丰 2张云慧 3代燕3
作者信息
- 1. 山西大学 分子科学研究所,山西 太原 030006;山西大学 环境科学研究所,山西 太原 030006
- 2. 山西大学 环境科学研究所,山西 太原 030006;山西省肿瘤医院分子生物室,山西 太原 030006
- 3. 山西大学 环境科学研究所,山西 太原 030006
- 折叠
摘要
纳米酶作为一类具有类生物酶活性的纳米材料是目前化学研究的新前沿.然而,纳米酶的应用受到其低催化活性的限制.因此,研制具有高催化活性的纳米酶成为目前该研究领域的热点.本研究通过固相研磨法成功制备出Cl―掺杂Co3O4纳米晶,其类过氧化物酶(Peroxidase,POD)初始反应速率较掺杂前增强了1.3倍.对反应机理的研究表明,Cl―掺杂使得Co3O4纳米晶催化H2O2分解产生超氧阴离子自由基(O2·―)的能力增强,同时还使得H2O2分解产生羟基自由基(·OH)的路径成为可能,而·OH的氧化性强于O2·―,因而Cl―掺杂后材料的类POD活性显著提高.电子顺磁共振谱(Electron Paramagnetic Resonance,EPR)及X射线光电子能谱(X-ray Photoelectron Spec-troscopy,XPS)的表征结果表明,Cl―掺杂后Co3O4纳米晶表面氧空位含量的增多及材料的电子结构的改变可能是其类POD活性增强的主要原因.同时,本研究成功地将基于固相研磨的卤素掺杂法应用到其他金属氧化物纳米晶的改性中,亦得到增强其类POD性能的有益效果.本研究开发出的金属氧化物纳米晶的改性方法有望为具有高效类POD性能的金属氧化物纳米酶的研制提供新途径.
Abstract
Nanozymes as nanomaterials with enzyme-like activity are a new frontier of chemical research.However,the low catalytic activity of nanozymes limits their application.Therefore,designing nanozymes with high catalytic activity has become a hot spot in this field.Herein,Cl― doped Co3O4 nanocrystals(NCs)were successfully prepared by the solid-phase grinding method.After doping,their peroxidase-like(POD-like)initial reaction rate was increased about 1.3 times.Cl― doping enhanced the H2O2 decomposition to superoxide anion radical(O2·―),making the production of hydroxyl radical(·OH)possible.As the·OH is more oxidizing than O2·―,the POD-like activity of Cl― doped Co3O4 NCs is significantly enhanced.The electron paramagnetic resonance(EPR)and X-ray photoelectron spectroscopy(XPS)investigations implied that the increase of oxygen vacancy and the change of electronic structure of Co3O4 NCs after doping were the primary reasons for the enhanced POD-like activity.At the same time,the solid-phase grinding-assisted halogen doping method was successfully applied to other metal oxide NCs,and the beneficial effect of enhancing their POD-like activities was also obtained.In this study,we developed a simple modification method for metal oxide NCs based on halogen doping.This method may provide a new way for the rational design of nanozyme with highly efficient POD-like activity.
关键词
固相研磨法/Cl―掺杂/Co3O4纳米晶/类过氧化物酶Key words
solid-phase grinding method/Cl― doping/Co3O4 nanocrystals/peroxidase-like引用本文复制引用
基金项目
山西省自然科学基金(202103021224014)
出版年
2024
国家科技期刊平台
NSTL
万方数据