ALBERT

Description: Methods for the determination of ship fuel sulphur content and NOx emission factors from remote measurements have been compared in the harbour of Rotterdam and compared to direct stack emission measurements on the ferry Stena Hollandica. The methods were selected based on a review of the available literature on ship emission measurements. They were either optical (LIDAR, DOAS, UV camera), combined with model based estimates of fuel consumption, or based on the so called "sniffer" principle, where SO2 or NOx emission factors are determined from simultaneous measurement of the increase of CO2 and SO2 or NOx concentrations in the plume of the ship compared to the background. The measurements were performed from stations at land, from a boat, and from a helicopter. Mobile measurement platforms were found to have important advantages compared to the landbased ones because they allow to optimize the sampling conditions and to sample from ships on the open sea. Although optical methods can provide reliable results, it was found that at the state of the art, the "sniffer" approach is the most convenient technique for determining both SO2 and NOx emission factors remotely. The average random error on the determination of SO2 emission factors comparing two identical instrumental set-ups was 6%. However, it was found that apparently minor differences in the instrumental characteristics, such as response time, could cause significant differences between the emission factors determined. Direct stack measurements showed that about 14% of the fuel sulphur content was not emitted as SO2. This was supported by the remote measurements and is in agreement with the results of other field studies.

Description: We present two Differential Optical Absorption Spectroscopy (DOAS) instruments built at RIVM, the RIVM DOAS and the miniDOAS. Both instruments provide virtually interference free measurements of NH3 concentrations in the atmosphere, since they measure over an open path, without suffering from inlet problems or interference problems by ammonium aerosols dissociating on tubes or filters. They measure concentrations up to at least 200 μg m−3, have a fast response, low maintenance demands, and a high up-time. The RIVM DOAS has a high accuracy of typically 0.15 μg m−3 for ammonia over 5-min averages and over a total light path of 100 m. The miniDOAS has been developed for application in measurement networks such as the Dutch National Air Quality Monitoring Network (LML). Compared to the RIVM DOAS it has a similar accuracy, but is significantly reduced in size, costs, and handling complexity. The RIVM DOAS and miniDOAS results showed excellent agreement (R2 = 0.996) during a field measurement campaign in Vredepeel, the Netherlands. This measurement site is located in an agricultural area and is characterized by highly variable, but on average high ammonia concentrations in the air. The RIVM-DOAS and miniDOAS results were compared to the results of the AMOR instrument, a continuous-flow wet denuder system, which is currently used in the LML. Averaged over longer time spans of typically a day the (mini)DOAS and AMOR results agree reasonably well, although an offset of the AMOR values compared to the (mini)DOAS results exists. On short time scales the (mini)DOAS shows a faster response and does not show the memory effects due to inlet tubing and transport of absorption fluids encountered by the AMOR. Due to its high accuracy, high uptime, low maintenance and its open path, the (mini)DOAS shows a good potential for flux measurements by using two (or more) systems in a gradient set-up and applying the aerodynamic gradient technique.

Description: From June to July 2009 more than thirty different in-situ and remote sensing instruments from all over the world participated in the Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI). The campaign took place at KNMI's Cabauw Experimental Site for Atmospheric Research in the Netherlands. Its main objectives were to determine the accuracy of state-of-the-art ground-based measurement techniques for the detection of atmospheric nitrogen dioxide (both in-situ and remote sensing), and to investigate their usability in satellite data validation. The expected outcomes are recommendations regarding the operation and calibration of such instruments, retrieval settings, and observation strategies for the use in ground-based networks for air quality monitoring and satellite data validation. Twenty-four optical spectrometers participated in the campaign, of which twenty-one had the capability to scan different elevation angles consecutively, the so-called Multi-axis DOAS systems, thereby collecting vertical profile information, in particular for nitrogen dioxide and aerosol. Various in-situ samplers simultaneously characterized the variability of atmospheric trace gases and the physical properties of aerosol particles. A large data set of continuous measurements of these atmospheric constituents has been collected under various meteorological conditions and air pollution levels. Together with the permanent measurement capability at the Cabauw site characterizing the meteorological state of the atmosphere, the CINDI campaign provided a comprehensive observational data set of atmospheric constituents in a highly polluted region of the world during summertime. First detailed comparisons performed with the CINDI data show that slant column measurements of NO2, O4 and HCHO with MAX-DOAS agree within 5 to 15%, vertical profiles of NO2 derived from several independent instruments agree within 25%, and MAX-DOAS aerosol optical thickness agrees within 20–30% with AERONET data. For the in-situ NO2 instrument using a molybdenum converter, a bias was found as large as 5 ppbv during day time, when compared to the other in-situ instruments using photolytic converters.

Description: In this paper we present the continued development of the miniDOAS, an active differential optical absorption spectroscopy (DOAS) instrument to measure ammonia concentrations in ambient air. The miniDOAS has been adapted for use in the Dutch National Air Quality Monitoring Network. The miniDOAS replaces the life-expired continuous-flow denuder ammonia monitor (AMOR). From September 2014 to December 2015, both instruments measured in parallel before the change from AMOR to miniDOAS was made. The instruments were deployed on six monitoring stations throughout the Netherlands. We report on the results of this intercomparison. Both instruments show a good uptime of ca. 90 %, adequate for an automatic monitoring network. Although both instruments produce minute values of ammonia concentrations, a direct comparison on short timescales such as minutes or hours does not give meaningful results, because the AMOR response to changing ammonia concentrations is slow. Comparisons between daily and monthly values show a good agreement. For monthly averages, we find a small average offset of 0.65 ± 0.28 µg m−3 and a slope of 1.034 ± 0.028, with the miniDOAS measuring slightly higher than the AMOR. The fast time resolution of the miniDOAS makes the instrument not only suitable for monitoring but also for process studies.

Description: Muliple Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) instruments can measure from the ground the absorption by nitrogen dioxide (NO2) of scattered sunlight seen in multiple viewing directions. This paper studies the potential of this technique to derive the vertical distribution of NO2 in the troposphere. Such profile information is essential in validation studies in which MAX-DOAS retrievals play a role. The retrieval algorithm used is based on a pre-calculated look-up table and assumes homogeneous mixing of aerosols and NO2 in layers extending from the surface to a variable height. Two retrieval models are compared: one including and one excluding an elevated NO2 layer at a fixed altitude in the free troposphere. An ensemble technique is applied to derive retrieved model uncertainties. Sensitivity studies demonstrate that MAX-DOAS based retrievals can make a distinction between an NO2 layer that extends from the surface to a certain height (having a constant mixing ratio, or a mixing ratio that decreases with altitude) and an elevated NO2 layer. The height of the elevated NO2 layer can only be retrieved accurately when the aerosol extinction profile is known and the measurement noise is low. The uncertainty in this elevated NO2 layer height provides the main source of uncertainty in the retrieval of the free tropospheric contribution to the tropospheric NO2 column. A comparison was performed with independent data, based on observations done at the CINDI campaign, held in the Netherlands in 2009. Comparison with lidar partial tropospheric NO2 columns showed a correlation of 0.78, and an average difference of 0.1× 1015 molec cm−2. The diurnal evolution of the NO2 volume mixing ratio measured by in-situ monitors at the surface and averaged over five days with cloud-free mornings, compares quite well to the MAX-DOAS retrieval: a correlation was found of 0.8, and an average difference of 0.2 ppb.