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

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Programming bulk enzyme heterojunctions for biosensor development with tetrahedral DNA framework.
Nature Communications ( IF 14.7 ) Pub Date : 2020-02-11 , DOI: 10.1038/s41467-020-14664-8
Ping Song _{1,

2} , Juwen Shen ₃ , Dekai Ye ₄ , Baijun Dong ₁ , Fei Wang ₂ , Hao Pei ₅ , Jianbang Wang ₂ , Jiye Shi ₄ , Lihua Wang _{4,

6} , Wei Xue ₁ , Yiran Huang ₁ , Gang Huang ₁ , Xiaolei Zuo _{1,

2} , Chunhai Fan _{1,

2}

Affiliation

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.

中文翻译：

使用四面体 DNA 框架对批量酶异质结进行编程，用于生物传感器的开发。

蛋白质-蛋白质相互作用在活细胞中受到空间调节，以实现高反应效率，如自然存在的电子转移链中所见。然而，人工装置接口处的化学/生化成分的排列不具有相同水平的控制。在这里，我们报告了一种支持四面体 DNA 框架的本体酶异质结 (BEH) 策略，用于对电化学生物传感器界面上的多酶催化级联进行编程。在毫米级电极界面构建BEH互穿网络使酶对的临界耦合长度（CCL）在~10 nm以内，从而将整体催化级联效率大大提高了~10倍。我们通过一系列酶对证明了 BEH 的通用性，用于电化学检测临床相关分子靶标。作为概念验证，基于 BEH 的肌氨酸传感器能够以超灵敏的方式单步检测肌氨酸代谢生物标志物，这具有精确诊断早期前列腺癌的潜力。

更新日期：2020-02-11

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