| Summary: | Precise regulation of biomimetic mineralization for highly ordered superstructures is one of the perpetual concerns in biomaterial synthesis and crystal engineering. Herein, we propose a ultra-homoporous interfacial crystallizer (UHIC) as a novel interfacial microdevice, which has realized high selective synthesis of CaCO3 superstructures during Gas–Liquid reactive crystallization process. This UHIC with ultra-uniform mass transfer porous channel and interfacial superhydrophilicity render the droplet ultra-homo nucleation site and coordinatively regulate the interfacial nucleation energy. The highly precise microchannel in UHIC can control the CO2 gas flow rate and sufficient interfacial Gas–Liquid diffusion of the CaCO3 pre-nucleation cluster (PNC). By coordinating the PNC diffusion, self-organization and nucleus growth, the proportion of synthesized CaCO3 crystals with spherical and polyhedral structures both increased to higher than 96.77 %, and the crystal size distribution was very uniform (minimum C.V. =11.7%). Fundamental theory of CaCO3 synthesis with UHIC as a desire interfacial reactive were then outlined, which can shed light on the high-selective synthesis of the microscale biomaterials.
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