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Programming bulk enzyme heterojunctions for biosensor development with tetrahedral DNA framework.


ABSTRACT: 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 ~10?nm, which in turn greatly improve the overall catalytic cascade efficiency by ~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.

SUBMITTER: Song P 

PROVIDER: S-EPMC7012893 | biostudies-literature | 2020 Feb

REPOSITORIES: biostudies-literature

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Programming bulk enzyme heterojunctions for biosensor development with tetrahedral DNA framework.

Song Ping P   Shen Juwen J   Ye Dekai D   Dong Baijun B   Wang Fei F   Pei Hao H   Wang Jianbang J   Shi Jiye J   Wang Lihua L   Xue Wei W   Huang Yiran Y   Huang Gang G   Zuo Xiaolei X   Fan Chunhai C  

Nature communications 20200211 1


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 constr  ...[more]

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