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Title: Organohalide Respiration with Chlorinated Ethenes under Low pH Conditions

Abstract

Bioremediation at chlorinated solvent sites often leads to groundwater acidification due to electron donor fermentation and enhanced dechlorination activity. The microbial reductive dechlorination process is robust at circumneutral pH, but activity declines at groundwater pH values below 6.0. Consistent with this observation, the activity of tetrachloroethene (PCE) dechlorinating cultures declined at pH 6.0 and was not sustained in pH 5.5 medium, with one notable exception. Sulf urospirillum multivorans dechlorinated PCE to cis-1,2-dichloroethene (cDCE) in pH 5.5 medium and maintained this activity upon repeated transfers. Microcosms established with soil and aquifer materials from five distinct locations dechlorinated PCE-to-ethene at pH 5.5 and pH 7.2. Dechlorination to ethene was maintained following repeated transfers at pH 7.2, but no ethene was produced at pH 5.5, and only the transfer cultures derived from the Axton Cross Superfund (ACS) microcosms sustained PCE dechlorination to cDCE as a final product. 16S rRNA gene amplicon sequencing of pH 7.2 and pH 5.5 ACS enrichments revealed distinct microbial communities, with the dominant dechlorinator being Dehalococcoides in pH 7.2 and Sulf urospirillum in pH 5.5 cultures. PCE-to-trichloroethene- (TCE-) and PCE-to-cDCEdechlorinating isolates obtained from the ACS pH 5.5 enrichment shared 98.6%, and 98.5% 16S rRNA gene sequence similarities to Sulfmore » urospirillum multivorans. Lastly, these findings imply that sustained Dehalococcoides activity cannot be expected in low pH (i.e., ≤ 5.5) groundwater, and organohalide-respiring Sulf urospirillum spp. are key contributors to in situ PCE reductive dechlorination under low pH conditions.« less

Authors:
 [1];  [2]; ORCiD logo [2];  [3];  [2]; ORCiD logo [4]
  1. Univ. of Tennessee, Knoxville, TN (United States). Center for Environmental Biotechnology, Dept. of Civil and Environmental Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Joint Inst. for Biological Sciences (JIBS)
  2. Tufts Univ., Medford, MA (United States). Dept. of Civil and Environmental Engineering
  3. Univ. of Tennessee, Knoxville, TN (United States). Center for Environmental Biotechnology, Dept. of Microbiology; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Joint Inst. for Biological Sciences (JIBS)
  4. Univ. of Tennessee, Knoxville, TN (United States). Center for Environmental Biotechnology, Dept. of Civil and Environmental Engineering, Dept. of Microbiology, Dept. of Biosystems Engineering and Soil Science; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Biosciences Division, and joint Inst. for Biological Sciences (JIBS)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE; USDoD
OSTI Identifier:
1399396
Grant/Contract Number:
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Environmental Science and Technology
Additional Journal Information:
Journal Volume: 51; Journal Issue: 15; Journal ID: ISSN 0013-936X
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Yang, Yi, Cápiro, Natalie L., Marcet, Tyler F., Yan, Jun, Pennell, Kurt D., and Löffler, Frank E. Organohalide Respiration with Chlorinated Ethenes under Low pH Conditions. United States: N. p., 2017. Web. doi:10.1021/acs.est.7b01510.
Yang, Yi, Cápiro, Natalie L., Marcet, Tyler F., Yan, Jun, Pennell, Kurt D., & Löffler, Frank E. Organohalide Respiration with Chlorinated Ethenes under Low pH Conditions. United States. doi:10.1021/acs.est.7b01510.
Yang, Yi, Cápiro, Natalie L., Marcet, Tyler F., Yan, Jun, Pennell, Kurt D., and Löffler, Frank E. Fri . "Organohalide Respiration with Chlorinated Ethenes under Low pH Conditions". United States. doi:10.1021/acs.est.7b01510.
@article{osti_1399396,
title = {Organohalide Respiration with Chlorinated Ethenes under Low pH Conditions},
author = {Yang, Yi and Cápiro, Natalie L. and Marcet, Tyler F. and Yan, Jun and Pennell, Kurt D. and Löffler, Frank E.},
abstractNote = {Bioremediation at chlorinated solvent sites often leads to groundwater acidification due to electron donor fermentation and enhanced dechlorination activity. The microbial reductive dechlorination process is robust at circumneutral pH, but activity declines at groundwater pH values below 6.0. Consistent with this observation, the activity of tetrachloroethene (PCE) dechlorinating cultures declined at pH 6.0 and was not sustained in pH 5.5 medium, with one notable exception. Sulf urospirillum multivorans dechlorinated PCE to cis-1,2-dichloroethene (cDCE) in pH 5.5 medium and maintained this activity upon repeated transfers. Microcosms established with soil and aquifer materials from five distinct locations dechlorinated PCE-to-ethene at pH 5.5 and pH 7.2. Dechlorination to ethene was maintained following repeated transfers at pH 7.2, but no ethene was produced at pH 5.5, and only the transfer cultures derived from the Axton Cross Superfund (ACS) microcosms sustained PCE dechlorination to cDCE as a final product. 16S rRNA gene amplicon sequencing of pH 7.2 and pH 5.5 ACS enrichments revealed distinct microbial communities, with the dominant dechlorinator being Dehalococcoides in pH 7.2 and Sulf urospirillum in pH 5.5 cultures. PCE-to-trichloroethene- (TCE-) and PCE-to-cDCEdechlorinating isolates obtained from the ACS pH 5.5 enrichment shared 98.6%, and 98.5% 16S rRNA gene sequence similarities to Sulf urospirillum multivorans. Lastly, these findings imply that sustained Dehalococcoides activity cannot be expected in low pH (i.e., ≤ 5.5) groundwater, and organohalide-respiring Sulf urospirillum spp. are key contributors to in situ PCE reductive dechlorination under low pH conditions.},
doi = {10.1021/acs.est.7b01510},
journal = {Environmental Science and Technology},
number = 15,
volume = 51,
place = {United States},
year = {Fri Jun 30 00:00:00 EDT 2017},
month = {Fri Jun 30 00:00:00 EDT 2017}
}

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  • Here we report that the genomes of two closely related Dehalobacter strains (strain CF and strain DCA) were assembled from the metagenome of an anaerobic enrichment culture that reductively dechlorinates chloroform (CF), 1,1,1-trichloroethane (1,1,1-TCA) and 1,1-dichloroethane (1,1-DCA). The 3.1 Mbp genomes of strain CF (that dechlorinates CF and 1,1,1-TCA) and strain DCA (that dechlorinates 1,1-DCA) each contain 17 putative reductive dehalogenase homologous (rdh) genes. These two genomes were systematically compared to three other available organohalide-respiring Dehalobacter genomes (Dehalobacter restrictus strain PER-K23, Dehalobacter sp. strain E1 and Dehalobacter sp. strain UNSWDHB), and to the genomes of Dehalococcoides mccartyi strain 195 andmore » Desulfitobacterium hafniense strain Y51. This analysis compared 42 different metabolic and physiological categories. The genomes of strains CF and DCA share 90% overall average nucleotide identity and >99.8% identity over a 2.9 Mbp alignment that excludes large insertions, indicating that these genomes differentiated from a close common ancestor. This differentiation was likely driven by selection pressures around two orthologous reductive dehalogenase genes, cfrA and dcrA, that code for the enzymes that reduce CF or 1,1,1-TCA and 1,1-DCA. The many reductive dehalogenase genes found in the five Dehalobacter genomes cluster into two small conserved regions and were often associated with Crp/Fnr transcriptional regulators. Specialization is on-going on a strain-specific basis, as some strains but not others have lost essential genes in the Wood-Ljungdahl (strain E1) and corrinoid biosynthesis pathways (strains E1 and PER-K23). The gene encoding phosphoserine phosphatase, which catalyzes the last step of serine biosynthesis, is missing from all five Dehalobacter genomes, yet D. restrictus can grow without serine, suggesting an alternative or unrecognized biosynthesis route exists. In contrast to D. mccartyi, a complete heme biosynthesis pathway is present in the five Dehalobacter genomes. This pathway corresponds to a newly described alternative heme biosynthesis route first identified in Archaea. Ultimately, this analysis of organohalide-respiring Firmicutes and Chloroflexi reveals profound evolutionary differences despite very similar niche-specific metabolism and function.« less
  • Dehalococcoides ethenogenes'' 195 can reductively dechlorinate tetrachloroethene (PCE) completely to ethene (ETH). When PCE-grown strain 195 was transferred (2% [vol/vol] inoculum) into growth medium amended with trichloroethene (TCE), cis-dichloroethene (DCE), 1,1-DCE, or 1,2-dichloroethane (DCA) as an electron acceptor, these chlorinated compounds were consumed at increasing rates over time, which indicated that growth occurred. Moreover, the number of cells increased when TCE, 1,1-DCE, or DCA was present. PCE, TCE, 1,1-DCE, and cis-DCE were converted mainly to vinyl chloride (VC) and then to ETH, while DCA was converted to ca. 99% ETH and 1% VC. cis-DCE was used at lower rates thanmore » PCE, TCE, 1,1-DCE, or DCA was used. When PCE-grown cultures were transferred to media containing VC or trans-DCE, products accumulated slowly, and there was no increase in the rate, which indicated that these two compounds did not support growth. When the intermediates in PCE dechlorination by strain 195 were monitored, TCE was detected first, followed by cis-DCE. After a lag, VC, 1,1-DCE, and trans-DCE accumulated, which is consistent with the hypothesis that cis-DCE is the precursor of these compounds. Both cis-DCE and 1,1-DCE were eventually consumed, and both of these compounds could be considered intermediates in PCE dechlorination, whereas the small amount of trans-DCE that was produced persisted. Cultures grown on TCE, 1,1-DCE, or DCA could immediately dechlorinate PCE, which indicated that PCE reductive dehalogenase activity was constitutive when these electron acceptors were used.« less
  • The purpose of this investigation was to determine whether tree-core analysis could be used to delineate shallow groundwater contamination by chlorinated ethenes. Analysis of tree cores from bald cypress [Taxodium distichum (L.) Rich], tupelo (Nyssa aquatica L.), sweet gum (Liquidambar stryaciflua L.), oak (Quercus spp.), sycamore (Platanus occidentalis L.), and loblolly pine (Pinus taeda L.) growing over shallow groundwater contaminated with cis-1,2-dichloroethene (cDCE) and trichloroethene (TCE) showed that those compounds also were present in the trees. The cores were collected and analyzed by headspace gas chromatography. Bald cypress, tupelo, and loblolly pine contained the highest concentrations of TCE, with lessermore » amounts in nearby oak and sweet gum. The concentrations of cDCE and TCE in various trees appeared to reflect the configuration of the chlorinated-solvent groundwater contamination plume. Bald cypress cores collected along 18.6-m vertical transects of the same trunks showed that TCE concentrations decline by 30--70% with trunk height. The ability of the tested trees to take up cDCE and TCE make tree coring a potentially cost-effective and simple approach to optimizing well placement at this site.« less
  • A study was conducted to enhance the performance of an advanced oxidation process in treating chlorinated ethenes in groundwater at IBM`s groundwater treatment system at its Essex Junction, Vermont facility. A model describing the reaction kinetics and mass transfer of a co-current ozone injection process is presented. This model, in conjunction with experiments, demonstrates that the treatment performance of the ozone treatment process at a given ozone/air concentration and ozone mass flowrate cannot be improved by varying process operating parameters such as number of ozone injectors utilized, use of a static mixer, or variation of groundwater flowrate through each injector.more » This is because dissolved ozone reaches equilibrium with the injected ozone/air mixture within two seconds of initial contact. Also, the Venturi-type ozone injection system presently in use destroys nearly half of the injected ozone. Injection of hydrogen peroxide in conjunction with ozone increases the overall tetrachloroethylene (PCE) treatment efficiency by a factor of four (in comparison to ozone alone) at a H{sub 2}O{sub 2}/O{sub 3} mass ratio of between 1 and 2. Treatment of trichloroethylene (TCE) is enhanced by a factor of two. This enhancement of the oxidative treatment process results in a reduction in solvent mass load to a granular activated carbon (GAC) adsorption system located downstream, thus potentially reducing the usage GAC and regeneration of spent GAC. However, residual hydrogen peroxide and/or hydroxyl free radicals from the oxidation process effluent may interact adversely with certain grades of GAC; the causes of this interaction and methods to attenuate it (i.e., the use of more resistant grades of GAC) are discussed. Overall O{sub 3}/H{sub 2}O{sub 2}/GAC system operating costs can potentially be reduced significantly (up to $20K annually). An economic analysis and system operation/cost optimization study are presented. 8 refs., 7 figs., 1 tab.« less