Construction Of Organic Micro-nano Electrogenerated Chemiluminescence Sensor And Its Application In Chiral Discrimination

Electrogenerated chemiluminescence(ECL),where an electronically excited state is generated electrochemically,is essentially a high-energy electron-transfer reaction between active material and co-reactant at an electrode surface,which has been usually used for the chemical and biological analysis due to its versatility,high stability,real-time analysis,low detection limit.Understanding of how interfacial reactions occurring in the interface of the working electrode are correlated with the noncovalent interaction becomes important,which not only offer a comprehensive understanding of the ECL reaction mechanism but also help to promote the development of ECL sensors in the chemical and biological analysis,thus having become a hot issue.In this dissertation,three typical organic materials were selected as active materials to prepare their micro/nano materials via molecular self-assembly process,in which their ECL properties and sensing applications were further studied.Then,the chiral proline enantiomers were selected as co-reactants to construct two different non-covalent reaction systems,and their ECL reaction mechanism was studied,detailedly.Whereafter through analyzing the ECL properties of these micro-nano materials,the application of ECL sensors in logic operation has been expanded and some important achievements which are as follows:(1)typical organic semiconductor material BPEA was used as building blocks to prepare two kinds of BPEA micro/nano materials with different structures via molecular self-assembly process.These developed BPEA micro/nano materials,chosen as ECL-active materials,are loaded onto a cleaned-ITO substrate for constructing reusable ECL sensors.The developed biosensor exhibits high ECL efficiency and excellent stability with tripropylamine(TPrA)as co-reactant,which would spur further application in detecting chiral molecules.The developed sensors exhibit high ECL activities for proline enantiomers,in which obvious difference on the ECL intensity towards L-Pro and D-Pro is observed,and thus achieving chiral discrimination.(2)Although there has been quite extensive interest focused on ECL mechanism,understanding of how interfacial reactions occurring in the interface of the working electrode are correlated with the noncovalent interaction still becomes important.Two kinds of organic chelate compounds were used as building blocks to prepare one-dimensional single structure system and aggregation-induced multi-structural system respectively via facile reprecipitation method and temperature-controlled PVT method.Using the obtained micro/nano materials,the non-covalent ECL sensors dominated by electrostatic force,electrostatic force and hydrogen bonding were constructed.In this context,chiral molecules with polar-(NH)s-essential for the formation hydrogen bonding,were selected as co-reactants,which is a suitable material to study the forming ability of hydrogen bonding,thus providing a good platform for studying chiral discrimination concerning different noncovalent interaction and enantiomeric stereoselectivity.(3)Logic gates,binary switches whose input conditions(0 or 1)determine their output state(0 or 1),are the basis of conventional computer microprocessors.WUsing aggregation-induced IrPA MSs sensors as a signal input and trace amount of the proline enantiomers as another signal input to construct logic gate operations with ECL intensity as the signal output.Compared with traditional sensing devices,intelligent logic gate sensors not only efficiently identify chiral molecules but also provide a new strategy for designing and constructing complex logic operations based on efficient organic dual-functional optoelectronic devices.