Unveiling the heavy-metal ion critical role in γ-dicalcium silicate: from solidification to early hydration.

The heavy-metal ion critical role in γ-dicalcium silicate (γ-C2S) both in terms of solidification mechanism and hydration is still unclear. In this work, the solidification mechanism and the effect on initiating hydration of these three heavy-metal ions (Ba, Cd, and Cr) in γ-C2S is systemically studied by well-defined ab initio calculations. The calculated results show that the solid solution tendency of ions originates from the charge contribution, and the charge localization caused by the doping of Cr ions weakens the surface water adsorption. These insights will provide theoretical guidance for the low-carbon cement development by γ-C2S.

An Upper Bound Visualization of Design Trade-Offs in Adsorbent Materials for Gas Separations: CO2 , N2 , CH4 , H2 , O2 , Xe, Kr, and Ar Adsorbents.

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 CO2 /N2 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 CO2 , N2 , CH4 , H2 , Xe, O2 , 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.

Enhanced Propulsion of Urease-Powered Micromotors by Multilayered Assembly of Ureases on Janus Magnetic Microparticles.

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.