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- Title
Globular pattern formation of hierarchical ceria nanoarchitectures.
- Authors
Aoyagi, Noboru; Motokawa, Ryuhei; Okumura, Masahiko; Ueda, Yuki; Saito, Takumi; Nishitsuji, Shotaro; Taguchi, Tomitsugu; Yomogida, Takumi; Sazaki, Gen; Ikeda-Ohno, Atsushi
- Abstract
Dissipative structures often appear as an unstable counterpart of ordered structures owing to fluctuations that do not form a homogeneous phase. Even a multiphase mixture may simultaneously undergo one chemical reaction near equilibrium and another one that is far from equilibrium. Here, we observed in real time crystal seed formation and simultaneous nanocrystal aggregation proceeding from CeIV complexes to CeO2 nanoparticles in an acidic aqueous solution, and investigated the resultant hierarchical nanoarchitecture. The formed particles exhibited two very different size ranges, resulting in further pattern formation with opalescence. The hierarchically assembled structures in solutions were CeO2 colloids, viz. primary core clusters (1–3 nm) of crystalline ceria and secondary clusters (20–30 nm) assembled through surface ions. Such self-assembly is widespread in multi-component complex fluids, paradoxically moderating hierarchical reactions. Stability and instability are not only critical but also complementary for co-optimisation around the nearby free energy landscape prior to bifurcation. For atomically precise nanoparticle synthesis, it is crucial to understand hierarchical interactions during nanostructure formation. Here, the authors observe the crystal seed formation and simultaneous nanocrystal aggregation of ceria from aqueous solution in real time to understand hierarchically different intra- and interparticle interactions governing the particle shapes.
- Subjects
CERIUM oxides; COMPLEX fluids; NANOPARTICLE synthesis; CHEMICAL reactions; AQUEOUS solutions
- Publication
Communications Chemistry, 2024, Vol 7, Issue 1, p1
- ISSN
2399-3669
- Publication type
Article
- DOI
10.1038/s42004-024-01199-y