突破单原子纳米酶的选择性障碍,通过平面外的配体协调
Seonhye Park1, Kyu In Shim2, Phuong Thy Nguyen3
1Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon, 34141, Republic of Korea.
Advanced materials (Deerfield Beach, Fla.)
|July 7, 2025
概括
新的单原子纳米酶 (SAzymes) 与联体显示出高的过氧化酶类活性和抑制的催化酶类活性. 这种选择性使近乎中性条件下的精确生物感知成为可能.
科学领域:
- 纳米材料科学 科学 纳米材料科学
- 催化剂是一种催化剂.
- 生物传感器是一种生物传感器.
背景情况:
- 类似过氧化酶 (POD) 的纳米酶为生物传感器中的自然酶提供了稳定,经济高效的替代品.
- 具有Fe-N4位点的单原子纳米酶 (SAzymes) 显示出高的催化活性,但受限于选择性和pH依赖性.
- 现有的SAzymes的2D活点在中性条件下阻碍了功能.
研究的目的:
- 开发具有增强过氧化酶类活性选择性的新型SA酶.
- 研究新纳米酶的催化机制和pH依赖性行为.
- 为了证明这些SAzymes对于精确的多生物标志物检测的实用性.
主要方法:
- 与联体 (RuNC_Cl) 协调的以为中心的SA酶的合成.
- 类似POD和类似催化酶 (CAT) 活动的表征.
- 密度函数理论 (DFT) 计算和巴德尔电荷分析以阐明反应机制.
主要成果:
- 与CAT类活动相比,RuNC_Cl的POD类活动 (38倍) 显著增加,显示出单一功能性能的表现.
- DFT的计算揭示了阻碍二次H2O2吸附的排斥力,增加了CAT类反应的能量屏障.
- 在接近中性的条件下,RuNC_Cl纳米酶能够精确地检测多个生物标志物的单级联检测.
结论:
- RuNC_Cl SA酶通过抑制竞争的CAT类反应来实现高度选择性的POD类活性.
- 抑制的CAT类活动归因于二次H2O2吸附的能量障碍增加.
- 这一进步提高了纳米酶在生理条件下的精确生物传感应用的实用性.
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