Journal
ANALYTICAL CHEMISTRY
Volume 93, Issue 51, Pages 17119-17126Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.1c04750
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Funding
- National Natural Science Foundation of China [22174054, 22172064, 22136002]
- National Key Research and Development Program of China [2018YFC1603001]
- Shandong Key Laboratory of Biochemical Analysis [SKLBA2101]
- National First-Class Discipline Program of Food Science and Technology [JUFSTR20180301]
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This study presents a new concept of invoking cathodic photoelectrochemistry using a spontaneously formed electron transporter, which successfully applied in biosensing to achieve improved photocurrent readout. The mechanism revealed a different perspective for signal transduction in cathodic photoelectrochemistry and may stimulate more interests in the design and construction of semiconductor/transporter counterparts for exquisite operation of photocathodic bioanalysis.
Most of the cathodic photoelectrochemical (PEC) bioassays rely on electron accepting molecules for signal stimuli; unfortunately, the performances of which are still undesirable. New signal transduction strategies are still highly expected for the further development of cathodic photoelectrochemistry as a potentially competitive method. This work represents a new concept of invoked cathodic photoelectrochemistry by a spontaneously formed electron transporter for innovative operation of the sensing strategy. Specifically, the hexacyanoferrate(II) in solution easily self-coordinated with CuO nanomaterials and formed electron transporting copper hexacyanoferrate (CuHCF) on the surface, which endowed improved carrier separation for presenting augmented photocurrent readout. Exemplified by the T4 polynucleotide kinase (T4 PNK) and its inhibitors as targets, a homogenous cathodic PEC biosensing platform was achieved with the distinctive merits of label-free, immobilization-free, and split-mode readout. The mechanism revealed here provided a totally different perspective for signal transduction in cathodic photoelectrochemistry. Hopefully, it may stimulate more interests in the design and construction of semiconductor/transporter counterparts for exquisite operation of photocathodic bioanalysis.
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