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Exploring the biochemical properties and remediation applications of the unusual explosive-degrading P450 system XpIA/B

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Exploring the biochemical properties and remediation applications of the unusual explosive-degrading P450 system XpIA/B. / Jackson, Rosamond G.; Rylott, Elizabeth L.; Fournier, Diane; Hawari, Jalal; Bruce, Neil C.

In: Proceedings of the National Academy of Sciences of the United States of America, Vol. 104, No. 43, 23.10.2007, p. 16822-16827.

Research output: Contribution to journalArticle

Harvard

Jackson, RG, Rylott, EL, Fournier, D, Hawari, J & Bruce, NC 2007, 'Exploring the biochemical properties and remediation applications of the unusual explosive-degrading P450 system XpIA/B', Proceedings of the National Academy of Sciences of the United States of America, vol. 104, no. 43, pp. 16822-16827.

APA

Jackson, R. G., Rylott, E. L., Fournier, D., Hawari, J., & Bruce, N. C. (2007). Exploring the biochemical properties and remediation applications of the unusual explosive-degrading P450 system XpIA/B. Proceedings of the National Academy of Sciences of the United States of America, 104(43), 16822-16827.

Vancouver

Jackson RG, Rylott EL, Fournier D, Hawari J, Bruce NC. Exploring the biochemical properties and remediation applications of the unusual explosive-degrading P450 system XpIA/B. Proceedings of the National Academy of Sciences of the United States of America. 2007 Oct 23;104(43):16822-16827.

Author

Jackson, Rosamond G. ; Rylott, Elizabeth L. ; Fournier, Diane ; Hawari, Jalal ; Bruce, Neil C. / Exploring the biochemical properties and remediation applications of the unusual explosive-degrading P450 system XpIA/B. In: Proceedings of the National Academy of Sciences of the United States of America. 2007 ; Vol. 104, No. 43. pp. 16822-16827.

Bibtex - Download

@article{665ae0687752465bafd555363e7bc87e,
title = "Exploring the biochemical properties and remediation applications of the unusual explosive-degrading P450 system XpIA/B",
abstract = "Widespread contamination of land and groundwater has resulted from the use, manufacture, and storage of the military explosive hexa-hydro-1,3,5-trinitro-1,3,5-triazine (RDX). This contamination has led to a requirement for a sustainable, low-cost method to remediate this problem. Here, we present the characterization of an unusual microbial P450 system able to degrade RDX, consisting of flavodoxin reductase XpIB and fused flavodoxin-cytochrome P450 XpIA. The affinity of XpIA for the xenobiotic compound RDX is high (K-d = 58 mu M) and comparable with the K. of other P450s toward their natural substrates (ranging from 1 to 500 mu M). The maximum turnover (k(cat)) is 4.44 per s, only 10-fold less than the fastest self-sufficient P450 reported, BM3. Interestingly, the presence of oxygen determines the final products of RDX degradation, demonstrating that the degradation chemistry is flexible, but both pathways result in ring cleavage and release of nitrite. Carbon monoxide inhibition is weak and yet the nitroaromatic explosive 2,4,6-trinitrotoluene (TNT) is a potent inhibitor. To test the efficacy of this system for the remediation of groundwater, transgenic Arabidopsis plants expressing both xpIA and xpIB were generated. They are able to remove saturating levels of RDX from liquid culture and soil leachate at rates significantly faster than those of untransformed plants and xpIA-only transgenic lines, demonstrating the applicability of this system for the phytoremediation of RDX-contaminated sites.",
keywords = "cytochrome p450, phytoremediation, hexa-hydro-1,3,5-trinitro1,35-triazine, SP STRAIN DN22, CYTOCHROME-P450, HEXAHYDRO-1,3,5-TRINITRO-1,3,5-TRIAZINE, BIODEGRADATION, REDUCTASE, RDX, ADRENODOXIN, ISOFORMS, OXYGEN",
author = "Jackson, {Rosamond G.} and Rylott, {Elizabeth L.} and Diane Fournier and Jalal Hawari and Bruce, {Neil C.}",
year = "2007",
month = "10",
day = "23",
language = "English",
volume = "104",
pages = "16822--16827",
journal = "Proceedings of the National Academy of Sciences of the United States of America",
issn = "0027-8424",
number = "43",

}

RIS (suitable for import to EndNote) - Download

TY - JOUR

T1 - Exploring the biochemical properties and remediation applications of the unusual explosive-degrading P450 system XpIA/B

AU - Jackson, Rosamond G.

AU - Rylott, Elizabeth L.

AU - Fournier, Diane

AU - Hawari, Jalal

AU - Bruce, Neil C.

PY - 2007/10/23

Y1 - 2007/10/23

N2 - Widespread contamination of land and groundwater has resulted from the use, manufacture, and storage of the military explosive hexa-hydro-1,3,5-trinitro-1,3,5-triazine (RDX). This contamination has led to a requirement for a sustainable, low-cost method to remediate this problem. Here, we present the characterization of an unusual microbial P450 system able to degrade RDX, consisting of flavodoxin reductase XpIB and fused flavodoxin-cytochrome P450 XpIA. The affinity of XpIA for the xenobiotic compound RDX is high (K-d = 58 mu M) and comparable with the K. of other P450s toward their natural substrates (ranging from 1 to 500 mu M). The maximum turnover (k(cat)) is 4.44 per s, only 10-fold less than the fastest self-sufficient P450 reported, BM3. Interestingly, the presence of oxygen determines the final products of RDX degradation, demonstrating that the degradation chemistry is flexible, but both pathways result in ring cleavage and release of nitrite. Carbon monoxide inhibition is weak and yet the nitroaromatic explosive 2,4,6-trinitrotoluene (TNT) is a potent inhibitor. To test the efficacy of this system for the remediation of groundwater, transgenic Arabidopsis plants expressing both xpIA and xpIB were generated. They are able to remove saturating levels of RDX from liquid culture and soil leachate at rates significantly faster than those of untransformed plants and xpIA-only transgenic lines, demonstrating the applicability of this system for the phytoremediation of RDX-contaminated sites.

AB - Widespread contamination of land and groundwater has resulted from the use, manufacture, and storage of the military explosive hexa-hydro-1,3,5-trinitro-1,3,5-triazine (RDX). This contamination has led to a requirement for a sustainable, low-cost method to remediate this problem. Here, we present the characterization of an unusual microbial P450 system able to degrade RDX, consisting of flavodoxin reductase XpIB and fused flavodoxin-cytochrome P450 XpIA. The affinity of XpIA for the xenobiotic compound RDX is high (K-d = 58 mu M) and comparable with the K. of other P450s toward their natural substrates (ranging from 1 to 500 mu M). The maximum turnover (k(cat)) is 4.44 per s, only 10-fold less than the fastest self-sufficient P450 reported, BM3. Interestingly, the presence of oxygen determines the final products of RDX degradation, demonstrating that the degradation chemistry is flexible, but both pathways result in ring cleavage and release of nitrite. Carbon monoxide inhibition is weak and yet the nitroaromatic explosive 2,4,6-trinitrotoluene (TNT) is a potent inhibitor. To test the efficacy of this system for the remediation of groundwater, transgenic Arabidopsis plants expressing both xpIA and xpIB were generated. They are able to remove saturating levels of RDX from liquid culture and soil leachate at rates significantly faster than those of untransformed plants and xpIA-only transgenic lines, demonstrating the applicability of this system for the phytoremediation of RDX-contaminated sites.

KW - cytochrome p450

KW - phytoremediation

KW - hexa-hydro-1,3,5-trinitro1,35-triazine

KW - SP STRAIN DN22

KW - CYTOCHROME-P450

KW - HEXAHYDRO-1,3,5-TRINITRO-1,3,5-TRIAZINE

KW - BIODEGRADATION

KW - REDUCTASE

KW - RDX

KW - ADRENODOXIN

KW - ISOFORMS

KW - OXYGEN

M3 - Article

VL - 104

SP - 16822

EP - 16827

JO - Proceedings of the National Academy of Sciences of the United States of America

JF - Proceedings of the National Academy of Sciences of the United States of America

SN - 0027-8424

IS - 43

ER -