Enzyme-powered micro/nanomotors propelled by biocompatible fuels generally show a weak propulsive force, which greatly limits their applications in complex biological environments. Herein, we have developed a novel and versatile approach to significantly enhance the propulsion of enzyme-powered micromotors by multilayered assembly of enzymes. As an example, multilayers of biotinylated ureases (BU) were asymmetrically immobilized on biotinylated Janus Au/magnetic microparticles (MMPs) with the assistance of streptavidin (SA). When the mass ratio of BU into SA and the amount of BU used in the assembly process are increased, the amount of urease immobilized on the biotinylated Janus Au/MMPs increased monotonously while the migration speed of the micromotor was augmented gradually until a saturated value. The as-optimized micromotors can be self-propelled with an average speed up to about 21.5 ± 0.8 μm/s at physiological urea concentrations (10 mM), which is five times faster than that of the monolayered counterparts and two times faster than that of the previously reported values. Owing to the enhanced thrust, the micromotors can move in liquids with viscosities similar to that of blood. In addition, with the inherent magnetic property of MMPs, the micromotors can exhibit fast magnetic separation and controllable motion direction by external magnetic fields. Our results provide a new pathway for designing high-efficient enzyme-powered micro/nanomotors and thereby promote their biomedical applications.
Switchable chemotaxis is vital for motile microorganisms seeking benefits or to avoid harm. Inspired by nature, and for the first time, we demonstrate an artificial enzyme-powered micromotor that can autonomously regulate the propulsion mechanism, as well as motion directionality, by solely sensing the change of fuel concentration (Cf) in its surroundings. The as-designed micromotors have a pot-like microstructure with ureases immobilized on the inner surface. With the confined effect of the pot-like microstructure and unique features of the urease catalytic reaction, the molecular products are further reacted into ions, and their propulsion mechanism can be reversibly adjusted between ionic diffusiophoresis and microbubble recoils when Cf changes. Consequently, the as-developed micromotors under magnetic field are able to self-turn back if the local Cf differs greatly in their surroundings, indicating the achievement of positive and negative chemotaxis by sensing local Cf. Meanwhile, the micromotors also show highly enhanced migration speed by microbubble ejection, up to 60 μm/s, around 30 body lengths per second at physiological urea concentrations. Furthermore, they have an outer surface of mesoporous silica which is easily functionalized for applications such as stimuli-responsive delivery-associated therapies. This work will promote “smart” artificial micro/nanomotors for in vivo biomedical applications.
The last 20 years have seen many publications investigating porous solids for gas adsorption and separation. The abundance of adsorbent materials (this work identifies 1608 materials for CO 2 /N 2 separation alone) provides a challenge to obtaining a comprehensive view of the field, identifying leading design strategies, and selecting materials for process modeling. In 2021, the empirical bound visualization technique was applied, analogous to the Robeson upper bound from membrane science, to alkane/alkene adsorbents. These bound visualizations reveal that adsorbent materials are limited by design trade-offs between capacity, selectivity, and heat of adsorption. The current work applies the bound visualization to adsorbents for a wider range of gas pairs, including CO 2 , N 2 , CH 4 , H 2 , Xe, O 2 , and Kr. How this visual tool can identify leading materials and place new material discoveries in the context of the wider field is presented. The most promising current strategies for breaking design trade-offs are discussed, along with reproducibility of published adsorption literature, and the limitations of bound visualizations. It is hoped that this work inspires new materials that push the bounds of traditional trade-offs while also considering practical aspects critical to the use of materials on an industrial scale such as cost, stability, and sustainability.
There are works have reported the crystal structures and mechanical properties of ferrite cement (C4AF) at the atomic scale with deviation owing to the omission of the Coulomb interaction effect (Ueff) between 3d electrons of Fe in C4AF. In this work, the DFT+U method was used to evaluate its effect on their electronic structures and mechanical properties of C4AF with two different phases I2mb (C4AF‐I) and Pnma (C4AF‐P). The Fe‐O bonds of the two phases are all weaker and display Ueff due to the presence of Fe ions. The mechanical properties of C4AF calculated using DFT+U method significantly differ from those obtained without considering Ueff, in which the former shows lower inferior mechanical properties than the latter. This work presents a comparative study the effect of Coulomb interaction to the internal electronic structures and mechanical properties, which will pave the way for designing high hydration reaction cement and high toughness materials.This article is protected by copyright. All rights reserved
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