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Front. Environ. Sci. Eng.    2021, Vol. 15 Issue (6) : 126    https://doi.org/10.1007/s11783-021-1414-6
REVIEW ARTICLE
δ15N-stable isotope analysis of NHx: An overview on analytical measurements, source sampling and its source apportionment
Noshan Bhattarai1,2, Shuxiao Wang1,2(), Yuepeng Pan3, Qingcheng Xu1,2, Yanlin Zhang4, Yunhua Chang4, Yunting Fang5
1. State Key Joint Laboratory of Environmental Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China
2. State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex, Beijing 100084, China
3. State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
4. Yale-NUIST Center on Atmospheric Environment, Nanjing University of Information Science & Technology, Nanjing 210044, China
5. CAS Key Laboratory of Forest Ecology and Management, Institute of Applied Ecology, Chinese Academy of Sciences, Shenyang 110016, China
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Abstract

• Challenges in sampling of NH3 sources for d15N analysis are highlighted.

• Uncertainties in the isotope-based source apportionment of NH3 and NH4+ are outlined.

• Characterizing dynamic isotopic fractionation may reduce uncertainties of NHx science.

Agricultural sources and non-agricultural emissions contribute to gaseous ammonia (NH3) that plays a vital role in severe haze formation. Qualitative and quantitative contributions of these sources to ambient PM2.5 (particulate matter with an aerodynamic equivalent diameter below 2.5 µm) concentrations remains uncertain. Stable nitrogen isotopic composition (δ15N) of NH3 and NH4+ (δ15N(NH3) and δ15N(NH4+), respectively) can yield valuable information about its sources and associated processes. This review provides an overview of the recent progress in analytical techniques for δ15N(NH3) and δ15N(NH4+) measurement, sampling of atmospheric NH3 and NH4+ in the ambient air and their sources signature (e.g., agricultural vs. fossil fuel), and isotope-based source apportionment of NH3 in urban atmosphere. This study highlights that collecting sample that are fully representative of emission sources remains a challenge in fingerprinting δ15N(NH3) values of NH3 emission sources. Furthermore, isotopic fractionation during NH3 gas-to-particle conversion under varying ambient field conditions (e.g., relative humidity, particle pH, temperature) remains unclear, which indicates more field and laboratory studies to validate theoretically predicted isotopic fractionation are required. Thus, this study concludes that lack of refined δ15N(NH3) fingerprints and full understanding of isotopic fractionation during aerosol formation in a laboratory and field conditions is a limitation for isotope-based source apportionment of NH3. More experimental work (in chamber studies) and theoretical estimations in combinations of field verification are necessary in characterizing isotopic fractionation under various environmental and atmospheric neutralization conditions, which would help to better interpret isotopic data and our understanding on NHx (NH3 + NH4+) dynamics in the atmosphere.
Keywords Aerosol ammonium      Atmospheric gaseous ammonia      Isotope fingerprinting      Isotope-based source apportionment      Ammonia gas-to-particle conversion     
Corresponding Author(s): Shuxiao Wang   
Issue Date: 17 March 2021
 Cite this article:   
Noshan Bhattarai,Shuxiao Wang,Yuepeng Pan, et al. δ15N-stable isotope analysis of NHx: An overview on analytical measurements, source sampling and its source apportionment[J]. Front. Environ. Sci. Eng., 2021, 15(6): 126.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-021-1414-6
https://academic.hep.com.cn/fese/EN/Y2021/V15/I6/126
No. Method NH4+ (µmol/L) N2O (nmole) Volume (mL) Standards replicates (±1σ ‰) References
1 Hypobromite-azide 0.5–10 10 20 0.3 Zhang et al.(2007)
2 Coupled denitrifier 10 20 20 0.7 Felix et al. (2013)
3 Hypobromite-hydroxylamine 10–20 60 4 0.3 Liu et al. (2014)
Tab.1  Summary of the parameters of δ15N(NH3)/δ15N(NH4+) laboratory experimental methods
Fig.1  Summary of previously reported δ15N source signature of NH3 (δ15N(NH3)) that were collected with passive or active sampling techniques. Dashed horizontal lines classify major sources of NH3 based on different sample collection methods utilized in previous studies. The δ15N(NH3) source signatures for sources listed in the figure (from top to bottom) are as following: Marine (–10.2‰ to 2.2‰) (Felix et al., 2013), livestock waste (active) (–15.2‰ to –8.9‰), livestock waste (passive) (–56.1‰ to –22.8‰), fertilizer use (passive) (–52.0‰ to –35.0‰) (Felix et al., 2013; Chang et al., 2016; Bhattarai et al., 2020), urban waste (passive) including human excreta (–39.6‰ to –37.3‰), solid waste (–37.6‰ to –29.9‰) and waste water (–42.0‰ to –39.2‰) (Chang et al., 2016), coal-fired power plants (CFPP/active) which includes NH3 slip from SCR equipped CFPP (–16.1‰ to –5.6‰) (Felix et al., 2013; Bhattarai et al., 2020) and coal combustion (–7.2‰ to 2‰) (Freyer, 1978), tailpipe emissions (active) (–9.3‰ to 9.0‰) (Berner and Felix, 2020), urban traffic (tunnel/active) (2.1‰ to 9.2‰) (Walters et al., 2020), and urban traffic (tunnel/passive) (–17.8‰ to –2.2‰) (Felix et al., 2013; Chang et al., 2016; Walters et al., 2020). δ15N(NH3) values of different sources were corrected for low bias in passive samplers by adding 15‰ to measured δ15N(NH3) values (Pan et al., 2020b; Walters et al., 2020).
Fig.2  Instantaneous δ15N(NH3) values in an NH3 volatilization experiment with liquid manure during the incubation periods (14 to 30 days in total) (Hristov et al., 2009; Lee et al., 2011) and range of δ15N(NH3) values previously observed during field studies (–56.1‰ to –22.8‰ and –41.1‰ to –7.8‰ (corrected)) (Freyer, 1978; Heaton, 1987; Felix et al., 2013; Chang et al., 2016; Bhattarai et al., 2020) for livestock waste (shaded area). During volatilization experiment, NH3 released from liquid manure was incubated and absorbed in a 0.5 mol/L H2SO4 scrubber to characterize d15N(NH3) values in previous studies (Hristov et al., 2009; Lee et al., 2011).
Location Sampling period Measured δ15N(NH3) (‰) Relative contribution (%) References
Agricultural a) Non-agricultural b)
Beijing
(China)		 18/10/2014 to 29/11/2014 –35.0±5.4 (n = 12) 54 46 Chang et al. (2016)
Indianapolis
(USA)		 07/2009 to 06/2010 –18.0 (n = 8)* 10 90 Felix et al. (2017)
Detroit
(USA)		 07/2009 to 06/2010 –14.3 (n = 11)* 4 96** Felix et al. (2017)
Shanghai
(China)		 07/2015 to 08/2015 –31.7±3.4 (n = 10) 47 53 Chang et al. (2019)
Texas
(USA)		 09/2016 to 08/2017 –19.1±10.9 (n = 22) 45 55*** Berner and Felix (2020)
Beijing
(China)		 03/2016 to 03/2017 –33.2±8.6
(n = 73)		 28 72 Zhang et al. (2020a)
Beijing
(China)		 03/2016 to 03/2017 –33.2±8.6
(n = 73)		 34 66 Pan et al. (2020a)
Beijing
(China)		 13/09/2018 to 09/10/2018 –28.9±1.5
(n = 8)		 37 63 Bhattarai et al. (2020)
Beijing
(China)		 03/01/2017 to 25/01/2017 _ 26 74 Zhang et al. (2020b)
Beijing
(China)		 07/02/2020 to 13/02/2020 and 25/03/2020 to 01/04/2020 _ 38 62 Zhang et al. (2020b)
Tab.2  Summary of recent isotope-based source apportionment studies on gaseous NH3 derived from measured δ15N(NH3) values observed in urban areas
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