Crystallization via Oriented Attachment of Nanoclusters with Short-Range Order in Solution

Hao Su, Paul H.H. Bomans, Heiner Friedrich, Yifei Xu (Corresponding author), Nico Sommerdijk

Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

6 Citaten (Scopus)

Samenvatting

Many mineral crystallization processes in aqueous solutions involve formation of nanoclusters with short-range order. Their transformation into crystalline products is not well understood. Here we investigate the formation of long-range crystalline order within networks of cobalt-based nanoclusters. High-resolution cryogenic transmission electron microscopy (cryoTEM) together with NMR and FTIR spectroscopies shows the formation of ∼0.8 nm sized (Co)(NH3)5CO3 complexes at the initial stage. By ligand exchange, those complexes become bridged by CO32-/OH- ligands and form ∼2 nm sized clusters, which subsequently aggregate into sheetlike networks due to the structural heterogeneity of the clusters. By further ligand change and adjustment in cluster orientations, long-range order is established, which leads to the nucleation of ammonium cobalt kambaldaite nanocrystals. Our observations demonstrate that nanoclusters with short-range order can form crystals via an oriented-attachment pathway, which provides new insights into multistep crystallization processes.

Originele taal-2Engels
Pagina's (van-tot)1143-1149
Aantal pagina's7
TijdschriftJournal of Physical Chemistry C
Volume125
Nummer van het tijdschrift1
DOI's
StatusGepubliceerd - 4 jan. 2021

Financiering

The authors gratefully acknowledge Shell Global Solutions and The Netherlands Association of Scientific Research (NWO) for funding through the CHIPP program. The research of Y.X. was supported by a Leverhulme research project grant (RPG-2017-178). The authors would like to thank Prof. Joseph Patterson (University of California, Irvine) for helpful discussions on the GOx cryoTEM experiments.

FinanciersFinanciernummer
European Union’s Horizon Europe research and innovation programme885795

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