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Mechanistic exploitation of a self-repairing, blocked proton transfer pathway in an O2-tolerant [NiFe]-hydrogenase

Abstract:

Catalytic long-range proton transfer in [NiFe]-hydrogenases has long been associated with a highly conserved glutamate (E) situated within 4 Å of the active site. Substituting for glutamine (Q) in the O2-tolerant [NiFe]-hydrogenase-1 from Escherichia coli produces a variant (E28Q) with unique properties that have been investigated using protein film electrochemistry, protein film infrared electrochemistry, and X-ray crystallography. At pH 7 and moderate potential, E28Q displays approximately ...

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Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1021/jacs.8b04798

Authors


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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; Inorganic Chemistry Laboratory
Role:
Author
ORCID:
0000-0001-5264-464X
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry; Inorganic Chemistry Laboratory
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry; Inorganic Chemistry Laboratory
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry; Inorganic Chemistry Laboratory
Role:
Author
ORCID:
0000-0001-6444-9382
More from this funder
Name:
Royal Society
Funding agency for:
Armstrong, F
Grant:
BB/L009722/1
More from this funder
Name:
Biotechnology and Biological Sciences Research Council
Funding agency for:
Armstrong, F
Grant:
BB/L009722/1
More from this funder
Name:
Engineering and Physical Sciences Research Council
Funding agency for:
Ash, P
Vincent, K
Grant:
EP/N013514/1
EP/N013514/1
More from this funder
Name:
Physical Sciences Research Council
Funding agency for:
Brooke, E
More from this funder
Name:
Global Innovation Initiative
Funding agency for:
Brooke, E
Publisher:
American Chemical Society
Journal:
Journal of the American Chemical Society More from this journal
Volume:
140
Issue:
32
Pages:
10208-10220
Publication date:
2018-08-02
Acceptance date:
2018-07-18
DOI:
EISSN:
1520-5126
ISSN:
0002-7863
Pmid:
30070475
Language:
English
Keywords:
Pubs id:
pubs:894328
UUID:
uuid:cb7e672c-f32f-4986-9e62-43df808d19c8
Local pid:
pubs:894328
Source identifiers:
894328
Deposit date:
2018-08-30

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