Impact of secondary ice in a frozen NaCl freeze-concentrated
solution on the extent of methylene blue aggregation

J 2024

Impact of secondary ice in a frozen NaCl freeze-concentrated solution on the extent of methylene blue aggregation

VESELÝ, Lukáš, Kamila ZAVACKA, Radim ŠTŮSEK, Martin OLBERT, Vilem NEDELA et. al.

Basic information

Original name

Impact of secondary ice in a frozen NaCl freeze-concentrated solution on the extent of methylene blue aggregation

Authors

VESELÝ, Lukáš (203 Czech Republic, belonging to the institution), Kamila ZAVACKA, Radim ŠTŮSEK (203 Czech Republic, belonging to the institution), Martin OLBERT, Vilem NEDELA, Evgenyi SHALAEV and Dominik HEGER (203 Czech Republic, guarantor, belonging to the institution)

Edition

International Journal of Pharmaceutics, AMSTERDAM, ELSEVIER, 2024, 0378-5173

Other information

Language

English

Type of outcome

Článek v odborném periodiku

Field of Study

10403 Physical chemistry

Country of publisher

Netherlands

Confidentiality degree

není předmětem státního či obchodního tajemství

References:

URL

Impact factor

Impact factor: 5.800 in 2022

Organization unit

Faculty of Science

DOI

http://dx.doi.org/10.1016/j.ijpharm.2023.123691

UT WoS

001138921200001

Keywords in English

Freezing; Lyophilization; Methylene blue; Ice morphology; Secondary ice; Freeze-concentrated solution

Abstract

V originále

Freezing and lyophilization have been utilized for decades to stabilize pharmaceutical and food products. Freezing a solution that contains dissolved salt and/or organic matter produces pure primary ice crystal grains separated by freeze-concentrated solutions (FCS). The microscopic size of the primary ice crystals depends on the cooling conditions and the concentration of the solutes. It is generally accepted that primary ice crystals size influences the rate of sublimation and also can impact physico-chemical behaviour of the species in the FCS. This article, however, presents a case where the secondary ice formed inside the FCS plays a critical role. We microscoped the structures of ice-cast FCS with an environmental scanning electron microscope and applied the aggregation-sensitive spectroscopic probe methylene blue to determine how the microstructure affects the mo-lecular arrangement. We show that slow cooling at-50 degrees C produces large salt crystals with a small specific surface, resulting in a high degree of molecular aggregation within the FCS. In contrast, fast liquid nitrogen cooling yields an ultrafine structure of salt crystals having a large specific surface area and, therefore, inducing smaller aggregation. The study highlights a critical role of secondary ice in solute aggregation and introduces methylene blue as a molecular probe to investigate freezing behaviour of aqueous systems with crystalline solute.

Links

MUNI/A/1594/2023, interní kód MU

Name: Vývoj metod a instrumentace pro analýzu biologicky významných látek 2024

Investor: Masaryk University

MUNI/C/0104/2023, interní kód MU

Name: Studie změn kyselosti po zamrazení vybraných vícesytných anorganických solí a kyselin

Investor: Masaryk University, Study of freezing-induced acidty changes of various polyprotic anorganic acids and salts, Excellent diploma thesis

Citovat

VESELÝ, Lukáš, Kamila ZAVACKA, Radim ŠTŮSEK, Martin OLBERT, Vilem NEDELA, Evgenyi SHALAEV and Dominik HEGER. Impact of secondary ice in a frozen NaCl freeze-concentrated solution on the extent of methylene blue aggregation. International Journal of Pharmaceutics. AMSTERDAM: ELSEVIER, 2024, vol. 650, JAN, p. 123691-123700. ISSN 0378-5173. Available from: https://dx.doi.org/10.1016/j.ijpharm.2023.123691.

@article{2371521,
   author = {Veselý, Lukáš and Zavacka, Kamila and Štůsek, Radim and Olbert, Martin and Nedela, Vilem and Shalaev, Evgenyi and Heger, Dominik},
   article_location = {AMSTERDAM},
   article_number = {JAN},
   doi = {http://dx.doi.org/10.1016/j.ijpharm.2023.123691},
   keywords = {Freezing; Lyophilization; Methylene blue; Ice morphology; Secondary ice; Freeze-concentrated solution},
   language = {eng},
   issn = {0378-5173},
   journal = {International Journal of Pharmaceutics},
   title = {Impact of secondary ice in a frozen NaCl freeze-concentrated solution on the extent of methylene blue aggregation},
   url = {https://www.sciencedirect.com/science/article/pii/S0378517323011134?via%3Dihub},
   volume = {650},
   year = {2024}
}

TY  - JOUR
ID  - 2371521
AU  - Veselý, Lukáš - Zavacka, Kamila - Štůsek, Radim - Olbert, Martin - Nedela, Vilem - Shalaev, Evgenyi - Heger, Dominik
PY  - 2024
TI  - Impact of secondary ice in a frozen NaCl freeze-concentrated solution on the extent of methylene blue aggregation
JF  - International Journal of Pharmaceutics
VL  - 650
IS  - JAN
SP  - 123691
EP  - 123691
PB  - ELSEVIER
SN  - 03785173
KW  - Freezing
KW  - Lyophilization
KW  - Methylene blue
KW  - Ice morphology
KW  - Secondary ice
KW  - Freeze-concentrated solution
UR  - https://www.sciencedirect.com/science/article/pii/S0378517323011134?via%3Dihub
N2  - Freezing and lyophilization have been utilized for decades to stabilize pharmaceutical and food products. Freezing a solution that contains dissolved salt and/or organic matter produces pure primary ice crystal grains separated by freeze-concentrated solutions (FCS). The microscopic size of the primary ice crystals depends on the cooling conditions and the concentration of the solutes. It is generally accepted that primary ice crystals size influences the rate of sublimation and also can impact physico-chemical behaviour of the species in the FCS. This article, however, presents a case where the secondary ice formed inside the FCS plays a critical role. We microscoped the structures of ice-cast FCS with an environmental scanning electron microscope and applied the aggregation-sensitive spectroscopic probe methylene blue to determine how the microstructure affects the mo-lecular arrangement. We show that slow cooling at-50 degrees C produces large salt crystals with a small specific surface, resulting in a high degree of molecular aggregation within the FCS. In contrast, fast liquid nitrogen cooling yields an ultrafine structure of salt crystals having a large specific surface area and, therefore, inducing smaller aggregation. The study highlights a critical role of secondary ice in solute aggregation and introduces methylene blue as a molecular probe to investigate freezing behaviour of aqueous systems with crystalline solute.
ER  -

VESELÝ, Lukáš, Kamila ZAVACKA, Radim ŠTŮSEK, Martin OLBERT, Vilem NEDELA, Evgenyi SHALAEV and Dominik HEGER. Impact of secondary ice in a frozen NaCl freeze-concentrated solution on the extent of methylene blue aggregation. \textit{International Journal of Pharmaceutics}. AMSTERDAM: ELSEVIER, 2024, vol.~650, JAN, p.~123691-123700. ISSN~0378-5173. Available from: https://dx.doi.org/10.1016/j.ijpharm.2023.123691.

Detailed Information on Publication Record