Yield of Protein Crystallization from Metastable Liquid–Liquid Phase Separation

Preparative protein crystallization is regarded as an economically sustainable protein purification alternative to chromatography in biotechnological downstream processing. However, protein crystallization is a not-well-understood process that is usually slow and poorly reproducible. A promising str...

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Main Authors: Shamberia Thomas, Joel A. Dougay, Onofrio Annunziata
Format: Article
Language:English
Published: MDPI AG 2025-05-01
Series:Molecules
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Online Access:https://www.mdpi.com/1420-3049/30/11/2371
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author Shamberia Thomas
Joel A. Dougay
Onofrio Annunziata
author_facet Shamberia Thomas
Joel A. Dougay
Onofrio Annunziata
author_sort Shamberia Thomas
collection DOAJ
description Preparative protein crystallization is regarded as an economically sustainable protein purification alternative to chromatography in biotechnological downstream processing. However, protein crystallization is a not-well-understood process that is usually slow and poorly reproducible. A promising strategy for enhancing protein crystallization is exploiting the metastable liquid–liquid phase separation (LLPS) of protein solutions. Here, we report an enhancement of lysozyme-crystallization yield by using a combination of two additives under LLPS conditions. The first additive, NaCl (0.15 M), is necessary to introduce protein–protein attractive interactions and induce LLPS by lowering temperature. The second additive, 4-(2-hydroxyethyl)-1-piperazineethanesulfonate (HEPES, 0.10 M, pH 7.4), accumulates in the metastable protein-rich liquid phase and thermodynamically stabilizes lysozyme crystals. We found that this combination of additives leads to crystallization yields of higher than 90% under LLPS conditions at a lysozyme concentration of 5% by weight and a fairly low ionic strength (0.2 M) within an operational time of the order of one hour. This crystallization yield is more than three-fold larger than that obtained from samples containing NaCl without HEPES at the same pH and ionic strength. Moreover, we determined crystallization yield as a function of incubation time, and temperature below and above the LLPS boundary. As crystallization temperature intersects with LLPS temperature, a significant increase in crystallization yield is observed. This is consistent with LLPS boosting protein crystallization. Our work suggests a possible strategy for increasing the crystallization success of other proteins, with applications in protein purification.
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spelling doaj-art-394aeb2d8689421ba03a4664dfcc8bcf2025-08-20T02:33:06ZengMDPI AGMolecules1420-30492025-05-013011237110.3390/molecules30112371Yield of Protein Crystallization from Metastable Liquid–Liquid Phase SeparationShamberia Thomas0Joel A. Dougay1Onofrio Annunziata2Department of Chemistry and Biochemistry, Texas Christian University, Fort Worth, TX 76109, USADepartment of Chemistry and Biochemistry, Texas Christian University, Fort Worth, TX 76109, USADepartment of Chemistry and Biochemistry, Texas Christian University, Fort Worth, TX 76109, USAPreparative protein crystallization is regarded as an economically sustainable protein purification alternative to chromatography in biotechnological downstream processing. However, protein crystallization is a not-well-understood process that is usually slow and poorly reproducible. A promising strategy for enhancing protein crystallization is exploiting the metastable liquid–liquid phase separation (LLPS) of protein solutions. Here, we report an enhancement of lysozyme-crystallization yield by using a combination of two additives under LLPS conditions. The first additive, NaCl (0.15 M), is necessary to introduce protein–protein attractive interactions and induce LLPS by lowering temperature. The second additive, 4-(2-hydroxyethyl)-1-piperazineethanesulfonate (HEPES, 0.10 M, pH 7.4), accumulates in the metastable protein-rich liquid phase and thermodynamically stabilizes lysozyme crystals. We found that this combination of additives leads to crystallization yields of higher than 90% under LLPS conditions at a lysozyme concentration of 5% by weight and a fairly low ionic strength (0.2 M) within an operational time of the order of one hour. This crystallization yield is more than three-fold larger than that obtained from samples containing NaCl without HEPES at the same pH and ionic strength. Moreover, we determined crystallization yield as a function of incubation time, and temperature below and above the LLPS boundary. As crystallization temperature intersects with LLPS temperature, a significant increase in crystallization yield is observed. This is consistent with LLPS boosting protein crystallization. Our work suggests a possible strategy for increasing the crystallization success of other proteins, with applications in protein purification.https://www.mdpi.com/1420-3049/30/11/2371NaClHEPESLLPS
spellingShingle Shamberia Thomas
Joel A. Dougay
Onofrio Annunziata
Yield of Protein Crystallization from Metastable Liquid–Liquid Phase Separation
Molecules
NaCl
HEPES
LLPS
title Yield of Protein Crystallization from Metastable Liquid–Liquid Phase Separation
title_full Yield of Protein Crystallization from Metastable Liquid–Liquid Phase Separation
title_fullStr Yield of Protein Crystallization from Metastable Liquid–Liquid Phase Separation
title_full_unstemmed Yield of Protein Crystallization from Metastable Liquid–Liquid Phase Separation
title_short Yield of Protein Crystallization from Metastable Liquid–Liquid Phase Separation
title_sort yield of protein crystallization from metastable liquid liquid phase separation
topic NaCl
HEPES
LLPS
url https://www.mdpi.com/1420-3049/30/11/2371
work_keys_str_mv AT shamberiathomas yieldofproteincrystallizationfrommetastableliquidliquidphaseseparation
AT joeladougay yieldofproteincrystallizationfrommetastableliquidliquidphaseseparation
AT onofrioannunziata yieldofproteincrystallizationfrommetastableliquidliquidphaseseparation