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Discovery of dark pH-dependent H+ migration in a [NiFe]-hydrogenase and its mechanistic relevance: mobilizing the hydrido ligand of the Ni-C intermediate

Abstract:

Despite extensive studies on [NiFe]-hydrogenases, the mechanism by which these enzymes produce and activate H2 so efficiently remains unclear. A well-known EPR-active state produced under H2 and known as Ni-C is assigned as a NiIII–FeII species with a hydrido ligand in the bridging position between the two metals. It has long been known that low-temperature photolysis of Ni-C yields distinctive EPR-active states, collectively...

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Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1021/jacs.5b03182

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Role:
Author
ORCID:
0000-0001-6341-9368
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Role:
Author
ORCID:
0000-0001-6794-3343
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Role:
Author
ORCID:
0000-0002-5291-4328
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Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Inorganic Chemistry
Role:
Author
ORCID:
0000-0002-9549-4220
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Inorganic Chemistry
Role:
Author
ORCID:
0000-0001-5264-464X
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Name:
Biotechnology and Biological Sciences Research Council
Grant:
BB/L009722/1
BB/I022309/1
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Name:
Engineering and Physical Sciences Research Council
Grant:
EP/L011972/1
EP/D048559/1
Publisher:
American Chemical Society
Journal:
Journal of the American Chemical Society More from this journal
Volume:
137
Issue:
26
Pages:
8484-8489
Place of publication:
United States
Publication date:
2015-06-23
Acceptance date:
2015-06-23
DOI:
EISSN:
1520-5126
ISSN:
0002-7863
Pmid:
26103582

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