Modelling trends in ammonia in the Netherlands over the 1990-2014

This study investigates to what extent emissions of ammonia, physicochemical processes and meteorology affect the trend in the atmospheric ammonia in the Netherlands between 1993 and 2014. Two distinct periods were distinguished: a period of declining ammonia concentrations between 1993 and 2004 and a period of slightly increasing ammonia concentrations between 2005 and 2014. In the first period, large emission reductions were reported, while the second period is characterized by smaller emission reductions. The Operational Priority Substances (OPS) model was used to quantify the effects of meteorology and physicochemical processes on atmospheric ammonia concentrations. The general performance of the OPS model for ammonia concentration, ammonium concentration and wet deposition of ammonia/ammonium is quite good when evaluated with observations over the whole period. For the period 1993-2004, model sensitivity runs show that the change in atmospheric chemical conditions and specific meteorological conditions can largely explain the smaller decline in ammonia concentrations compared with the decline in ammonia emissions. Uncertainties in emissions such as changes in the timing of manure applications and uncertainties in the estimated excretion and grazing emissions might partly explain remaining differences at the beginning of the period. Low-emission manure spreading techniques have an important reducing effect on the atmospheric ammonia concentration. Without these techniques, the ammonia concentrations at the measurement stations would have been about 3.5-41.1,mu g m(-3) higher in recent years. In the period between 2005 and 2014 emissions declined at a much lower rate, but the observed concentrations increased slightly. One third of the observed difference in trends can again be explained by the changed chemical conditions while no explanation has yet been found for the rest. (C) 2017 The Authors. Published by Elsevier Ltd.