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Title: Iron- and aluminium-induced depletion of molybdenum in acidic environments impedes the nitrogen cycle: Mo depletion by Fe/Al precipitation at ORR

Abstract

Anthropogenic nitrate contamination is a serious problem in many natural environments. Nitrate removal by microbial action is dependent on the metal molybdenum (Mo), which is required by nitrate reductase for denitrification and dissimilatory nitrate reduction to ammonium. The soluble form of Mo, molybdate (MoO4 2- ), is incorporated into and adsorbed by iron (Fe) and aluminium (Al) (oxy) hydroxide minerals. Herein we used Oak Ridge Reservation (ORR) as a model nitrate-contaminated acidic environment to investigate whether the formation of Fe- and Al-precipitates could impede microbial nitrate removal by depleting Mo. We demonstrate that Fe and Al mineral formation that occurs as the pH of acidic synthetic groundwater is increased, decreases soluble Mo to low picomolar concentrations, a process proposed to mimic environmental diffusion of acidic contaminated groundwater. Analysis of ORR sediments revealed recalcitrant Mo in the contaminated core that co-occurred with Fe and Al, consistent with Mo scavenging by Fe/Al precipitates. Nitrate removal by ORR isolate Pseudomonas fluorescens N2A2 is virtually abolished by Fe/Al precipitate-induced Mo depletion. The depletion of naturally occurring Mo in nitrate- and Fe/Al-contaminated acidic environments like ORR or acid mine drainage sites has the potential to impede microbial-based nitrate reduction thereby extending the duration of nitratemore » in the environment.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [2];  [2];  [1]; ORCiD logo [3];  [4];  [5];  [5];  [6];  [6];  [2]; ORCiD logo [4]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of Georgia, Athens, GA (United States)
  2. Univ. of Missouri, Columbia, MO (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Univ. of Tennessee, Knoxville, TN (United States)
  5. Univ. of Washington, Seattle, WA (United States)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1528691
Alternate Identifier(s):
OSTI ID: 1483016; OSTI ID: 1580350
Grant/Contract Number:  
AC05-00OR22725; AC02‐05CH11231; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Environmental Microbiology
Additional Journal Information:
Journal Volume: 21; Journal Issue: 1; Journal ID: ISSN 1462-2912
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 59 BASIC BIOLOGICAL SCIENCES

Citation Formats

Ge, Xiaoxuan, Vaccaro, Brian J., Thorgersen, Michael P., Poole, Farris L., Majumder, Erica L., Zane, Grant M., De León, Kara B., Lancaster, W. Andrew, Moon, Ji Won, Paradis, Charles J., von Netzer, Frederick, Stahl, David A., Adams, Paul D., Arkin, Adam P., Wall, Judy D., Hazen, Terry C., and Adams, Michael W. W. Iron- and aluminium-induced depletion of molybdenum in acidic environments impedes the nitrogen cycle: Mo depletion by Fe/Al precipitation at ORR. United States: N. p., 2018. Web. doi:10.1111/1462-2920.14435.
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Ge, Xiaoxuan, Vaccaro, Brian J., Thorgersen, Michael P., Poole, Farris L., Majumder, Erica L., Zane, Grant M., De León, Kara B., Lancaster, W. Andrew, Moon, Ji Won, Paradis, Charles J., von Netzer, Frederick, Stahl, David A., Adams, Paul D., Arkin, Adam P., Wall, Judy D., Hazen, Terry C., & Adams, Michael W. W. Iron- and aluminium-induced depletion of molybdenum in acidic environments impedes the nitrogen cycle: Mo depletion by Fe/Al precipitation at ORR. United States. doi:10.1111/1462-2920.14435.
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Ge, Xiaoxuan, Vaccaro, Brian J., Thorgersen, Michael P., Poole, Farris L., Majumder, Erica L., Zane, Grant M., De León, Kara B., Lancaster, W. Andrew, Moon, Ji Won, Paradis, Charles J., von Netzer, Frederick, Stahl, David A., Adams, Paul D., Arkin, Adam P., Wall, Judy D., Hazen, Terry C., and Adams, Michael W. W. Fri . "Iron- and aluminium-induced depletion of molybdenum in acidic environments impedes the nitrogen cycle: Mo depletion by Fe/Al precipitation at ORR". United States. doi:10.1111/1462-2920.14435. https://www.osti.gov/servlets/purl/1528691.
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@article{osti_1528691,
title = {Iron- and aluminium-induced depletion of molybdenum in acidic environments impedes the nitrogen cycle: Mo depletion by Fe/Al precipitation at ORR},
author = {Ge, Xiaoxuan and Vaccaro, Brian J. and Thorgersen, Michael P. and Poole, Farris L. and Majumder, Erica L. and Zane, Grant M. and De León, Kara B. and Lancaster, W. Andrew and Moon, Ji Won and Paradis, Charles J. and von Netzer, Frederick and Stahl, David A. and Adams, Paul D. and Arkin, Adam P. and Wall, Judy D. and Hazen, Terry C. and Adams, Michael W. W.},
abstractNote = {Anthropogenic nitrate contamination is a serious problem in many natural environments. Nitrate removal by microbial action is dependent on the metal molybdenum (Mo), which is required by nitrate reductase for denitrification and dissimilatory nitrate reduction to ammonium. The soluble form of Mo, molybdate (MoO4 2- ), is incorporated into and adsorbed by iron (Fe) and aluminium (Al) (oxy) hydroxide minerals. Herein we used Oak Ridge Reservation (ORR) as a model nitrate-contaminated acidic environment to investigate whether the formation of Fe- and Al-precipitates could impede microbial nitrate removal by depleting Mo. We demonstrate that Fe and Al mineral formation that occurs as the pH of acidic synthetic groundwater is increased, decreases soluble Mo to low picomolar concentrations, a process proposed to mimic environmental diffusion of acidic contaminated groundwater. Analysis of ORR sediments revealed recalcitrant Mo in the contaminated core that co-occurred with Fe and Al, consistent with Mo scavenging by Fe/Al precipitates. Nitrate removal by ORR isolate Pseudomonas fluorescens N2A2 is virtually abolished by Fe/Al precipitate-induced Mo depletion. The depletion of naturally occurring Mo in nitrate- and Fe/Al-contaminated acidic environments like ORR or acid mine drainage sites has the potential to impede microbial-based nitrate reduction thereby extending the duration of nitrate in the environment.},
doi = {10.1111/1462-2920.14435},
journal = {Environmental Microbiology},
number = 1,
volume = 21,
place = {United States},
year = {2018},
month = {10}
}
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Journal Article:
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DOI:  10.1111/1462-2920.14435
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Cited by: 3 works
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Figures / Tables:

Fig. 1 Fig. 1: Mo in the nitrogen cycle and at ORR. (a) Mo-dependent steps in the nitrogen cycle are indicated by bold black arrows while dashed arrows are independent of Mo. (b) Model of Mo depletion at the ORR contaminated site. The large background arrow indicates pH change of contaminated groundwatermore » from lower pH (red) to higher pH (pink to white). Two methods of Mo depletion by Fe or Al precipitates are proposed: incorporation and adsorption as indicated by blue arrows.« less
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