磁铁矿纳米粒子的润湿性指导稳定的无定形水铁矿的生长,Journal of the American Chemical Society

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磁铁矿纳米粒子的润湿性指导稳定的无定形水铁矿的生长
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-07-15 , DOI: 10.1021/jacs.1c02687
Lucas Kuhrts ₁ , Sylvain Prévost ₂ , Daniel M Chevrier _{1,

3} , Péter Pekker ₄ , Oliver Spaeker ₁ , Mathias Egglseder ₁ , Jens Baumgartner ₁ , Mihály Pósfai ₄ , Damien Faivre _{1,

3}

Affiliation

通过无定形前体形成晶体是设计具有良好控制的尺寸和形态的纳米粒子的长期追捧的途径。生物矿化生物，如趋磁细菌，遵循这种非经典的结晶途径来生产具有在环境条件下合成努力无法比拟的复杂程度的磁铁矿纳米颗粒。在这里，就地使用小角 X 射线散射，我们展示了在磁铁矿纳米颗粒的合成形成中添加聚（精氨酸）如何诱导生物矿化回忆途径。添加聚（精氨酸）可稳定无定形水铁矿前体，将磁铁矿形成途径从热力学控制转变为动力学控制。通过催化 pH 依赖性前体附着改变磁铁矿形成的能量景观，我们不断调整磁铁矿纳米颗粒的尺寸，超过了在趋磁细菌中观察到的尺寸。我们在此发现的这种机制转变进一步允许通过调节液体状水铁矿和新生磁铁矿纳米颗粒之间的 pH 依赖性界面相互作用来控制晶体形态，从而建立控制纳米颗粒形态的新策略。

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Wettability of Magnetite Nanoparticles Guides Growth from Stabilized Amorphous Ferrihydrite

Crystal formation via amorphous precursors is a long-sought-after gateway to engineer nanoparticles with well-controlled size and morphology. Biomineralizing organisms, like magnetotactic bacteria, follow such a nonclassical crystallization pathway to produce magnetite nanoparticles with sophistication unmatched by synthetic efforts at ambient conditions. Here, using in situ small-angle X-ray scattering, we demonstrate how the addition of poly(arginine) in the synthetic formation of magnetite nanoparticles induces a biomineralization-reminiscent pathway. The addition of poly(arginine) stabilizes an amorphous ferrihydrite precursor, shifting the magnetite formation pathway from thermodynamic to kinetic control. Altering the energetic landscape of magnetite formation by catalyzing the pH-dependent precursor attachment, we tune magnetite nanoparticle size continuously, exceeding sizes observed in magnetotactic bacteria. This mechanistic shift we uncover here further allows for crystal morphology control by adjusting the pH-dependent interfacial interaction between liquidlike ferrihydrite and nascent magnetite nanoparticles, establishing a new strategy to control nanoparticle morphology. Synthesizing compact single crystals at wetting conditions and unique semicontinuous single-crystalline nanoparticles at dewetting conditions in combination with an improved control over magnetite crystallite size, we demonstrate the versatility of bio-inspired, kinetically controlled nanoparticle formation pathways.

更新日期：2021-07-28

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