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Engineering Proximal vs Distal Heme-NO Coordination via Dinitrosyl Dynamics: Implications for NO Sensor Design

Overview of attention for article published in Chemical Science, January 2017
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Title
Engineering Proximal vs Distal Heme-NO Coordination via Dinitrosyl Dynamics: Implications for NO Sensor Design
Published in
Chemical Science, January 2017
DOI 10.1039/c6sc04190f
Pubmed ID
Authors

Demet Kekilli, David Petersen, David Pixton, Dlzar Gahfoor, Gaylany Hikmat Abdullah, Florian Dworkowski, Michael Wilson, Derren Heyes, Samantha Hardman, Loretta Murphy, Richard William Strange, Nigel S Scrutton, Colin R. Andrew, Michael Hough, Christine A. Petersen, David A. Pixton, Dlzar D. Ghafoor, Gaylany H. Abdullah, Florian S. N. Dworkowski, Michael T. Wilson, Derren J. Heyes, Samantha J. O. Hardman, Loretta M. Murphy, Richard W. Strange, Nigel S. Scrutton, Michael A. Hough

Abstract

Proximal vs. distal heme-NO coordination is a novel strategy for selective gas response in heme-based NO-sensors. In the case of Alcaligenes xylosoxidans cytochrome c' (AXCP), formation of a transient distal 6cNO complex is followed by scission of the trans Fe-His bond and conversion to a proximal 5cNO product via a putative dinitrosyl species. Here we show that replacement of the AXCP distal Leu16 residue with smaller or similar sized residues (Ala, Val or Ile) traps the distal 6cNO complex, whereas Leu or Phe residues lead to a proximal 5cNO product with a transient or non-detectable distal 6cNO precursor. Crystallographic, spectroscopic, and kinetic measurements of 6cNO AXCP complexes show that increased distal steric hindrance leads to distortion of the Fe-N-O angle and flipping of the heme 7-propionate. However, it is the kinetic parameters of the distal NO ligand that determine whether 6cNO or proximal 5cNO end products are formed. Our data support a 'balance of affinities' mechanism in which proximal 5cNO coordination depends on relatively rapid release of the distal NO from the dinitrosyl precursor. This mechanism, which is applicable to other proteins that form transient dinitrosyls, represents a novel strategy for 5cNO formation that does not rely on an inherently weak Fe-His bond. Our data suggest a general means of engineering selective gas response into biologically-derived gas sensors in synthetic biology.

Twitter Demographics

The data shown below were collected from the profile of 1 tweeter who shared this research output. Click here to find out more about how the information was compiled.

Mendeley readers

The data shown below were compiled from readership statistics for 13 Mendeley readers of this research output. Click here to see the associated Mendeley record.

Geographical breakdown

Country Count As %
Japan 1 8%
Unknown 12 92%

Demographic breakdown

Readers by professional status Count As %
Student > Ph. D. Student 4 31%
Researcher 4 31%
Unspecified 2 15%
Lecturer 2 15%
Professor 1 8%
Other 0 0%
Readers by discipline Count As %
Chemistry 7 54%
Unspecified 3 23%
Agricultural and Biological Sciences 2 15%
Biochemistry, Genetics and Molecular Biology 1 8%

Attention Score in Context

This research output has an Altmetric Attention Score of 1. This is our high-level measure of the quality and quantity of online attention that it has received. This Attention Score, as well as the ranking and number of research outputs shown below, was calculated when the research output was last mentioned on 17 November 2016.
All research outputs
#6,587,050
of 8,647,833 outputs
Outputs from Chemical Science
#1,598
of 1,954 outputs
Outputs of similar age
#202,992
of 295,763 outputs
Outputs of similar age from Chemical Science
#83
of 97 outputs
Altmetric has tracked 8,647,833 research outputs across all sources so far. This one is in the 13th percentile – i.e., 13% of other outputs scored the same or lower than it.
So far Altmetric has tracked 1,954 research outputs from this source. They typically receive a little more attention than average, with a mean Attention Score of 5.9. This one is in the 8th percentile – i.e., 8% of its peers scored the same or lower than it.
Older research outputs will score higher simply because they've had more time to accumulate mentions. To account for age we can compare this Altmetric Attention Score to the 295,763 tracked outputs that were published within six weeks on either side of this one in any source. This one is in the 19th percentile – i.e., 19% of its contemporaries scored the same or lower than it.
We're also able to compare this research output to 97 others from the same source and published within six weeks on either side of this one. This one is in the 5th percentile – i.e., 5% of its contemporaries scored the same or lower than it.