Chemistry - A European Journal
10.1002/chem.201902812
FULL PAPER
valent hydroxide-bridged dinuclear clusters are capable oxidants
and match the kinetic reactivity of the most reactive comparable
oxo-bridged entities, turning the tables in the current
understanding of the activity of several metallo-enzymes. We
continue to explore the reactivity properties and mechanism of
oxidation by these complexes and their relevance to biological
diamond core clusters.
[10] F. F. Pfaff, F. Heims, S. Kundu, S. Mebs, K. Ray, Chem. Commun. 2012,
48, 3730-3732.
[
[
11] S. Hikichi, M. Yoshizawa, Y. Sasakura, M. Akita, Y. Moro-oka, J. Am.
Chem. Soc. 1998, 120, 10567-10568.
12] a) Y. Morimoto, Y. Takagi, T. Saito, T. Ohta, T. Ogura, N. Tohnai, M.
Nakano, S. Itoh, Angew. Chem. Int. Ed. 2018, 57, 7640-7643; b) S. Itoh,
H. Bandoh, M. Nakagawa, S. Nagatomo, T. Kitagawa, K. D. Karlin, S.
Fukuzumi, J. Am. Chem. Soc. 2001, 123, 11168-11178; c) S. Itoh, H.
Bandoh, S. Nagatomo, T. Kitagawa, S. Fukuzumi, J. Am. Chem. Soc.
1999, 121, 8945-8946.
[
[
13] B. S. Mandimutsira, J. L. Yamarik, T. C. Brunold, W. Gu, S. P. Cramer,
C. G. Riordan, J. Am. Chem. Soc. 2001, 123, 9194-9195.
14] S. K. Padamati, D. Angelone, A. Draksharapu, G. Primi, D. J. Martin, M.
Tromp, M. Swart, W. R. Browne, J. Am. Chem. Soc. 2017, 139, 8718-
8724.
Acknowledgements
This publication has emanated from research supported by
European
Research
Council
(ERC-2015-STG-678202).
Research in the McDonald lab is supported in part by a research
grant from Science Foundation Ireland (SFI/15/RS-URF/3307).
XAS experiments were conducted at SSRL beamline 7-3 (SLAC
National Accelerator Laboratory, USA), with support from the
DOE Office of Science (DE-AC02-76SF00515), DOE Office of
Science Office of Biological and Environmental Research and
NIH (P41-GM-103393 and P30-EB-009998). We are grateful to
COST Action CM1305 (ECOSTBio) for networking support. We
thank Prof. Robert Barkley for training on and use of an EPR
spectrometer. We wish to acknowledge the Irish Centre for High-
End Computing (ICHEC) for the provision of computational
facilities and support.
[15] H. Zhang, Y. Dong, Pat. WO2012CN01001 20120726, KBP BioSciences
Co., Ltd., Peop. Rep. China . 2012, p. 73 pp.
[
16] W. K. Anderson, R. Kasliwal, D. M. Houston, Y.-s. Wang, V. L.
Narayanan, R. D. Haugwitz, J. Plowman, J. Med. Chem. 1995, 38, 3789-
3797.
[
[
[
17] F. Cotton, R. Francis, J. Am. Chem. Soc. 1960, 82, 2986-2991.
18] L. Yang, D. R. Powell, R. P. Houser, Dalton Trans. 2007, 955-964.
19] Y. Li, L. Jiang, L. Wang, H. Gao, F. Zhu, Q. Wu, Appl. Organomet. Chem.
2006, 20, 181-186.
[20] C. Jaeheung, F. Hideki, F. Shuhei, S. Masatatsu, Angew. Chem. Int. Ed.
004, 43, 3300-3303.
2
[
21] R. M. Silverstein, F. X. Webster, D. J. Kiemle, D. L. Bryce, Spectrometric
identification of organic compounds, 8th ed., John wiley & sons, 2014.
22] a) E. Carmona, J. M. Marin, P. Palma, M. Paneque, M. L. Poveda, Inorg.
Chem. 1989, 28, 1895-1900; b) N. Kitajima, S. Hikichi, M. Tanaka, Y.
Morooka, J. Am. Chem. Soc. 1993, 115, 5496-5508.
[
Keywords: high-valent oxidant • diamond core • bis-μ-hydroxo-
[23] J. Ferrando-Soria, O. Fabelo, M. Castellano, J. Cano, S. Fordham, H. C.
Zhou, Chem. Commun. 2015, 51, 13381-13384.
Ni
2
• hydrocarbon oxidation • bioinorganic chemistry
[
24] K. Honda, J. Cho, T. Matsumoto, J. Roh, H. Furutachi, T. Tosha, M. Kubo,
S. Fujinami, T. Ogura, T. Kitagawa, M. Suzuki, Angew. Chem. Int. Ed.
[
1]
a) L. Que, Jr., W. B. Tolman, Nature 2008, 455, 333-340; b) M. O. Ross,
A. C. Rosenzweig, J. Biol. Inorg. Chem. 2017, 22, 307-319.
S. Sirajuddin, A. C. Rosenzweig, Biochemistry 2015, 54, 2283-2294.
G. E. Cutsail, 3rd, R. Banerjee, A. Zhou, L. Que, Jr., J. D. Lipscomb, S.
DeBeer, J Am Chem Soc 2018, 140, 16807-16820.
2009, 48, 3304-3307.
[
[
[
25] R. Schenker, B. S. Mandimutsira, C. G. Riordan, T. C. Brunold, J. Am.
Chem. Soc. 2002, 124, 13842-13855.
[
[
2]
3]
26] a) R. I. Haines, A. McAuley, Coord. Chem. Rev. 1981, 39, 77-119; b) S.
A. Jacobs, D. W. Margerum, Inorg. Chem. 1984, 23, 1195-1201.
27] a) G. J. Colpas, M. J. Maroney, C. Bagyinka, M. Kumar, W. S. Willis, S.
L. Suib, P. K. Mascharak, N. Baidya, Inorg. Chem. 1991, 30, 920-928; b)
P. Mondal, P. Pirovano, A. Das, E. R. Farquhar, A. R. McDonald, J. Am.
Chem. Soc. 2018, 140, 1834-1841; c) S. Kundu, F. F. Pfaff, E. Miceli, I.
Zaharieva, C. Herwig, S. Yao, E. R. Farquhar, U. Kuhlmann, E. Bill, P.
Hildebrandt, H. Dau, M. Driess, C. Limberg, K. Ray, Angew. Chem. Int.
Ed. 2013, 52, 5622-5626.
[
4]
a) C. Deville, S. K. Padamati, J. Sundberg, V. McKee, W. R. Browne, C.
J. McKenzie, Angew. Chem. Int. Ed. 2016, 55, 545-549; b) R. A. Baglia,
K. A. Prokop-Prigge, H. M. Neu, M. A. Siegler, D. P. Goldberg, J. Am.
Chem. Soc. 2015, 137, 10874-10877; c) D. E. Lansky, D. P. Goldberg,
Inorg. Chem. 2006, 45, 5119-5125.
[
5]
a) M. Costas, M. P. Mehn, M. P. Jensen, L. Que, Chem. Rev. 2004, 104,
9
39-986; b) J.-U. Rohde, J.-H. In, M. H. Lim, W. W. Brennessel, M. R.
Bukowski, A. Stubna, E. Münck, W. Nam, L. Que, Science 2003, 299,
037-1039; c) J. E. M. N. Klein, L. Que, in Encyclopedia of Inorganic and
[
[
[
[
28] A. Roe, D. Schneider, R. Mayer, J. Pyrz, J. Widom, L. Que Jr, J. Am.
Chem. Soc. 1984, 106, 1676-1681.
1
Bioinorganic Chemistry, 2016, pp. 1-22; d) M. R. Mills, A. C. Weitz, M. P.
Hendrich, A. D. Ryabov, T. J. Collins, J Am Chem Soc 2016, 138, 13866-
29] G. Shulman, Y. Yafet, P. Eisenberger, W. Blumberg, Proc. Natl. Acad.
Sci. 1976, 73, 1384-1388.
13869; e) W. Nam, Acc. Chem. Res. 2015, 48, 2415-2423; f) S. Hong, K.
30] J. Cho, R. Sarangi, J. Annaraj, S. Y. Kim, M. Kubo, T. Ogura, E. I.
Solomon, W. Nam, Nat. Chem. 2009, 1, 568.
D. Sutherlin, J. Park, E. Kwon, M. A. Siegler, E. I. Solomon, W. Nam, Nat.
Commun. 2014, 5, 5440; g) D. C. Lacy, R. Gupta, K. L. Stone, J. Greaves,
J. W. Ziller, M. P. Hendrich, A. Borovik, J. Am. Chem. Soc. 2010, 132,
31] L. R. Furenlid, M. W. Renner, E. Fujita, Physica B Condens. Matter 1995,
208, 739-742.
12188-12190.
[
[
32] R. A. Scott, M. K. Eidsness, Comments Inorg. Chem. 1988, 7, 235-267.
33] K. Shiren, S. Ogo, S. Fujinami, H. Hayashi, M. Suzuki, A. Uehara, Y.
Watanabe, Y. Moro-oka, J. Am. Chem. Soc. 2000, 122, 254-262.
[
[
6]
7]
A. W. Pierpont, T. R. Cundari, Inorg. Chem. 2010, 49, 2038-2046.
P. Pirovano, E. R. Farquhar, M. Swart, A. R. McDonald, J. Am. Chem.
Soc. 2016, 138, 14362-14370.
[
34] S. Mahapatra, J. A. Halfen, E. C. Wilkinson, G. Pan, X. Wang, V. G.
Young, C. J. Cramer, L. Que, W. B. Tolman, J. Am. Chem. Soc. 1996,
[
[
8]
9]
T. Corona, F. F. Pfaff, F. Acuna-Pares, A. Draksharapu, C. J. Whiteoak,
V. Martin-Diaconescu, J. Lloret-Fillol, W. R. Browne, K. Ray, A. Company,
Chem. Eur. J. 2015, 21, 15029-15038.
118, 11555-11574.
[
[
[
35] L. Que Jr, W. B. Tolman, Angew. Chem. Int. Ed. 2002, 41, 1114-1137.
36] P. Pirovano, A. R. McDonald, Eur. J. Inorg. Chem. 2018, 2018, 547-560.
37] A. Ohta, K. Hattori, Y. Kusumoto, T. Kawase, T. Kobayashi, H. Naito, C.
Kitamura, Chem. Lett. 2012, 41, 674-676.
T. Corona, A. Draksharapu, S. K. Padamati, I. Gamba, V. Martin-
Diaconescu, F. Acuna-Pares, W. R. Browne, A. Company, J Am Chem
Soc 2016, 138, 12987-12996.
This article is protected by copyright. All rights reserved.