Programming bulk enzyme heterojunctions for biosensor development with tetrahedral DNA framework

Ping Song, Juwen Shen, Dekai Ye, Baijun Dong, Fei Wang, Hao Pei, Jianbang Wang, Jiye Shi, Lihua Wang, Wei Xue, Yiran Huang, Gang Huang, Xiaolei Zuo () and Chunhai Fan ()
Additional contact information
Ping Song: Shanghai Jiao Tong University
Juwen Shen: East China Normal University
Dekai Ye: Division of Physical Biology, CAS Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Baijun Dong: Shanghai Jiao Tong University
Fei Wang: Shanghai Jiao Tong University
Hao Pei: East China Normal University
Jianbang Wang: Shanghai Jiao Tong University
Jiye Shi: Division of Physical Biology, CAS Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Lihua Wang: Division of Physical Biology, CAS Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Wei Xue: Shanghai Jiao Tong University
Yiran Huang: Shanghai Jiao Tong University
Gang Huang: Shanghai Jiao Tong University
Xiaolei Zuo: Shanghai Jiao Tong University
Chunhai Fan: Shanghai Jiao Tong University

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-14664-8

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