Hydrate Transformation via Anhydrate Pairs

Thornton, Alyssa M.; Hall, Victoria M.; Swift, Jennifer A.

doi:10.1021/acs.cgd.0c00655

Cited by 2 publications

(4 citation statements)

References 30 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The crystallographic data and refinement details are presented in Table S3. It was found that MC crystallizes in the space group P2 1 /c including one UA and two water molecules, which is consistent with previous reports (Parkin & Hope, 1998;Artioli et al, 1997;Thornton et al, 2020;Izatulina et al, 2019). But here we also found the presence of disordered UA molecules in the crystal structure with the chemical occupancy 0.688:0.312, as shown in Fig.…”

Section: Mechanism Of the Core-shell Phase Transitionsupporting

confidence: 93%

“…The metastable phase UAD can spontaneously transform to UAA through either solid-state dehydration in air or solvent-mediated phase transformation in aqueous solution (Zellelow et al, 2010a;Presores & Swift, 2014). A recent study by Swift and coworkers suggested that the defects induced by trace amounts of 2,4-diaminopyrimidine may impact the kinetics of the solid-state dehydration transition from UAD to UAA (Thornton et al, 2020). However, the unique core-shell phase transition reported in this work was not observed in any of these investigations.…”

contrasting

confidence: 52%

“…The Raman spectrum of UAA crystals is similar to that of UAD (Fig. S1 of the supporting information), but two characteristic peaks can be identified in the range 1200-1800 cm À1 where UAD displays characteristic peaks at 1431 and 1640 cm À1 , but these two bands shift to 1404 and 1650 cm À1 , respectively, in UAA (Thornton et al, 2020). We found the MC initially formed [Fig.…”

Section: Resultsmentioning

confidence: 53%

See 2 more Smart Citations

Unusual shape-preserved pathway of a core-shell phase transition triggered by orientational disorder

Tang

2023

Int Union Crystallogr J

View full text Add to dashboard Cite

The ubiquitous presence of crystal defects provides great potential and opportunities to construct the desired structure (hence with the desired properties) and tailor the synthetic process of crystalline materials. However, little is known about their regulation role in phase transition and crystallization pathways. It was generally thought that a phase transition in solution proceeds predominantly via the solvent-mediated phase-transformation pathway due to energetically high-cost solid-state phase transitions (if any). Herein, we report an unprecedented finding that an orientational disorder defect present in the crystal structure triggers an unusual pathway of a core-shell phase transition with apparent shape-preserved evolution. In the pathway, the solid-state dehydration phase transition occurs inside the crystal prior to its competitive transformation approach mediated by solvent, forming an unconventional core-shell structure. Through a series of combined experimental and computational techniques, we revealed that the presence of crystal defects, introduced by urate tautomerism over the course of crystallization, elevates the metastability of uric acid dihydrate (UAD) crystals and triggers UAD dehydration to the uric acid anhydrate (UAA) phase in the crystal core which precedes with surface dissolution of the shell UAD crystal and recrystallization of the core phase. This unique phase transition could also be related to defect density, which appears to be influenced by the thickness of UAD crystals and crystallization driving force. The discovery of an unusual pathway of the core-shell phase transition suggests that the solid-state phase transition is not necessarily slower than the solvent-mediated phase transformation in solution and provides an alternative approach to constructing the core-shell structure. Moreover, the fundamental role of orientational disorder defects on the phase transition identified in this study demonstrates the feasibility to tailor phase transition and crystallization pathways by strategically importing crystal defects, which has broad applications in crystal engineering.

show abstract

Section: Mechanism Of the Core-shell Phase Transitionsupporting

confidence: 93%

contrasting

confidence: 52%

Section: Resultsmentioning

confidence: 53%

See 1 more Smart Citation

Unusual shape-preserved pathway of a core-shell phase transition triggered by orientational disorder

Tang

2023

Int Union Crystallogr J

View full text Add to dashboard Cite

show abstract

“…S1†), stronger characteristic peaks (590, 630, 1012, 1062 cm −1 ) of MSUM appear close to those of UAA and UAD at 550–630 cm −1 and 1000–1065 cm −1 , respectively. In addition, the Raman spectra between UAD and UAA appear quite similar and the discernible differences are at 1431–1640 cm −1 and 1404–1650 cm −1 corresponding to UAD and UAA, 41 respectively (Fig. 2b).…”

Section: Resultsmentioning

confidence: 87%