Size- and Shape-Controlled Synthesis of Calcium Silicate Particles Enables Self-Assembly and Enhanced Mechanical and...

Calcium silicate (CS)-based materials are ubiquitous in diverse industries ranging from cementitious materials to bone tissue engineering and drug delivery. As a symbolic example, concrete is the most widely used synthetic material on the planet. This large consumption entails significant negative environmental footprint, which calls for innovative strategies to develop greener concrete with improved properties (to do more with less). Herein, we focus on the physicochemical properties of novel spherical calcium silicate particles with an extremely narrow size distribution and report their promising potential as fundamental building blocks. We demonstrate a scalable size- and shape-controlled synthesis protocol to yield highly spherical CS submicron particles, leading to favorable aggregation mechanisms and thus self-assembly of the bulk ensemble. This optimized kinetics-controlled synthesis is governed by suitable stoichiometric ratio of calcium over silicon, type and concentration of the surfactant, and molar ratio of the alkaline solution. Our extensive nano/micro/macro-characterization results show that the bulk ensemble exhibits many superior properties, such as improved strength, toughness, ductility, and durability, paving the path for bottom-up science-based engineering of concrete.