森林地区PM<sub>2.5</sub>中氨基酸的水平、来源及转化

Abstract
Figure/Table
References
Related Citation (15)

Download: PDF (592 KB) HTML (1 KB)
Export: BibTeX | EndNote (RIS)

Abstract In this study, PM_2.5 samples were collected in a forest area of Nanchang (28.75°N, 115.71°E) in spring, The concentrations of combined amino acids (CAAs), free amino acids (FAAs) and the nitrogen isotopes of glycine (Gly) were determined. The result showed that the concentrations of total CAAs and the concentrations of total FAAs were 272.8~4761.5pmol/m³, and 56.4~494.0pmol/m³in the atmospheric aerosols, respectively. The fractional percentage of CAAs, Pro, Gly, Glu, Leu and Ala in the total CAAs were (19.5 ±12.0)%, (19.4 ±10.6)%, (15.3 ±4.9)%, (12.8 ±5.4)% and (9.1 ±1.6)%, respectively. Gly was the most abundant amino acid, accounting for (71.1 ±9.2)% of the total FAAs. However, the fractional percentage of other FAAs was very small (proportion range of 0.1%~14.3%). The proportion of neutral amino acids was much higher in FAAs than that in CAAs, which might be related to the photochemical reaction during long-distance transport. According to the correlations between amino acid and O₃, NO₂ and temperature, we found that the formation of FAAs was associated with atmospheric photochemical processes and thermal reactions in the forest areas. The δ¹⁵N_C_-_Glyvalue (-1.0‰~+17.5‰) and δ¹⁵N_F_-_Gly value (-5.5‰~+13.0‰) in aerosol were close to the δ¹⁵N_Gly value from soil sources, indicating that the main source of amino acids in PM_2.5 might be from soil emission in the forest areas.

Key words： combined amino acids free amino acids PM_2.5 O₃ δ¹⁵N_Gly

Received: 22 May 2020

PACS:

X513

	Service

	E-mail this article
	Add to my bookshelf
	Add to citation manager
	E-mail Alert
	RSS
	Articles by authors
	ZHU Yu-wen
	ZHU Ren-guo
	FANG Xiao-zheng
	PAN Yuan-yuan
	WEN Ze-qun

Cite this article:

ZHU Yu-wen,ZHU Ren-guo,FANG Xiao-zheng等. The levels, sources and atmospheric photochemical processes of amino acids in PM_2.5 in forest areas[J]. CHINA ENVIRONMENTAL SCIENCECE, 2021, 41(1): 81-90.

URL:

http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2021/V41/I1/81

[1]	Zhang Q, Carroll J J, Dixon A J, et al. Aircraft measurements of nitrogen and phosphorus in and around the Lake Tahoe Basin:Implications for possible sources of atmospheric pollutants to Lake Tahoe[J]. Environmental Science & Technology, 2002,36(23):49814989.
[2]	Zhang Q, Anastasio C, Jimenez-Cruz M. Water-soluble organic nitrogen in atmospheric fine particles (PM2.5) from Northern California[J]. Journal of Geophysical Research:Atmospheres, 2002,107(D11):AAC3-1-AAC 3-9.
[3]	Zhang Q, Anastasio C. Chemistry of fog waters in California's Central Valley-Part 3:concentrations and speciation of organic and inorganic nitrogen[J]. Atmospheric Environment, 2001,35(32):5629-5643.
[4]	Cornell S, Mace K, Coeppicus S, et al. Organic nitrogen in Hawaiian rain and aerosol[J]. Journal of Geophysical Research:Atmospheres, 2001,106(D8):7973-7983.
[5]	Weathers K C, Lovett G M, Likens G E, et al. Cloudwater inputs of nitrogen to forest ecosystems in southern Chile:forms, fluxes, and sources[J]. Ecosystems, 2000,3(6):590-595.
[6]	Anastasio C, Mcgregor K G. Photodestruction of dissolved organic nitrogen species in fog waters[J]. Aerosol Science & Technology, 2000,32(2):106-119.
[7]	Chan M N, Choi M Y, Ng N L, et al. Hygroscopicity of water-soluble organic compounds in atmospheric aerosols:Amino acids and biomass burning derived organic species[J]. Environmental Science & Technology, 2005,39(6):1555-1562.
[8]	Szyrmer W, Zawadzki I. Biogenic and anthropogenic sources of ice-forming nuclei:A review[J]. Bulletin of the American Meteorological Society, 1997,78(2):209-228.
[9]	Després V, Huffman J A, Burrows S M, et al. Primary biological aerosol particles in the atmosphere:a review[J]. Tellus B:Chemical and Physical Meteorology, 2012,64(1):15598.
[10]	Matos J T, Duarte R M, Duarte A C. Challenges in the identification and characterization of free amino acids and proteinaceous compounds in atmospheric aerosols:a critical review[J]. TrAC Trends in Analytical Chemistry, 2016,75:97-107.
[11]	Barbaro E, Feltracco M, Cesari D, et al. Characterization of the water soluble fraction in ultrafine, fine, and coarse atmospheric aerosol[J]. Science of the Total Environment, 2019,658:1423-1439.
[12]	Scalabrin E, Zangrando R, Barbaro E, et al. Amino acids in Arctic aerosols[J]. Atmospheric Chemistry and Physics, 2012,12(21):1045310463.
[13]	Wedyan M A, Preston M R. The coupling of surface seawater organic nitrogen and the marine aerosol as inferred from enantiomer-specific amino acid analysis[J]. Atmospheric Environment, 2008,42(37):86988705.
[14]	Kuznetsova M, Lee C, Aller J. Characterization of the proteinaceous matter in marine aerosols[J]. Marine Chemistry, 2005,96(3/4):359377.
[15]	Matsumoto K, Uematsu M. Free amino acids in marine aerosols over the western North Pacific Ocean[J]. Atmospheric Environment, 2005,39(11):2163-2170.
[16]	Mcgregor K G, Anastasio C. Chemistry of fog waters in California's Central Valley:2. Photochemical transformations of amino acids and alkyl amines[J]. Atmospheric Environment, 2001,35(6):1091-1104.
[17]	Milne P J, Zika R G. Amino acid nitrogen in atmospheric aerosols:Occurrence, sources and photochemical modification[J]. Journal of Atmospheric Chemistry, 1993,16(4):361-398.
[18]	Mopper K, Zika R G. Free amino acids in marine rains:evidence for oxidation and potential role in nitrogen cycling[J]. Nature, 1987, 325(6101):246.
[19]	Zhang Q, Anastasio C. Free and combined amino compounds in atmospheric fine particles (PM2.5) and fog waters from Northern California[J]. Atmospheric Environment, 2003,37(16):2247-2258.
[20]	Wang S, Song T, Shiraiwa M, et al. Occurrence of aerosol proteinaceous matter in urban Beijing:An investigation on composition, sources, and atmospheric processes during the "APEC Blue" period[J]. Environmental Science & Technology, 2019,53(13):7380-7390.
[21]	Ho K, Ho S S H, Huang R-J, et al. Characteristics of water-soluble organic nitrogen in fine particulate matter in the continental area of China[J]. Atmospheric Environment, 2015,106:252-261.
[22]	Di Filippo P, Pomata D, Riccardi C, et al. Free and combined amino acids in size-segregated atmospheric aerosol samples[J]. Atmospheric Environment, 2014,98:179-189.
[23]	Samy S, Robinson J, Rumsey I C, et al. Speciation and trends of organic nitrogen in southeastern US fine particulate matter (PM2.5)[J]. Journal of Geophysical Research:Atmospheres, 2013,118(4):19962006.
[24]	Kang H, Xie Z, Hu Q. Ambient protein concentration in PM10 in Hefei, central China[J]. Atmospheric Environment, 2012,54:73-79.
[25]	Menetrez M, Foarde K, Dean T, et al. An evaluation of the protein mass of particulate matter[J]. Atmospheric Environment, 2007,41(37):8264-8274.
[26]	Yang H, Yu J Z, Ho S S H, et al. The chemical composition of inorganic and carbonaceous materials in PM2.5 in Nanjing, China[J]. Atmospheric Environment, 2005,39(20):3735-3749.
[27]	Yu J, Schauer J. Chemical characterization of water soluble organic compounds in particulate matters in Hong Kong[M]. Report from Hong Kong Environmental Protection Department, Hong Kong University. 2002:31-36.
[28]	Belan B, Borodulin A, Buryak G, et al. Annual changes in concentration of protein content of atmospheric aerosol in the South of Western Siberia[J]. Journal of Aerosol Science, 2000,31:S963-S964.
[29]	Mace K A, Artaxo P, Duce R a J J O G R A. Water-soluble organic nitrogen in Amazon Basin aerosols during the dry (biomass burning) and wet seasons[J]. Journal of Geophysical Research:Atmospheres, 2003,108(D16):4512.
[30]	Shar S, James R, D H M. An advanced LC-MS (Q-TOF) technique for the detection of amino acids in atmospheric aerosols[J]. Analytical and Bioanalytical Chemistry, 2011,401(10):3103-3113.
[31]	Song T, Wang S, Zhang Y, et al. Proteins and amino acids in fine particulate matter in rural Guangzhou, Southern China:seasonal cycles, sources, and atmospheric processes[J]. Environmental Science & Technology, 2017,51(12):6773-6781.
[32]	Mandalakis M, Apostolaki M, Tziaras T, et al. Free and combined amino acids in marine background atmospheric aerosols over the Eastern Mediterranean[J]. Atmospheric Environment, 2011,45(4):1003-1009.
[33]	Barbaro E, Zangrando R, Moret I, et al. Free amino acids in atmospheric particulate matter of Venice, Italy[J]. Atmospheric Environment, 2011,45(28):5050-5057.
[34]	Shi J, Gao H, Qi J, et al. Sources, compositions, and distributions of water-soluble organic nitrogen in aerosols over the China Sea[J]. Journal of Geophysical Research, 2010,115(D17):1-13.
[35]	Yang H, Xu J, Wu W-S, et al. Chemical characterization of watersoluble organic aerosols at Jeju Island collected during ACE-Asia[J]. Environmental Chemistry, 2004,1(1):13-17.
[36]	Mace K A, Kubilay N, Duce R A. Organic nitrogen in rain and aerosol in the eastern Mediterranean atmosphere:An association with atmospheric dust[J]. Journal of Geophysical Research, 2003,108(D10):1-11.
[37]	Mace K A, Duce R A, Tindale N W. Organic nitrogen in rain and aerosol at Cape Grim, Tasmania, Australia[J]. Journal of Geophysical Research, 2003,108(D11):1-14.
[38]	Barbaro E, Zangrando R, Vecchiato M, et al. Free amino acids in Antarctic aerosol:potential markers for the evolution and fate of marine aerosol[J]. Atmospheric Chemistry and Physics, 2015,15(10):5457-5469.
[39]	Helin A, Sietiö O-M, Heinonsalo J, et al. Characterization of free amino acids, bacteria and fungi in size-segregated atmospheric aerosols in boreal forest:seasonal patterns, abundances and size distributions[J]. Atmospheric Chemistry and Physics, 2017,17:1308913101.
[40]	Samy S, Robinson J, Hays M D. An advanced LC-MS (Q-TOF) technique for the detection of amino acids in atmospheric aerosols[J]. Analytical and Bioanalytical Chemistry, 2011,401(10):3103-3113.
[41]	Franze T, Weller M G, Niessner R, et al. Protein nitration by polluted air[J]. Environmental Science & Technology, 2005,39(6):1673-1678.
[42]	Sharma V K, Graham N J. Oxidation of amino acids, peptides and proteins by ozone:a review[J]. Ozone:Science & Engineering, 2010,32(2):81-90.
[43]	Manabu S, Kathrin S, Hong Y, et al. Multiphase chemical kinetics of the nitration of aerosolized protein by ozone and nitrogen dioxide[J]. Environment Science & Technology, 2012,46(12):72-80.
[44]	J K C, Fobang L, Kathrin R-S, et al. Protein cross-linking and oligomerization through dityrosine formation upon exposure to ozone[J]. Environment Science & Technology, 2015,49(18):59-66.
[45]	Mumford R A, Lipke H, Laufer D A, et al. Ozone-induced changes in corn pollen[J]. Environmental Science & Technology, 2002,(5):427430.
[46]	Isabelle B, Susanne J, Stefanie G, et al. High environmental ozone levels lead to enhanced allergenicity of birch pollen[J]. PloS One, 2013,8(11):e80147.
[47]	Liu F, Lakey P S, Berkemeier T, et al. Atmospheric protein chemistry influenced by anthropogenic air pollutants:nitration and oligomerization upon exposure to ozone and nitrogen dioxide[J]. Faraday Discussions, 2017,200:413-427.
[48]	Reinmuth-Selzle K, Kampf C J, Lucas K, et al. Air pollution and climate change effects on allergies in the anthropocene:abundance, interaction, and modification of allergens and adjuvants[J]. Environmental Science & Technology, 2017,51(8):4119-4141.
[49]	Liu F, Lai S, Tong H, et al. Release of free amino acids upon oxidation of peptides and proteins by hydroxyl radicals[J]. Analytical and Bioanalytical Chemistry, 2017,409(9):2411-2420.
[50]	Guicherit R, Roemer M J C-G C S. Tropospheric ozone trends[J]. Chemosphere-Global Change Science, 2000,2(2):167-183.
[51]	Lai S, Zhao Y, Ding A, et al. Characterization of PM2.5 and the major chemical components during a 1-year campaign in rural Guangzhou, Southern China[J]. Atmospheric Research, 2016,167:208-215.
[52]	Xiao H-Y, Tang C-G, Xiao H-W, et al. Stable sulphur and nitrogen isotopes of the moss Haplocladium microphyllum at urban, rural and forested sites[J]. Atmospheric Environment, 2010,44(34):4312-4317.
[53]	Liu X-Y, Xiao H-Y, Liu C-Q, et al. Tissue N content and 15N natural abundance in epilithic mosses for indicating atmospheric N deposition in the Guiyang area, SW China[J]. Applied Geochemistry, 2008,23(9):2708-2715.
[54]	Zhu R-G, Xiao H-Y, Lv Z, et al. Nitrogen isotopic composition of free Gly in aerosols at a forest site[J]. Atmospheric Environment, 2020, 222:117179.
[55]	Ren L, Bai H, Yu X, et al. Molecular composition and seasonal variation of amino acids in urban aerosols from Beijing, China[J]. Atmospheric Research, 2018,203:28-35.
[56]	Takano Y, Kashiyama Y, Ogawa N O, et al. Isolation and desalting with cation-exchange chromatography for compound-specific nitrogen isotope analysis of amino acids:application to biogeochemical samples[J]. Rapid Commun Mass Spectrom, 2010,24(16):2317-2323.
[57]	Hare P E, Fogel M L, Stafford Jr T W, et al. The isotopic composition of carbon and nitrogen in individual amino acids isolated from modern and fossil proteins[J]. Journal of Archaeological Science, 1991, 18(3):277-292.
[58]	Zhu R-G, Xiao H-Y, Zhang Z, et al. Compound-specific δ 15N composition of free amino acids in moss as indicators of atmospheric nitrogen sources[J]. Scientific reports, 2018,8(1):14347.
[59]	Zhu R G, Xiao H Y, Zhu Y, et al. Sources and transformation processes of proteinaceous matter and free amino acids in PM2.5[J]. Journal of Geophysical Research:Atmospheres, 2020,125(5):e2020JD032375.
[60]	Rosas I, Yela A, Salinas E, et al. Preliminary assessment of protein associated with airborne particles in Mexico City[J]. Aerobiología, 1995,11(2):81-86.
[61]	Miguel A G, Cass G R, Glovsky M M, et al. Allergens in paved road dust and airborne particles[J]. Environmental science & technology, 1999,33(23):4159-4168.
[62]	Yan G, Kim G, Kim J, et al. Dissolved total hydrolyzable enantiomeric amino acids in precipitation:Implications on bacterial contributions to atmospheric organic matter[J]. Geochimica et Cosmochimica Acta, 2015,153:1-14.
[63]	Dauwe B, Middelburg J J, Herman P M, et al. Linking diagenetic alteration of amino acids and bulk organic matter reactivity[J]. Limnology and Oceanography, 1999,44(7):1809-1814.
[64]	Mace K A, Artaxo P, Duce R A. Water-soluble organic nitrogen in Amazon Basin aerosols during the dry (biomass burning) and wet seasons[J]. Journal of Geophysical Research:Atmospheres, 2003, 108(D16):1-14.
[65]	Hong Z, Li M, Wang H, et al. Characteristics of atmospheric volatile organic compounds (VOCs) at a mountainous forest site and two urban sites in the southeast of China[J]. Science of the Total Environment, 2019,657:1491-1500.
[66]	Wu F, Yu Y, Sun J, et al. Characteristics, source apportionment and reactivity of ambient volatile organic compounds at Dinghu Mountain in Guangdong Province, China[J]. Science of the Total Environment, 2016,548:347-359.
[67]	余应新,文晟,吕辉雄,等.广州森林大气中VOCs昼夜变化特征及对O3的影响[J]. 环境科学与技术, 2009,32(3):94-98. Yu Y X, Wen C, Lv H X, et al. Diurnal variations of VOCs and relative contribution to ozone in forest of Guangzhou[J]. Environmental Science and Technology, 2009,32(3):94-98.
[68]	李美娟,周晓晶,韩烈保,等.鹫峰国家森林公园大气中VOCs的组成与特点[J]. 环境化学, 2007,(3):399-402. Li M J, Zhou X J, Han L B, et al. The composition and characteristics of VOCs in the atmosphere of Jiufeng National Forest Park[J]. Environmental Chemistry, 2007,(3):399-402.
[69]	张渊钰,王新明,刘晓玲,等.新疆独山子区VOCs组成及其对O3和SOA的贡献[J]. 中国环境科学, 2020,40(5):1915-1923. Zhang Y Y, Wang X M, Liu X L, et al. Volatile organic compounds (VOCs) in Dushanzi, Xinjiang:Compositions and contributions to the formation of O3 and SOA[J]. China Environmental Science, 2020, 40(5):1915-1923.
[70]	司雷霆,王浩,李洋,等.太原市夏季大气VOCs污染特征及臭氧生成潜势[J]. 中国环境科学, 2019,39(9):3655-3662. Si L T, Wang H, Li Y, et al. Pollution characteristics and ozone formation potential of ambient VOCs in summer in Taiyuan[J]. China Environmental Science, 2019,39(9):3655-3662.
[71]	虞小芳,程鹏,古颖纲,等.广州市夏季VOCs对臭氧及SOA生成潜势的研究[J]. 中国环境科学, 2018,38(3):830-837. Yu X F, Cheng P, Gu Y G, et al. Formation potential of ozone and secondary organic aerosol from VOCs oxidation in summer in Guangzhou, China[J]. China Environmental Science, 2018,38(3):830837.
[72]	Pommié C, Levadoux S, Sabatier R, et al. IMGT standardized criteria for statistical analysis of immunoglobulin V-REGION amino acid properties[J]. Journal of Molecular Recognition, 2004,17(1):17-32.