Wang Ying, Cho Ara, Jia Guangri, Cui Xiaoqiang, Shin Junhyeop, Nam Inho, Noh Kyung-Jong, Park Byoung Joon, Huang Rui, Han Jeong Woo
Department of Chemical Engineering, Pohang University of Science and Technology (POSTECH), Pohang, Gyeongbuk, 37673 (Republic of, Korea.
State Key Laboratory of Automotive Simulation and Control, School of Materials Science and Engineering, Key Laboratory of Automobile Materials of MOE, Jilin University, Changchun, Jilin, 130012, China.
Angew Chem Int Ed Engl. 2023 Apr 3;62(15):e202300119. doi: 10.1002/anie.202300119. Epub 2023 Mar 2.
Single-atom nanozymes (SAzymes) are promising in next-generation nanozymes, nevertheless, how to rationally modulate the microenvironment of SAzymes with controllable multi-enzyme properties is still challenging. Herein, we systematically investigate the relationship between atomic configuration and multi-enzymatic performances. The constructed Mn -N -coordinated SAzymes (Mn -N -C) exhibits much more remarkable oxidase-, peroxidase-, and glutathione oxidase-like activities than that of Mn -N -C. Based on experimental and theoretical results, these multi-enzyme-like behaviors are highly dependent on the coordination number of single atomic Mn sites by local charge polarization. As a consequence, a series of colorimetric biosensing platforms based on Mn -N -C SAzymes is successfully built for specific recognition of biological molecules. These findings provide atomic-level insight into the microenvironment of nanozymes, promoting rational design of other demanding biocatalysts.
单原子纳米酶在下一代纳米酶领域颇具前景，然而，如何合理调控具有可控多酶性质的单原子纳米酶的微环境仍是一项挑战。在此，我们系统地研究了原子构型与多酶性能之间的关系。构建的锰-氮配位单原子纳米酶（Mn-N-C）展现出比Mn-N-C更显著的氧化酶、过氧化物酶和谷胱甘肽氧化酶样活性。基于实验和理论结果，这些多酶样行为高度依赖于通过局部电荷极化的单原子锰位点的配位数。因此，基于Mn-N-C单原子纳米酶成功构建了一系列用于生物分子特异性识别的比色生物传感平台。这些发现为纳米酶的微环境提供了原子层面的见解，推动了其他所需生物催化剂的合理设计。
