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Title: Electrophoretic and potentiometric signatures of multistage CaCO3 nucleation

Journal Article · · Journal of Colloid and Interface Science
 [1];  [2]; ORCiD logo [3];  [3];  [2];  [1]; ORCiD logo [4]
  1. Polish Academy of Sciences (PAS), Warsaw (Poland). Inst. of Physical Chemistry
  2. Józef Piłsudski Univ. of Physical Education, Warsaw (Poland). Dept. of Chemistry and Biochemistry
  3. Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy and Management
  4. Polish Academy of Sciences (PAS), Warsaw (Poland). Inst. of Physical Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Geosciences Division

HYPOTHESIS:Calcium carbonate nucleation is often a complex and multistep process that is difficult to follow in situ. The time-resolved electrochemical and electrophoretic methods can provide a new insight into the nucleation pathway. EXPERIMENTS:Here, we used a combination of speciation calculations with time-resolved electrophoretic and potentiometric methods to monitor calcium carbonate precipitation from a slightly supersaturated solution. FINDINGS:After an initial mixing period of three minutes in which metastable CaCO3 phases may have nucleated and subsequently dissolved due to locally-high supersaturations, bulk solution pH and Ca2+ concentrations stabilize before decreasing in tandem with the precipitation of a CaCO3 phase. After an hour, the precipitate is dominated by calcite that grows at the expense of dissolving vaterite. The time-dependent electrokinetic potential shows analogous signatures of multistage nucleation process: initial rapid changes in ζ-potential are followed by much slower equilibration starting about one hour after reagents are mixed. The changes in ζ-potential, solution pH, saturation indexes, and particle morphology are consistent with vaterite to calcite transformation via dissolution of the former and recrystallization of the latter. These findings highlight the potential use of ζ-potential measurements for monitoring polymorphic transformations of carbonate phases in-situ.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1569471
Alternate ID(s):
OSTI ID: 1635998
Journal Information:
Journal of Colloid and Interface Science, Vol. 544, Issue C; ISSN 0021-9797
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 9 works
Citation information provided by
Web of Science

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