A closed-loop catalytic nanoreactor system on a transistor

Author:

Wang Xuejun123ORCID,Xia Binbin4ORCID,Hao Zhuang56ORCID,Kang Hua123,Liu Wentao123,Chen Yiheng123,Jiang Qunfeng7ORCID,Liu Jingyuan8,Gou Jian9ORCID,Dong Baijun4ORCID,Wee Andrew Thye Shen9ORCID,Liu Yunqi3ORCID,Wei Dacheng123ORCID

Affiliation:

1. State Key Laboratory of Molecular Engineering of Polymers, Fudan University, Shanghai 200433, China.

2. Department of Macromolecular Science, Fudan University, Shanghai 200433, China.

3. Laboratory of Molecular Materials and Devices, Fudan University, Shanghai 200433, China.

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

5. School of Mechanical Engineering and Automation, Beihang University, Beijing 100191, China.

6. School of Mechatronics Engineering, Harbin Institute of Technology, Harbin 150001, China.

7. Department of Physics, Fudan University, Shanghai 200433, China.

8. Global Clinical Operation, Johnson & Johnson, Shanghai 200233, China.

9. Department of Physics, National University of Singapore, Singapore 117542, Singapore.

Abstract

Precision chemistry demands miniaturized catalytic systems for sophisticated reactions with well-defined pathways. An ideal solution is to construct a nanoreactor system functioning as a chemistry laboratory to execute a full chemical process with molecular precision. However, existing nanoscale catalytic systems fail to in situ control reaction kinetics in a closed-loop manner, lacking the precision toward ultimate reaction efficiency. We find an inter-electrochemical gating effect when operating DNA framework-constructed enzyme cascade nanoreactors on a transistor, enabling in situ closed-loop reaction monitoring and modulation electrically. Therefore, a comprehensive system is developed, encapsulating nanoreactors, analyzers, and modulators, where the gate potential modulates enzyme activity and switches cascade reaction “ON” or “OFF.” Such electric field-effect property enhances catalytic efficiency of enzyme by 343.4-fold and enables sensitive sarcosine assay for prostate cancer diagnoses, with a limit of detection five orders of magnitude lower than methodologies in clinical laboratory. By coupling with solid-state electronics, this work provides a perspective to construct intelligent nano-systems for precision chemistry.

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

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