Characteristics of Total Gaseous Mercury (TGM) Concentrations in An

1 Supporting Information for 2 3 4 Characteristics of total gaseous mercury (TGM) concentrations in an 5 industrial complex in southern Korea: Impacts from local sources 6 7 Yong-Seok Seo1, 2, Seung-Pyo Jeong1, Thomas M. Holsen3, Young-Ji Han4, Eunhwa Choi5, Eun 8 Ha Park1, Tae Young Kim1, Hee-Sang Eum1, Dae Gun Park1, Eunhye Kim6, Soontae Kim6, 9 Jeong-Hun Kim7, Jaewon Choi8, Seung-Muk Yi1, 2, * 10 11 1Department of Environmental Health, Graduate School of Public Health, Seoul National 12 University, 1 Gwanak, Gwanak-ro, Gwanak-gu, Seoul 151-742, South Korea 13 14 2Institute of Health and Environment, Seoul National University, 1 Gwanak, Gwanak-ro, 15 Gwanak-gu, Seoul 151-742, South Korea 16 17 3Department of Civil and Environmental Engineering, Clarkson University, Potsdam, 18 NY13699, USA 19 20 4Department of Environmental Science, Kangwon National University, 192-1, Hyoja-2-dong, 21 Chuncheon, Kangwondo, 200-701, South Korea 22 23 5Asian Institute for Energy, Environment & Sustainability, Seoul National University, 1 24 Gwanak-ro, Gwanak-gu, Seoul 151-742, South Korea 25 26 6Department of Environmental, Civil and Transportation Engineering, Ajou University, 27 Woncheon-dong, Yeongtong-gu, Suwon, 443-749, South Korea 28 29 7Division of Air Pollution Engineering, Department of Climate and Air Quality Research, 30 National Institute of Environmental Research, Hwangyong-ro 42, Seogu, Incheon, 404-708, 31 South Korea 32 33 8University of Pennsylvania, Philadelphia, PA19104, USA 34 35 36 37 38 39 40 41 42 43 *Address correspondence to Dr. Seung-Muk Yi, Graduate School of Public Health, Seoul 44 National University, 1 Gwanak, Gwanak-ro, Gwanak-gu, Seoul 151-742, South Korea 45 E-mail) [email protected] 46 Telephone) 82-2-880-2736 47 Fax) 82-2-745-9104

49 Fig. S1. Frequency of counts of measured wind direction occurrence by season in this 50 study. 51

53 Fig. S2. Sectoral contribution of emissions of (a) South Korea, (b) Gyeongsangbuk-do 54 and (c) Pohang for CO, NOx, SOx, TSP VOC and NH3. 55

56 Sectoral contribution of emissions

57 In South Korea, the NOx emissions were highest, followed by VOC, CO, SOx, NH3, TSP,

58 PM10 and PM2.5 (Fig. S2(a)). In Gyeongsangbuk-do, the NOx emissions were highest,

59 followed by CO, VOC, SOx, NH3, and TSP, PM10 and PM2.5 which is similar trend to South

60 Korea (Fig. S2(b)). However, Pohang showed a different pattern with the highest NOx

61 emissions, followed by SOx, VOC, CO, TSP, PM10, PM2.5 and NH3 (Fig. S2(c)).

62 Point source (combustion in energy industries + combustion in manufacturing industries +

63 production processes + waste treatment and disposal) in South Korea accounted for

64 1,226,609 tons (34.6% of total emissions in South Korea) of the air pollutants.

65 Gyeongsangbuk-do has a similar trend with 106,439 tons (35.8% of total emissions in

66 Gyeongsangbuk-do) of the air pollutants. However, Pohang has a significantly high

67 contribution with 56,144 tons (69.2% of total emissions in Pohang) of the air pollutants.

68 Area source (non-industrial combustion + storage and distribution of fuels + solvent

69 utilization + agriculture + other area sources) in South Korea accounted for 1,055,461 tons

70 (29.8% of total emissions in South Korea) of the air pollutants. Gyeongsangbuk-do has a

71 similar trend with 90,982 tons (30.6% of total emissions in Gyeongsangbuk-do) of the air

72 pollutants. However, Pohang has a less contribution with 6,903 tons (8.5% of total emissions

73 in Pohang) of the air pollutants.

74 Mobile source (road transport + non-road transport) in South Korea accounted for

75 1,261,782 tons (35.6% of total emissions in South Korea) of the air pollutants.

76 Gyeongsangbuk-do has a similar contribution with 99,709 tons (33.6% of total emissions in

77 Gyeongsangbuk-do) of the air pollutants. Pohang also has a lower contribution with 18,048

78 tons (22.3% of total emissions in Pohang) of the air pollutants.

80 Table S1. Source Classification Categories (SCC) in CAPSS. The fugitive dust and 81 biomass were excluded.

Emission SCC1 (11) SCC2 (42) SCC3 (173) characteristics - Public power Combustion in - District heating plants 4 energy industries - Petroleum refining plants - Commercial power - Process furnace Combustion in - Combustion plants 44 manufacturing industries - Other - Processes in other industries - Processes in wood, paper and pulp industries Point source - Processes in inorganic chemical industries - Processes in petroleum industries Production processes 44 - Processes in food and drink industries - Ammonia consumption - Processes in organic chemical industries - Processes in iron and steel industries - Waste incineration Waste treatment and disposal 5 - Other waste treatment - Commercial and institutional plants Non-industrial combustion - Plants in agriculture, forestry and aquaculture 5 - Residential plants Storage and distribution of - Gasoline distribution 3 fuels - Paint application Area source -Electronic Degreaser Solvent utilization 15 - Dry cleaning - Other use of solvents and related activities - Enteric fermentation Agriculture 10 - Cultures with fertilizers - Forest and other vegetation fires Other area sources 3 - Animals - Passenger cars - Light-duty vehicles - Recreational vehicles - Taxis Road transport 18 - Buses - Special purpose vehicles Mobile source - Trucks - Motorcycles - Construction machinery and equipment - Agricultural machinery Non-road transport - Ships 22 - Railways - Aircrafts 82 *The numbers represent the number of sources.

Fig. S3. Frequency distribution of TGM during sampling period. Note that TGM was measured every 5-min.

85 86 Fig. S4. Comparisons of CPF and CBPF plots for TGM and CO higher than average 87 concentration. The radial axes of CPF and CBPF are the probability and the wind 88 speed (m s-1), respectively.

89 90 Fig. S5. The diurnal variations of co-pollutants concentrations and 91 meteorological data during the sampling periods. The error bars represent 92 standard error. 93

40 100

80 30 ) -3 60

20 conc. (ppb) 2 40 NO TGMconc. (ng m 10 20

0 0

Fall (daytime) Fall (daytime) Fall (nighttime) Total (daytime) Fall (nighttime) Total (daytime) Spring (daytime) Winter (daytime) Total (nighttime) Spring (daytime) Winter (daytime) Total (nighttime) Spring (nighttime)Summer (daytime) Winter (nighttime) Spring (nighttime)Summer (daytime) Winter (nighttime) Summer (nighttime) Summer (nighttime) 100 4000

80 3000

2000 conc. (ppb) 3 40 O COconc. (ppb)

1000 20

0 0

Fall (daytime) Fall (daytime) Fall (nighttime) Fall (nighttime) Total (daytime) Spring (daytime) Winter (daytime) Spring (daytime) Winter (daytime) Total (nighttime) Spring (nighttime)Summer (daytime) Winter (nighttime) Spring (nighttime)Summer (daytime) Winter (nighttime) Summer (nighttime) Summer (nighttime) 200 50

40 150 ) -3

g m g 30  100 conc. (ppb) 2 conc. ( conc.

10 20 SO PM 50 10

0 0

10 ℃ ) Temperature ( Temperature

-10

Fall (daytime) Fall (nighttime) Total (daytime) Spring (daytime) Winter (daytime) Total (nighttime) Spring (nighttime)Summer (daytime) Winter (nighttime) Summer (nighttime) 94 95 Fig. S6. Comparison of TGM, co-pollutants and meteorological data between daytime 96 and nighttime. Note that TGM was presented with hourly average concentration.