Drivers for spatial, temporal and long-term trends in atmospheric ammonia and ammonium in the UK
A unique long-term dataset from the UK National Ammonia Monitoring Network (NAMN) is used here to assess spatial, seasonal and long-term variability in atmospheric ammonia (NH3: 1998–2014) and particulate ammonium (NH4+: 1999–2014) across the UK. Extensive spatial heterogeneity in NH3 concentrations...
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| Published in | Atmospheric chemistry and physics Vol. 18; no. 2; pp. 705 - 733 |
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| Main Authors | , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
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Katlenburg-Lindau
Copernicus GmbH
22.01.2018
Copernicus Publications |
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| Abstract | A unique long-term dataset from the UK National Ammonia Monitoring Network (NAMN) is used here to assess spatial, seasonal and long-term variability in atmospheric ammonia (NH3: 1998–2014) and particulate ammonium (NH4+: 1999–2014) across the UK. Extensive spatial heterogeneity in NH3 concentrations is observed, with lowest annual mean concentrations at remote sites (< 0.2 µg m−3) and highest in the areas with intensive agriculture (up to 22 µg m−3), while NH4+ concentrations show less spatial variability (e.g. range of 0.14 to 1.8 µg m−3 annual mean in 2005). Temporally, NH3 concentrations are influenced by environmental conditions and local emission sources. In particular, peak NH3 concentrations are observed in summer at background sites (defined by 5 km grid average NH3 emissions < 1 kg N ha−1 yr−1) and in areas dominated by sheep farming, driven by increased volatilization of NH3 in warmer summer temperatures. In areas where cattle, pig and poultry farming is dominant, the largest NH3 concentrations are in spring and autumn, matching periods of manure application to fields. By contrast, peak concentrations of NH4+ aerosol occur in spring, associated with long-range transboundary sources. An estimated decrease in NH3 emissions by 16 % between 1998 and 2014 was reported by the UK National Atmospheric Emissions Inventory. Annually averaged NH3 data from NAMN sites operational over the same period (n = 59) show an indicative downward trend, although the reduction in NH3 concentrations is smaller and non-significant: Mann–Kendall (MK), −6.3 %; linear regression (LR), −3.1 %. In areas dominated by pig and poultry farming, a significant reduction in NH3 concentrations between 1998 and 2014 (MK: −22 %; LR: −21 %, annually averaged NH3) is consistent with, but not as large as the decrease in estimated NH3 emissions from this sector over the same period (−39 %). By contrast, in cattle-dominated areas there is a slight upward trend (non-significant) in NH3 concentrations (MK: +12 %; LR: +3.6 %, annually averaged NH3), despite the estimated decline in NH3 emissions from this sector since 1998 (−11 %). At background and sheep-dominated sites, NH3 concentrations increased over the monitoring period. These increases (non-significant) at background (MK: +17 %; LR: +13 %, annually averaged data) and sheep-dominated sites (MK: +15 %; LR: +19 %, annually averaged data) would be consistent with the concomitant reduction in SO2 emissions over the same period, leading to a longer atmospheric lifetime of NH3, thereby increasing NH3 concentrations in remote areas. The observations for NH3 concentrations not decreasing as fast as estimated emission trends are consistent with a larger downward trend in annual particulate NH4+ concentrations (1999–2014: MK: −47 %; LR: −49 %, p < 0.01, n = 23), associated with a lower formation of particulate NH4+ in the atmosphere from gas phase NH3. |
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| AbstractList | A unique long-term dataset from the UK National Ammonia Monitoring Network (NAMN) is used here to assess spatial, seasonal and long-term variability in atmospheric ammonia (NH3: 1998–2014) and particulate ammonium (NH4+: 1999–2014) across the UK. Extensive spatial heterogeneity in NH3 concentrations is observed, with lowest annual mean concentrations at remote sites (< 0.2 µg m−3) and highest in the areas with intensive agriculture (up to 22 µg m−3), while NH4+ concentrations show less spatial variability (e.g. range of 0.14 to 1.8 µg m−3 annual mean in 2005). Temporally, NH3 concentrations are influenced by environmental conditions and local emission sources. In particular, peak NH3 concentrations are observed in summer at background sites (defined by 5 km grid average NH3 emissions < 1 kg N ha−1 yr−1) and in areas dominated by sheep farming, driven by increased volatilization of NH3 in warmer summer temperatures. In areas where cattle, pig and poultry farming is dominant, the largest NH3 concentrations are in spring and autumn, matching periods of manure application to fields. By contrast, peak concentrations of NH4+ aerosol occur in spring, associated with long-range transboundary sources. An estimated decrease in NH3 emissions by 16 % between 1998 and 2014 was reported by the UK National Atmospheric Emissions Inventory. Annually averaged NH3 data from NAMN sites operational over the same period (n = 59) show an indicative downward trend, although the reduction in NH3 concentrations is smaller and non-significant: Mann–Kendall (MK), −6.3 %; linear regression (LR), −3.1 %. In areas dominated by pig and poultry farming, a significant reduction in NH3 concentrations between 1998 and 2014 (MK: −22 %; LR: −21 %, annually averaged NH3) is consistent with, but not as large as the decrease in estimated NH3 emissions from this sector over the same period (−39 %). By contrast, in cattle-dominated areas there is a slight upward trend (non-significant) in NH3 concentrations (MK: +12 %; LR: +3.6 %, annually averaged NH3), despite the estimated decline in NH3 emissions from this sector since 1998 (−11 %). At background and sheep-dominated sites, NH3 concentrations increased over the monitoring period. These increases (non-significant) at background (MK: +17 %; LR: +13 %, annually averaged data) and sheep-dominated sites (MK: +15 %; LR: +19 %, annually averaged data) would be consistent with the concomitant reduction in SO2 emissions over the same period, leading to a longer atmospheric lifetime of NH3, thereby increasing NH3 concentrations in remote areas. The observations for NH3 concentrations not decreasing as fast as estimated emission trends are consistent with a larger downward trend in annual particulate NH4+ concentrations (1999–2014: MK: −47 %; LR: −49 %, p < 0.01, n = 23), associated with a lower formation of particulate NH4+ in the atmosphere from gas phase NH3. A unique long-term dataset from the UK National Ammonia Monitoring Network (NAMN) is used here to assess spatial, seasonal and long-term variability in atmospheric ammonia (NH.sub.3 : 1998-2014) and particulate ammonium (NH.sub.4 .sup.+ : 1999-2014) across the UK. Extensive spatial heterogeneity in NH.sub.3 concentrations is observed, with lowest annual mean concentrations at remote sites (< 0.2 µg m.sup.-3) and highest in the areas with intensive agriculture (up to 22 µg m.sup.-3 ), while NH.sub.4 .sup.+ concentrations show less spatial variability (e.g. range of 0.14 to 1.8 µg m.sup.-3 annual mean in 2005). Temporally, NH.sub.3 concentrations are influenced by environmental conditions and local emission sources. In particular, peak NH.sub.3 concentrations are observed in summer at background sites (defined by 5 km grid average NH.sub.3 emissions < 1 kg N ha.sup.-1 yr.sup.-1) and in areas dominated by sheep farming, driven by increased volatilization of NH.sub.3 in warmer summer temperatures. In areas where cattle, pig and poultry farming is dominant, the largest NH.sub.3 concentrations are in spring and autumn, matching periods of manure application to fields. By contrast, peak concentrations of NH.sub.4 .sup.+ aerosol occur in spring, associated with long-range transboundary sources. An estimated decrease in NH.sub.3 emissions by 16 % between 1998 and 2014 was reported by the UK National Atmospheric Emissions Inventory. Annually averaged NH.sub.3 data from NAMN sites operational over the same period (n = 59) show an indicative downward trend, although the reduction in NH.sub.3 concentrations is smaller and non-significant: Mann-Kendall (MK), -6.3 %; linear regression (LR), -3.1 %. In areas dominated by pig and poultry farming, a significant reduction in NH.sub.3 concentrations between 1998 and 2014 (MK: -22 %; LR: -21 %, annually averaged NH.sub.3) is consistent with, but not as large as the decrease in estimated NH.sub.3 emissions from this sector over the same period (-39 %). By contrast, in cattle-dominated areas there is a slight upward trend (non-significant) in NH.sub.3 concentrations (MK: +12 %; LR: +3.6 %, annually averaged NH.sub.3 ), despite the estimated decline in NH.sub.3 emissions from this sector since 1998 (-11 %). At background and sheep-dominated sites, NH.sub.3 concentrations increased over the monitoring period. These increases (non-significant) at background (MK: +17 %; LR: +13 %, annually averaged data) and sheep-dominated sites (MK: +15 %; LR: +19 %, annually averaged data) would be consistent with the concomitant reduction in SO.sub.2 emissions over the same period, leading to a longer atmospheric lifetime of NH.sub.3, thereby increasing NH.sub.3 concentrations in remote areas. The observations for NH.sub.3 concentrations not decreasing as fast as estimated emission trends are consistent with a larger downward trend in annual particulate NH.sub.4 .sup.+ concentrations (1999-2014: MK: -47 %; LR: -49 %, p < 0.01, n = 23), associated with a lower formation of particulate NH.sub.4 .sup.+ in the atmosphere from gas phase NH.sub.3. A unique long-term dataset from the UK National Ammonia Monitoring Network(NAMN) is used here to assess spatial, seasonal and long-term variability inatmospheric ammonia (NH3: 1998–2014) and particulate ammonium(NH4+: 1999–2014) across the UK. Extensive spatial heterogeneity inNH3 concentrations is observed, with lowest annual mean concentrationsat remote sites (< 0.2 µg m−3) and highest in theareas with intensive agriculture (up to 22 µg m−3), whileNH4+ concentrations show less spatial variability (e.g. range of 0.14to 1.8 µg m−3 annual mean in 2005). Temporally, NH3concentrations are influenced by environmental conditions and local emissionsources. In particular, peak NH3 concentrations are observed in summerat background sites (defined by 5 km grid average NH3 emissions< 1 kg N ha−1 yr−1) and in areas dominated by sheepfarming, driven by increased volatilization of NH3 in warmer summertemperatures. In areas where cattle, pig and poultry farming is dominant, thelargest NH3 concentrations are in spring and autumn, matching periods ofmanure application to fields. By contrast, peak concentrations ofNH4+ aerosol occur in spring, associated with long-rangetransboundary sources. An estimated decrease in NH3 emissions by16 % between 1998 and 2014 was reported by the UK National AtmosphericEmissions Inventory. Annually averaged NH3 data from NAMN sitesoperational over the same period (n = 59) show an indicative downwardtrend, although the reduction in NH3 concentrations is smaller andnon-significant: Mann–Kendall (MK), −6.3 %; linear regression (LR),−3.1 %. In areas dominated by pig and poultry farming, a significantreduction in NH3 concentrations between 1998 and 2014 (MK: −22 %;LR: −21 %, annually averaged NH3) is consistent with, but not aslarge as the decrease in estimated NH3 emissions from this sector overthe same period (−39 %). By contrast, in cattle-dominated areas thereis a slight upward trend (non-significant) in NH3 concentrations (MK:+12 %; LR: +3.6 %, annually averaged NH3), despite theestimated decline in NH3 emissions from this sector since 1998(−11 %). At background and sheep-dominated sites, NH3concentrations increased over the monitoring period. These increases(non-significant) at background (MK: +17 %; LR: +13 %, annuallyaveraged data) and sheep-dominated sites (MK: +15 %; LR: +19 %,annually averaged data) would be consistent with the concomitant reduction inSO2 emissions over the same period, leading to a longer atmosphericlifetime of NH3, thereby increasing NH3 concentrations in remoteareas. The observations for NH3 concentrations not decreasing as fast asestimated emission trends are consistent with a larger downward trend inannual particulate NH4+ concentrations (1999–2014: MK: −47 %;LR: −49 %, p < 0.01, n = 23), associated with alower formation of particulateNH4+ in the atmosphere from gas phase NH3. A unique long-term dataset from the UK National Ammonia Monitoring Network (NAMN) is used here to assess spatial, seasonal and long-term variability in atmospheric ammonia (NH3: 1998–2014) and particulate ammonium (NH4+: 1999–2014) across the UK. Extensive spatial heterogeneity in NH3 concentrations is observed, with lowest annual mean concentrations at remote sites (< 0.2 µg m-3) and highest in the areas with intensive agriculture (up to 22 µg m-3), while NH4+ concentrations show less spatial variability (e.g. range of 0.14 to 1.8 µg m-3 annual mean in 2005). Temporally, NH3 concentrations are influenced by environmental conditions and local emission sources. In particular, peak NH3 concentrations are observed in summer at background sites (defined by 5 km grid average NH3 emissions < 1 kg N ha-1 yr-1) and in areas dominated by sheep farming, driven by increased volatilization of NH3 in warmer summer temperatures. In areas where cattle, pig and poultry farming is dominant, the largest NH3 concentrations are in spring and autumn, matching periods of manure application to fields. By contrast, peak concentrations of NH4+ aerosol occur in spring, associated with long-range transboundary sources. An estimated decrease in NH3 emissions by 16 % between 1998 and 2014 was reported by the UK National Atmospheric Emissions Inventory. Annually averaged NH3 data from NAMN sites operational over the same period (n= 59) show an indicative downward trend, although the reduction in NH3 concentrations is smaller and non-significant: Mann–Kendall (MK), -6.3 %; linear regression (LR),-3.1 %. In areas dominated by pig and poultry farming, a significant reduction in NH3 concentrations between 1998 and 2014 (MK: -22 %; LR: -21 %, annually averaged NH3) is consistent with, but not as large as the decrease in estimated NH3 emissions from this sector over the same period (-39 %). By contrast, in cattle-dominated areas there is a slight upward trend (non-significant) in NH3 concentrations (MK:+12 %; LR: +3.6 %, annually averaged NH3), despite the estimated decline in NH3 emissions from this sector since 1998 (-11 %). At background and sheep-dominated sites, NH3 concentrations increased over the monitoring period. These increases (non-significant) at background (MK: +17 %; LR: +13 %, annually averaged data) and sheep-dominated sites (MK: +15 %; LR: +19 %, annually averaged data) would be consistent with the concomitant reduction in SO2 emissions over the same period, leading to a longer atmospheric lifetime of NH3, thereby increasing NH3 concentrations in remote areas. The observations for NH3 concentrations not decreasing as fast as estimated emission trends are consistent with a larger downward trend in annual particulate NH4+ concentrations (1999–2014: MK: -47 %; LR: -49 %, p < 0.01, n= 23), associated with a lower formation of particulate NH4+ in the atmosphere from gas phase NH3. |
| Audience | Academic |
| Author | Vincent, Keith Tang, Yuk S. van Dijk, Netty Heal, Mathew R. Keenan, Patrick O. Dos Santos Pereira, Gloria Braban, Christine F. Sutton, Mark A. Conolly, Christopher Poskitt, Janet Smith, Rognvald I. Dragosits, Ulrike Dore, Anthony J. Simmons, Ivan |
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| Title | Drivers for spatial, temporal and long-term trends in atmospheric ammonia and ammonium in the UK |
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