Acefylline activates filaggrin deimination by peptidylarginine deiminases in the upper epidermis

•Screening of a large chemical library identified xanthines as PAD potential activators.•Deimination of human filaggrin was enhanced by caffeine, theobromine and acefylline.•Topical application of acefylline on reconstructed human epidermis improved deimination.•Acefylline is the first identified ac...

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Published in:Journal of dermatological science Vol. 81; no. 2; pp. 101 - 106
Main Authors: Méchin, Marie-Claire, Cau, Laura, Galliano, Marie-Florence, Daunes-Marion, Sylvie, Poigny, Stéphane, Vidaluc, Jean-Louis, Bessou-Touya, Sandrine, Takahara, Hidenari, Serre, Guy, Duplan, Hélène, Simon, Michel
Format: Journal Article
Language:English
Published: Netherlands Elsevier Ireland Ltd 01.02.2016
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ISSN:0923-1811, 1873-569X, 1873-569X
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Abstract •Screening of a large chemical library identified xanthines as PAD potential activators.•Deimination of human filaggrin was enhanced by caffeine, theobromine and acefylline.•Topical application of acefylline on reconstructed human epidermis improved deimination.•Acefylline is the first identified activator of PAD1 and PAD3. Peptidylarginine deiminases (PADs) catalyze deimination (or citrullination), a calcium-dependent post-translational modification involved in several physiological processes and human diseases, such as rheumatoid arthritis and cancer. Deimination of filaggrin (FLG) by PAD1 and PAD3 during the last steps of keratinocyte differentiation is a crucial event for the epidermis function and homeostasis. This allows the complete degradation of FLG, leading to the production of free amino acids and their derivatives that are essential for epidermal photoprotection and moisturizing of the stratum corneum. To increase the flux of this catabolic pathway, we searched for activators of PADs. A large chemical library was screened first in silico and then by using an automated assay based on an indirect colorimetric measurement of recombinant human PAD activity. Potential activators were then confirmed using a recombinant human FLG as a substrate, and secondly after topical application at the surface of three-dimensional reconstructed human epidermis. The data obtained after the library screening pointed to xanthine derivatives as potential PAD activators. Among seven xanthine derivatives tested at 50–300μM, caffeine, theobromine and acefylline proved to be the most potent enhancers of in vitro deimination of FLG by PAD1 and PAD3. After topical application of a gel formulation containing 3% acefylline at the surface of reconstructed epidermis, immunoblotting analysis showed an increase in the total amount of deiminated proteins, and confocal microscopy showed an enhanced deimination in the stratum corneum. This demonstrated the activation of PADs in living cells. As a PAD activator, acefylline will be useful to study the role of deimination and could be proposed to increase or correct the hydration of the cornified layers of the epidermis.
AbstractList Peptidylarginine deiminases (PADs) catalyze deimination (or citrullination), a calcium-dependent post-translational modification involved in several physiological processes and human diseases, such as rheumatoid arthritis and cancer. Deimination of filaggrin (FLG) by PAD1 and PAD3 during the last steps of keratinocyte differentiation is a crucial event for the epidermis function and homeostasis. This allows the complete degradation of FLG, leading to the production of free amino acids and their derivatives that are essential for epidermal photoprotection and moisturizing of the stratum corneum.BACKGROUNDPeptidylarginine deiminases (PADs) catalyze deimination (or citrullination), a calcium-dependent post-translational modification involved in several physiological processes and human diseases, such as rheumatoid arthritis and cancer. Deimination of filaggrin (FLG) by PAD1 and PAD3 during the last steps of keratinocyte differentiation is a crucial event for the epidermis function and homeostasis. This allows the complete degradation of FLG, leading to the production of free amino acids and their derivatives that are essential for epidermal photoprotection and moisturizing of the stratum corneum.To increase the flux of this catabolic pathway, we searched for activators of PADs.OBJECTIVETo increase the flux of this catabolic pathway, we searched for activators of PADs.A large chemical library was screened first in silico and then by using an automated assay based on an indirect colorimetric measurement of recombinant human PAD activity. Potential activators were then confirmed using a recombinant human FLG as a substrate, and secondly after topical application at the surface of three-dimensional reconstructed human epidermis.METHODSA large chemical library was screened first in silico and then by using an automated assay based on an indirect colorimetric measurement of recombinant human PAD activity. Potential activators were then confirmed using a recombinant human FLG as a substrate, and secondly after topical application at the surface of three-dimensional reconstructed human epidermis.The data obtained after the library screening pointed to xanthine derivatives as potential PAD activators. Among seven xanthine derivatives tested at 50-300μM, caffeine, theobromine and acefylline proved to be the most potent enhancers of in vitro deimination of FLG by PAD1 and PAD3. After topical application of a gel formulation containing 3% acefylline at the surface of reconstructed epidermis, immunoblotting analysis showed an increase in the total amount of deiminated proteins, and confocal microscopy showed an enhanced deimination in the stratum corneum. This demonstrated the activation of PADs in living cells.RESULTSThe data obtained after the library screening pointed to xanthine derivatives as potential PAD activators. Among seven xanthine derivatives tested at 50-300μM, caffeine, theobromine and acefylline proved to be the most potent enhancers of in vitro deimination of FLG by PAD1 and PAD3. After topical application of a gel formulation containing 3% acefylline at the surface of reconstructed epidermis, immunoblotting analysis showed an increase in the total amount of deiminated proteins, and confocal microscopy showed an enhanced deimination in the stratum corneum. This demonstrated the activation of PADs in living cells.As a PAD activator, acefylline will be useful to study the role of deimination and could be proposed to increase or correct the hydration of the cornified layers of the epidermis.CONCLUSIONAs a PAD activator, acefylline will be useful to study the role of deimination and could be proposed to increase or correct the hydration of the cornified layers of the epidermis.
•Screening of a large chemical library identified xanthines as PAD potential activators.•Deimination of human filaggrin was enhanced by caffeine, theobromine and acefylline.•Topical application of acefylline on reconstructed human epidermis improved deimination.•Acefylline is the first identified activator of PAD1 and PAD3. Peptidylarginine deiminases (PADs) catalyze deimination (or citrullination), a calcium-dependent post-translational modification involved in several physiological processes and human diseases, such as rheumatoid arthritis and cancer. Deimination of filaggrin (FLG) by PAD1 and PAD3 during the last steps of keratinocyte differentiation is a crucial event for the epidermis function and homeostasis. This allows the complete degradation of FLG, leading to the production of free amino acids and their derivatives that are essential for epidermal photoprotection and moisturizing of the stratum corneum. To increase the flux of this catabolic pathway, we searched for activators of PADs. A large chemical library was screened first in silico and then by using an automated assay based on an indirect colorimetric measurement of recombinant human PAD activity. Potential activators were then confirmed using a recombinant human FLG as a substrate, and secondly after topical application at the surface of three-dimensional reconstructed human epidermis. The data obtained after the library screening pointed to xanthine derivatives as potential PAD activators. Among seven xanthine derivatives tested at 50–300μM, caffeine, theobromine and acefylline proved to be the most potent enhancers of in vitro deimination of FLG by PAD1 and PAD3. After topical application of a gel formulation containing 3% acefylline at the surface of reconstructed epidermis, immunoblotting analysis showed an increase in the total amount of deiminated proteins, and confocal microscopy showed an enhanced deimination in the stratum corneum. This demonstrated the activation of PADs in living cells. As a PAD activator, acefylline will be useful to study the role of deimination and could be proposed to increase or correct the hydration of the cornified layers of the epidermis.
Background: Peptidylarginine deiminases (PADs) catalyze deimination (or citrullination), a calcium-dependent post-translational modification involved in several physiological processes and human diseases, such as rheumatoid arthritis and cancer. Deimination of filaggrin (FLG) by PAD1 and PAD3 during the last steps of keratinocyte differentiation is a crucial event for the epidermis function and homeostasis. This allows the complete degradation of FLG, leading to the production of free amino acids and their derivatives that are essential for epidermal photoprotection and moisturizing of the stratum corneum. Objective: To increase the flux of this catabolic pathway, we searched for activators of PADs. Methods: A large chemical library was screened first in silico and then by using an automated assay based on an indirect colorimetric measurement of recombinant human PAD activity. Potential activators were then confirmed using a recombinant human FLG as a substrate, and secondly after topical application at the surface of three-dimensional reconstructed human epidermis. Results: The data obtained after the library screening pointed to xanthine derivatives as potential PAD activators. Among seven xanthine derivatives tested at 50-300μM, caffeine, theobromine and acefylline proved to be the most potent enhancers of in vitro deimination of FLG by PAD1 and PAD3. After topical application of a gel formulation containing 3% acefylline at the surface of reconstructed epidermis, immunoblotting analysis showed an increase in the total amount of deiminated proteins, and confocal microscopy showed an enhanced deimination in the stratum corneum. This demonstrated the activation of PADs in living cells. Conclusion: As a PAD activator, acefylline will be useful to study the role of deimination and could be proposed to increase or correct the hydration of the cornified layers of the epidermis.
Peptidylarginine deiminases (PADs) catalyze deimination (or citrullination), a calcium-dependent post-translational modification involved in several physiological processes and human diseases, such as rheumatoid arthritis and cancer. Deimination of filaggrin (FLG) by PAD1 and PAD3 during the last steps of keratinocyte differentiation is a crucial event for the epidermis function and homeostasis. This allows the complete degradation of FLG, leading to the production of free amino acids and their derivatives that are essential for epidermal photoprotection and moisturizing of the stratum corneum. To increase the flux of this catabolic pathway, we searched for activators of PADs. A large chemical library was screened first in silico and then by using an automated assay based on an indirect colorimetric measurement of recombinant human PAD activity. Potential activators were then confirmed using a recombinant human FLG as a substrate, and secondly after topical application at the surface of three-dimensional reconstructed human epidermis. The data obtained after the library screening pointed to xanthine derivatives as potential PAD activators. Among seven xanthine derivatives tested at 50-300μM, caffeine, theobromine and acefylline proved to be the most potent enhancers of in vitro deimination of FLG by PAD1 and PAD3. After topical application of a gel formulation containing 3% acefylline at the surface of reconstructed epidermis, immunoblotting analysis showed an increase in the total amount of deiminated proteins, and confocal microscopy showed an enhanced deimination in the stratum corneum. This demonstrated the activation of PADs in living cells. As a PAD activator, acefylline will be useful to study the role of deimination and could be proposed to increase or correct the hydration of the cornified layers of the epidermis.
Highlights • Screening of a large chemical library identified xanthines as PAD potential activators. • Deimination of human filaggrin was enhanced by caffeine, theobromine and acefylline. • Topical application of acefylline on reconstructed human epidermis improved deimination. • Acefylline is the first identified activator of PAD1 and PAD3.
Author Galliano, Marie-Florence
Vidaluc, Jean-Louis
Serre, Guy
Daunes-Marion, Sylvie
Duplan, Hélène
Méchin, Marie-Claire
Takahara, Hidenari
Bessou-Touya, Sandrine
Simon, Michel
Cau, Laura
Poigny, Stéphane
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  email: michel.simon@udear.cnrs.fr
  organization: Paul Sabatier University (UPS), Toulouse, France
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Issue 2
Keywords FLG
Post-translational modification
PAD
Epidermal barrier
LUT
Skin
Xanthine
Filaggrin
lookup table
peptidylarginine deiminase
filaggrin
Language English
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SSID ssj0005249
Score 2.176896
Snippet •Screening of a large chemical library identified xanthines as PAD potential activators.•Deimination of human filaggrin was enhanced by caffeine, theobromine...
Highlights • Screening of a large chemical library identified xanthines as PAD potential activators. • Deimination of human filaggrin was enhanced by caffeine,...
Peptidylarginine deiminases (PADs) catalyze deimination (or citrullination), a calcium-dependent post-translational modification involved in several...
Background: Peptidylarginine deiminases (PADs) catalyze deimination (or citrullination), a calcium-dependent post-translational modification involved in...
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SubjectTerms Administration, Cutaneous
Cells, Cultured
Computer Simulation
Dermatology
Dose-Response Relationship, Drug
Enzyme Activation
Enzyme Activators - administration & dosage
Enzyme Activators - chemistry
Enzyme Activators - pharmacology
Epidermal barrier
Epidermal Cells Epidermis / drug effects
Epidermis - cytology
Epidermis - drug effects
Epidermis - enzymology
Filaggrin
Human health and pathology
Humans
Humans Hydrolases / metabolism
Hydrolases - metabolism
Infectious diseases
Intermediate Filament Proteins - chemistry
Intermediate Filament Proteins - metabolism
Keratinocytes - drug effects
Keratinocytes - enzymology
Life Sciences
Models, Molecular
Post-translational modification
Protein Conformation
Protein Processing, Post-Translational
Protein-Arginine Deiminases
Skin
Small Molecule Libraries
Structure-Activity Relationship
Theophylline - administration & dosage
Theophylline - analogs & derivatives
Theophylline - chemistry
Theophylline - pharmacology
Xanthine
Title Acefylline activates filaggrin deimination by peptidylarginine deiminases in the upper epidermis
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Volume 81
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