2 publications

2 publications

Exploring and Adapting the Molecular Selectivity of Artificial Metalloenzymes

Review

Tanaka, K.

BCSJ 2021, 94, 382-396, 10.1246/bcsj.20200316

In recent years, artificial metalloenzymes (ArMs) have become a major research interest in the field of biocatalysis. With the ability to facilitate new-to-nature reactions, researchers have generally prepared them either through intensive protein engineering studies or through the introduction of abiotic transition metals. The aim of this review will be to summarize the major types of ArMs that have been recently developed, as well as to highlight their general reaction scope. A point of emphasis will also be made to discuss the promising ways that the molecular selectivity of ArMs can be applied to in areas of pharmaceutical synthesis, diagnostics, and drug therapy.


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Molecular Design and Regulation of Metalloenzyme Activities through Two Novel Approaches: Ferritin and P450s

Review

Watanabe, Y.

BCSJ 2020, 93, 379-392, 10.1246/bcsj.20190305

We have developed two novel approaches for the construction of artificial metalloenzymes showing either unique catalytic activities or substrate specificity. The first example is the use of a hollow cage of apo-ferritin as a reaction vessel for hydrogenation of olefins, Suzuki-Miyaura C-C coupling and phenylacetylene polymerization by employing Pd0 nano-clusters, Pd2+(η3-C3H5) complexes and Rh1+(nbd) (nbd = norbornadiene) complexes introduced in the hollow cage, respectively. The second approach is the use of “decoy molecules” to change substrate specificity of P450s, allowing epoxidation and hydroxylation activities toward nonnative organic substrates in P450SPα, P450BSβ and P450BM3 without the mutation of any amino acid. Finally, the decoy strategy has been applied to an in vivo system of P450, i.e., the use of P450BM3 expressed in the whole cell of E. coli to oxidize benzene to phenol.


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