eg电子占有率指导设计基于尖晶石氧化物的高效类过氧化物酶及其生物分析应用

对具有类过氧化物酶活性的纳米酶研究虽然取得了一些实质性进展，但长期以来研究者们对其构效关系和催化机理所知甚少，因而在纳米酶设计和合成时往往采用经验和试错的方法，这导致目前的纳米酶活性普遍偏低。为了获得高活性的纳米酶，需要发展可用于纳米酶理性设计的活性描述符。最近，申请人发现钙钛矿氧化物中过渡金属离子的eg电子个数可用作其类过氧化物酶活性的描述符来指导纳米酶的理性设计。然而，eg这一活性描述符目前只在钙钛矿氧化物中得到了证实，其普适性还有待于证实；另外，受制备方法所限，钙钛矿氧化物尺寸偏大，且难以进行表面修饰，这极大限制了其在生物分析中的进一步应用。因此，针对eg电子占有率指导纳米酶设计所面临的挑战，本项目拟以尖晶石氧化物作为研究对象，系统研究尖晶石氧化物中金属阳离子的eg电子占有率对其过氧化物酶活性的影响，理性设计并合成能够高效模拟过氧化物酶的尖晶石氧化物，进而将其应用于生物分析领域。

Despite of the substantial progress, peroxidase-like nanozymes were generally developed by trail-and-error strategies because nanozymes’ catalytic mechanism and structure-activity relationship remain largely unknown. As a result, the catalytic activities of current nanozymes were generally low. To search for peroxidase-mimicking nanozymes with excellent catalytic activities, it is necessary to develop activity descriptors for the rational design of nanozymes. Recently, we found that eg occupancy of transition metal site could serve as a descriptor for designing peroxidase-mimicking perovskites. However, the eg principle is only demonstrated in perovskite oxides, and its universality needs to be further exploited. In addition, due to the limitation of the preparation method, the size of the perovskite oxides is too large and it is also difficult to perform surface modification, which greatly limits their further application for bioanalysis. To address these challenges, in this project we choose spinel oxides as a model system to study the relationship between eg occupancies and their peroxidase-like activities. Spinel oxides with high peroxidase-like activities will be designed by eg occupancy. Further, biosensing platform will be constructed using peroxidase-mimicking spinel oxides.