Paper based modification-free photoelectrochemical sensing platform with single-crystalline aloe like TiO₂ as...

By controlling target-induced signal quencher release, a label-free and modification-free microfluidic paper based photoelectrochemical analytical device (μ-PAD) for cardiac troponin-I (cTnI) detection was designed for the first time. To achieve it, cellulose paper based single-crystalline three-dimensional aloe like TiO₂ arrays (PSATs) were firstly fabricated as the electron transporting material, providing direct pathways for the charge carriers transfer, and subsequently coupled with CdS to form PSATs/CdS heterojunction for extending the solar spectrum response. Meanwhile, positive charged mesoporous silica nanoparticles (PMSNs) were prepared as the nanocarrier to efficient entrap the Cu²⁺ which could be regarded as signal quencher due to their reaction with CdS to form Cu_xS. Single stranded DNAs (ssDNAs), which could bind specifically with the target of cTnI, were then introduced to couple with the PMSNs and used as the bio-gate to encapsulate the signal quencher of Cu²⁺, endowing the functional PMSNs with responsiveness to cTnI. When the cTnI existed, the ssDNAs were dissociated from PMSNs due to the formation of cTnI-ssDNAs complexes, triggering controllable release of the trapped Cu²⁺, and further decreasing the photocurrent signal caused by the formation of Cu_xS. Accordingly, the concentration of cTnI could be accurately quantified via the photocurrent, realizing the target-induced modification-free μ-PAD assay. We believe this work could provide an ingenious idea to construct the easy-to-use novel modification-free μ-PAD.