| The rapid development of science and technology has brought convenience to the production and life of human beings.At the same time,it also causes serious damages to the environment and human.In order to increase the yields of crop,reduce the flammability of building materials,electronic products and daily necessities,a variety of chemical reagents were added in the process of the production or preservation.Due to the excessive and inappropriate use of chemical reagents,many contaminants were exposed to the environment.Unfortunately,they could accumulate and enter into the human body,greatly impacting the health of human.For example,exposure to organic phosphorus flame retardants(OPFRs)has been proved to cause serious damage to the immune and reproductive system;Persistent organic pollutants(POPs),such as perfluorooctanesulfonate(PFOS)can cause liver toxicity,neurotoxicity.Currently,rapid determination and reliable quantification of these typical contaminants has aroused high concern and become increasingly important in environmental monitoring.Therefore,to develop a simple,cheap and sensitive analytical method for fast screening of typical contaminants residues in water is urgently desirable.Based on the above understanding,the following works were carried out.The novel photoelectrochemical(PEC)single/dual channel analysis strategies have been developed for the determination of OPFRs and the coexisted PFOS in water,respectively.1.Triphenyl Phosphate(TPhP),as a typical model of OPFRs,has been regarded as emerging environmental contaminants of health concern.In this study,a rapid and highly sensitive visible-light-response PEC sensor has been developed for the detection of TPhP using electrospun template directed molecularly imprinted nanofibers modified BiOI nanoflake arrays(BiOINFs)as a photoactive electrode.The molecularly imprinted electrospun nanofibers(MI-ESNFs)were carefully characterized by scanning electron microscopy(SEM),UV spectra,FTIR spectra measurements and various electrochemical techniques.Under the optimized experimental conditions,the PEC response was linearly proportional to the logarithm value of TPhP concentrations in the range of 0.01 ng mL-1 to 500.0 ng mL-1.Meanwhile,the sensor exhibited high selectivity and stability.2.As another typical model of OPFRs,the determination of tris(2-chloroethyl)phosphate(TCEP)has aroused great concern.To meet the requirements of performing rapid "in-situ" analyses,the integration of PEC sensor into well-designed monitoring systems,even disposable sensing strips have gained great attention.In this study,a disposable PEC sensing strip has been fabricated by a one-step electrodeposition of visible-light-responsive BiOI0.5Cl0.5 nanoflake arrays(BiOIClNFs)onto the surface of screen-printed electrode(SPE)array,and then subsequently grafted the molecule tags of TCEP,i.e.the molecularly imprinted polymers(MIP),labeled as MIP@BiOIClNFs/SPE.The as-prepared MIP@BiOIClNFs/SPE-based sensing strip exhibits high sensitivity and selectivity for the determination of TCEP.The PEC analysis is highly linear over the TCEP concentration ranging from 0.01 to 200.0 ng mL-1.Toward practical applications,this low-cost and sensitive assay was successfully applied to measure TCEP in real water samples.3.To further meet the requirements of performing high throughput and rapid analyses,the integration of PEC sensor into well-designed monitoring systems have gained great attention.Based on the previous single PEC detection of OPFRs,in this study,a dual channel PEC sensor has been developed for the simultaneous detection of TPhP and PFOS.The combination of hydrothermal synthesis method,electrospinning technique,and molecular imprinting technology yields a novel nanostructured hybrid of MIP@BiOI/g-C3N4 as the photoactive sensing probe.The as-prepared MIP@BiOI/g-C3N4-based sensing probe exhibits high selectivity and sensitivity for the detection of TPhP and PFOS.Such a newly designed dual-channel PEC sensing probe realized the simultaneous detection of TPhP and PFOS with cost-effective,short time and high throughput.And moreover,this low-cost and sensitive dual-channel assay was successfully applied to measure TPhP and PFOS in real water samples. |