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81.
Effect of the Morphology of the High-Surface-Area Support on the Performance of the Oxygen-Evolution Reaction for Iridium Nanoparticles
Leonard Moriau, Marjan Bele, Živa Marinko, Francisco Ruiz-Zepeda, Gorazd Koderman, Martin Šala, Angelija Kjara Šurca, Janez Kovač, Iztok Arčon, Primož Jovanovič, Nejc Hodnik, Luka Suhadolnik, 2021, original scientific article

Abstract: The development of affordable, low-iridium-loading, scalable, active, and stable catalysts for the oxygen-evolution reaction (OER) is a requirement for the commercialization of proton-exchange membrane water electrolyzers (PEMWEs). However, the synthesis of high-performance OER catalysts with minimal use of the rare and expensive element Ir is very challenging and requires the identification of electrically conductive and stable high-surface-area support materials. We developed a synthesis procedure for the production of large quantities of a nanocomposite powder containing titanium oxynitride (TiONx) and Ir. The catalysts were synthesized with an anodic oxidation process followed by detachment, milling, thermal treatment, and the deposition of Ir nanoparticles. The anodization time was varied to grow three different types of nanotubular structures exhibiting different lengths and wall thicknesses and thus a variety of properties. A comparison of milled samples with different degrees of nanotubular clustering and morphology retention, but with identical chemical compositions and Ir nanoparticle size distributions and dispersions, revealed that the nanotubular support morphology is the determining factor governing the catalyst’s OER activity and stability. Our study is supported by various state-of-the-art materials’ characterization techniques, like X-ray photoelectron spectroscopy, scanning and transmission electron microscopies, Xray powder diffraction and absorption spectroscopy, and electrochemical cyclic voltammetry. Anodic oxidation proved to be a very suitable way to produce high-surface-area powder-type catalysts as the produced material greatly outperformed the IrO2 benchmarks as well as the Ir-supported samples on morphologically different TiONx from previous studies. The highest activity was achieved for the sample prepared with 3 h of anodization, which had the most appropriate morphology for the effective removal of oxygen bubbles.
Found in: osebi
Keywords: electrocatalysis, oxygen-evolution reaction, TiONx-Ir powder catalyst, iridium nanoparticles, anodic oxidation, morphology−activity correlation
Published: 04.01.2021; Views: 1706; Downloads: 0
.pdf Fulltext (6,36 MB)

82.
Multiresponsive nonvolatile memories based on optically switchable ferroelectric organic field-effect transistors
Martin Herder, Alex Dixon, Marco Carroli, Egon Pavlica, Stefan Hecht, Gvido Bratina, Emanuele Orgiu, Paolo Samorì, 2021, original scientific article

Abstract: Organic transistors are key elements for flexible, wearable, and biocompatible logic applications. Multiresponsivity is highly sought‐after in organic electronics to enable sophisticated operations and functions. Such a challenge can be pursued by integrating more components in a single device, each one responding to a specific external stimulus. Here, the first multiresponsive organic device based on a photochromic–ferroelectric organic field‐effect transistor, which is capable of operating as nonvolatile memory with 11 bit memory storage capacity in a single device, is reported. The memory elements can be written and erased independently by means of light or an electric field, with accurate control over the readout signal, excellent repeatability, fast response, and high retention time. Such a proof of concept paves the way toward enhanced functional complexity in optoelectronics via the interfacing of multiple components in a single device, in a fully integrated low‐cost technology compatible with flexible substrates.
Found in: osebi
Keywords: organic transistors, memory, time-dependent
Published: 11.03.2021; Views: 1318; Downloads: 0
.pdf Fulltext (281,34 KB)

83.
Elucidating local pollution and site representativeness at the Jungfraujoch, Switzerland through parallel aerosol measurements at an adjacent mountain ridge
Martin Gysel, Maxime Hervo, Urs Baltensperger, Markus Christian Leuenberger, Martine Collaud Coen, Stéphane Affolter, Günther Wehrle, Griša Močnik, Benjamin Brem, Nicolas Bukowiecki, 2021, original scientific article

Abstract: Many long-term air pollution and climate monitoring stations face the issue of increasing anthropogenic activities in their vicinity. Furthermore, the spatial representativeness of the sites is often not entirely understood especially in mountainous terrain with complex topographic features. This study presents a 5-year comparison of parallel aerosol measurements (total particle number concentration and equivalent black carbon mass concentration) at the Jungfraujoch in the Swiss Alps (JFJ, 3580 m a.s.l.), and an adjacent mountain ridge, the Jungfrau East Ridge (JER, 3705 m a.s.l.), in 1000 m air-line distance to the main site. The parallel aerosol measurements reveal characteristic differences in the diurnal variations between the two sites under certain specific meteorological conditions. Our analysis estimates that on 20-40% of the days local activities at the Jungfraujoch have a clear influence on the measured time series of the total aerosol number concentration and the equivalent black carbon mass concentration. This influence is mainly seen in form of strong isolated spikes rather than by an increase in the on-site background concentration. They can thus be flagged during the data quality assurance process and filtered from those measurement parameters available at high time resolution. Removing the spikes from the original time series results in daily mean values for the total aerosol number concentration and equivalent black carbon mass concentration that are 5-10 % lower compared to the original signals. During nighttime with hardly any local pollution sources that cause spikes this percentage decreases towards 0%. The signal baselines at the Jungfraujoch and Jungfrau East Ridge correlate well during more than 50% of the days.
Found in: osebi
Keywords: aerosol long-term monitoring, equivalent black carbon, aerosol number concentration, spatial variation
Published: 15.03.2021; Views: 1209; Downloads: 59
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84.
The impact of cloudiness and cloud type on the atmospheric heating rate of black and brown carbon in the Po Valley
Niccolò Losi, Ezio Bolzacchini, Gian Paolo Gobbi, Luca Di Liberto, Luca Ferrero, Asta Gregorič, Griša Močnik, Francesca Barnaba, Sergio Cogliati, Martin Rigler, 2021, original scientific article

Abstract: We experimentally quantified the impact of cloud fraction and cloud type on the heating rate (HR) of black and brown carbon (HRBC and HRBrC). In particular, we examined in more detail the cloud effect on the HR detected in a previous study (Ferrero et al., 2018). High-time-resolution measurements of the aerosol absorption coefficient at multiple wavelengths were coupled with spectral measurements of the direct, diffuse and surface reflected irradiance and with lidar–ceilometer data during a field campaign in Milan, Po Valley (Italy). The experimental set-up allowed for a direct determination of the total HR (and its speciation: HRBC and HRBrC) in all-sky conditions (from clear-sky conditions to cloudy). The highest total HR values were found in the middle of winter (1.43 ± 0.05 K d−1), and the lowest were in spring (0.54 ± 0.02 K d−1). Overall, the HRBrC accounted for 13.7 ± 0.2 % of the total HR, with the BrC being characterized by an absorption Ångström exponent (AAE) of 3.49 ± 0.01. To investigate the role of clouds, sky conditions were classified in terms of cloudiness (fraction of the sky covered by clouds: oktas) and cloud type (stratus, St; cumulus, Cu; stratocumulus, Sc; altostratus, As; altocumulus, Ac; cirrus, Ci; and cirrocumulus–cirrostratus, Cc–Cs). During the campaign, clear-sky conditions were present 23 % of the time, with the remaining time (77 %) being characterized by cloudy conditions. The average cloudiness was 3.58 ± 0.04 oktas (highest in February at 4.56 ± 0.07 oktas and lowest in November at 2.91 ± 0.06 oktas). St clouds were mostly responsible for overcast conditions (7–8 oktas, frequency of 87 % and 96 %); Sc clouds dominated the intermediate cloudiness conditions (5–6 oktas, frequency of 47 % and 66 %); and the transition from Cc–Cs to Sc determined moderate cloudiness (3–4 oktas); finally, low cloudiness (1–2 oktas) was mostly dominated by Ci and Cu (frequency of 59 % and 40 %, respectively). HR measurements showed a constant decrease with increasing cloudiness of the atmosphere, enabling us to quantify for the first time the bias (in %) of the aerosol HR introduced by the simplified assumption of clear-sky conditions in radiative-transfer model calculations. Our results showed that the HR of light-absorbing aerosol was ∼ 20 %–30 % lower in low cloudiness (1–2 oktas) and up to 80 % lower in completely overcast conditions (i.e. 7–8 oktas) compared to clear-sky ones. This means that, in the simplified assumption of clear-sky conditions, the HR of light-absorbing aerosol can be largely overestimated (by 50 % in low cloudiness, 1–2 oktas, and up to 500 % in completely overcast conditions, 7–8 oktas). The impact of different cloud types on the HR was also investigated. Cirrus clouds were found to have a modest impact, decreasing the HRBC and HRBrC by −5 % at most. Cumulus clouds decreased the HRBC and HRBrC by −31 ± 12 % and −26 ± 7 %, respectively; cirrocumulus–cirrostratus clouds decreased the HRBC and HRBrC by −60 ± 8 % and −54 ± 4 %, which was comparable to the impact of altocumulus (−60 ± 6 % and −46 ± 4 %). A higher impact on the HRBC and HRBrC suppression was found for stratocumulus (−63 ± 6 % and −58 ± 4 %, respectively) and altostratus (−78 ± 5 % and −73 ± 4 %, respectively). The highest impact was associated with stratus, suppressing the HRBC and HRBrC by −85 ± 5 % and −83 ± 3 %, respectively. The presence of clouds caused a decrease of both the HRBC and HRBrC (normalized to the absorption coefficient of the respective species) of −11.8 ± 1.2 % and −12.6 ± 1.4 % per okta. This study highlights the need to take into account the role of both cloudiness and different cloud types when estimating the HR caused by both BC and BrC and in turn decrease the uncertainties associated with the quantification of their impact on the climate.
Found in: osebi
Keywords: black carbon, brown carbon, cloud, atmospheric heating rate, climate change
Published: 29.03.2021; Views: 1484; Downloads: 0
.pdf Fulltext (8,61 MB)

85.
Determination of Aethalometer multiple-scattering enhancement parameters and impact on source apportionment during the winter 2017/18 EMEP/ACTRIS/COLOSSAL campaign in Milan
Asta Gregorič, Dario Massabo, Griša Močnik, Paolo Prati, Martin Rigler, Luca Santagostini, Ezio Bolzacchini, Alice Corina Forello, Vera Bernardoni, Luca Ferrero, 2021, original scientific article

Abstract: In the frame of the EMEP/ACTRIS/COLOSSAL campaign in Milan during winter 2018, equivalent black carbon measurements using the Aethalometer 31 (AE31), the Aethalometer 33 (AE33), and a Multi-Angle Absorption Photometer (MAAP) were carried out together with levoglucosan analyses on 12 h resolved PM2.5 samples collected in parallel. From AE31 and AE33 data, the loading-corrected aerosol attenuation coefficients (bATN) were calculated at seven wavelengths (λ, where λ values are 370, 470, 520, 590, 660, 880, and 950 nm). The aerosol absorption coefficient at 637 nm (babs_MAAP) was determined by MAAP measurements. Furthermore, babs was also measured at four wavelengths (405, 532, 635, 780 nm) on the 12 h resolved PM2.5 samples by a polar photometer (PP_UniMI). After comparing PP_UniMI and MAAP results, we exploited PP_UniMI data to evaluate the filter multiple-scattering enhancement parameter at different wavelengths for AE31 and AE33. We obtained instrument- and wavelength-dependent multiple-scattering enhancement parameters by linear regression of the Aethalometer bATN against the babs measured by PP_UniMI. We found significant dependence of the multiple-scattering enhancement parameter on filter material, hence on the instrument, with a difference of up to 30 % between the AE31 and the AE33 tapes. The wavelength dependence and day–night variations were small – the difference between the smallest and largest value was up to 6 %. Data from the different instruments were used as input to the so-called “Aethalometer model” for optical source apportionment, and instrument dependence of the results was investigated. Inconsistencies among the source apportionment were found fixing the AE31 and AE33 multiple-scattering enhancement parameters to their usual values. In contrast, optimised multiple-scattering enhancement parameters led to a 5 % agreement among the approaches. Also, the component apportionment “MWAA model” (Multi-Wavelength Absorption Analyzer model) was applied to the dataset. It was less sensitive to the instrument and the number of wavelengths, whereas significant differences in the determination of the absorption Ångström exponent for brown carbon were found (up to 22 %).
Found in: osebi
Keywords: black carbon, filter photometer, Aethalometer, source apportionment
Published: 16.04.2021; Views: 1448; Downloads: 0
.pdf Fulltext (1,95 MB)

86.
Consistent determination of the heating rate of light-absorbing aerosol using wavelength- and time-dependent Aethalometer multiple-scattering correction
Martin Rigler, Asta Gregorič, Griša Močnik, Dario Massabò, Sara Valentini, Francesca Soldan, Sergio Cogliati, Luca Santagostini, Vera Bernardoni, Luca Ferrero, 2021, original scientific article

Abstract: Accurate and temporally consistent measurements of light absorbing aerosol (LAA) heating rate (HR) and of its source apportionment (fossil-fuel, FF; biomass-burning, BB) and speciation (black and brown Carbon; BC, BrC) are needed to evaluate LAA short-term climate forcing. For this purpose, wavelength- and time-dependent accurate LAA absorption coefficients are required. HR was experimentally determined and apportioned (sources/species) in the EMEP/ACTRIS/COLOSSAL-2018 winter campaign in Milan (urban-background site). Two Aethalometers (AE31/AE33) were installed together with a MAAP, CPC, OPC, a low volume sampler (PM2.5) and radiation instruments. AE31/AE33 multiple-scattering correction factors (C) were determined using two reference systems for the absorption coefficient: 1) 5-wavelength PP_UniMI with low time resolution (12 h, applied to PM2.5 samples); 2) timely-resolved MAAP data at a single wavelength. Using wavelength- and time-independent C values for the AE31 and AE33 obtained with the same reference device, the total HR showed a consistency (i.e. reproducibility) with average values comparable at 95% probability. However, if different reference devices/approaches are used, i.e. MAAP is chosen as reference instead of a PP_UniMI, the HR can be overestimated by 23-30% factor (by both AE31/AE33). This became more evident focusing on HR apportionment: AE33 data (corrected by a wavelength- and time-independent C) showed higher HRFF (+24±1%) and higher HRBC (+10±1%) than that of AE31. Conversely, HRBB and HRBrC were -28±1% and -29±1% lower for AE33 compared to AE31. These inconsistencies were overcome by introducing a wavelength-dependent Cλ for both AE31 and AE33, or using multi-wavelength apportionment methods, highlighting the need for further studies on the influence of wavelength corrections for HR determination. Finally, the temporally-resolved determination of C resulted in a diurnal cycle of the HR not statistically different whatever the source- speciation- apportionment used.
Found in: osebi
Keywords: climate change, heating rate, black carbon, light absorbing aerosols
Published: 09.06.2021; Views: 1189; Downloads: 0
.pdf Fulltext (2,02 MB)

87.
88.
Determination of the multiple-scattering correction factor and its cross-sensitivity to scattering and wavelength dependence for different AE33 Aethalometer filter tapes
Andres Alastuey, Griša Močnik, Vera Bernardoni, Jesús Yus-Díez, Davide Ciniglia, Matic Ivančič, Xavier Querol, Noemí Perez, Cristina Reche, Martin Rigler, Roberta Vecchi, Sara Valentini, Marco Pandolfi, 2021, original scientific article

Abstract: Providing reliable observations of aerosol particles' absorption properties at spatial and temporal resolutions suited to climate models is of utter importance to better understand the effects that atmospheric particles have on climate. Nowadays, one of the instruments most widely used in international monitoring networks for in situ surface measurements of light absorption properties of atmospheric aerosol particles is the multi-wavelength dual-spot Aethalometer, AE33. The AE33 derives the absorption coefficients of aerosol particles at seven different wavelengths from the measurements of the optical attenuation of light through a filter where particles are continuously collected. An accurate determination of the absorption coefficients from the AE33 instrument relies on the quantification of the non-linear processes related to the sample collection on the filter. The multiple-scattering correction factor (C), which depends on the filter tape used and on the optical properties of the collected particles, is the parameter with both the greatest uncertainty and the greatest impact on the absorption coefficients derived from the AE33 measurements. Here we present an in-depth analysis of the AE33 multiple-scattering correction factor C and its wavelength dependence for two different and widely used filter tapes, namely the old, and most referenced, TFE-coated glass, or M8020, filter tape and the currently, and most widely used, M8060 filter tape. For performing this analysis, we compared the attenuation measurements from AE33 with the absorption coefficients measured with different filter-based techniques. On-line co-located multi-angle absorption photometer (MAAP) measurements and off-line PP_UniMI polar photometer measurements were employed as reference absorption measurements for this work. To this aim, we used data from three different measurement stations located in the north-east of Spain, namely an urban background station (Barcelona, BCN), a regional background station (Montseny, MSY) and a mountaintop station (Montsec d'Ares, MSA). The median C values (at 637 nm) measured at the three stations ranged between 2.29 (at BCN and MSY, lowest 5th percentile of 1.97 and highest 95th percentile of 2.68) and 2.51 (at MSA, lowest 5th percentile of 2.06 and highest 95th percentile of 3.06). The analysis of the cross-sensitivity to scattering, for the two filter tapes considered here, revealed a large increase in the C factor when the single-scattering albedo (SSA) of the collected particles was above a given threshold, up to a 3-fold increase above the average C values. The SSA threshold appeared to be site dependent and ranged between 0.90 to 0.95 for the stations considered in the study. The results of the cross-sensitivity to scattering displayed a fitted constant multiple-scattering parameter, Cf, of 2.21 and 1.96, and a cross-sensitivity factor, ms, of 1.8 % and 3.4 % for the MSY and MSA stations, respectively, for the TFE-coated glass filter tape. For the M8060 filter tape, Cf values of 2.50, 1.96 and 1.82 and ms values of 1.6 %, 3.0 % and 4.9 % for the BCN, MSY and MSA stations, respectively, were obtained. SSA variations also influenced the spectral dependence of C, which showed an increase with wavelength when SSA was above the site-dependent threshold. Below the SSA threshold, no statistically significant dependence of C on the wavelength was observed. For the measurement stations considered here, the wavelength dependence of C was to some extent driven by the presence of dust particles during Saharan dust outbreaks that had the potential to increase the SSA above the average values. At the mountaintop station, an omission of the wavelength dependence of the C factor led to an underestimation of the absorption Ångström exponent (AAE) by up to 12 %. Differences in the absorption coefficient determined from AE33 measurements at BCN, MSY and MSA of around 35 %–40 % can be expected when using the site-dependent experimentally obtained C value instead of the nominal C value. Due to the fundamental role that the SSA of the particles collected on the filter tape has in the multiple-scattering parameter C, we present a methodology that allows the recognition of the conditions upon which the use of a constant and wavelength-independent C is feasible.
Found in: osebi
Keywords: black carbon, aerosol absorption, filter photometer, artifact
Published: 01.10.2021; Views: 1049; Downloads: 0
.pdf Fulltext (1,76 MB)

89.
Black carbon emission factors of diesel vehicles
Martin Rigler, Irena Ježek, Asta Gregorič, Matic Ivančič, Bálint Alföldy, 2021, published scientific conference contribution abstract

Found in: osebi
Keywords: black carbon, emission factor, aethalometer
Published: 17.11.2021; Views: 910; Downloads: 4
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90.
Optical absorption properties of mineral dust particles generated by storm events in a desert environment
Martin Rigler, Asta Gregorič, Matic Ivančič, Mohamed M. Mahfouz, Bálint Alföldy, 2021, published scientific conference contribution abstract

Found in: osebi
Keywords: mineral dust, optical absorption
Published: 17.11.2021; Views: 942; Downloads: 43
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