生物传感器
肌氨酸
级联
DNA
模板
异质结
酶
纳米技术
计算机科学
材料科学
化学
组合化学
光电子学
生物化学
氨基酸
色谱法
甘氨酸
作者
Ping Song,Ji Shen,Dekai Ye,Baijun Dong,Fei Wang,Hao Pei,Jianbang Wang,Jiye Shi,Lihua Wang,Wei Xue,Yiran Huang,Gang Huang,Xiaolei Zuo,Chunhai Fan
标识
DOI:10.1038/s41467-020-14664-8
摘要
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.
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