Identification and analysis of a bottleneck in PCB biodegradation

被引:75
作者
Dai, SD
Vaillancourt, FH
Maaroufi, H
Drouin, HM
Neau, DB
Snieckus, V
Bolin, JT [1 ]
Eltis, LD
机构
[1] Purdue Univ, Dept Biol Sci, Markey Ctr Struct Biol, W Lafayette, IN 47907 USA
[2] Univ British Columbia, Dept Microbiol, Vancouver, BC V6T 1Z3, Canada
[3] Univ British Columbia, Dept Biochem, Vancouver, BC V6T 1Z3, Canada
[4] Univ Laval, Dept Biochem, Quebec City, PQ G1K 7P4, Canada
[5] Queens Univ, Dept Chem, Kingston, ON K7L 3N6, Canada
基金
美国国家卫生研究院; 加拿大自然科学与工程研究理事会;
关键词
D O I
10.1038/nsb866
中图分类号
Q5 [生物化学]; Q7 [分子生物学];
学科分类号
071010 ; 081704 ;
摘要
The microbial degradation of polychlorinated biphenyls (PCBs) provides the potential to destroy these widespread, toxic and persistent environmental pollutants. For example, the four-step upper bphpathway transforms some of the more than 100 different PCBs found in commercial mixtures and is being engineered for more effective PCB degradation. In the critical third step of this pathway, 2,3-dihydroxybiphenyl (DHB) 1,2-dioxygenase (DHBD; EC 1.13.11.39) catalyzes aromatic ring cleavage. Here we demonstrate that ortho-chlorinated PCB metabolites strongly inhibit DHBD, promote its suicide inactivation and interfere with the degradation of other compounds. For example, k(cat)(app) for 2',6'-diCl DHB was reduced by a factor of similar to7,000 relative to DHB, and it bound with sufficient affinity to competitively inhibit DHB cleavage at nanomolar concentrations. Crystal structures of two complexes of DHBD with ortho-chlorinated metabolites at 1.7 Angstrom resolution reveal an explanation for these phenomena, which have important implications for bioremediation strategies.
引用
收藏
页码:934 / 939
页数:6
相关论文
共 35 条
[1]   AEROBIC AND ANAEROBIC BIODEGRADATION OF PCBS - A REVIEW [J].
ABRAMOWICZ, DA .
CRITICAL REVIEWS IN BIOTECHNOLOGY, 1990, 10 (03) :241-249
[2]  
Arcaro KF, 1999, J CELL BIOCHEM, V72, P94, DOI 10.1002/(SICI)1097-4644(19990101)72:1<94::AID-JCB10>3.3.CO
[3]  
2-P
[4]   Family shuffling of a targeted bphA region to engineer biphenyl dioxygenase [J].
Barriault, D ;
Plante, MM ;
Sylvestre, M .
JOURNAL OF BACTERIOLOGY, 2002, 184 (14) :3794-3800
[5]  
BOLIN JT, 2001, HDB METALLOPROTEINS, P632
[6]   DEGRADATION OF HIGHLY CHLORINATED PCBS BY PSEUDOMONAS STRAIN LB400 [J].
BOPP, LH .
JOURNAL OF INDUSTRIAL MICROBIOLOGY, 1986, 1 (01) :23-29
[7]   Crystallography & NMR system:: A new software suite for macromolecular structure determination [J].
Brunger, AT ;
Adams, PD ;
Clore, GM ;
DeLano, WL ;
Gros, P ;
Grosse-Kunstleve, RW ;
Jiang, JS ;
Kuszewski, J ;
Nilges, M ;
Pannu, NS ;
Read, RJ ;
Rice, LM ;
Simonson, T ;
Warren, GL .
ACTA CRYSTALLOGRAPHICA SECTION D-BIOLOGICAL CRYSTALLOGRAPHY, 1998, 54 :905-921
[8]   Solving the riddle of the intradiol and extradiol catechol dioxygenases: how do enzymes control hydroperoxide rearrangements? [J].
Bugg, TDH ;
Lin, G .
CHEMICAL COMMUNICATIONS, 2001, (11) :941-952
[9]   Assessing the role of ortho-substitution on polychlorinated biphenyl binding to transthyretin, a thyroxine transport protein [J].
Chauhan, KR ;
Kodavanti, PRS ;
McKinney, JD .
TOXICOLOGY AND APPLIED PHARMACOLOGY, 2000, 162 (01) :10-21
[10]  
Cornish-Bowden A., 1995, ANAL ENZYME KINETIC