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

Ping Song1,2, Juwen Shen3, Dekai Ye4

  • 1Institute of Molecular Medicine, Department of Urology, Department of Nuclear Medicine, Renji Hospital, School of Medicine, Shanghai Jiao Tong University, 200127, Shanghai, China.

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Summary

This study introduces a tetrahedral DNA framework strategy for bulk enzyme heterojunctions (BEH) in electrochemical biosensors. This method enhances enzyme proximity, boosting catalytic cascade efficiency for sensitive biomarker detection, including sarcosine for prostate cancer diagnosis.

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Area of Science:

  • Biochemical Engineering
  • Nanotechnology
  • Biosensor Technology

Background:

  • Cellular processes achieve high efficiency through spatial regulation of protein-protein interactions.
  • Artificial devices lack precise control over the arrangement of biochemical components at interfaces.
  • Optimizing enzyme proximity is crucial for efficient multi-enzyme catalytic cascades.

Purpose of the Study:

  • To develop a novel strategy for programming multi-enzyme catalytic cascades at electrochemical biosensor interfaces.
  • To enhance the efficiency of enzyme-catalyzed reactions by controlling spatial arrangement.
  • To demonstrate the utility of this approach for sensitive detection of clinically relevant biomarkers.

Main Methods:

  • Utilized a tetrahedral DNA framework to create bulk enzyme heterojunctions (BEH).
  • Engineered interpenetrating networks of BEH at millimeter-scale electrode interfaces.
  • Brought enzyme pairs within a critical coupling length (~10 nm) for enhanced interaction.

Main Results:

  • Achieved a ~10-fold improvement in overall catalytic cascade efficiency.
  • Demonstrated the versatility of the BEH strategy with various enzyme pairs.
  • Developed a BEH-based sarcosine sensor for ultrasensitive, single-step detection of a prostate cancer biomarker.

Conclusions:

  • The BEH strategy effectively programs multi-enzyme cascades at biosensor interfaces.
  • This approach significantly enhances catalytic efficiency and enables sensitive molecular detection.
  • The developed sarcosine sensor shows potential for precision diagnosis of early-stage prostate cancer.