Cite this paper:
Xie Chengjun, Song Guodong, Liu Sumei, Tang Jiyao, Zhang Guiling. Self-assembled membrane injection mass spectrometry system and its application on the study of dissimilatory nitrate reduction in sandy sediments[J]. Haiyang Xuebao, 2020, 42(2): 22-29

Self-assembled membrane injection mass spectrometry system and its application on the study of dissimilatory nitrate reduction in sandy sediments

Xie Chengjun1,2,3, Song Guodong1,2, Liu Sumei1,2, Tang Jiyao1,2,3, Zhang Guiling1,2
1. Key Laboratory of Marine Chemistry Theory and Technology, Ministry of Education/Institute for Advanced Ocean Study, Ocean University of China, Qingdao 266100, China;
2. Laboratory for Marine Ecology and Environmental Science, Pilot National Laboratory for Marine Science and Technology (Qingdao), Qingdao 266237, China;
3. College of Chemistry and Chemical Engineering, Ocean University of China, Qingdao 266100, China
Dissimilatory nitrate reduction processes in sediments play a crucial role in marine nitrogen cycle. The most popular method to determine the rates of different dissimilatory nitrate reduction processes is the 15N labeled technique. Therefore, accurate and rapid determination the concentration of 15N-labeled products, such as 29N2 and 30N2, is the key to quantify the rate of each dissimilatory nitrate reduction process. In this study, we set up a membrane injection mass spectrometry (MIMS) and optimize the operating condition of the MIMS for the determination of 29N2 and 30N2. The optimization experiment results indicated that, when the peristaltic pump for sampling flow rate is 0.80 mL/min, the sampling time is 3~3.5 min, the thermostat water bath temperature is 20~25℃, and the copper reduction furnace temperature is 300~600℃, the precision (expressed in coefficient of variation) of the measured 29N2/28N2 and 30N2/28N2 can be controlled less than 0.1% and 1%, respectively. We used the self-assembled MIMS and combined the 15N labeling technique to study the dissimilatory nitrate reduction processes in the sandy sediment of the Shilaoren beach in Qingdao. There is no significant aerobic denitrification in the Shilaoren sand that can completely reduce nitrate to N2. The potential rates of anammox, anaerobic denitrification and dissimilatory nitrate reduction to ammonium (DNRA) are (0.05±0.01) nmol/(cm3·h), (2.32±0.21) nmol/(cm3·h) and (1.02±0.15) nmol/(cm3·h) (N,wet sed.), respectively. Anaerobic denitrification is the major contributor to nitrate dissimilatory reduction, with a ratio of nearly 70%, followed by DNRA, with a ratio of up to 30%, while anammox has the lowest contribution of only 1%. In the N2 production, the main contributor is anaerobic denitrification, and the contribution of anammox is only 2%.
Key words:    membrane injection mass spectrometry (MIMS)    sandy sediment    denitrification    anammox    dissimilatory nitrate reduction to ammonium   
Received: 2019-04-05   Revised: 2019-05-30
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[1] Gruber N, Galloway J N. An earth-system perspective of the global nitrogen cycle[J]. Nature, 2008, 451(7176):293-296.
[2] Cai Weijun, Hu Xinping, Huang W J, et al. Acidification of subsurface coastal waters enhanced by eutrophication[J]. Nature Geoscience, 2011, 4(11):766-770.
[3] Seitzinger S P, Phillips L. Nitrogen stewardship in the Anthropocene[J]. Science, 2017, 357(6349):350-351.
[4] Breitburg D, Levin L A, Oschlies A, et al. Declining oxygen in the global ocean and coastal waters[J]. Science, 2018, 359(6371):eaam7240.
[5] Seitzinger S P. Denitrification in freshwater and coastal marine ecosystems:ecological and geochemical significance[J]. Limnology and Oceanography, 1988, 33:702-724.
[6] Codispoti L A. An oceanic fixed nitrogen sink exceeding 400 Tg N a-1 vs the concept of homeostasis in the fixed-nitrogen inventory[J]. Biogeosciences, 2007, 4(2):233-253.
[7] Devol A H. Denitrification, anammox, and N2 production in marine sediments[J]. Annual Review of Marine Science, 2015, 7:403-423.
[8] Gao Hang, Schreiber F, Collins G, et al. Aerobic denitrification in permeable Wadden Sea sediments[J]. The ISME Journal, 2010, 4(3):417-426.
[9] Marchant H K, Holtappels M, Lavik G, et al. Coupled nitrification-denitrification leads to extensive N loss in subtidal permeable sediments[J]. Limnology and Oceanography, 2016, 61(3):1033-1048.
[10] Huettel M, Berg P, Kostka J E. Benthic exchange and biogeochemical cycling in permeable sediments[J]. Annual Review of Marine Science, 2014, 6:23-51.
[11] Sokoll S, Lavik G, Sommer S, et al. Extensive nitrogen loss from permeable sediments off North-West Africa[J]. Journal of Geophysical Research:Biogeosciences, 2016, 121(4):1144-1157.
[12] Robertson E K, Bartoli M, Brüchert V, et al. Application of the isotope pairing technique in sediments:Use, challenges, and new directions[J]. Limnology and Oceanography:Methods, 2019, 17(2):112-136.
[13] Nielsen L P. Denitrification in sediment determined from nitrogen isotope pairing[J]. FEMS Microbiology Letter, 1992, 86(4):357-362.
[14] Thamdrup B, Dalsgaard T. Production of N2 through anaerobic ammonium oxidation coupled to nitrate reduction in marine sediments[J]. Applied and Environmental Microbiology, 2002, 68(3):1312-1318.
[15] Kana T M, Darkangelo C, Hunt M D, et al. Membrane inlet mass spectrometer for rapid high-precision determination of N2, O2, and Ar in environmental water samples[J]. Analytical Chemistry, 1994, 66(23):4166-4170.
[16] br>Chen Nengwang, Wu Jiezhong, Duan Hengyi, et al. N2:Ar method for direct measurement of denitrification product (dissolved N2) using membrane inlet mass spectrometry (MIMS)[J]. Acta Scientiae Circumstantiae, 2010, 30(12):2479-2483
[17] br>Zheng Wenjing, Han Yu, Qin Chuan, et al. Continuous underway measurements of sea surface O2/Ar and pCO2 by membrane inlet mass spectrometry[J]. Marine Environmental Science, 2016, 35(4):611-617
[18] An S, Gardner W S, Kana T. Simultaneous measurement of denitrification and nitrogen fixation using isotope pairing with membrane inlet mass spectrometry analysis[J]. Applied and Environmental Microbiology, 2001, 67(3):1171-1178.
[19] Yin Guoyu, Hou Lijun, Liu Min, et al. A novel membrane inlet mass spectrometer method to measure 15NH4+ for isotope-enrichment experiments in aquatic ecosystems[J]. Environmental Science & Technology, 2014, 48(16):9555-9562.
[20] Lin Xianbiao, Liu Min, Hou Lijun, et al. Nitrogen losses in sediments of the East China Sea:spatiotemporal variations, controlling factors, and environmental implications[J]. Journal of Geophysical Research:Biogeosciences, 2017, 122(10):2699-2715.
[21] br>Zhao Yongqiang, Xia Yongqiu, Li Bolun, et al. Simultaneous determination of denitrification and anaerobic ammonium oxidation in river sediments using membrane inlet mass spectrometry[J]. Journal of Agro-Environment Science, 2014, 33(4):794-802
[22] Eyre B D, Rysgaard S, Dalsgaard T, et al. Comparison of isotope pairing and N2:Ar methods for measuring sediment denitrification-assumption, modifications, and implications[J]. Estuaries, 2002, 25(6):1077-1087.
[23] Song G D, Liu S M, Marchant H, et al. Anammox, denitrification and dissimilatory nitrate reduction to ammonium in the East China Sea sediment[J]. Biogeosciences, 2013, 10(11):6851-6864.
[24] Song Guodong, Liu Sumei, Zhu Zhuoyi, et al. Sediment oxygen consumption and benthic organic carbon mineralization on the continental shelves of the East China Sea and the Yellow Sea[J]. Deep Sea Research Part II:Topical Studies in Oceanography, 2016, 124:53-63.
[25] Thamdrup B, Dalsgaard T. The fate of ammonium in anoxic manganese oxide-rich marine sediment[J]. Geochimica et Cosmochimica Acta, 2000, 64(24):4157-4164.
[26] Sgouridis F, Stott A, Ullah S. Application of the 15N gas-flux method for measuring in situ N2 and N2O fluxes due to denitrification in natural and semi-natural terrestrial ecosystems and comparison with the acetylene inhibition technique[J]. Biogeosciences, 2016, 13(6):1821-1835.
[27] Lunstrum A, Aoki L R. Oxygen interference with membrane inlet mass spectrometry may overestimate denitrification rates calculated with the isotope pairing technique[J]. Limnology and Oceanography:Methods, 2016, 14(7):425-431.
[28] Kana T M, Weiss D L, Eyre B D, et al. Comment on "Comparison of isotope pairing and N2:Ar methods for measuring sediment denitrification" by B. D. Eyre, S. Rysgaard, T. Dalsgaard, and P. Bondo Christensen. 2002. Estuaries 25:1077-1087[J]. Estuaries, 2004, 27(1):173-176.
[29] Song G D, Liu S M, Kuypers M M M, et al. Application of the isotope pairing technique in sediments where anammox, denitrification, and dissimilatory nitrate reduction to ammonium coexist[J]. Limnology and Oceanography:Methods, 2016, 14(12):801-815.
[30] Nicholls J C, Trimmer M. Widespread occurrence of the anammox reaction in estuarine sediments[J]. Aquatic Microbial Ecology, 2009, 55(2):105-113.
[31] Cook P L M, Kessler A J, Eyre B D. Does denitrification occur within porous carbonate sand grains?[J]. Biogeosciences, 2017, 14(18):4061-4069.
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