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Muonium Chemistry at Diiron Subsite Analogues of [FeFe]‐Hydrogenase
Author(s) -
Wright Joseph A.,
Peck Jamie N. T.,
Cottrell Stephen P.,
Jablonskytė Aušra,
Oganesyan Vasily S.,
Pickett Christopher J.,
Jayasooriya Upali A.
Publication year - 2016
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201607109
Subject(s) - muonium , hydride , chemistry , protonation , hydrogenase , metal , microsecond , hydrogen , catalysis , photochemistry , inorganic chemistry , computational chemistry , ion , organic chemistry , physics , astronomy
The chemistry of metal hydrides is implicated in a range of catalytic processes at metal centers. Gaining insight into the formation of such sites by protonation and/or electronation is therefore of significant value in fully exploiting the potential of such systems. Here, we show that the muonium radical (Mu . ), used as a low isotopic mass analogue of hydrogen, can be exploited to probe the early stages of hydride formation at metal centers. Mu . undergoes the same chemical reactions as H . and can be directly observed due to its short lifetime (in the microseconds) and unique breakdown signature. By implanting Mu . into three models of the [FeFe]‐hydrogenase active site we have been able to detect key muoniated intermediates of direct relevance to the hydride chemistry of these systems.