Construction Of Novel Chemiluminescent Censor Based On Transition Metal Nanocatalysts For Biochemical Analysis

Chemiluminescence?CL?is a phenomenon of light radiation that occurs during a chemical reaction.When chemiluminescence is used to analyze actual samples,it has the advantages of does not need of external light source,high sensitivity,wide linear range,fast analysis speed,simple equipment and so on,which makes it one of the most effective technologies in the field of sensing,and has been widely applied to the field of medical examination,environmental moitoring,pharmaceutical analysis and so on.It is well known that the levels of small bioactive molecules,DNA,proteins and enzymes produced by the human body's metabolic activities are closely related to many diseases in the body.Therefore,it is of great significance to build a high sensitivity and highly selectivity sensing platform for these bioactive molecules in the field of analytical chemistry.Because of its high quantum yield and the good water solubility,luminol has become one of the most extensively studied CL system and widely used chemiluminescence reagents among many well-established chemiluminescence systems.Unfortunately,the chemiluminescence emission produced by luminol in an aqueous solution alone or mixed with hydrogen peroxide is very feeble,and an appropriate catalyst needs to be added to the CL system to increase the luminous intensity.In recent years,with the rapid development of nanotechnology,catalysts such as metal nanomaterials,metal oxide nanomaterials,semiconductor nanomaterials,and carbon nanomaterials have been widely used and the CL intensity of luminol can be strongly enhanced by those catalysts.Therefore,the sensitivity of luminescence analysis methods has greatly improved and its application research also be broadened.And made outstanding contributions to the development of the field of chemiluminescence analysis.However,how to use nanomaterial catalysts to build chemiluminescence systems with higher sensitivity and further broaden the application research of chemiluminescence method is still a huge challenge.Based on the above facts,we has carried out a series of applied researches on the subject of"Construction of novel chemiluminescent censor based on transition metal nanocatalysts for biochemical analysis".In this paper,a luminol-hydrogen peroxide chemiluminescence system was used as a model system,and a sensing platform for detecting bioactive molecules was constructed based on highly catalytically active transition metal nanomaterials.In combination with linear discriminant analysis,a chemiluminescence sensor array that recognizes multiple enzymes was build,which are of great significance to broaden the application of chemiluminescence.The main research results in this paper are as follows:1.Engineering FeCo alloy@N-doped carbon layers by directly pyrolyzing Prussian blue analogue:new peroxidase mimetic for chemiluminescence glucose biosensing.Herein,we report the synthesis of FeCo alloy@N-doped carbon layers?FeCo@NC?,a new peroxidase mimetic,by directly pyrolyzing the Fe^III–Co Prussian blue analogue(Fe^III–Co PBA).The FeCo@NC composite showed excellent peroxidase-like activity due to its highly active FeCo alloy,M–N species?Co–N and Fe–N?and N-doped carbon layers with hierarchical pore nanostructures,which were formed via simple heat treatment of Fe^III–Co PBA without additional C and N sources.In particular,the obtained FeCo@NC hybrid presented high CL activity with more than85-fold enhancement in the CL emission of the H₂O₂–luminol system,and long-term stability compared with FeCo alloy nanoparticles.The CL response showed a linear range of 0.01–40?M H₂O₂ with a limit of detection of 2.5 nM.When coupled with glucose oxidase,we developed a new CL sensing method for the detection of glucose in the linear range of 10 nM to 10?M with a detection limit of 8.5 nM.This FeCo@NC-based glucose biosensor displayed rapidity,high precision and good reproducibility when utilized to analyze real biological samples.Expectedly,FeCo@NC,as a new peroxidase mimetic,exhibits great potential for monitoring glucose levels in clinical diagnosis.2.Chemiluminescence sensor arrays for oxidases discrimination based on the enhancment of luminol–H₂O₂.The efficient identification of oxidases is of considerable significance in clinical diagnosis.Herein,three different ternary transition metal sulfide?TTMS?nanoparticles were synthesized,which presented high CL activity with 3 orders of magnitude enhancing in the CL emission intensity for luminol–H₂O₂ system.Thus,a CL sensing platform for ultrasensitive detection of H₂O₂ was developed based on TTMS and the detection limits reached 0.5 pM.Simultaneously,a novel CL sensor array was developed for the detection and discrimination of oxidases based on the different substrates/corresponding oxidases produced different amounts of H₂O₂ due to their different affinities.The sensor array successfully discriminated different oxidases both in buffer and serum samples using linear discriminant analysis.It provides new ideas for designing new analytical detection chemiluminescence analysis methods,and is of great significance.