Department of Chemistry, Laboratory of Advanced Materials, Shanghai Key Lab of Molecular Catalysis and Innovative Materials and State Key Laboratory of Molecular Engineering of Polymers, College of Chemistry and Materials, Fudan University, Shanghai 200433, P. R. China.
Material Science and Technology Program, College of Arts and Sciences, Qatar University, P.O. Box 2713, Doha, Qatar.
J Am Chem Soc. 2022 Mar 9;144(9):3892-3901. doi: 10.1021/jacs.1c11749. Epub 2022 Feb 22.
As one of the most important parameters of the nanomotors' motion, precise speed control of enzyme-based nanomotors is highly desirable in many bioapplications. However, owing to the stable physiological environment, it is still very difficult to in situ manipulate the motion of the enzyme-based nanomotors. Herein, inspired by the brakes on vehicles, the near-infrared (NIR) "optical brakes" are introduced in the glucose-driven enzyme-based mesoporous nanomotors to realize remote speed regulation for the first time. The novel nanomotors are rationally designed and fabricated based on the Janus mesoporous nanostructure, which consists of the SiO@Au core@shell nanospheres and the enzymes-modified periodic mesoporous organosilicas (PMOs). The nanomotor can be driven by the biofuel of glucose under the catalysis of enzymes (glucose oxidase/catalase) on the PMO domain. Meanwhile, the Au nanoshell at the SiO@Au domain enables the generation of the local thermal gradient under the NIR light irradiation, driving the nanomotor by thermophoresis. Taking advantage of the unique Janus nanostructure, the directions of the driving force induced by enzyme catalysis and the thermophoretic force induced by NIR photothermal effect are opposite. Therefore, with the NIR optical speed regulators, the glucose-driven nanomotors can achieve remote speed manipulation from 3.46 to 6.49 μm/s (9.9-18.5 body-length/s) at the fixed glucose concentration, even after covering with a biological tissue. As a proof of concept, the cellar uptake of the such mesoporous nanomotors can be remotely regulated (57.5-109 μg/mg), which offers great potential for designing smart active drug delivery systems based on the mesoporous frameworks of this novel nanomotor.
作为纳米马达运动的最重要参数之一,在许多生物应用中,精确控制基于酶的纳米马达的速度是非常理想的。然而,由于稳定的生理环境,仍然很难在原位操纵基于酶的纳米马达的运动。在此,受车辆刹车的启发,首次在葡萄糖驱动的基于酶的介孔纳米马达中引入近红外(NIR)“光刹车”来实现远程速度调节。新型纳米马达是基于 Janus 介孔纳米结构合理设计和制造的,该结构由 SiO@Au 核壳纳米球和酶修饰的周期性介孔有机硅(PMO)组成。纳米马达可以在 PMO 域上的酶(葡萄糖氧化酶/过氧化氢酶)的催化下,由生物燃料葡萄糖驱动。同时,SiO@Au 域上的 Au 纳米壳在近红外光照射下产生局部热梯度,通过热泳驱动纳米马达。利用独特的 Janus 纳米结构,酶催化产生的驱动力方向和近红外光热效应产生的热泳力方向相反。因此,通过近红外光速度调节器,在固定的葡萄糖浓度下,葡萄糖驱动的纳米马达可以实现远程速度调节,速度范围为 3.46 至 6.49 μm/s(9.9-18.5 体长/s),甚至在覆盖生物组织后仍可调节。作为概念验证,这种介孔纳米马达的细胞摄取可以远程调节(57.5-109 μg/mg),这为设计基于新型纳米马达介孔框架的智能主动药物输送系统提供了巨大的潜力。