A01：Emergence of novel functions through integration of bio-metal complexes and nucleic acids and its application to exploring the role of bio-metal ions in abiogenesis
Yasuhiko YAMAMOTO
（Department of Chemistry, University of Tsukuba）
Lab website
Heme is perhaps the most ubiquitous and abundant cofactor found in nature and the most functionally diverse. Heme is incorporated, as a prosthetic group, into various apoproteins to form a series of hemoproteins that play vital roles in biological systems. Despite such ubiquitous occurrence of heme in nature, no functional role in vivo has yet been attributed to heme incorporated into nucleic acids. The RNA world hypothesis has provided a strong stimulus for exploring new catalytic properties of nucleic acids. Incorporation of cofactors into nucleic acids is expected to contribute to such a study, and heme is most likely an ancient compound and a likely player in the postulated RNA world. Heme binds selectively to G-quadruplex nucleic acids to form complexes which exhibit one-electron (peroxidase) and two-electron (peroxygenase) oxidation reactions. Thus, the heme-bound nucleic acids recapitulate at least two of the known catalytic functions of contemporary hemoproteins, lending credence to heme’s link to a primordial RNA world. In my study, the role of bio-metal ions in abiogenesis will be explored.
Major publications
K. Hayasaka, T. Shibata, A. Momotake, T. Matsui, S, Neya, T. Ishizuka, Y. Xu, Y. Yamamoto
“Characterization of Structure and Catalytic Activity of a Complex between Heme and an All Parallel-Stranded Tetrameric G-Quadruplex Formed from DNA/RNA Chimera Sequence d(TTA)r(GGG)dT”
Bull. Chem. Soc. Jpn. 2020, 93, 621-629
doi:10.1246/bcsj.20190157
R. Shinomiya, H. Araki, A. Momotake, H. Kotani, T. Kojima, Y. Yamamoto
“Identification of Intermediates in Peroxidase Catalytic Cycle of a DNAzyme Possessing Heme”
Bull. Chem. Soc. Jpn. 2019, 92, 1729-1736
doi:10.1246/bcsj.20200013
C.-D. Xiao, T. Shibata, Y. Yamamoto, Y. Xu
“An intramolecular antiparallel G-quadruplex formed by human telomere RNA”
Chem. Commun. 2018, 54, 3944-3946
doi:10.1039/c8cc01427b
Y. Yamamoto, H. Araki, R. Shinomiya, K. Hayasaka, Y. Nakayama, K. Ochi, T. Shibata, A. Momotake, T. Ohyama, M. Hagihara, H. Hemmi
“Structures and Catalytic Activities of Complexes between Heme and All Parallel-Stranded Monomeric G-Quadruplex DNAs”
Biochemistry 2018, 57, 5938-5948
doi:10.1021/acs.biochem.8b00792
R. Shinomiya, Y. Katahira, H. Araki, T. Shibata, A. Momotake, S. Yanagisawa, T. Ogura, A. Suzuki, S. Neya, Y. Yamamoto
“Characterization of Catalytic Activities and Heme Coordination Structures of Heme-DNA Complexes Composed of Some Chemically Modified Hemes and an All Parallel-Stranded Tetrameric G-Quadruplex DNA Formed from d(TTAGGG)”
Biochemistry 2018, 57, 5930-5937
doi:10.1021/acs.biochem.8b00793