Biomorphic triangulations: constructing an additional formation pathway to achieve hierarchical self-evolution in biomorphs

Biomimetic morphologies constructed in pure inorganic systems, called biomorphs, provide a promising approach to produce advanced biomimetic materials via bottom-up self-organization. Although existing biomorphs show the potential to imitate complex and/or hierarchical micro-architectures, they can only be achieved by changing the conditions manually during the reaction, not an intelligent morphological self-evolution. In this contribution, we propose a strategy to introduce more than one type of initial variable for the construction of different formation/transition pathways to realize a hierarchical architecture via self-evolution. A hierarchical architecture with unique triangular branches was obtained successfully by initial control of both the temperature and Mg2+ doping, highlighting two pathways for the textured growth of polycrystals and single crystals in different hierarchies led by CO2 and MgCO3, respectively. Our findings lay the foundation for the future construction of materials with new complex hierarchical architectures via a self-evolution approach realized by rational pathway design.