Tracing molybdenum attenuation in mining environments using

Apr 18, 2019 - Elliott K Skierszkan , Jared Robertson , Matthew B.J. Lindsay , Justin S. Stockwell , John W. Dockrey , Soumya Das , Dominique Weis , R...
0 downloads 0 Views 1MB Size
Subscriber access provided by UniSA Library

Characterization of Natural and Affected Environments

Tracing molybdenum attenuation in mining environments using molybdenum stable isotopes Elliott K Skierszkan, Jared Robertson, Matthew B.J. Lindsay, Justin S. Stockwell, John W. Dockrey, Soumya Das, Dominique Weis, Roger Daniel Beckie, and K. Ulrich Mayer Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.9b00766 • Publication Date (Web): 18 Apr 2019 Downloaded from http://pubs.acs.org on April 20, 2019

Just Accepted “Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. The American Chemical Society provides “Just Accepted” as a service to the research community to expedite the dissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscripts appear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have been fully peer reviewed, but should not be considered the official version of record. They are citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offered to authors. Therefore, the “Just Accepted” Web site may not include all articles that will be published in the journal. After a manuscript is technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Note that technical editing may introduce minor changes to the manuscript text and/or graphics which could affect content, and all legal disclaimers and ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts.

is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties.

Page 1 of 32

Environmental Science & Technology

1

Tracing molybdenum attenuation in mining environments using

2

molybdenum stable isotopes

3 4

Elliott K. Skierszkan,1,2,* Jared M. Robertson,3,4 Matthew B. J. Lindsay,3 Justin S. Stockwell,2

5

John W. Dockrey,2 Soumya Das,3 Dominique Weis,1,5 Roger D. Beckie,1 and

6

K. Ulrich Mayer1

7

1Department

8

Main Mall, Vancouver, BC, Canada, V6T 1Z4

9

2Lorax

of Earth, Ocean and Atmospheric Sciences, University of British Columbia, 2020-2207

Environmental Services Ltd., 2289 Burrard Street, Vancouver, BC, Canada, V6J 3H9

10

3Department

11

Canada, S7N 5E2

12

4O’Kane

13

5Pacific

14

Sciences, University of British Columbia, 2020-2207 Main Mall, Vancouver, BC, Canada, V6T 1Z4

of Geological Sciences, University of Saskatchewan, 114 Science Place, Saskatoon, SK,

Consultants Inc., 112 Research Drive, Saskatoon, SK, Canada, S7N 3R3

Centre for Isotopic and Geochemical Research, Department of Earth, Ocean and Atmospheric

15 16

Corresponding Author

17

*E-mail: [email protected]

18

1 ACS Paragon Plus Environment

Environmental Science & Technology

20

Abstract

21

Molybdenum contamination is a concern in mining regions worldwide. Better

22

understanding of processes controlling Mo mobility in mine wastes is critical for assessing

23

potential impacts and developing water-quality management strategies associated to this element.

24

Here, we used Mo stable isotope (δ98/95Mo) analyses to investigate geochemical controls on Mo

25

mobility within a tailings management facility (TMF) featuring oxic and anoxic environments.

26

These isotopic analyses were integrated with X-ray absorption spectroscopy, X-ray diffraction,

27

Raman spectroscopy, transmission electron microscopy, and aqueous chemical data. Dissolved

28

Mo concentrations were inversely correlated with δ98/95Mo values such that enrichment of heavy

29

Mo isotopes in solution reflected attenuation processes. Inner-sphere complexation of Mo(VI)

30

with ferrihydrite was the primary driver of Mo removal and was accompanied by a circa 1 ‰

31

isotope fractionation. Limited Mo attenuation and isotope fractionation was observed in Fe(II)-

32

and Mo-rich anoxic TMF seepage, while attenuation and isotope fractionation were greatest

33

during discharge and oxidation of this seepage after discharge into a pond where Fe-

34

(oxyhydr)oxide precipitation promoted Mo sorption. Overall, this study highlights the role of

35

sorption onto Fe-(oxyhydr)oxides in attenuating Mo in oxic environments, a process which can

36

be traced by Mo isotope analyses.

37 38 39 40 41 2 ACS Paragon Plus Environment

Page 2 of 32

Page 3 of 32

42

Environmental Science & Technology

Graphical Abstract

43

44

1

Introduction

45

Oxidative weathering of sulfide mine wastes can release potentially hazardous elements

46

including molybdenum (Mo) to the environment.1–4 Natural fresh waters typically contain