期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 20, 期 51, 页码 17019-17024出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201404765
关键词
amphiphiles; carbon dioxide; enzyme catalysis; self-assembly; sequestration
资金
- Korean Research Foundation - Korean Government [NRF-2013R1A1A2006459]
- National Research Foundation of Korea [2013R1A1A2006459] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
A biomimetic catalyst was prepared through the self-assembly of a bolaamphiphilic molecule with histidine moieties for the sequestration of carbon dioxide. The histidyl bolaamphiphilic molecule bis(N-alpha-amidohistidine)-1,7-heptane dicarboxylate has been synthesized and self-assembled to produce analogues of the active sites of carbonic anhydrase (CA) after association with Zn2+ ions. Spectroscopic analysis demonstrated the coordination of the Zn2+ ions with histidine imidazole moieties, which is the core conformation of CA active sites. The Zn-associated self-assembly worked as a CA-mimetic catalyst that shows catalytic activity for CO2 hydration. Evaluation of the kinetics of using para-ni-trophenylacetate revealed that the kinetic parameters of the CA-mimetic catalyst were maximized at the optimal Zn concentration and that excess Zn ions resulted in deteriorated catalytic activity. The performance of the CA-mimetic catalyst was enhanced by changing the pH value and temperature of the reaction, which implies that the hydrolysis of the substrate is the rate-determining step. The catalyst-assisted sequestration of CO2 was demonstrated by CaCO3 precipitation upon the addition of Ca2+ ions. This study offers an easy way to prepare enzyme analogues for CO2 sequestration through the self-assembly of bolaamphiphile molecules with designer biochemical moieties.
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