Controlling autonomous propulsion of microswimmers is essential for targeted drug delivery and applications of micro/nanomachines in environmental remediation and beyond. Herein, we report two-dimensional (2D) carbon nitride-based Janus particles as highly efficient, light-driven microswimmers in aqueous media. Due to the superior photocatalytic properties of poly(heptazine imide) (PHI), the microswimmers are activated by both visible and ultraviolet (UV) light in conjunction with different capping materials (Au, Pt, and SiO2) and fuels (H2O2 and alcohols). Assisted by photoelectrochemical analysis of the PHI surface photoreactions, we elucidate the dominantly diffusiophoretic propulsion mechanism and establish the oxygen reduction reaction (ORR) as the major surface reaction in ambient conditions on metal-capped PHI and even with TiO2-based systems, rather than the hydrogen evolution reaction (HER), which is generally invoked as the source of propulsion under ambient conditions with alcohols as fuels. Making use of the intrinsic solar energy storage ability of PHI, we establish the concept of photocapacitive Janus microswimmers that can be charged by solar energy, thus enabling persistent light-induced propulsion even in the absence of illumination—a process we call “solar battery swimming”—lasting half an hour and possibly beyond. We anticipate that this propulsion scheme significantly extends the capabilities in targeted cargo/drug delivery, environmental remediation, and other potential applications of micro/nanomachines, where the use of versatile earth-abundant materials is a key prerequisite.
We propose two-dimensional poly(heptazine imide) (PHI) carbon nitride microparticles as light-driven microswimmers in various ionic and biological media. Their high-speed (15 to 23 micrometer per second; 9.5 ± 5.4 body lengths per second) swimming in multicomponent ionic solutions with concentrations up to 5 M and without dedicated fuels is demonstrated, overcoming one of the bottlenecks of previous light-driven microswimmers. Such high ion tolerance is attributed to a favorable interplay between the particle’s textural and structural nanoporosity and optoionic properties, facilitating ionic interactions in solutions with high salinity. Biocompatibility of these microswimmers is validated by cell viability tests with three different cell lines and primary cells. The nanopores of the swimmers are loaded with a model cancer drug, doxorubicin (DOX), resulting in a high (185%) loading efficiency without passive release. Controlled drug release is reported under different pH conditions and can be triggered on-demand by illumination. Light-triggered, boosted release of DOX and its active degradation products are demonstrated under oxygen-poor conditions using the intrinsic, environmentally sensitive and light-induced charge storage properties of PHI, which could enable future theranostic applications in oxygen-deprived tumor regions. These organic PHI microswimmers simultaneously address the current light-driven microswimmer challenges of high ion tolerance, fuel-free high-speed propulsion in biological media, biocompatibility, and controlled on-demand cargo release toward their biomedical, environmental, and other potential applications.
Light‐driven microswimmers have garnered attention for their potential use in various applications, such as environmental remediation, hydrogen evolution, and targeted drug delivery. Janus hollow mesoporous TiO2/Au (JHP–TiO2–Au) microswimmers with enhanced swimming speeds under low‐intensity ultraviolet (UV) light are presented. The swimmers show enhanced swimming speeds both in presence and absence of H2O2. The microswimmers move due to self‐electrophoresis when UV light is incident on them. There is a threefold increase in speed of JHP–TiO2–Au microswimmers in comparison with Janus solid TiO2/Au (JS–TiO2–Au) microswimmers. This increase in their speed is due to the increase in surface area of the porous swimmers and their hollow structure. These microswimmers are also made steerable by using a thin Co magnetic layer. They can be used in potential environmental applications for active photocatalytic degradation of methylene blue and targeted active drug delivery of an anticancer drug (doxurobicin) in vitro in H2O2 solution. Their increased speed from the presence of a hollow mesoporous structure is beneficial for future potential applications, such as hydrogen evolution, selective heterogeneous photocatalysis, and targeted cargo delivery.
The motion of nanomotors triggered by light sources will provide new alternative routes to power nanoarchitectures without the need of chemical fuels. However, most light-driven nanomotors are triggered by UV-light, near infrared reflection (NIR) or laser sources. We demonstrate that nanocap shaped Au/TiO2 nanomotors (175 nm in diameter) display increased Brownian motion in the presence of broad spectrum visible light. The motion results from the surface plasmon resonance (SPR) effect leading to self-electrophoresis between the Au and TiO2 layers, a mechanism called plasmonic photocatalytic effect in the field of photocatalysis. This mechanism has been experimentally characterized by electron energy loss spectroscopy (EELS), energy-filtered transmission electron microscopy (EFTEM) and optical video tracking. We also studied this mechanism in a more theoretical manner using numerical finite-difference timedomain (FDTD) simulations. The ability to power nanomaterials with visible light may result in entirely new applications for externally powered micro/nanomotors.
While current light-driven microswimmers require high-intensity light, UV light, or toxic fuels to propel them, powering them with low-intensity UV-free visible light without fuels is essential to enable their potential high-impact applications. Therefore, in this study, a new material for light-driven microswimmers in the form of CoO is introduced. Janus CoO–TiO2 microswimmers powered with low-intensity, UV-free visible light inside water without using any toxic fuels like H2O2 is proposed. The microswimmers show propulsion under full spectrum of visible light with 17 times lower intensity than the mean solar intensity. They propel by breaking down water into oxygen and oxide radicals, which enables their potential applications for photocatalysis and drug delivery. The microswimmers are multiwavelength responsive, from the ultraviolet to the infrared region. The direction of swimming changes with the change in the illumination from the visible to UV light. In addition to being responsive, they are wavelength steerable and exhibit inherent magnetic properties enabling magnetic steering control of the CoO–TiO2 microswimmers. Thus, these microswimmers, which are propelled under low-intensity visible light, have direction-changing capability using light of different wavelengths, and have steering control capability by external magnetic fields, could be used in future potential applications, such as active and local cargo delivery, active photocatalysis, and hydrogen evolution.
Wireless magnetic microrobots are envisioned to revolutionize minimally invasive medicine. While many promising medical magnetic microrobots are proposed, the ones using hard magnetic materials are not mostly biocompatible, and the ones using biocompatible soft magnetic nanoparticles are magnetically very weak and, therefore, difficult to actuate. Thus, biocompatible hard magnetic micro/nanomaterials are essential toward easy‐to‐actuate and clinically viable 3D medical microrobots. To fill such crucial gap, this study proposes ferromagnetic and biocompatible iron platinum (FePt) nanoparticle‐based 3D microprinting of microrobots using the two‐photon polymerization technique. A modified one‐pot synthesis method is presented for producing FePt nanoparticles in large volumes and 3D printing of helical microswimmers made from biocompatible trimethylolpropane ethoxylate triacrylate (PETA) polymer with embedded FePt nanoparticles. The 30 μm long helical magnetic microswimmers are able to swim at speeds of over five body lengths per second at 200 Hz, making them the fastest helical swimmer in the tens of micrometer length scale at the corresponding low‐magnitude actuation fields of 5–10 mT. It is also experimentally in vitro verified that the synthesized FePt nanoparticles are biocompatible. Thus, such 3D‐printed microrobots are biocompatible and easy to actuate toward creating clinically viable future medical microrobots.
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While micromachines with tailored functionalities enable therapeutic applications in biological environments, their controlled motion and targeted drug delivery in biological media require sophisticated designs for practical applications. Covalent organic frameworks (COFs), a new generation of crystalline and nanoporous polymers, offer new perspectives for light-driven microswimmers in heterogeneous biological environments including intraocular fluids, thus setting the stage for biomedical applications such as retinal drug delivery. Two different types of COFs, uniformly spherical TABP-PDA-COF sub-micrometer particles and texturally nanoporous, micrometer-sized TpAzo-COF particles are described and compared as lightdriven microrobots. They can be used as highly efficient visible-light-driven drug carriers in aqueous ionic and cellular media. Their absorption ranging down to red light enables phototaxis even in deeper and viscous biological media, while the organic nature of COFs ensures their biocompatibility. Their inherently porous structures with ≈2.6 and ≈3.4 nm pores, and large surface areas allow for targeted and efficient drug loading even for insoluble drugs, which can be released on demand. Additionally, indocyanine green (ICG) dye loading in the pores enables photoacoustic imaging, optical coherence tomography, and hyperthermia in operando conditions. This real-time visualization of the drug-loaded COF microswimmers enables unique insights into the action of photoactive porous drug carriers for therapeutic applications.
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