Geochemical evidence for sources of surface dust deposited on the Laohugou glacier, Qilian Mountains

Geochemical evidence for sources of surface dust deposited on the Laohugou glacier, Qilian Mountains

Accepted Manuscript Geochemical evidence for sources of surface dust deposited on the Laohugou glacier, Qilian Mountains Ting Wei, Zhiwen Dong, Shicha...

8MB Sizes 0 Downloads 28 Views

Accepted Manuscript Geochemical evidence for sources of surface dust deposited on the Laohugou glacier, Qilian Mountains Ting Wei, Zhiwen Dong, Shichang Kang, Xiang Qin, Zhilong Guo PII:

S0883-2927(16)30428-0

DOI:

10.1016/j.apgeochem.2017.01.024

Reference:

AG 3816

To appear in:

Applied Geochemistry

Received Date: 23 October 2016 Revised Date:

21 January 2017

Accepted Date: 30 January 2017

Please cite this article as: Wei, T., Dong, Z., Kang, S., Qin, X., Guo, Z., Geochemical evidence for sources of surface dust deposited on the Laohugou glacier, Qilian Mountains, Applied Geochemistry (2017), doi: 10.1016/j.apgeochem.2017.01.024. This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.

ACCEPTED MANUSCRIPT

4

Ting Wei a, Zhiwen Dong a*, Shichang Kang a, b, Xiang Qin a, c, Zhilong Guo a

5

a

6

Eco-Environment and Resources, Chinese Academy of Sciences, Lanzhou 730000,

7

China.

8

b

9

c

State

Key

Laboratory

of

Cryospheric

Sciences,

Northwest

Institute

of

CAS Center for Excellence in Tibetan Plateau Earth Sciences, Beijing 100101, China

SC

2

RI PT

3

Geochemical evidence for sources of surface dust deposited on the Laohugou Glacier, Qilian Mountains

1

Qilian Shan Station of Glaciology and Ecologic Environment, Chinese Academy of

Sciences, Lanzhou 730000, China.

11

*Corresponding Author. Address: State Key Laboratory of Cryospheric Sciences,

12

Northwest Institute of Eco-Environment and Resources, Chinese Academy of

13

Sciences, Lanzhou 730000, China.

14

Email: [email protected]

15

Abstract

16

Atmospheric dust deposited on glacier surfaces can decrease snow albedo by

17

enhancing lighting absorption and by forming cryoconites via microbial activity,

18

which accelerates glacier melt. Using snow and cryoconite sampled from the

19

Laohugou Glacier No.12 in the Qilian Mountains during spring 2012 and summer

20

2014, this work investigates the Sr-Nd isotopic and rare earth element (REE)

21

geochemistry of dust and its environmental significance. Results demonstrate that

22

dust REEs possess lower Eu/Eu* and L/HREE, and higher (Gd/Yb)N values compared

23

with that of the Mu Us and Hobq Deserts but yield higher (La/Yb)N, L/HREE,

24

(La/Sm)N and (La/Yb)N ratios than that of the Taklimakan Desert. The REE

25

composition of glacier surface dust is similar to the material from nearby arid regions,

26

such as the Qaidam Basin and the Tengger and Badain Jaran Deserts surrounding the

27

eastern Tibetan Plateau. The εNd(0) values of glacial dust resemble the isotopic ratios

AC C

EP

TE D

M AN U

10

1

ACCEPTED MANUSCRIPT 28

of the Qaidam, Badain Jaran, Tengger Deserts and local dust (εNd(0) value of -13.6)

29

but differ from that of the Taklimakan Desert, which has higher

30

Analysis of air mass trajectory also indicates a potential dust input from the

31

surrounding areas to the alpine glaciers in the Qilian Mountains. These results

32

strongly indicate that the dust source from the arid, northern Tibetan Plateau region

33

was the dominant contributor to atmospheric dust deposition on the glacier surface,

34

rather than dust originating from the long-range transport of Taklimakan Desert

35

material.

36

Keywords: Surface dust; REEs; Sr-Nd isotopes; Dust source; glacier melt

37

1. Introduction

38

Mineral dust exerts a significant influence on the climate system and biosphere by

39

affecting the chemical composition of the troposphere (Bauer et al., 2004; Dentener et

40

al., 1996; Zhang et al., 2015), potentially reducing precipitation by increasing

41

cloudiness with smaller droplets (Rosenfeld et al., 2001) and changing the radiative

42

balance of the atmosphere by absorbing solar radiation and scattering terrestrial

43

radiation (Sokolik and Toon, 1999; Sullivan et al., 2007).

Sr/86Sr ratios.

TE D

M AN U

SC

RI PT

87

The Cryosphere plays an important role in the Earth’s climate system, affecting the

45

hydrological cycle and energy balance (Di Mauro et al., 2015), and is sensitive even

46

to small climate changes. Glaciers, the largest component of the Cryosphere, are

47

currently experiencing dramatic melting attributed to increasing temperatures and

48

decreasing snow accumulation. Mineral dust, one type of Light Absorbing Impurity

49

(LAI) deposited on glaciers, is an important factor influencing glacier melt (Kaspari et

50

al., 2015; Wang et al., 2013). Specifically, iron oxides in dust such as goethite and

51

hematite enhance absorption of shortwave spectra (ultraviolet and visible wavelengths)

52

in snow and thus lead to reduced snow albedo and glacier melt (Zhang et al., 2015;

53

Wu et al., 2015). Previous studies indicated that snow albedo and radiative forcing of

54

dust have a greater influence on climate warming than does black carbon when

55

impurity contents are low (Kaspari et al., 2014; Ramanathan and Carmichael, 2008).

56

Mineral dust in the Solu-Khumbucan decrease snow albedo by 40-42% (Kaspari et al.,

AC C

EP

44

2

ACCEPTED MANUSCRIPT 2014). Other studies showed that dust deposited onto an Alpine glacier reduced the

58

mean annual albedo of snow by less than 0.01 (Gabbi et al., 2015). Iron oxide mineral

59

dust has a significant effect on the melting of snow and glaciers. The mineralogical

60

properties of surface dust on glaciers have a strong effect on glacier ablation.

61

However, many previous studies focused more on biological properties and less on

62

mineralogy, which depends on dust source and transport. Therefore, to constrain the

63

influence of dust on glacier ablation, the provenance of dust deposited onto glaciers

64

must be identified.

RI PT

57

Rare earth elements (REEs) and strontium and neodymium isotopic compositions

66

are powerful tools for determining dust origin (Piper et al., 2013). Like isotopes,

67

REEs possess identical external electronic configurations and therefore display

68

essentially identical chemical properties. Owing to their low solubility, REEs are

69

generally in the particulate phase during transport (Henderson, 1984). These

70

properties impose limitations on REE fractionation during weathering and diagenesis.

71

Similarly,

72

properties and less on alteration due to surficial processes, including weathering,

73

transport and deposition. These isotopes are therefore utilized as fingerprints for dust

74

sources (Grousset and Biscaye, 2005; Nie et al., 2012). Using REE compositions and

75

Sr-Nd isotopes, we can both determine dust composition and trace the source of

76

mineral dust deposited onto glaciers (Dong et al., 2015; Dong et al., 2016; Du et al.,

77

2015; Wu et al., 2015; Tepe et al., 2015). We therefore employ a multi-parameter

78

method to address provenance (Nie et al. 2012).

143

M AN U

Sr/86Sr and

Nd/144Nd isotopic signatures mainly depend on geological

EP

TE D

87

AC C

79

SC

65

Laohugou (LHG) glacier No.12 is a mountain glacier in northern China that has

80

gradually retreated over the last 50 years (Du et al., 2008). This dramatic glacier melt

81

is attributed to a rise in temperature, a reduction in snow accumulation and the

82

deposition of LAIs such as mineral dust (Kaspari et al., 2015). Therefore, tracing the

83

provenance of dust on the glacier is important for understanding both glacial change,

84

and regional atmospheric circulation. Previous studies have mainly focused on tracing

85

sources and analyzing the physicochemical composition of snow dust, as well as the

86

microbial process of cryoconite formation in the upper portion of the glacier (Dong et 3

ACCEPTED MANUSCRIPT al., 2014; Xu et al., 2012). However, little research has been done on the provenance

88

of glacier surface dust, including on snow dust and cryoconites from LHG glacier

89

No.12. In addition, very limited Sr-Nd isotopic and REE composition data have been

90

reported for dust on local glacier surfaces. Therefore, this study aims for a

91

comprehensive understanding of dust geochemical composition over the entire glacier

92

and discusses the potential dust transport mechanism in the larger region of western

93

and northern China.

94

2. Sampling and Methodology

95

2.1. Sampling glacier surface dust

96

The Qilian Mountains, located in the northwestern Tibetan Plateau (TP), are

97

surrounded by several large sand deserts. To the northwest and west are the

98

Gurbantunggut and the Taklimakan Deserts, respectively, the largest two deserts in

99

central Asia. The Qaidam Desert is located immediately to the southwest of the Qilian

100

Mountains, and to the southeast are the Badain Jaran and Tengger Deserts. The LHG

101

Glacier No.12 (39.438N, 96.568E), with a length of 10.1 km and an area of 21.9 km2,

102

is the largest glacier in the LHG basin and is separated into two branches at 4560 m

103

above sea level (asl). A typical continental climate characterizes the northern Qilian

104

Mountains, and the southeasterly winds prevailing in the area are mainly controlled

105

by Westerlies.

EP

TE D

M AN U

SC

RI PT

87

In June 2012 and August 2014, we collected snow pit and cryoconite samples at

107

LHG glacier No.12 (Figure 1, Table 1). Thirteen samples were acquired, including

108

seven cryoconite samples from 5 cm in depth and six snow pit samples from 95 and

109

120 cm in depth. Cryoconite samples were collected between 4386 and 4850 m asl

110

and snow pit samples at 5040 m asl. Samples were collected using a pre-cleaned

111

stainless-steel shovel and polyethylene gloves, then put into pre-cleaned low-density

112

polyethylene (LDPE) bottles (Thermo Scientific). All samples were kept frozen until

113

they were analyzed at the Analytical Laboratory of Beijing Research Institute of

114

Uranium Geology.

AC C

106

4

ACCEPTED MANUSCRIPT 115

2.2. REE parameters and Sr-Nd isotopes REEs are a group of 14 elements ranging from La to Lu with similar ionic radii and

117

valance states. According to their mass number, REEs are divided into light REEs

118

(LREE: La, Ce, Pr, Nd, Sm, Eu) and heavy REEs (HREE: Gd, Tb, Dy, Ho, Er, Tm,

119

Yb, Lu). Chondrite-normalization of REEs was used to eliminate the odd-even effect.

120

In this study, several REE composition parameters were applied to determine the

121

potential sources of REEs in the dust of both the study region and the potential source

122

areas. Ratios of L/HREE and (La/Yb)N can reflect the differential degree of REEs.

123

The (La/Sm)N ratio represents the differential degree of LREEs, with a positive

124

correlation between the ratio and the differential degree. Alternatively, (Gd/Yb)N

125

indicates the differential degree of HREE and is negatively correlated with differential

126

degree. Additionally, Eu/Eu*(=EuN/(SmN ∗ GdN)1/2) values can not only indicate

127

sedimentary environment but also parent rock characteristics (Zhang, 1997).

M AN U

SC

RI PT

116

Radiogenic Sr and radiogenic Nd isotopic compositions are expressed in ratios of

128 87

Sr/86Sr and 143Nd/144Nd. In general, 143Nd/144Nd ratios possess little variation and are

130

represented as a ten thousand part deviation from the

131

chondrites

132

143

133

affected by surficial processes, the cycling of crustal material or grain size. In contrast,

134

Sr isotopes are easily altered by weathering, wind sorting and grain size effects (Chen

135

et al., 2011). Moreover, Sr isotopes are weakly affected by the reaction of dust with

136

acid aerosols during atmospheric transport, and acid leaching during pretreatments

137

(Meyer et al., 2011; Revel-Rolland et al., 2006). Therefore, our discussion will

138

principally focus on the comparison of εNd (0) values of dust samples and the deserts.

139

2.3. Geochemical analyses

TE D

129

(0.512638):

143

Nd/144Nd ratio of modern

εNd=((143Nd/144Nd)sample/143Nd/144Nd)CHUR)−1)×104.

The

AC C

EP

Nd/144Nd ratio is mainly controlled by crust-mantle differentiation age and is not

140

REEs in dust samples were measured by inductively coupled plasma-mass

141

spectrometry (ICP-MS, Thermo Scientific Element/XR). To improve data accuracy

142

and ensure the credibility of results, non-powder vinyl clean room gloves and masks

143

were worn during sample analysis to avoid potential contamination. Experimental 5

ACCEPTED MANUSCRIPT 144

blank analyses showed that contamination produced during sampling, transportation

145

and analysis was negligible. This methodology has been described in detail by Dong

146

et al. (2015). Thermal ionization mass spectrometry (TIMS) measurement of Sr-Nd isotopes was

148

performed at the same laboratory as REE analysis. Dissolution was carried out in

149

PTFE screw-top bombs with a mixture of ultra-pure HF + HClO4 at 120℃for seven

150

days on a hot plate. Then, Sr-Nd isotopes were isolated in quartz columns by

151

ion-exchange chromatography. Isotopes of Sr were measured using single Re

152

filaments and a Ta activator in static mode. The 87Sr/86Sr and

153

corrected for internal mass bias to

154

87

155

which has a recommended value of 0.710248. The 143Nd/144Nd ratio for the reference

156

material ShinEtsu was 0.512095±9 (2σ, n=10), which has a recommended value of

157

0.512110. For convenience, the

158

εNd(0)=[(143Nd/144Nd) /0.512638–1] x104.

159

3. Results and Discussion

160

3.1 REE composition of dust deposited on the glacier surface

161

The LHG glacier No.12 is located near the central Asian dust sources and may be

162

significantly affected by dust emissions from these deserts. However, the deserts

163

differ in their influence on dust transport to the study site because of geographic

164

location, meteorological conditions and mineralogical properties. The deserts have

165

distinct mineral compositions, such as goethite and hematite, which are LAIs on

166

glacier and snow surfaces (Maher et al., 2009). The sources of dust transported to

167

LHG Glacier No.12 should be identified in order to establish iron oxide indicators and

168

to determine the influence of iron oxides on glacier and snow melt.

RI PT

147

Nd/144Nd data were

SC

87

143

Sr/86Sr =0.1194 and

143

Nd/144Nd =0.7219. The

Nd/144Nd ratios were normalized and denoted as

AC C

EP

TE D

143

M AN U

Sr/86Sr ratio for the reference material NBS 987 was 0.710229±13 (2σ, n=10),

169

The REE characteristics of glacier surface dust from LHG Glacier No.12 vary

170

widely but are different from the Hobq and Mu Us Deserts in their lower Eu/Eu* and

171

L/HREE values, and higher (Gd/Yb)N values (Figure 2 and Figure 3). The Taklimakan

172

Desert, the main Asian dust source, can be roughly distinguished from samples 6

ACCEPTED MANUSCRIPT collected at the glacier by higher (La/Yb)N, L/HREE and (La/Sm)N ratios (Figure 2

174

and Figure 3). However, several samples yield REE data that are similar to those of

175

the northern and southern Taklimakan Desert, indicating a potential contribution of

176

Taklimakan Desert dust to the Laohugou basin (Figure 2 and Figure 3). Furthermore,

177

the samples have lower (La/Yb)N and L/HREE ratios, but higher (Gd/Yb)N ratios,

178

than the western Tibetan Plateau (TP), suggesting that it contributes little to the

179

glacier surface dust loading at the study site. However, REE composition of glacier

180

surface dust is similar to the Qaidam Basin, Tengger and Badain Jaran Deserts and the

181

eastern TP with respect to L/HREE, (Gd/Yb)N, (La/Sm)N and (La/Yb)N. Additionally,

182

one of the glacial dust samples possesses a distinct REE signature compared to the

183

above deserts and the TP, which potentially implies other unknown dust sources.

184

3.2 Sr-Nd compositions

185

Isotopes of Sr-Nd are considered to be the most effective and reliable indicators for

186

tracing dust source. Generally, Sr isotopes are easily altered by weathering and wind

187

sorting during transportation and deposition (Chen et al., 2011). The Sr isotopes are

188

also weakly affected by the reaction of dust with acid aerosols during atmospheric

189

transportation and by acid leaching during pretreatments (Meyer et al., 2011;

190

Revel-Rolland et al., 2006). In this work, an acid leaching pretreatment was used for

191

mineral cryoconites formed on the glaciers of the TP in order to remove carbonates

192

(Wu et al., 2010; Schettler et al., 2009). According to a previous study on the TP (Wu

193

et al., 2010), the carbonate content of dust deposited onto glaciers is very low, which

194

suggests that the effect of acid leaching on Sr isotopic composition is negligible. It is

195

noteworthy that Sr isotopic compositions are heavily dependent on grain size (Dasch,

196

1969; Chen et al., 2007; Feng et al., 2009; Újvári et al., 2012). The grain size effect

197

has a significant influence on the

198

size fractions have similar

199

2007). Chen et al. (2007) divided dust from potential source areas into <75µm and

200

<5µm fractions, and Dong et al. (2016) found that most LHG glacier surface dust is

201

<75µm in diameter. Therefore, the studied grain sizes of the potential dust sources and

AC C

EP

TE D

M AN U

SC

RI PT

173

87

87

Sr/86Sr ratio of particles <2µm, while other grain

Sr/86Sr compositions to the bulk size range (Chen et al.,

7

ACCEPTED MANUSCRIPT 143

Nd/144Nd isotopes

glacier surface dust are similar. In a contrast with Sr isotopes,

203

experience limited alteration during the processes of transportation, deposition and

204

eluviation (Chen et al., 2011). Therefore, our discussion will principally focus on the

205

comparison of εNd(0) values of dust samples and the deserts. The Sr-Nd isotopic

206

signatures vary widely, with 87Sr/86Sr ratios of 0.715324 to 0.723112 and εNd(0) values

207

of -14.96 to -9.09 (Figure 4). The isotopic composition of glacier surface dust is more

208

radiogenic than that of the Ordos Plateau (the Hobq and Mu Us Deserts) with εNd(0)

209

values from -16.3 to -10.5, but is lower than the Gurbantunggut Desert with εNd(0)

210

values from -6.3 to -1.2. Some samples from the LHG Glacier No.12 are

211

geochemically similar to the deserts on the northern margin of the TP (the Qaidam,

212

Badain Jaran, and Tengger Deserts), which have εNd(0) values ranging from -12.8 to

213

-7.4 and

214

similar to the local soil, indicating that this could be the primary source of glacier dust.

215

It is noteworthy that different regions within a desert have dramatically different

216

provenance and geochemical characteristics. Nie et al. (2015) and Stevens et al. (2013)

217

revealed different provenances for the western and eastern Mu Us Desert. Therefore, a

218

list of sampling sites of the potential source areas is presented in Table 2. The upper

219

reach of the Yellow River shares similar geochemical properties to the western Mu Us

220

Desert. Thus, we infer that upper reach Yellow River sediments are a potential dust

221

source for the glacier (Nie et al., 2015).

222

3.3 Principal component analysis (PCA) for REE composition in surface dust

223

Principal component analysis (PCA) is a well-established multivariate statistical

224

method that reduces dimensionality of the data to produce a new set of variables while

225

retaining the features of the dataset (Jolliffe, 2002). This is useful for further analysis

226

of the geochemical composition of dust with a relatively complex source. A

227

mathematical algorithm in SPSS 22.0 was used to describe the similarities between

228

dust sink and potential source areas (Du et al., 2015). In this study, three principle

229

components (PCs) were extracted using SPSS 22.0, yielding a 56.0%, 21.2% and 17.4%

230

variance of PC1, PC2 and PC3, respectively, and an eigenvalue higher than 1 (Figure

Sr/86Sr ratios from 0.713 to 0.722. However, the remaining samples are

AC C

EP

TE D

87

M AN U

SC

RI PT

202

8

ACCEPTED MANUSCRIPT 5). The first three PCs together account for a variance of 94.6% (Table 3). The

232

loadings of (La/Sm)N, (La/Yb)N, L/HREE and Ce/Yb are higher than 0.839, except for

233

(Gd/Yb)N and Eu/Yb in the PC1 column. The (La/Sm)N, L/HREE and Ce/Yb loadings

234

for PC2 are negative, and the absolute values of (Gd/Yb)N and Eu/Yb are significantly

235

greater than 0.653 (Table 4). Using these results, the first two PCs are identified as

236

possessing the original characteristics of both the studied samples and potential source

237

regions. The PCA1 scores are negative for the Qaidam, Tengger, Badain Jaran Deserts

238

and eastern TP, indicating that these deserts and the eastern TP are the major sources

239

of surface dust deposited onto LHG glacier No.12. In contrast, the PCA1 scores are

240

positive for the Taklimakan Desert, suggesting that it is a minor contributor to the

241

glacier surface dust (Figure 5).

242

3.4 Discussion of the possible sources of glacier surface dust

243

Geochemical composition (Sr-Nd isotope and REEs) is generally a highly effective

244

and reliable dust source tracer. Samples from LHG glacier No.12 are distinct from the

245

Mu Us and Hobq Deserts, with very different REE parameters (higher (Gd/Yb)N and

246

lower Eu/Eu* and L/HREE) (Figure 2 and Figure 3). The Sr-Nd isotopic compositions

247

of the samples show variable εNd(0) values that are higher than the εNd(0) values

248

(-16.3 to -10.9) of the Mu Us and Hobq Deserts (Honda et al., 2004; Rao et al., 2008;

249

Yang et al., 2007) (Figure 4). Both deserts are located to the northeast of LHG glacier

250

No.12 and are perennially dominated by northwesterly and westerly winds. It is

251

therefore inferred that the Mu Us and Hobq Deserts could not be the source of surface

252

dust in the study area.

SC

M AN U

TE D

EP

AC C

253

RI PT

231

Deserts on the northern margin of the TP include the Qaidam, Badain Jaran and

254

Tengger Deserts. Figure 3 shows that some or all samples have very similar REE

255

signatures to the Qaidam, Badain Jaran and Tengger Deserts, but only near or just

256

within the Taklimakan Desert field. Furthermore, Sr-Nd isotopic compositions show

257

that the samples collected at LHG glacier No.12 resemble the Qaidam (-10.2 on

258

average εNd(0) values), Badain Jaran (-9.31 on average εNd(0) values) and Tengger

259

(-8.56 in average εNd(0) values) Deserts in εNd(0) values but can be distinguished from 9

ACCEPTED MANUSCRIPT 87

Sr/86Sr ratios (Figure 4). The study region is

the Taklimakan Desert by its higher

261

close to the Qaidam, Badain Jaran and Tengger Deserts (Figure 1). Additionally, the

262

aeolian deposits in the Badain Jaran Desert are predominantly derived from the Qilian

263

Mountain via fluvial processes, which further supports the Badain Jaran Desert as a

264

surface dust source for the study site (Hu and Yang, 2016). Although the Tengger and

265

Badain Jaran Deserts are generally located downwind of LHG glacier No.12, local

266

circulation in both deserts may transport dust to the glacier. Back trajectory analyses

267

of air masses support this interpretation. These results confirm that the Qaidam,

268

Badain Jaran and Tengger Deserts are the major dust sources for LHG glacier No.12.

269

However, Figure 4 and Figure 5 show that the Taklimakan Desert is a minor

270

contributor to dust composition. The LHG glacier No.12 is located at a high altitude

271

(>4200 m asl) in the northeastern TP, whereas the Taklimakan desert is adjacent to the

272

northwestern TP. Dust storm events in the Tarim Basin (Taklimakan Desert) occur

273

frequently and with a longer duration than in other areas, with dust emissions from the

274

desert accounting for 21% of all Asian dust emissions (Zhang et al., 2003; Wang et al.,

275

2005). Satellite observations indicate that dust layers emerge most frequently at

276

approximately 4 to 7 km a.s.l. Portions of dust storms occurring in the Taklimakan

277

Desert can be lifted to the level of the TP by westerly winds, which are transported to

278

LHG glacier No.12, while the remaining storm components are blocked by the TP

279

(approximately 3 to 6 km a.s.l.). However, dust emissions from the Qaidam, Badain

280

Jaran and Tengger Deserts amount to 31% of total Asian dust emissions, which is

281

greater than that of the Taklimakan Desert (Zhang et al., 2003). Therefore, the Qaidam,

282

Badain Jaran and Tengger Deserts are major sources for dust deposited on the study

283

glacier, and the Taklimakan Desert is a minor source. The eastern TP and local soil are

284

also major dust sources, judging from their similarity to REE parameters (Eu/Eu*,

285

L/HREE, (Gd/Yb)N, (La/Sm)N) and to Sr-Nd isotopic compositions of samples

286

collected from LHG glacier No.12 (Figure 4 and Figure 5). Although the Tengger and

287

the Badain Jaran Deserts are located downwind of LHG glacier No.12, the

288

near-surface atmospheric circulation in both deserts may transport dust to the alpine

289

glacier area. Air mass back trajectory confirms this result. The Hysplit4 back

AC C

EP

TE D

M AN U

SC

RI PT

260

10

ACCEPTED MANUSCRIPT trajectory model (http://ready.arl.noaa.gov/) indicates that dust on LHG glacier No.12

291

is mainly from the Qaidam, Badain Jaran, and Tengger Deserts as well as the

292

Taklimakan Desert. This is confirmed by air mass back trajectory from the north and

293

from local wind circulation (Figure 6).

294

4. Conclusions

295

Using REEs and Sr-Nd isotope geochemical tracers, this study investigates the

296

provenance of surface dust on LHG glacier No.12, which is located in a dust source

297

area of east-central Asia. The REE characteristics of the surface dust vary widely but

298

are distinguished from the Mu Us and Hobq Deserts by the lower Eu/Eu* and

299

L/HREE and higher (Gd/Yb)N of those deserts. One sample from the study site is

300

similar to the Taklimakan Desert, while the remainder differ in that they possess lower

301

(La/Yb)N, L/HREE and (La/Sm)N ratios. However, the REE characteristics of glacier

302

surface dust are similar to that of the Qaidam Basin, Tengger, and Badain Jaran

303

Deserts and the eastern TP. The Sr-Nd isotopic signatures of the samples possess great

304

variability, ranging from 0.715324 to 0.723112 in 87Sr/86Sr ratios and -14.96 to -9.09

305

in εNd(0) values. These values are more radiogenic than the Ordos Plateau, which has

306

εNd(0) values from -16.3 to -10.5 but are lower than the Gurbantunggut Desert, with

307

εNd(0) values from -6.3 to -1.2.

TE D

M AN U

SC

RI PT

290

Our data clearly show that dust sample characteristics from LHG Glacier No.12 are

309

somewhat close to those of deserts on the northern margin of the Tibetan Plateau

310

(including the Qaidam, Badain Jaran, and Tengger Deserts), ranging from -12.8 to

311

-7.4 in εNd(0) values and 0.713 to 0.722 in

312

geochemistry can be attributed to the local soil surrounding LHG glacier No.12. It is

313

therefore inferred that the glacier surface dust may be derived from the Qaidam,

314

Badain Jaran, Tengger Deserts and eastern TP crust, as well as local soil, while the

315

Taklimakan Desert may have contributed little dust.

316

Acknowledgments

317

This work was funded by the National Natural Science Foundation of China

318

(41421061, 41671062), the Chinese Academy of Sciences (KJZD-EW-G03-04), and

AC C

EP

308

11

87

Sr/86Sr. Much of the remaining dust

ACCEPTED MANUSCRIPT the State Key Laboratory of Cryosphere Sciences (SKLCS-ZZ-2016). The authors

320

also would like to thank the summer 2014 field work team on the Tibetan Plateau for

321

their logistical field work. We also thank anonymous reviewers and the Editor, Dr.

322

Michael Kersten, for their helpful comments and suggestions.

323

References

324

Bauer S E, Balkanski Y, Schulz M, et al., 2004. Global modeling of heterogeneous

325

chemistry on mineral aerosol surfaces: Influence on tropospheric ozone chemistry and

326

comparison to observations. Journal of Geophysical Research: Atmospheres. 109(D2).

327

DOI: 10.1029/2003JD003868.

328

Chen J, Li G, Yang J, Rao W, Lu H, Balsam W, Sun Y, Ji J, 2007. Nd and Sr isotopic

329

characteristics of Chinese deserts: implications for the provenances of Asian dust.

330

Geochimica et Cosmochimica Acta. 71(15): 3904-3914.

331

Chen J, Li G J, 2011. Geochemical studies on the source region of Asian dust. Science

332

China Earth Sciences. 54(9): 1279-1301.

333

Dasch E J, 1969. Strontium isotopes in weathering profiles, deep-sea sediments, and

334

sedimentary rocks. Geochimica et Cosmochimica Acta. 33(12): 1521-1552.

335

Dentener F J, Carmichael G R, Zhang Y, et al., 1996. Role of mineral aerosol as a

336

reactive surface in the global troposphere. Journal of Geophysical Research:

337

Atmospheres. 101(D17): 22869-22889.

338

Dong Z, Qin D, Chen J, et al., 2014. Physicochemical impacts of dust particles on

339

alpine glacier meltwater at the Laohugou Glacier basin in western Qilian Mountains,

340

China. Science of the Total Environment. 493: 930-942.

341

Dong Z, Kang S, Qin X, et al., 2015. New insights into trace elements deposition in

342

the snow packs at remote alpine glaciers in the northern Tibetan Plateau, China.

343

Science of the Total Environment. 529: 101-113.

344

Dong Z, Kang S, Qin D, et al., 2016. Provenance of cryoconite deposited on the

345

glaciers of the Tibetan Plateau: new insights from Nd‐Sr isotopic composition and

AC C

EP

TE D

M AN U

SC

RI PT

319

12

ACCEPTED MANUSCRIPT size

distribution.

Journal

of

Geophysical

Research:

Atmospheres.

DOI:

347

10.1002/2016JD024944.

348

Di Mauro B, Fava F, Ferrero L, et al., 2015. Mineral dust impact on snow radiative

349

properties in the European Alps combining ground, UAV, and satellite observations.

350

Journal of Geophysical Research: Atmospheres. 120(12): 6080-6097.

351

Du W., Qin X., Liu Y. et al., 2008. Variation of the Laohugou Glacier No. 12 in the

352

Qilian Mountains. Journal of Glaciology and Geocryology. 30(3): 373-379. (In

353

Chinese).

354

Du Z, Xiao C, Liu Y, et al., 2015. Geochemical characteristics of insoluble dust as a

355

tracer in an ice core from Miaoergou Glacier, east Tien Shan. Global and Planetary

356

Change. 127: 12-21. 5

357

Feng, J.L., Zhu, L.P., Zhen, X.L., Hu, Z.G., 2009. Grain size effect on Sr and Nd

358

isotopic compositions in eolian dust: implications for tracing dust provenance and Nd

359

model age. Geochemical Journal 43, 123–131.

360

Ferrat M, Weiss D J, Strekopytov S, et al., 2011. Improved provenance tracing of

361

Asian dust sources using rare earth elements and selected trace elements for

362

palaeomonsoon studies on the eastern Tibetan Plateau. Geochimica et Cosmochimica

363

Acta. 75(21): 6374-6399.

364

Gabbi J, Huss M, Bauder A, et al., 2015. The impact of Saharan dust and black carbon

365

on albedo and long-term mass balance of an Alpine glacier. The Cryosphere. 9(4):

366

1385-1400.

367

Grousset F E, Biscaye P E, 2005. Tracing dust sources and transport patterns using Sr,

368

Nd and Pb isotopes. Chemical Geology. 222(3): 149-167.

369

Henderson, P. (Ed.), 1984. Rare Earth Element Geochemistry. Elsevier Science,

370

Amsterdam.

371

Honda M, Yabuki S, Shimizu H, 2004. Geochemical and isotopic studies of aeolian

372

sediments in China. Sedimentology. 51(2): 211-230.

AC C

EP

TE D

M AN U

SC

RI PT

346

13

ACCEPTED MANUSCRIPT Hu F, and Yang X, 2016. Geochemical and geomorphological evidence for the

374

provenance of aeolian deposits in the Badain Jaran Desert, northwestern China.

375

Quaternary Science Reviews. 131: 179-192.

376

Jolliffe I, 2002. Principal component analysis. John Wiley & Sons, Ltd.

377

Kaspari S, Painter T H, Gysel M, et al., 2014Seasonal and elevational variations of

378

black carbon and dust in snow and ice in the Solu-Khumbu, Nepal and estimated

379

radiative forcings. Atmospheric Chemistry and Physics. 14(15): 8089-8103.

380

Kaspari S, McKenzie Skiles S, Delaney I, et al., 2015.Accelerated glacier melt on

381

Snow Dome, Mount Olympus, Washington, USA, due to deposition of black carbon

382

and

383

Atmospheres.120(7): 2793-2807.

384

Kwon Y I, Lee S G, Yu K M, et al., 2004.Geochemical characteristics of the surface

385

sediments of Ordos and Alashan deserts, China: eolian sediment provenance and

386

fingerprint. Journal of Geological Society of Korea. 40: 119-132.

387

Li C, Kang S, Zhang Q, 2009. Elemental composition of Tibetan Plateau top soils and

388

itseffect on evaluating atmospheric pollution transport. Environmental pollution

389

157(8): 2261-2265.

390

Maher B A, Mutch T J, Cunningham D, 2009. Magnetic and geochemical

391

characteristics of Gobi Desert surface sediments: Implications for provenance of the

392

Chinese Loess Plateau. Geology, 37(3): 279-282.

393

Meyer I, Davies G R, Stuut J B W, 2011. Grain size control on Sr-Nd isotope

394

provenance studies and impact on paleoclimate reconstructions: An example from

395

deep-sea sediments offshore NW Africa. Geochemistry, Geophysics, Geosystems

396

12(3). DOI: 10.1002/2016JD024944.

397

Nakano T, Yokoo Y, Nishikawa M, Koyanagi H, 2004. Regional Sr–Nd isotopic ratios

398

of soil minerals in northern China as Asian dust fingerprints. Atmospheric

399

Environment, 38(19): 3061-3067.

wildfire.

Journal

of

Geophysical

Research:

M AN U

from

TE D

dust

AC C

EP

mineral

SC

RI PT

373

14

ACCEPTED MANUSCRIPT Nie J, Stevens T, Rittner M, et al., 2015, Loess plateau storage of northeastern Tibetan

401

plateau-derived yellow river sediment. Nature communications, 6. DOI: 10.1038

402

/ncomms9511

403

Nie J, Horton B K, Saylor J E, et al., 2012. Integrated provenance analysis of a

404

convergent retroarc foreland system: U–Pb ages, heavy minerals, Nd isotopes, and

405

sandstone compositions of the Middle Magdalena Valley basin, northern Andes,

406

Colombia. Earth Science Reviews, 110(1): 111-126.

407

Piper D Z, Bau M, 2013. Normalized rare earth elements in water, sediments, and

408

wine: identifying sources and environmental redox conditions. American Journal of

409

Analytical Chemistry .DOI:10.4236/ajac.2013.410A1009

410

Ramanathan, V. and Carmichael, G. R, 2008. Global and regional climate changes due

411

to black carbon, Nat. Geosci. 1, 221-227.

412

Rao W, Chen J, Yang J, Ji J, Li G, Tan H, 2008. Sr-Nd isotopic characteristics of

413

eolian deposits in the Erdos Desert and Chinese Loess Plateau: Implications for their

414

provenances. Geochemical Journal. 42(3): 273-282.

415

Revel-Rolland M, De Deckker P, Delmonte B, et al., 2006. Eastern Australia: a

416

possible source of dust in East Antarctica interglacial ice. Earth and Planetary Science

417

Letters. 249(1): 1-13.

418

Rosenfeld D, Rudich Y, Lahav R, 2001. Desert dust suppressing precipitation: A

419

possible desertification feedback loop. Proceedings of the National Academy of

420

Sciences, 98(11), 5975-5980.

421

Sokolik I N, Toon O B, 1999. Incorporation of mineralogical composition into models

422

of the radiative properties of mineral aerosol from UV to IR wavelengths. Journal of

423

Geophysical Research, 104(D8), 9423-9444.

424

Stevens T, Carter A, Watson T P, et al., 2013. Genetic linkage between the Yellow

425

River, the Mu Us desert and the Chinese Loess Plateau. Quaternary Science Reviews,

426

78: 355-368.

AC C

EP

TE D

M AN U

SC

RI PT

400

15

ACCEPTED MANUSCRIPT Sullivan R C, Guazzotti S A, Sodeman D A, et al., 2007. Direct observations of the

428

atmospheric processing of Asian mineral dust. Atmospheric Chemistry and Physics,

429

7(5), 1213-1236.

430

Tepe N, Bau M, 2015. Distribution of rare earth elements and other high field strength

431

elements in glacial meltwater and sediments from the western Greenland Ice Sheet:

432

Evidence for different sources of particles and nanoparticles. Chemical Geology, 412:

433

59-68.

434

Xu J, Yu G, Kang S, et al., 2012. Sr-Nd isotope evidence for modern aeolian dust

435

sources in mountain glaciers of western China. Journal of Glaciology, 58(211):

436

859-865.

437

Yang X, Liu Y, Li C, et al., 2007a. Rare earth elements of aeolian deposits in Northern

438

China and their implications for determining the provenance of dust storms in Beijing.

439

Geomorphology, 87(4): 365-377.

440

Yang X, Zhu B, White P D, 2007b. Provenance of aeolian sediment in the Taklimakan

441

Desert of western China, inferred from REE and major-elemental data. Quaternary

442

International, 175(1), 71-85.

443

Yang J, Chen J, Rao W, et al., 2007. Isotopic partition characteristics of Chinese

444

deserts. Geochimica, 5, 84-92. (In Chinese)

445

Újvári, G., Varga, A., Ramos, F.C., Kovács, J., Németh, T., Stevens, T., 2012.

446

Evaluating the use of clay mineralogy, Sr–Nd isotopes and zircon U–Pb ages in

447

tracking dust provenance: An example from loess of the Carpathian Basin. Chemical

448

Geology, 304–305.

449

Wang S, Wang J, Zhou Z, et al., 2005. Regional characteristics of three kinds of dust

450

storm events in China. Atmospheric Environment, 39(3), 509-520.

451

Wang X, Doherty S J, Huang J, 2013. Black carbon and other light‐absorbing

452

impurities in snow across Northern China. Journal of Geophysical Research:

453

Atmospheres, 118(3): 1471-1492.

AC C

EP

TE D

M AN U

SC

RI PT

427

16

ACCEPTED MANUSCRIPT Wu G, Zhang C, Zhang X, et al., 2010. Sr and Nd isotopic composition of dust in

455

Dunde ice core, Northern China: implications for source tracing and use as an

456

analogue of long-range transported Asian dust. Earth and Planetary Science Letters,

457

299(3): 409-416.

458

Wu G, Zhang C, Zhang X, et al., 2015. The environmental implications for dust in

459

high-alpine snow and ice cores in Asian mountains. Global and Planetary Change, 124:

460

22-29.

461

Zhang X Y, Gong S L, Zhao T L, et al., 2003. Sources of Asian dust and role of

462

climate change versus desertification in Asian dust emission. Geophysical Research

463

Letters. 30(24).

464

Zhang, H, 1997. The Superficial Elemental Geochemistry and Theoretical Principles.

465

Lanzhou University Press, Lanzhou, pp. 130–131 (in Chinese).

466

Zhang X L, Wu G J, Zhang C L, et al., 2015. What is the real role of iron oxides in the

467

optical properties of dust aerosols? Atmospheric Chemistry and Physics, 15(21):

468

12159-12177.

471 472 473 474

SC

M AN U

TE D EP

470

AC C

469

RI PT

454

475 476 477 478 17

ACCEPTED MANUSCRIPT 479 480

Tables Table 1 Sampling of snow and cryoconite dust from Laohugou Glacier No.12. Altitude Sample no.

Sample data

Depth (cm)

Sample type

(m a.s.l.) 2014/7/29

5

cryoconite

LHG30-6

4592

2014/7/30

5

cryoconite

LHG29-4

4450

2014/7/29

5

cryoconite

LHG29-3

4386

2014/7/29

5

cryoconite

LHG30-4

4698

2014/7/30

5

LHG30-1

4849

2014/7/30

5

LHG8-4

4850

2014/8/8

5

LHG-01

5040

2012/6/21

120

LHG-02

5040

2012/6/21

120

LHG-03

5040

2012/6/21

LHG-04

5040

2012/6/21

LHG-05

5040

2012/6/21

LHG-06

5040

RI PT

4590

cryoconite cryoconite cryoconite snow pit

SC

snow pit snow pit

95

snow pit

95

snow pit

M AN U

120

2012/6/21

95

snow pit

Table 2 Sampling sites for dust Sr-Nd isotopic and REE compositions in the arid dust source regions of China. Location

Parameters

References

Gurbantunggut Desert

west of the desert

Sr-Nd isotope/REE

Honda et al., 2004

45.06-45.6N, 87.46-89.11E

Sr-Nd isotope

Chen et al., 2007

37.45-37.68N,104.97-105.5E

Sr-Nd isotope

Chen et al., 2007

38.35-38.64N, 102.33-105E

Sr-Nd isotope

Honda et al., 2004

39N,103.5E

REE

Ferrat et al., 2011

38.34-39N, 102.5-102.54E

Sr-Nd isotope

Nakano et al., 2004

39.4-42.02N, 100.63-103.23E

Sr-Nd isotope

Chen et al., 2007

39.2N,103E

REE

Ferrat et al., 2011

36.8-37.99N, 93.75-97.69E

Sr-Nd isotope

Chen et al., 2007

36N, 95E

REE

Ferrat et al., 2011

whole range

Sr-Nd isotope/REE

Honda et al., 2004

38.5-39.15N, 107.56-108.5E

Sr-Nd isotope

Nakano et al., 2004

38.22-40.33N,108.08-111.35E

Sr-Nd isotope

Chen et al., 2007

40.05-41.45N, 106.77-109.7E

Sr-Nd isotope

Chen et al., 2007

39.65-41.45N, 107.02-111.35E

Sr-Nd isotope

Rao et al., 2008

whole range

REE

Kwon et al., 2004

36.41-39.69N, 81.84-94.35E

Sr-Nd isotope

Chen et al., 2007

37.5-40N, 77.5-94.8E

Sr-Nd isotope

Honda et al., 2004

Gobi

40.43-43.7N, 105-114.5E

Sr-Nd isotope

Nakano et al., 2004

western Tibetan Plateau

29.5-37.5N, 87.5-79.5E

REE

Li et al., 2009

Tengger Desert

EP

Badain Jaran Desert

TE D

Sources

Qaidam Basin

AC C

481 482 483

LHG29-1

Mu Us Desert

Hobq Desert

Taklimakan Desert

18

ACCEPTED MANUSCRIPT REE

Ferrat et al., 2011

Northern Taklimakan Desert

42N,83E

REE

Yang et al., 2007b

Southern Taklimakan Desert

38N,81.5E

REE

Ferrat et al., 2011

Table 3 Total variance explained in principal component analysis. Eigenvalue

Variance%

Cumulative%

1.000

3.362

56.033

56.033

2.000

1.270

21.167

3.000

1.043

17.390

4.000

0.228

3.805

5.000

0.079

1.317

6.000

0.017

0.286

RI PT

Component

77.200 94.591

98.396 99.713

SC

486 487

32N,101E

100.000

Table 4 Loadings of each element upon each of three significant principal components.

M AN U

484 485

East of the Tibetan Plateau

Component

Index 1

3

-0.284

0.192

0.842

-0.492

0.653

0.739

0.206

0.019

0.884

(Gd/Yb)N

0.130

Eu/Yb

0.077

(La/Yb)N

0.970

L/HREE

0.956

-0.108

0.186

Ce/Yb

0.839

-0.006

-0.428

TE D

(La/Sm)N

EP

488 489 490 491

2

Figure Captions

493

Figure 1 Location of Laohugou Glacier No.12, sampled for surface dust deposition.

494

Figure 2 The REE composition (correlation between Gd/Yb and Eu/Eu*, and La/Yb)

495

of surface dust from LHG glacier No.12 and from potential source regions, including

496

the northern and southern Taklimakan Desert, Junggar Basin, eastern and western TP,

497

Qaidam Basin, Tengger Desert, Badain Jaran Desert, Mu Us Desert and Hobq Desert.

498

Figure 3 The REE signatures (correlations between La/Sm and L/HREE, La/Yb and

499

L/HREE) of surface dust from LHG glacier No.12.

AC C

492

19

ACCEPTED MANUSCRIPT Figure 4 Comparison of Sr-Nd isotopic compositions of surface dust from Laohugou

501

Glacier No.12 with the Gobi Desert and deserts from northern and northwestern

502

China. Dotted areas represent d<5 µm fractions of the Chinese deserts, and the

503

remaining data are the d<75 µm fractions of dust particles in arid regions. Some data

504

are from Xu et al., 2012.

505

Figure 5 The PCA scores of each site in three principal components, indicating

506

potential dust sources.

507

Figure 6 Three-day backward trajectories of LHG Glacier No.12 during the

508

high-frequency dust storm season (March to July) in 2012 and 2014, showing the

509

potential dust transport to the Qilian Mountains glacier area from surrounding regions.

SC

RI PT

500

AC C

EP

TE D

M AN U

510

20

AC C

EP

TE D

M AN U

SC

RI PT

ACCEPTED MANUSCRIPT

AC C

EP

TE D

M AN U

SC

RI PT

ACCEPTED MANUSCRIPT

AC C

EP

TE D

M AN U

SC

RI PT

ACCEPTED MANUSCRIPT

AC C

EP

TE D

M AN U

SC

RI PT

ACCEPTED MANUSCRIPT

AC C

EP

TE D

M AN U

SC

RI PT

ACCEPTED MANUSCRIPT

AC C

EP

TE D

M AN U

SC

RI PT

ACCEPTED MANUSCRIPT

ACCEPTED MANUSCRIPT Highlights: : 1. We present new geochemical data of surface dust on glacier in Qilian Mountains 2. Glacier dust were mainly from the Qaidam, Badain Jaran and Tengger Deserts

AC C

EP

TE D

M AN U

SC

RI PT

4. Near surface circulation may transport arid dust from downwind areas