Investigation of laccase activity in cholinium-based ionic liquids using experimental and molecular dynamics techniques

resumo

Laccases hold great potential for biotechnological applications, particularly in environmental pollutant remediation. Laccase activity is governed by the solvent environment, and ionic liquids (ILs) emerge as a versatile solvent for activation or stabilization of enzymes. Herein, effects of cholinium-based ILs formulated with carboxylic acids, inorganic acid, and amino acids as anionic species, on the catalytic activity of laccase from Trametes versicolor were investigated by experimental and computational approaches. Experimental results showed that laccase activity was enhanced by 21.39 % in 0.5 M cholinium dihydrogen citrate ([Cho][DHC]), in relation to the laccase activity in phosphate buffer medium. However, cholinium aminoate ILs negatively affected laccase activity, as evidenced by the partial deactivation of laccase in both cholinium glycinate and cholinium phenylalaninate, at concentrations of 0.1 M and 0.5 M, respectively. Molecular dynamics studies revealed that the enhancement of laccase activity in [Cho][DHC] might be attributed to the highly stabilized and compact structure of laccase, facilitating a better internal electron transfer during the laccase-substrate interactions. Enhanced catalytic performance of laccase in [Cho][DHC] was postulated to be driven by the high accumulation level of dihydrogen citrate anions around laccase's surface. [Cho][DHC] holds great promise as a cosolvent in laccase-catalyzed biochemical reactions.

palavras-chave

LIGNIN MODEL COMPOUNDS; TRAMETES-VERSICOLOR; CATALYTIC-ACTIVITY; ELECTRON-TRANSFER; ORGANIC-SOLVENTS; MEDIATOR SYSTEMS; STABILITY; SIMULATION

categoria

Biochemistry & Molecular Biology; Chemistry; Polymer Science

autores

Chan, KK; Pereira, AF; Valente, AI; Tavares, APM; Coutinho, JAP; Ooi, CW

Grupos

G4 - Materiais Renováveis e Economia Circular
G5 - Materiais Biomiméticos, Biológicos e Vivos

Projectos

CICECO - Aveiro Institute of Materials (UIDB/50011/2020)

CICECO - Aveiro Institute of Materials (UIDP/50011/2020)

agradecimentos

The authors acknowledge the Fundamental Research Grant Scheme (FRGS) [FRGS/1/2018/STG04/MUSM/02/1] by the Ministry of Higher Education (MOHE) Malaysia and Monash University Malaysia-ASEAN Research Grant Scheme 2021 (ASE-000010) . The authors also express their gratitude to Monash University Malaysia High-Performance Computing for providing computational resources for this work. research received partial support from the Monash eResearch Centre eSolutions-Research Support Services through the utilization of MonARCH HPC Cluster. K.K. Chan acknowledges the Monash Global Mobility program in providing financial support to conduct research CICECO-Aveiro Institute of Materials, University of Aveiro, Portugal. This work was partly within the scope of the project CICECO-Aveiro Institute of Materials, UIDB/50011/2020 (DOI 10.54499/UIDB/50011/2020) , UIDP/50011/2020 (DOI 10.54499/UIDP/50011/2020) & P/0006/2020 (DOI 10.54499/LA/P/0006/2020) , financed by national funds through the FCT/MCTES (PIDDAC) . Ana P.M. Tavares acknowledges FCT for the research contract CEECIND/01867/2020 .54499/2020.01867.CEECIND/CP1589/CT0013) under the ScientificEmployment Stimulus-Individual Calls. Ana F. Pereira and Ana Valente acknowledge FCT for the PhD grant 2022/13247/BD 2021.08352.BD (DOI:10.54499/2021.08352.BD) , respectively.r Employment Stimulus-Individual Calls. Ana F. Pereira and Ana Valente acknowledge FCT for the PhD grant 2022/13247/BD 2021.08352.BD (DOI:10.54499/2021.08352.BD) , respectively.