Yiming Gao, Weifeng Fang, Xurong Xu, Ruikang Tang, Zhaoming Liu
Bulk ceramic fabrication commonly relies on interparticle adhesion via high-temperature sintering or the addition of binders; however, inorganic adhesives yield stiff-but-brittle monoliths, whereas soft organic binders severely compromise overall stiffness and strength. Biominerals provide elegant solutions to this dilemma, such as nacre featuring a "brick-and-mortar" structure that exhibits a synergistic interfacial adhesion that combines a soft organic matrix for energy dissipation and stiff mineral bridges for load bearing. Inspired by this, we developed a stiff-yet-elastic organic-inorganic adhesive interface among ceramic particles, achieving the preparation of ceramic composite bulks and their synergistic strengthening and toughening. Specifically, by employing thioctic acid-calcium carbonate (TA-CCO) hybrid molecules as a reactive binder, the in situ polymerization constructs a stiff-yet-elastic adhesive interface, featuring a molecular-scale organic-inorganic bicontinuous network, thereby transforming isotropic, disordered powders into cohesive ceramic composite bulks. This stiff-yet-elastic hybrid adhesive interface simultaneously facilitates load bearing and energy dissipation, significantly strengthening and toughening the resulting bulks. Notably, for platelet-shaped particles capable of forming layered structures, the mechanical reinforcement is further amplified. By this approach, we successfully upcycle industrial solid waste powders (blast furnace slag and fly ash) into ceramic composite bulks that mechanically outperform conventional clay bricks and high-strength concrete, while the dynamic nature of the adhesive interface endows the monoliths with thermoplastic-like recyclability. This work validates a transformative paradigm: reshaping the mechanical essence of the interparticle adhesive interface provides a universal, sustainable, and energy-efficient pathway for high-performance ceramic composite manufacturing.