Diel variation in mercury stable isotope ratios records photoreduction of PM2.5-bound mercury

Qiang Huang, Jiubin Chen, Weilin Huang, John Reinfelder, Pingqing Fu, Shengliu Yuan, Zhongwei Wang, Wei Yuan, Hongming Cai, Hong Ren, Yele Sun, Li He

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Abstract

Mercury (Hg) bound to fine aerosols (PM 2.5 -Hg) may undergo photochemical reaction that causes isotopic fractionation and obscures the initial isotopic signatures. In this study, we quantified Hg isotopic compositions for 56 PM 2.5 samples collected between 15 September and 16 October 2015 from Beijing, China, among which 26 were collected during daytime (between 08:00 and 18:30 LT) and 30 during night (between 19:00 and 07:30 LT). The results show that diel variation was statistically significant (p< 0.05) for Hg content, δ199Hg and δ200Hg, with Hg content during daytime (0.32±0.14 μg g -1 ) lower than at night (0.48±0.24 μg g -1 ) and δ199Hg and δ200Hg values during daytime (mean of 0.26 ±0.40 and 0.09 ±0.06, respectively) higher than during nighttime (0.04 ±0.22 and 0.06 ±0.05, respectively), whereas PM 2.5 concentrations and δ202Hg values showed insignificant (p< &gt;< 0.05) diel variation. Geochemical characteristics of the samples and the air mass backward trajectories (PM 2.5 source related) suggest that diel variation in δ199Hg values resulted primarily from the photochemical reduction of divalent PM 2.5 -Hg, rather than variations in emission sources. The importance of photoreduction is supported by the strong correlations between δ199Hg and (i) δ201Hg (positive, slope Combining double low line 1.1), (ii) δ202Hg (positive, slope Combining double low line 1.15), (iii) content of Hg in PM 2.5 (negative), (iv) sunshine durations (positive) and (v) ozone concentration (positive) observed for consecutive day-night paired samples. Our results provide isotopic evidence that local, daily photochemical reduction of divalent Hg is of critical importance to the fate of PM 2.5 -Hg in urban atmospheres and that, in addition to variation in sources, photochemical reduction appears to be an important process that affects both the particle mass-specific abundance and isotopic composition of PM 2.5 -Hg.

Original languageEnglish (US)
Pages (from-to)315-325
Number of pages11
JournalAtmospheric Chemistry and Physics
Volume19
Issue number1
DOIs
StatePublished - Jan 9 2019

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diel variation
stable isotope
isotopic composition
urban atmosphere
isotopic fractionation
air mass
trajectory
ozone
aerosol
mercury

All Science Journal Classification (ASJC) codes

  • Atmospheric Science

Cite this

Huang, Qiang ; Chen, Jiubin ; Huang, Weilin ; Reinfelder, John ; Fu, Pingqing ; Yuan, Shengliu ; Wang, Zhongwei ; Yuan, Wei ; Cai, Hongming ; Ren, Hong ; Sun, Yele ; He, Li. / Diel variation in mercury stable isotope ratios records photoreduction of PM2.5-bound mercury. In: Atmospheric Chemistry and Physics. 2019 ; Vol. 19, No. 1. pp. 315-325.
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abstract = "Mercury (Hg) bound to fine aerosols (PM 2.5 -Hg) may undergo photochemical reaction that causes isotopic fractionation and obscures the initial isotopic signatures. In this study, we quantified Hg isotopic compositions for 56 PM 2.5 samples collected between 15 September and 16 October 2015 from Beijing, China, among which 26 were collected during daytime (between 08:00 and 18:30 LT) and 30 during night (between 19:00 and 07:30 LT). The results show that diel variation was statistically significant (p< 0.05) for Hg content, δ199Hg and δ200Hg, with Hg content during daytime (0.32±0.14 μg g -1 ) lower than at night (0.48±0.24 μg g -1 ) and δ199Hg and δ200Hg values during daytime (mean of 0.26 ±0.40 and 0.09 ±0.06, respectively) higher than during nighttime (0.04 ±0.22 and 0.06 ±0.05, respectively), whereas PM 2.5 concentrations and δ202Hg values showed insignificant (p< >< 0.05) diel variation. Geochemical characteristics of the samples and the air mass backward trajectories (PM 2.5 source related) suggest that diel variation in δ199Hg values resulted primarily from the photochemical reduction of divalent PM 2.5 -Hg, rather than variations in emission sources. The importance of photoreduction is supported by the strong correlations between δ199Hg and (i) δ201Hg (positive, slope Combining double low line 1.1), (ii) δ202Hg (positive, slope Combining double low line 1.15), (iii) content of Hg in PM 2.5 (negative), (iv) sunshine durations (positive) and (v) ozone concentration (positive) observed for consecutive day-night paired samples. Our results provide isotopic evidence that local, daily photochemical reduction of divalent Hg is of critical importance to the fate of PM 2.5 -Hg in urban atmospheres and that, in addition to variation in sources, photochemical reduction appears to be an important process that affects both the particle mass-specific abundance and isotopic composition of PM 2.5 -Hg.",
author = "Qiang Huang and Jiubin Chen and Weilin Huang and John Reinfelder and Pingqing Fu and Shengliu Yuan and Zhongwei Wang and Wei Yuan and Hongming Cai and Hong Ren and Yele Sun and Li He",
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Diel variation in mercury stable isotope ratios records photoreduction of PM2.5-bound mercury. / Huang, Qiang; Chen, Jiubin; Huang, Weilin; Reinfelder, John; Fu, Pingqing; Yuan, Shengliu; Wang, Zhongwei; Yuan, Wei; Cai, Hongming; Ren, Hong; Sun, Yele; He, Li.

In: Atmospheric Chemistry and Physics, Vol. 19, No. 1, 09.01.2019, p. 315-325.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Diel variation in mercury stable isotope ratios records photoreduction of PM2.5-bound mercury

AU - Huang, Qiang

AU - Chen, Jiubin

AU - Huang, Weilin

AU - Reinfelder, John

AU - Fu, Pingqing

AU - Yuan, Shengliu

AU - Wang, Zhongwei

AU - Yuan, Wei

AU - Cai, Hongming

AU - Ren, Hong

AU - Sun, Yele

AU - He, Li

PY - 2019/1/9

Y1 - 2019/1/9

N2 - Mercury (Hg) bound to fine aerosols (PM 2.5 -Hg) may undergo photochemical reaction that causes isotopic fractionation and obscures the initial isotopic signatures. In this study, we quantified Hg isotopic compositions for 56 PM 2.5 samples collected between 15 September and 16 October 2015 from Beijing, China, among which 26 were collected during daytime (between 08:00 and 18:30 LT) and 30 during night (between 19:00 and 07:30 LT). The results show that diel variation was statistically significant (p< 0.05) for Hg content, δ199Hg and δ200Hg, with Hg content during daytime (0.32±0.14 μg g -1 ) lower than at night (0.48±0.24 μg g -1 ) and δ199Hg and δ200Hg values during daytime (mean of 0.26 ±0.40 and 0.09 ±0.06, respectively) higher than during nighttime (0.04 ±0.22 and 0.06 ±0.05, respectively), whereas PM 2.5 concentrations and δ202Hg values showed insignificant (p< >< 0.05) diel variation. Geochemical characteristics of the samples and the air mass backward trajectories (PM 2.5 source related) suggest that diel variation in δ199Hg values resulted primarily from the photochemical reduction of divalent PM 2.5 -Hg, rather than variations in emission sources. The importance of photoreduction is supported by the strong correlations between δ199Hg and (i) δ201Hg (positive, slope Combining double low line 1.1), (ii) δ202Hg (positive, slope Combining double low line 1.15), (iii) content of Hg in PM 2.5 (negative), (iv) sunshine durations (positive) and (v) ozone concentration (positive) observed for consecutive day-night paired samples. Our results provide isotopic evidence that local, daily photochemical reduction of divalent Hg is of critical importance to the fate of PM 2.5 -Hg in urban atmospheres and that, in addition to variation in sources, photochemical reduction appears to be an important process that affects both the particle mass-specific abundance and isotopic composition of PM 2.5 -Hg.

AB - Mercury (Hg) bound to fine aerosols (PM 2.5 -Hg) may undergo photochemical reaction that causes isotopic fractionation and obscures the initial isotopic signatures. In this study, we quantified Hg isotopic compositions for 56 PM 2.5 samples collected between 15 September and 16 October 2015 from Beijing, China, among which 26 were collected during daytime (between 08:00 and 18:30 LT) and 30 during night (between 19:00 and 07:30 LT). The results show that diel variation was statistically significant (p< 0.05) for Hg content, δ199Hg and δ200Hg, with Hg content during daytime (0.32±0.14 μg g -1 ) lower than at night (0.48±0.24 μg g -1 ) and δ199Hg and δ200Hg values during daytime (mean of 0.26 ±0.40 and 0.09 ±0.06, respectively) higher than during nighttime (0.04 ±0.22 and 0.06 ±0.05, respectively), whereas PM 2.5 concentrations and δ202Hg values showed insignificant (p< >< 0.05) diel variation. Geochemical characteristics of the samples and the air mass backward trajectories (PM 2.5 source related) suggest that diel variation in δ199Hg values resulted primarily from the photochemical reduction of divalent PM 2.5 -Hg, rather than variations in emission sources. The importance of photoreduction is supported by the strong correlations between δ199Hg and (i) δ201Hg (positive, slope Combining double low line 1.1), (ii) δ202Hg (positive, slope Combining double low line 1.15), (iii) content of Hg in PM 2.5 (negative), (iv) sunshine durations (positive) and (v) ozone concentration (positive) observed for consecutive day-night paired samples. Our results provide isotopic evidence that local, daily photochemical reduction of divalent Hg is of critical importance to the fate of PM 2.5 -Hg in urban atmospheres and that, in addition to variation in sources, photochemical reduction appears to be an important process that affects both the particle mass-specific abundance and isotopic composition of PM 2.5 -Hg.

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