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Programming bulk enzyme heterojunctions for biosensor development with tetrahedral DNA framework
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DOI：10.1038/s41467-020-14664-8.png)
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Abstract
En 中文
Protein-protein interactions are spatially regulated in living cells to realize high reaction efficiency, as seen in naturally existing electron-transfer chains. Nevertheless, arrangement of chemical/biochemical components at the artificial device interfaces does not possess the same level of control. Here we report a tetrahedral DNA framework-enabled bulk enzyme heterojunction (BEH) strategy to program the multi-enzyme catalytic cascade at the interface of electrochemical biosensors. The construction of interpenetrating network of BEH at the millimeter-scale electrode interface brings enzyme pairs within the critical coupling length (CCL) of similar to 10nm, which in turn greatly improve the overall catalytic cascade efficiency by similar to 10-fold. We demonstrate the BEH generality with a range of enzyme pairs for electrochemically detecting clinically relevant molecular targets. As a proof of concept, a BEH-based sarcosine sensor enables single-step detection of the metabolic biomarker of sarcosine with ultrasensitivity, which hold the potential for precision diagnosis of early-stage prostate cancer.
Keywords:
GLUCOSE-RESPONSIVE INSULIN
PROSTATE-CANCER
SARCOSINE
CELLS
NANOSTRUCTURES
METABOLISM
LIPOSOMES
MECHANISM
BIOMARKER
MACHINES
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