Electrostatic Effect of Functional Surfaces on the Activity of Adsorbed Enzymes: Simulations and Experiments
| Autor: | Jin-Yi Zhong, Shengjiang Yang, Jian Zhou, Zhe Zhang, He Zheng, Yan Cui, Yong-Chao Zheng |
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| Rok vydání: | 2020 |
| Předmět: |
Models
Molecular Materials science Hydrolases Surface Properties Static Electricity Rational design Substrate (chemistry) 02 engineering and technology Enzymes Immobilized 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences 0104 chemical sciences Enzyme catalysis Catalysis Adsorption Chemical engineering Rhodococcus Surface modification General Materials Science 0210 nano-technology Haloalkane dehalogenase Protein adsorption |
| Zdroj: | ACS Applied Materials & Interfaces. 12:35676-35687 |
| ISSN: | 1944-8252 1944-8244 |
| DOI: | 10.1021/acsami.0c08080 |
| Popis: | The efficient immobilization of haloalkane dehalogenase (DhaA) on carriers with retaining of its catalytic activity is essential for its application in environmental remediation. In this work, adsorption orientation and conformation of DhaA on different functional surfaces were investigated by computer simulations; meanwhile, the mechanism of varying the catalytic activity was also probed. The corresponding experiments were then carried out to verify the simulation results. (The simulations of DhaA on SAMs provided parallel insights into DhaA adsorption in carriers. Then, the theory-guided experiments were carried out to screen the best surface functional groups for DhaA immobilization.) The electrostatic interaction was considered as the main impact factor for the regulation of enzyme orientation, conformation, and enzyme bioactivity during DhaA adsorption. The synergy of overall conformation, enzyme substrate tunnel structural parameters, and distance between catalytic active sites and surfaces codetermined the catalytic activity of DhaA. Specifically, it was found that the positively charged surface with suitable surface charge density was helpful for the adsorption of DhaA and retaining its conformation and catalytic activity and was favorable for higher enzymatic catalysis efficiency in haloalkane decomposition and environmental remediation. The neutral, negatively charged surfaces and positively charged surfaces with high surface charge density always caused relatively larger DhaA conformation change and decreased catalytic activity. This study develops a strategy using a combination of simulation and experiment, which can be essential for guiding the rational design of the functionalization of carriers for enzyme adsorption, and provides a practical tool to rationally screen functional groups for the optimization of adsorbed enzyme functions on carriers. More importantly, the strategy is general and can be applied to control behaviors of different enzymes on functional carrier materials. |
| Databáze: | OpenAIRE |
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