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https://doi.org/10.1007/s11270-019-4176-z
Abstract Whereas mining and non-mining sourced enrichment factors (ratios of PM concentrations to
particulate metal/metalloids (PM) (> 0.45 μm) are ubiquitous metals such as aluminum), lead isotopes,
present in the tributaries of the San Juan River, color, and particle size, were used to tie layers in a
USA, the individual contributions of PM from the San Juan River sediment core to upstream tributary
San Juan River tributaries to the sediment of the San sources. Tributary PM concentrations and loads were
Juan River Delta of Lake Powell were previously compared to Lower San Juan River suspended PM
unknown. Suspended PM signatures, including loads to estimate the relative contribution of tributary
PM (both mining and non-mining sourced) directly
Highlights upstream of Lake Powell. Results suggest elevated
•Contributions of suspended particulate metals and metalloids to enrichment factors of lead, cadmium, copper, and
the San Juan River from mined and unmined tributaries were zinc in deposited sediment were sourced from mined
determined using tributary geochemical signatures that reflected tributaries, whereas elevated manganese in deposited
legacy mining impacts or the predominant underlying geology.
•Suspended particulates in tributaries were linked to layers in San sediment was sourced from unmined tributaries. Sed-
Juan River Delta sediment cores through geochemical signatures, iment Pb isotope ratios reflected the depleted signa-
such as depleted Pb isotopes and elevated Pb to Al, Cd to Al, and ture of the mineralized vein (present in the headwa-
Zn to Al ratios reflective of mining impact, as well as enriched Pb ters of mined tributaries), the enriched signature of
isotopes, elevated Mn to Al, and red color reflective of unmined
sources the Chinle Sandstone (predominant underlying geol-
•Approximately 10% of PM deposited in a sediment core was ogy of unmined tributaries), or a mixture of these two
attributed to mining sources, whereas approximately 80% of PM endmembers. These independent lines of evidence
deposited in a sediment core was attributed to a mixture of sources. were used to link probable tributary source and run-
•Seasonal accumulation in sediment traps indicated that the 3.37-
m core was deposited over approximately 1.3 years off category to sediment layers, where ~ 10% and 5%
of the overall PM deposited in the sediment core was
Electronic supplementary material The online version of this attributed to mining versus non-mining sources, re-
article (https://doi.org/10.1007/s11270-019-4176-z) contains
supplementary material, which is available to authorized users. spectively. Because traditional dating methods were
not possible, runoff category signatures were used to
L. Frederick : W. P. Johnson (*) : T. Cerling : estimate that the 3.37 m San Juan River Delta core
D. Fernandez was deposited over ~ 1.3 years.
Department of Geology and Geophysics, University of Utah, Salt
Lake City, UT 84112, USA
e-mail: william.johnson@utah.edu
Keywords Particulate metals/metalloid concentration .
J. VanDerslice Sediment cores . Sediment traps . Lead isotopes .
Department of Family and Preventative Medicine, School of
Principal component analysis . Lake Powell
Medicine, University of Utah, Salt Lake City, UT 84112, USA
128 Page 2 of 18 Water Air Soil Pollut (2019) 230:128
Animas
UT CO McElmo
La Plata Navajo
Mancos Dam
AZ NM
Core 3
Core 2
Core 1 Lake
Up
Down Mid Powell
0 5 10 km
et al. 1997). In the San Juan River, the ratio of total Pb to change with runoff category (i.e., snowmelt, rainfall, or
total Al was used to track the passage of a mining waste baseflow), yielding distinct layers in sediment traps and
plume (2015 Gold King Mine Spill) beyond the distance sediment cores at the downstream end of the system.
at which it was not visually apparent (Sullivan et al. Because mining tends to occur in high elevations,
2017). snowmelt-activated PM loads and PM concentrations
from mined tributaries are posited to have elemental
1.2 Source Identification in Lacustrine Sediment signatures, e.g., elevated Pb, Cd, As, Zn, and Pb isotope
ratio (corresponding to mineralized vein), that can be
In order to differentiate natural, industrial, and/or used to link downstream sediment layers to mining
mining-sourced PM, sediment source identification in origin.
lacustrine systems has been performed using elemental In order to link deposited sediment to upstream trib-
concentrations in principal component analysis (PCA) utaries, PM signatures of suspended sediment were
(Christensen and Juracek 2001; Palau Estevan et al. established for each tributary watershed and runoff cat-
2012; Wang et al. 2015), lead (Pb) isotopes (Graney egory (e.g., snowmelt, rainfall, and/or baseflow). PM
et al. 1995), and enrichment factors relative to major signatures in the deposited sediment of Lake Powell
lithogenic elements that are non-reactive during trans- were linked to upstream tributary sources using PM
port (conservative) (Riba et al. 2002; Wang et al. 2015). concentrations/ratios and Pb isotopes. This strategy as-
Similar to elemental ratios, enrichment factors normal- sumes that reductive elemental mobilization following
ize concentrations of metals to conservative elements, deposition in Lake Powell does not reposition original
e.g., Fe, Al, and Mn, can be used to determine inputs of strata.
anthropogenic and mining-sourced PM among contam- The percent contribution of tributary PM (both min-
inated and background lakes (Wang et al. 2015; Riba ing and non-mining sourced) to suspended sediment in
et al. 2002). PCA is a statistical tool to reduce multidi- the Lower San Juan River was estimated by comparing
mensional datasets through the generation of principal tributary suspended PM loads to Lower San Juan River
components (PCs), which represent linear combinations suspended PM loads during each runoff category. This
of input variables (e.g., concentrations, elemental, or watershed-scale approach assumes that PM concentra-
isotopic ratios) (Li and Zhang 2010; Wang et al. tions collected in stream samples from a given tributary
2015). PCA performed with elemental concentrations during a given runoff category are representative of that
was used to differentiate sources (e.g., mining, industri- runoff category for that given tributary; PM remains in
al, or natural), where sample categories occupied dis- particulate form during transit through the San Juan
tinct PC space (Wang et al. 2015). Additionally, PCA River; and high flow during large rainfall and snowmelt
probability ellipses (also referred to as convex hulls) events transmits a portion of PM to Lake Powell.
represent the confidence interval within PC space of a Whereas some material will likely be deposited along
given sample category and can be used to predict cate- the reach of the San Juan River, layers of sediment
gorical association of an independent data set (Palau deposited in Lake Powell represent a signal of mobilized
Estevan et al. 2012). Similar to source identification in PM that can be tied to upstream sources.
surface water, stable isotopes of Pb, which do not frac- Justification for these assumptions are explored in the
tionate during transport/deposition, have been utilized in Supporting Information (Appendix A). Briefly, varia-
both alluvial and lacustrine sediment to attribute sources tion in average suspended PM loads and concentrations
(e.g., a mineralized vein) (Graney et al. 1995; Church for each runoff category (one standard deviation) were
et al. 1997). compared to ensure the average tributary suspended PM
signatures were representative for each runoff category.
1.3 Hypotheses and Assumptions Additionally, transport modeling in the San Juan River
suggests that PM transits the majority of the system
Layers in sediment deposited in the San Juan River during high flow (~ 1500 cfs) (Sullivan et al. 2017;
Delta of Lake Powell are posited to reflect distinct USGS 2018). As San Juan River flow during snowmelt
sources from upstream tributaries. Because elevations and rainfall events often surpass 1500 cfs, a signal of
and lithologies range among tributaries, PM loads and mobilized PM should be deposited during these high
PM concentrations from a given tributary are posited to flow events.
Water Air Soil Pollut (2019) 230:128 Page 5 of 18 128
By understanding the percent contribution of mining three sediment cores in August 2010 ranging in depth
versus non-mining sourced PM during different runoff from 1.48 to 4.6 m (Hornewer 2014) (Fig. 1). The three
events in the Lower San Juan River, the percent of sediment cores (USGS 371712110364200, USGS
deposited PM sourced from mining versus non-mining 371425110382699, and USGS 371545110410700)
sources was estimated. As the San Juan River and each of showed variation in elemental concentration with depth;
its contributing tributaries represent complex systems, however, a sediment accumulation history was not de-
this work serves as a first order estimate to compare termined (Hornewer 2014). Additionally, in response to
PM sources from mined versus non-mined tributaries. the 2015 Gold King Mine spill, the USGS deployed
sediment traps at three locations (upstream, mid-stream,
and downstream, Fig. 1) in the San Juan River Delta
2 Background during baseflow with intermittent rainfall and snowmelt
(Supporting Information Fig. SI3) (UDWQ et al. 2018).
2.1 Tributaries of the San Juan River Lower San Juan River baseflow conditions punctuated
by four rainfall events in the watershed were captured in
The seven main tributaries of the San Juan River (Upper 48 cm at the upstream location from 8/23/2015 to 11/19/
San Juan River, Animas River, La Plata River, Mancos 2015 (USGS MRP-15078). Snowmelt runoff in the
River, McElmo Creek, Chaco Creek, and Chinle Creek) Lower San Juan River (5/17/2016 to 7/14/2016) was
can be characterized by prevalence of precious metal min- captured with three sediment traps (upstream, mid-
ing, predominant underlying geologic unit, as well as runoff stream, and downstream locations), where 12.7 cm were
type (i.e., snowmelt, rainfall, or baseflow) in the tributary deposited in each trap over 59 days (USGS MRP-
(Supporting Information Fig. SI1 and SI2, Table SI1). 15597). Lower San Juan River baseflow conditions
Mined tributaries, defined as > 50 precious metal mines, punctuated by a large rainfall event and two smaller
include the Animas, Upper San Juan, Mancos, and La Plata rainfall events in the watershed (7/14/2016 to 10/26/
Rivers, whereas unmined tributaries, defined as < 50 pre- 2016) were captured in 3.5, 6, and 2 cm from the
cious metal mines, include McElmo, Chinle, and Chaco upstream, mid-stream, and downstream locations, re-
Creeks. The watersheds of McElmo Creek, Mancos River, spectively (USGS MRP-16105).
and La Plata River are predominantly underlain (> 50% Sediment deposition rates in Lake Powell are high
area) by the Mancos Shale, a Cretaceous-age marine shale (meter per year range) and vary substantially within and
naturally high in As and Se (US DOE 2011; Larrick and between years (Stanford and Ward 1991; Potter and Drake
Ashmore 2012; Dyer et al. 2016; MRDS 2017), whereas 1989; Vernieu 1997). For example, USGS sediment traps
the watersheds of Chinle Creek and Chaco Creek are collected during baseflow with intermittent rainfall show
predominantly underlain (> 50% area) by the Chinle Sand- interannual variation in deposition rates, e.g., 1.97 m/year
stone, a Pennsylvanian to Cretaceous age sandstone natu- in 2015 and 0.21 m/year in 2016. Average sediment
rally high in Al, As, cobalt (Co), chromium (Cr), Fe, accumulation rates in the San Juan River Delta were
vanadium (V), and Zn (Newman 1962; MRDS 2017) reported to range from 0.48 to 2 m/year (Potter and
(Supporting Information Fig. SI1, Table SI1). Drake 1989; Stanford and Ward 1991; Vernieu 1997).
Stream hydrographs in snowmelt-dominated water- The high observed sedimentation rates in the San Juan
sheds (Upper San Juan and Animas) are characterized River Delta lead to an expectation that the USGS sediment
by sustained high flow during spring, whereas cores (ranging in length from 1.48 to 4.6 m) likely repre-
hydrographs from rainfall-dominated watersheds (La sent less than a decade of sediment deposition. Whereas
Plata, McElmo, Chinle, and Chaco) are characterized cesium (Cs)-137 and Pb-210 isotopes are commonly used
by short high intensity flow events (Supporting to determine sediment accumulation rates in modern lake
Information Fig. SI2). records (post-1950) (e.g., Malher et al. 2006; Bloesch and
Evans 1982; USGS 2016), the combination of fluctuating
2.2 San Juan River Delta of Lake Powell deposition rates and the decade (short) timescale make
traditional dating methods unfeasible. Therefore, seasonal
In order to document the presence of elevated elemental signatures of San Juan River tributaries may help in
concentrations in San Juan River deltaic sediment, the estimation of deposition time in the San Juan River Delta
United States Geological Survey (USGS) collected sediment cores.
128 Page 6 of 18 Water Air Soil Pollut (2019) 230:128
for each runoff category, where conservative transport 10 samples at 4- to 5-cm increments. Sediment deposit-
with no deposition was assumed. ed during peak snowmelt at the upstream location was
The three sediment cores collected from the San Juan sub-sectioned by visual layer (total of three subsec-
River Delta of Lake Powell in August 2010 (Core 1, tions), whereas the sediment from the other two loca-
Core 2, and Core 3) (Fig. 1) (Hornewer 2014) had tions was homogenized. Collection and analysis of the
individual thickness of 1.48 m, 3.37 m, and 4.60 m, sediment traps were performed by the USGS indepen-
respectively. The complete sampling methodology and dent from and prior to our project (MPR-15078, MPR-
coring procedure are given in Hornewer (2014) and Hart 15597, and MPR-16105). Sediment deposited during
et al. (2005). Various strata were subsampled (20, 32, rainfall/baseflow 2016 was homogenized and analyzed
and 49 subsamples, for cores 1, 2, and 3, respectively), separately for each trap location. All sediment trap sam-
dried, digested via total digestion (HCl, HNO3, HClO4, ples were dried, digested via total digestion, and ana-
and HF at low temperature), and analyzed via inductive- lyzed via ICP-AES-MS multi-acid (ICP-42) (USGS
ly coupled plasma atomic emission spectrometry (ICP- method 19-42, USGS 2018).
AES) (Hornewer 2014). Additional sediment samples PCA was performed in R (R Core Team 2013) to
were sub-sectioned from the frozen cores in Fall 2017 at generate linear combinations of sediment elemental con-
the USGS laboratory in Boulder, CO (6, 19, and 15 centrations, where PC1 accounts for the majority of
samples from cores 1, 2, and 3, respectively). variance among elemental concentrations,and PC2 ac-
Because the three sediment cores have similar aver- counts for the largest remaining variance orthogonal to
age elemental concentrations (Student t test p > 0.05) PC1. Because sediment elemental concentrations
(Supporting Information, Fig. SI 5), Core 2 was selected spanned multiple orders of magnitude, elemental con-
and analyzed for elemental concentration and Pb iso- centrations were log transformed to avoid
topes via ICP-MS with a 10% HCl digestion for 48 h at overweighting of large concentrations. PCA was per-
22 °C. Grain size was analyzed via Sympa Tec Lixell formed for the sediment trap elemental concentrations
Helos/KF laser diffraction using two lenses, which cap- in order to generate runoff-specific probability ellipses
tured particles sizes 0.25 to 87.5 μm and 0.5 to 350 μm, representing 95% confidence interval. PC1 and PC2
respectively. Particle sphericity was analyzed via Sympa weights were then applied to log-transformed sediment
Tec Lixell QICPIC. core elemental concentrations (also measured via total
Sediment color was assigned based on Munsell Soil digestion).
Color Charts (Munsell Color x-rite 2009). Water content Enrichment factors, PCA, and Pb isotopes were
and bulk density of the sediment samples were deter- used as independent lines of evidence for source iden-
mined by weighing a known volume of sample before tification of San Juan River Delta sediment layers.
and after drying. Sediment elemental concentrations Enrichment factors, Pb isotopes, sediment color, and
were then corrected to represent the dry elemental con- grain size tie sediment deposited in the San Juan River
centration. A 10% HCl leaching was assumed to extract Delta to upstream tributaries, where enrichment fac-
only the metal/metalloid coating on the mineral (e.g., tors, Pb isotopes, and color will characterize the
elements that precipitate upon mixing acidic mine waste bioavailable/redox sensitive component of sediment
with circum-neutral river water) (extractable phase), (extractable phase). Enrichment factors and color of
rather than the entire mineral matrix (total digestion). San Juan River Delta sediment layers may record
While inclusion of an oxidizing extractant (nitric acid) changes in PM source, where distinct PM concentra-
might have recovered additional trace elements via de- tions and/or color exists between tributaries or between
struction of organic matter, increased chloride, and pro- runoff categories (assuming no diagenetic processes).
ton concentration (via HCl) also promotes trace element Pb isotopes in San Juan River Delta sediment may
release from organic matter. In this way, suspended PM reflect the mineralized vein (sourced from mined trib-
concentrations in the water, also digested via 10% HCl, utaries), predominant underlying geologic unit
can be directly compared to sediment elemental (sourced from unmined tributaries), or a combination
concentrations. of sources. Sediment trap elemental concentration
Sediment traps were sub-sectioned and analyzed by PCA (total digestion) establishes runoff category
the USGS (UDWQ et al. 2018), where layers deposited trends in deposited sediment to be used predictively
during rainfall/baseflow 2015 were sub-sectioned into for San Juan River Delta sediment.
128 Page 8 of 18 Water Air Soil Pollut (2019) 230:128
<0.05
<0.05
<0.05
<0.05
<0.05
<0.05
<0.05
<0.05
<0.05 <0.05
<0.05
<0.05 <0.05
<0.05
<0.05
<0.05 <0.05
<0.05
<0.05 <0.05
<0.05
c
Fig. 2 Average PM concentration in the tributary watersheds shown. Tributary PM concentrations are only present for runoff
during rainfall (a), snowmelt (b), and baseflow (c) shaded from categories occurring within the tributary (e.g., no Chinle baseflow
upstream (dark blue) to downstream (red). Statistically significant PM concentrations exist). PM concentrations not shown in Fig. 2
differences (p < 0.05) between average PM concentrations are are given in Supporting Information (Fig. SI6)
samples 2–01, 2–12, 2–13, 2–15, and 2–18 (Fig. 4a) and were not normally distributed (Supporting
may reflect sediment sourced from Chinle Creek. Information, Fig. SI 10). The median suspended sedi-
Median (P50) grain size in Core 2 ranged from 4 to ment size in Chinle and Chaco Creeks was smaller than
150 μm with a majority of the sediment < 10 μm in size those observed in sediment Core 2 (P50 2.9 ± 0.12and
(Fig. 4c). Median grain size was used because particles 3.4 ± 0.05 μm, respectively), while Upper San Juan
were observed over the entire size range (0.25 μm to River, Animas River, Mancos River, La Plata River,
87.5 μm or 0.5 μm to 350 μm, dependent on lens used) and McElmo Creek mobilized particles with median
128 Page 10 of 18 Water Air Soil Pollut (2019) 230:128
<0.05
<0.05
Fig. 3 Average PM concentrations (mgmetal/mgsed) in the Animas River during rainfall (red), snowmelt (blue), and baseflow (gray).
Statistically significant differences (p < 0.05) between average PM concentrations are shown
size ranging from 8.5 to 39.0 μm (Supporting the sediment matrix and not on the coating, with less
Information, Fig. SI11). Core 2 sphericity measure- than 10% of Al, Cr, Sb, and V on the coating (low ratio
ments were not useful in differentiating tributary source of extractable to digested, Fig. 4d).
(mean sphericity 0.71 ± 0.01) and are provided in the Similar to elemental concentrations, color, and grain
Supporting Information (Fig. SI12). size, sediment Pb isotope ratios linked deposited sedi-
Sediment elemental concentrations in the extractable ment to PM in upstream tributaries. Suspended PM Pb
phase were 1 to 1000 times lower than those determined isotope ratios from mined San Juan River tributaries
by dissolution of the matrix (Hornewer 2014) (Fig. 4d). generally reflected Pb isotopes in the mined mineralized
In general, over 50% of elemental concentration was in vein (Eureka Graben) (Church et al. 1997), whereas Pb
Sample Color/ID Metal:Al rao P50 Grain Size (μm) Extractable:Digested (%)
a b c d
Fig. 4 a Dominant Munsell color of sediment (Munsell Color x- the top of the core (m) with the lens size range in gray; and d
rite 2009) and sample ID as a function of depth from the top of the Percent of metal in extractable phases relative to full digestion as a
core (m); b ratio of extractable As (gold), Cd (orange), Cu (green), function of depth from the top of the core (m). The lesser number
Pb (light blue), Mo (dark blue), Ni (purple), and Se (pink) to Al as of samples in D reflects lesser samples fully digested (Hornewer
a function of depth from the top of the core (m); c Median (P50) 2014)
grain size (μm) for samples (black line) as a function of depth from
Water Air Soil Pollut (2019) 230:128 Page 11 of 18 128
isotope ratios in unmined tributaries reflected the pre- concentrations (lower PC1) than sediment deposited
dominant underlying geologic unit (Fig. 5). Suspended during baseflow with intermittent rainfall, which were
sediment in the Animas, Upper San Juan, La Plata, and higher in Fe, Al, and Ni concentrations (higher PC1)
McElmo Rivers had Pb isotope ratios that reflected the (Fig. 7a). Rainfall/baseflow sediment deposited in 2015
mineralized vein (Church et al. 1997), which is present had higher Fe, Al, and Ni concentrations (higher PC1)
in the headwaters of each tributary except McElmo than sediment deposited during rainfall/baseflow in
Creek (Fig. 5). The Dolores River, headwaters underlain 2016 (Fig. 7a), possibly reflecting the larger 2015 rain-
by the mineralized vein, is diverted to McElmo Creek to fall events resulting in significant flow in Chinle Creek
maintain year-round flow (Larrick 2010) and appears to (Supporting Information, Fig. SI2) (UDWQ et al. 2018).
dominate the McElmo Pb signature. The Mancos River Additionally, the significantly higher sedimentation rate
Pb isotope ratios reflected a combination of the miner- captured in 2015 rainfall/baseflow trap than in 2016
alized vein and the Mancos Shale, which has relatively rainfall/baseflow trap (1.97 m/year versus 0.21 m/year,
enriched 208Pb/204Pb and 206Pb/204Pb (Church et al. respectively) indicates the activation of a large sediment
1997) (Fig. 5). Chinle and Chaco Creeks Pb isotope source (e.g., Chinle Creek) during the 2015 deployment.
ratios were enriched, potentially reflecting the Chinle Sediment trap periods were not further differentiated
Sandstone (Fig. SI5). in PC2, as sediment deposited during both snowmelt
Pb isotope ratios in core 2 spanned Pb isotope ratios and baseflow with intermittent rainfall spanned PC2
measured in tributary suspended sediment (Fig. 6), (Fig. 7a). Unlike sediment trap period, sediment trap
where Pb isotope ratios for samples 2–02 and 2–03 location (upstream, midstream, and downstream) did
reflected the mineralized vein, and samples 2–01, 2– not occupy distinct PCA spaces (Fig. 7a), where colors
12, 2–13, 2–15, and 2–18 reflected the Chinle Sand- corresponding to sediment trap location were mixed
stone (Fig. 6). Pb isotopes measured in 2–04 and 2–05 throughout the PCA space.
represented a transition, similar to the Pb isotope ratios Core 2 sediment PM concentrations (total digestion),
measured in the Mancos River (Fig. 6). occupied similar PCA space to sediment traps, except-
ing 2–07 which was lower in all PM concentrations
4.2 Sediment Matrix Signatures in PCA Space (Fig. 7b). Samples 2–01, 2–13, 2–15, 2–17, and 2–18
occupied PC space within the probability ellipse
Runoff category signatures were established through assigned to 2015 rainfall/baseflow sediment traps, indi-
PCA of sediment trap PM concentrations (via total cating that these sample concentrations were similar
digestion) (mgmetal/mgsed), which were deployed during (95% confidence) (Fig. 7b). Whereas samples 2–03
baseflow with intermittent rainfall and peak snowmelt and 2–16 occur outside the probability ellipse for peak
(UDWQ et al. 2018). Sediment trap periods occupied snowmelt sediment, these samples occupied a similar
distinct PC spaces (Fig. 7a); where sediment deposited PC2 space (higher Pb, Zn, Mo, and As) as that occupied
during snowmelt had higher Pb, Zn, V, Mo, and As by early and peak snowmelt samples (Fig. 7b). Samples
a b
2–09 and 2–19 occurred in the 2016 rainfall/baseflow thickness. Tributary suspended PM loads were com-
probability ellipse, indicating similar concentrations pared to Lower San Juan River suspended PM loads to
(Fig. 7b). estimate the relative contribution of PM from different
tributaries (both mining and non-mining sourced) to PM
4.3 Average Tributary Suspended PM Loads loads directly upstream of Lake Powell.
The contribution of upstream tributaries to the Lower
Whereas PM concentrations link geochemical signa- San Juan River suspended PM load changed with runoff
tures in suspended sediment to geochemical signatures category (Fig. 8), even though overall Lower San Juan
in deposited sediment, suspended PM loads, in contrast, River PM loads were similar regardless of runoff category
link suspended material mass to deposited layer (p > 0.05, Supporting Information Fig SI13). During
Trap Period
Rainfall/baseflow
Early snowmelt Cores
Peak snowmelt Core 2
Trap Locaon Trap Period
Upstream Rainfall/baseflow
Mid-stream Early snowmelt
Downstream Peak snowmelt
a b
Fig. 7 a PCA for USGS sediment traps deployed over three 29.2% of the variance, respectively. PC3 explained 14.5% of the
periods: 2015 rainfall/baseflow (circles), 2016 snowmelt variance; b Sediment core samples were assigned PC1 and PC2
(squares), and 2016 rainfall/baseflow (triangles), collected at three weights generated by sediment traps (blue diamonds) and graphed
locations: upstream (red), mid-stream (green), and downstream with sediment deposited during 2015 rainfall/baseflow (black
(blue) (Fig. 1). Graphical representation of elemental PC weights circles), 2016 snowmelt (squares), and 2016 rainfall/baseflow
(solid lines) are given, where vectors denote weight and direction (triangles). Probability ellipses, representing the 95% confidence
of PC1 and PC2 weights. PC1 and PC2 explained 48.3% and interval, are given for the distinct sediment trap categories
Water Air Soil Pollut (2019) 230:128 Page 13 of 18 128
b
Baseflow
snowmelt, the Animas River was the dominant source of rainfall events, the Animas River contributed the largest
Lower San Juan River PM loads (> 50% contribution of PM loads of As, Be and Se (32%, 89%, and 78%, respec-
As, Cd, Cr, Cu, Pb, Se, Tl, and Zn) (Fig. 8a). The Upper tively), the Upper San Juan River contributed the second
San Juan River contributed the second largest loads of Cr largest PM loads of Se and Zn (20% and 22%, respective-
and Cu in the Lower San Juan River during snowmelt ly), McElmo Creek contributed the largest PM loads of Fe
(30% and 36% contribution, respectively), whereas (48%) and Tl (93%), and the Chaco Creek contributed the
Mancos River snowmelt PM loads were even less signif- largest PM load of Cd (30%). The La Plata River and
icant (< 20% contribution for each element). Unaccounted Mancos River did not contribute any significant rainfall
PM loads (Fig. 8 open bars) are examined in Supporting PM loads. Whereas the Animas River contributed the
Information (Appendix I). largest loads of Be and Tl during baseflow conditions
During rainfall events, Chinle Creek was the dominant (99% and 68%, respectively), a majority of the Lower
source (> 50% contribution) of Lower San Juan River PM San Juan River baseflow PM loads were not attributable
loads for Al, Cr, Cu, Pb, Ni, V, and Zn (Fig. 8b). During to an upstream tributary (Fig. 8c).
128 Page 14 of 18 Water Air Soil Pollut (2019) 230:128
The overall percent PM load contributions from each Mancos Watershed (Clow and Stephens 2005) were not
tributary to the Lower San Juan River during a given apparent in downstream Mancos River PM loads
runoff category did not vary significantly when one (Fig. 8), possibly due to dilution by loads from the
standard deviation of the average PM load was consid- unmined West Fork tributaries as well as differences in
ered (Supporting Information Fig. SI14). The propor- partitioning among dissolved versus particulate phases.
tionality of average PM loads to standard deviation PM Reported elevated As and Se concentrations (mgmetal/L)
loads suggests that PM loads were consistent within in Mancos Shale (Dyer et al. 2016; U.S. Department of
runoff events and that PM source was not limited. When Energy 2011; Larrick and Ashmore 2012) were
considering discrete samples, PM load and discharge reflected in Mancos As and Se PM concentrations,
were directly related (power law, R2 > 0.68, e.g., Al which rivaled those of the Animas River (Supporting
PM load = 221.32*discharge0.75) in each tributary re- Information Fig. SI7). In contrast, As and Se PM loads
gardless of runoff category, indicating consistency of from the Mancos River were minor fractions of the As
PM concentrations among runoff categories. An excep- and Se PM load of the Lower San Juan River, reflecting
tion was rainfall in the Animas River, where both high the relatively low flow in the Mancos River compared to
and low PM loads occurred at low discharge the Animas River (Fig. 8).
(Supporting Information, Fig. SI15). In contrast to snowmelt-dominated watersheds,
Chinle Creek and other unmined tributaries dominated
PM contributions to the San Juan River during rainfall
5 Discussion events (e.g., Al, As, Cr, Co, Cu, Fe, Pb, Ni, V, and Zn)
(Fig. 8). The association of Chinle Creek rainfall PM
5.1 Mined versus Unmined Tributary Signatures loads (Fig. 8) to elements associated with the Chinle
Sandstone (Newman 1962) and Chinle and Chaco
During snowmelt, discharge (Supporting Information Creek Pb isotope with the Chinle Sandstone (Fig. 5)
Fig. SI12), PM load (Fig. 8), and Pb isotope ratio links Chinle and Chaco Creek rainfall PM loads to
(Fig. 5) of the Lower San Juan River each reflected the unmined sources. McElmo Creek Fe and Tl PM rainfall
Animas River. The association of Animas snowmelt PM loads (Fig. 8) may reflect both mined and unmined
loads (Fig. 8) and Pb-isotope with mining activity terranes. Whereas McElmo Watershed is unmined, it is
(Fig. 5) (Church et al. 1997), as well as the fact that supplemented by water from the Dolores River, which is
snowmelt runoff predominantly originated in high ele- mined (Larrick 2010), and this was reflected in the Pb
vation, mining-intensive terrain, links Animas, and isotope ratio (Fig. 5).
Lower San Juan River snowmelt PM to mining legacy.
Animas River snowmelt PM load contributions domi- 5.2 Linking Sediment Core Layers to PM of Upstream
nated those of the other mined tributaries (Upper San Tributaries
Juan, La Plata, and Mancos Rivers) (Fig. 8) due to
relatively insignificant flows in the La Plata and Mancos Elemental and isotopic signatures in Lake Powell sedi-
Rivers, as well as trapping by the Navajo Dam in the ment were linked to those of PM in upstream tributaries.
Upper San Juan River (Supporting Information Fig. The 0.66-m layer near the top of core 2, represented by
SI2). That the Upper San Juan River Pb isotope ratio samples 2–02 and 2–03, likely reflected Animas River
was representative of the mineralized vein (Fig. 5) sug- snowmelt PM, where the Pb isotope ratios represented
gests that not all mining-sourced PM is trapped by the mineralized vein present in the headwaters of the
Navajo Dam and the ~ 30% contributions of Upper Animas River (Fig. 5). As well, ratios of Pb to Al, Cd to
San Juan River snowmelt PM loads of Cu, Cr, and Cd Al, Cu to Al, and Zn to Al were characteristic of the
are potentially mining-sourced (Fig. 8). Animas River (Fig. 4b), and elemental concentrations
That the Mancos River Pb isotope ratio reflected a occupied similar PC space as sediment deposited during
combination of Mancos Shale and mineralized vein snowmelt (Fig. 7).
(Fig. 5) (Church et al. 1997) suggests that both mining The dominance of the Animas River PM signature in
and non-mined terranes contributed to Mancos River the Lower San Juan River during snowmelt (Supporting
PM loads. Reported elevated dissolved concentrations Information, SI17) in addition to the low deposition
of Cu and Ag attributed to mining in the east fork of the rates modeled in the San Juan River during high flow
Water Air Soil Pollut (2019) 230:128 Page 15 of 18 128
typical of snowmelt (Sullivan et al. 2017) would allow rainfall and snowmelt (Fig. 7) and Pb isotopes were
Animas River snowmelt PM signatures to be deposited enriched compared to the Chinle Sandstone (Fig. 6)
as a layer in the sediment of the San Juan River Delta. (i.e., samples 2–08, 2–11, 2–14, and 2–19). Sediment
The 0.24-m layer deposited before the snowmelt layer, core sample 2–16 occupied similar PC space as sedi-
represented by samples 2–04 and 2–05, possibly ment deposited during snowmelt but had a Pb isotope
reflected Animas River early snowmelt PM as the Pb ratio reflective of the Chinle Sandstone, potentially in-
isotope ratio was mixed (Fig. 6), but no excursions in dicating a mixture of sources.
elemental concentration were noted. Because Animas River snowmelt PM loads in the
Sediment core layers with enriched Pb isotope ratios San Juan River can be attributed to mining in the head-
(Fig. 6), red color (Fig. 4), and enriched Mn to Al waters of the Animas River, sediment layers reflecting
(Supporting Information Fig. SI8) likely reflected the Animas River snowmelt signature may also be at-
Chinle and Chaco Creek PM sources (i.e., layers repre- tributed to mining sources. Conversely, because rainfall
sented by samples 2–01, 2–12, 2–13, 2–15, 2–17, and PM loads sourced from the Chinle and Chaco tributaries
2–18). These samples also had elemental concentrations can be attributed to non-mining sources, sediment
that occupied similar PC space as sediment deposited reflecting Chinle and Chaco Creek rainfall signatures
during 2015 rainfall/baseflow (Fig. 6), suggesting the may be attributed to non-mining sources.
dominance of Chinle Creek PM during large rainfall Therefore, the percent of PM sourced from mining
events. That Chinle Creek (farthest downstream tribu- and non-mining sources was estimated from the percent
tary at ~ 20-km upstream of Lower San Juan) dominated contribution of mining and non-mining sourced PM in
rainfall layers deposited in the San Juan River Delta the Lower San Juan River (Fig. 8), the length of each
sediment, indicates that short duration high intensity sediment layer (Hornewer 2014), and the bulk density
flow events transmit PM across (~20 km) the system. (Supporting Information, Fig. SI19) of each sediment
Whereas the red color of core 2 layers could potentially layer. Assuming each subsample PM concentration rep-
reflect post-depositional oxidation of iron, it more likely resented the average PM concentration for a given layer,
reflects the red color of Chinle Creek PM, since PCA the percent of mining and non-mining sourced PM over
and Pb isotope ratios for red sediment layers also sug- Core 2 was calculated. For Core 2, 0.2% Al, 4% As, 5%
gested Chinle Creek as a source. Cu, 1% Fe, 10% Pb, and 8% Zn was attributed to mining
The 0.57-m-thick sandy layer, represented by sam- sources and 5% Al, 2% As, 7% Cu, 1% Fe, 3% Pb, and
ples 2–06 and 2–07, cannot be attributed to a runoff 4% Zn was attributed to non-mining sources. The re-
category because PM concentrations were lower than maining PM was likely sourced from a mixture of
those measured in any sediment trap (Fig. 7); however, mining and non-mining sources. As this is a first attempt
the Pb isotope ratios were representative of the Chinle at attributing mining and non-mining source PM in the
Sandstone (Fig. 5). The median grain size of the sandy sediment of Lake Powell, future work is needed to refine
layer (154 μm and 90 μm, for sample 2–06 and 2–07, estimates made here.
respectively) (Fig. 4C) was larger than any median
tributary particle size, suggesting that events mobilizing 5.3 Age of the Core
coarse sand particles were rare, or that coarse particles
were not successfully collected using the grab sampling Our results suggest that Core 2 was deposited in only ~
technique in upstream tributaries. Either possibility is 1.3 years, which reflects the high sedimentation rates
consistent with the good agreement in PM concentra- reported to occur during some years in the San Juan
tions measured between sampling composited and grab River delta. Core 2 was collected in mid-August 2010,
samples (UDEQ et al. 2018), since coarse particles have indicating that the 2010 snowmelt signature was repre-
low extractable elemental concentrations (Fig. 4d). No- sented in samples 2–03 to 2–04 (near the top of the
tably, no sand layers were observed in sediment traps, record). No other snowmelt layer was detected in core 2,
suggesting that coarse particles were not suspended in suggesting that the 2009 snowmelt was not represented.
the water column. 2009 was a low snowmelt year in the Lower San Juan
Other layers likely reflect a mixture of sources de- River, with peak flow ending in early May rather than
posited during baseflow, where sediment PM concen- the typical June or July (Supporting Information Fig.
trations were lower than both baseflow with intermittent SI20), (USGS 2018). Core 2 was collected directly after
128 Page 16 of 18 Water Air Soil Pollut (2019) 230:128
a large precipitation event (08/03/2010) where flow in source identification and apportionment study.
Chemosphere, 59, 669–678.
the Lower San Juan River exceeded 5000 cfs (USGS
Axtmann, E. V., & Luoma, S. N. (1991). Large-scale distribution
2018) and flow in Chinle Creek reached ~ 100 cfs, likely of metal contamination in the fine-grained sediments of the
yielding the layer represented by sample 2–01. A similar Clark Fork River, Montana, U.S.A. Applied Geochemistry, 6,
age for this core, 1.4 years, was determined using bathy- 75–88.
metric survey elevation and average sedimentation rates Besser, J. M., & Leib, K. J. (2007). Toxicity of metals in water and
sediment to aquatic biota. In Integrated investigations of
(UDWQ et al. 2018). environmental effects of historical mining in the Animas
Whereas Pb isotopes, particle sizes, and enrichment River Wa ters ehd , S an Jua n Cou nt y, C olo ra do .
factors were determined for core 2, these attributes were (Professional Paper 1651) (pp. 837–849). Reston: U.S.
not determined for cores 1 and 3. PCA was performed Department of the Interior, U.S. Geological Survey.
Bliesner, R., & Lamarra, V. (2000). San Juan River basin recovery
for cores 1 and 3 (Supporting Information, Fig. SI21).
implementation program: hydrology, geomorphology and
Both core 1 and core 3 had a single sample fall within habitat studies. U.S: Fish and Wildlife Services.
the probability ellipse established by 2016 snowmelt, Bloesch, J., & Evans, R. D. (1982). Lead-210 dating of sediments
and multiple samples fall within the probability ellipses compared with accumulation rates estimated by natural
established by 2015 and 2016 rainfall/baseflow sedi- markers and measured with sediment traps. Hydrobiologia,
92, 579–586.
ment traps. Whereas future work will examine the re- Borrok, D. M., Wanty, R. B., Ridely, W. I., Lamothe, P. J.,
cord provided in these sediment cores, the detection of Kimball, B. A., Verplanck, P. L., & Runkel, R. L. (2009).
an Animas River snowmelt layer in core 2 suggests that Application of iron and zinc isotopes to track the sources and
high flow, typical of spring runoff, is needed for up- mechanisms of metal loading in a mountain watershed.
Applied Geochemistry, 24, 1270–1277.
stream signatures (above Chinle Creek) to be preserved
Christensen, V. G., & Juracek, K. E. (2001). Variability of metals
in the downstream sediment record. in reservoir sediment from two adjacent basins in the central
Great Plains. Environmental Geology, 40(4–5), 470–481.
Church, S. E., Kimball, B. A., Fey, D. L., Ferderer, D. A., Yager, T.
J., & Vaughn, R. B. (1997). Source, transport, and
6 Conclusions
partitioning of metals between water, colloids, and bed sed-
iment of the Animas River, Colorado. United States
San Juan River Delta sediment PM reflects mining and Geological Survey, 97–151.
non-mining sources from the tributaries of the San Juan Clow, S., & Stephens, D. B. (2005). Nonpoint source assessment
River. Tributary Pb isotopes and PM concentrations, of the Ute Mountain Ute Reservation of Colorado, New
Mexico and Utah. Ute Mountain Ute Tribe and Stephens
which differ with runoff category, were used to link and Associates, Inc.
sediment core layers to upstream tributaries, where the Coulthard, T. J., & Macklin, M. G. (2003). Modeling long-term
3.37 m core examined here represented approximately contamination in river systems from historical metal mining.
1.3 years of sediment deposition. Approximately 10% Geological Society of America, 31(5), 451–454.
Covelli, S., & Fontolan, G. (1997). Application of a normalization
of the overall PM deposited in the sediment core was
procedure in determining regional geochemical baselines,
attributed to mining sources, with ~ 80% of the overall Gulf of Trieste, Italy. Environmental Geology, 30(1–2), 34–
PM reflecting a mixture of mining and non-mining 45.
sources. Czuba, J. A., Magirl, C. S., Czuba, C. R., Grossman, E. E., Curran,
C. A., Gendaszek, A. S., & Dinicola, R. S. (2011). Sediment
Acknowledgements This research was supported by the Utah load from major rivers into Puget Sound and its adjacent
Department of Environmental Quality (Contract #171990). The waters. US Department of the Interior, US Geological
authors wish to thank the scientists at the NNEPA, USGS, and Survey.
DEQ for their support. Dologopolova, A., Weiss, D. J., Seltmann, R., Kober, B., Mason,
T. F. D., Coles, B., & Stanley, C. J. (2006). Use of isotope
ratios to assess sources of Pb and Zn dispersed in the envi-
ronment during mining and ore processing with the Orlovka-
Spokoinoe mining site (Russia). Applied Geochemistry, 21,
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