Snapshots of Ce70 Toroid Assembly from Solids and SolutionClick to copy article linkArticle link copied!
- Ian ColliardIan ColliardDepartment of Chemistry, Oregon State University, Corvallis, Oregon 97331, United StatesMore by Ian Colliard
- Jessica C. BrownJessica C. BrownDepartment of Chemistry, Oregon State University, Corvallis, Oregon 97331, United StatesMore by Jessica C. Brown
- Dylan B. FastDylan B. FastDepartment of Chemistry, Oregon State University, Corvallis, Oregon 97331, United StatesMore by Dylan B. Fast
- A. Kirstin SockwellA. Kirstin SockwellDepartment of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame, Notre Dame, Indiana 46556, United StatesMore by A. Kirstin Sockwell
- Amy E. HixonAmy E. HixonDepartment of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame, Notre Dame, Indiana 46556, United StatesMore by Amy E. Hixon
- May Nyman*May Nyman*Email: [email protected]Department of Chemistry, Oregon State University, Corvallis, Oregon 97331, United StatesMore by May Nyman
Abstract
Crystallization at the solid–liquid interface is difficult to spectroscopically observe and therefore challenging to understand and ultimately control at the molecular level. The Ce70-torroid formulated [CeIV70(OH)36(O)64(SO4)60(H2O)10]4–, part of a larger emerging family of MIV70-materials (M = Zr, U, Ce), presents such an opportunity. We elucidated assembly mechanisms by the X-ray scattering (small-angle scattering and total scattering) of solutions and solids as well as crystallizing and identifying fragments of Ce70 by single-crystal X-ray diffraction. Fragments show evidence for templated growth (Ce5, [Ce5(O)3(SO4)12]10-) and modular assembly from hexamer (Ce6) building units (Ce13, [Ce13(OH)6(O)12(SO4)14(H2O)14]6– and Ce62, [Ce62(OH)30(O)58(SO4)58]14-). Ce62, an almost complete ring, precipitates instantaneously in the presence of ammonium cations as two torqued arcs that interlock by hydrogen boding through NH4+, a structural motif not observed before in inorganic systems. The room temperature rapid assemblies of both Ce70 and Ce62, respectively, by the addition of Li+ and NH4+, along with ion-exchange and redox behavior, invite exploitation of this emerging material family in environmental and energy applications.
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