Programming bulk enzyme heterojunctions for biosensor development with tetrahedral DNA framework

被引:130
作者
Song, Ping [1 ,2 ]
Shen, Juwen [3 ]
Ye, Dekai [4 ]
Dong, Baijun [1 ]
Wang, Fei [2 ]
Pei, Hao [5 ]
Wang, Jianbang [2 ]
Shi, Jiye [4 ]
Wang, Lihua [4 ,6 ]
Xue, Wei [1 ]
Huang, Yiran [1 ]
Huang, Gang [1 ]
Zuo, Xiaolei [1 ,2 ]
Fan, Chunhai [1 ,2 ]
机构
[1] Shanghai Jiao Tong Univ, Inst Mol Med, Dept Urol, Dept Nucl Med,Renji Hosp,Sch Med, Shanghai 200127, Peoples R China
[2] Shanghai Jiao Tong Univ, Frontiers Sci Ctr Transformat Mol, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China
[3] East China Normal Univ, Shanghai Key Lab Regulatory Biol, Inst Biomed Sci, Sch Life Sci, Shanghai 200241, Peoples R China
[4] Chinese Acad Sci, Shanghai Inst Appl Phys, CAS Key Lab Interfacial Phys & Technol, Div Phys Biol, Shanghai 201800, Peoples R China
[5] East China Normal Univ, Shanghai Key Lab Green Chem & Chem Proc, Sch Chem & Mol Engn, Shanghai 200241, Peoples R China
[6] Chinese Acad Sci, Shanghai Adv Res Inst, Zhangjiang Lab, Bioimaging Ctr,Shanghai Synchrotron Radiat Facil, Shanghai 201210, Peoples R China
关键词
GLUCOSE-RESPONSIVE INSULIN; PROSTATE-CANCER; SARCOSINE; CELLS; NANOSTRUCTURES; METABOLISM; LIPOSOMES; MECHANISM; BIOMARKER; MACHINES;
D O I
10.1038/s41467-020-14664-8
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
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 similar to 10nm, which in turn greatly improve the overall catalytic cascade efficiency by similar to 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.
引用
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页数:10
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