Measurement report: Determination of Black Carbon concentration in PM<sub>2.5</sub> fraction by Multi-wavelength absorption black carbon instrument (MABI)

Ryś, Anna; Samek, Lucyna

doi:https://doi.org/10.5194/acp-2021-766

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https://doi.org/10.5194/acp-2021-766

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11 Oct 2021

| 11 Oct 2021

Status: this preprint has been withdrawn by the authors.

Measurement report: Determination of Black Carbon concentration in PM_2.5 fraction by Multi-wavelength absorption black carbon instrument (MABI)

Anna Ryś and Lucyna Samek

Abstract. The evaluation of black carbon (BC) sources is very important, especially in environmental sciences. This study shows how the contributions of biomass burning and fossil fuel/traffic to PM_2.5 mass can be assessed. MABI was used for this purpose and gave the possibility to measure the transmission of light at different wavelengths. Absorption coefficients were calculated from measurements data and recalculated for concentrations of eBC. The samples of PM_2.5 fraction were collected from February 1, 2020 to March 27, 2021 every third day in Krakow, Poland (50°04' N, 19°54'47" E). The concentrations of equivalent BC (eBC) from fossil fuel/traffic and biomass burning were in the range 0.82–11.64 μg m⁻³) and 0.007–0.84 μg m⁻³, respectively. At the same time, PM_2.5 concentrations varied from 3.14 to 55.24 μg m⁻³. It means that about 18 % of PM_2.5 mass belongs to eBC and 11.3 % of this value comes from biomass burning. The eBC contribution is the significant part of PM_2.5 mass and we observed seasonal variation of the eBC concentration during the year with the peak in winter. The contribution of biomass burning to PM_2.5 mass is more stable during the whole year. The eBC concentration during workdays is a bit higher than during weekend days but biomass burning is similar for both days (work and weekend taken as the mean for the whole period).

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Received: 07 Sep 2021 – Discussion started: 11 Oct 2021

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Anna Ryś and Lucyna Samek

Interactive discussion

Status: closed

CC1:
'Comment on acp-2021-766', Cheng Wu, 01 Nov 2021
This study (acp-2021-766) reported a one-year eBC measurement study in Poland using a multiwavelength absorption black carbon instrument (MABI). MABI is a newly developed offline filter-based absorption photometer that provides more wavelengths (7λ) than the existing OT-21 (2λ) and MWAA (3λ). The application of MABI could provide more information to study the spectral characteristics of light-absorbing aerosols. However, the following concerns need to be addressed.
Line 105. The assumption of the multi-scattering correction factor C_ref =1 is arbitrary. C_ref is not only filter type specific (Presler-Jur et al., 2017), but also site specific (Coen et al., 2010). Teflon filter usually has a C_ref value smaller than the quartz filter (Pandey et al., 2019). The exact value of C_ref can only be determined through co-located field comparisons with a reference instrument (e.g. photo-acoustic spectrometry).

The MAE_eBC used in this study (6.036 m²g^-1 @ 639 nm) lacks scientific evidence. Neither the MABI manual nor the recent MABI paper (Manohar et al., 2021) had shown how MAE_eBC was derived. The key question is that for the MAE_eBC used in MABI, which EC protocol is aligning with? For example, the MAE_eBC used in the aethalometer was aligning with EC determined by Lawrence Berkeley Laboratory evolved gas analysis (EGA) protocol (Gundel et al., 1984). The MAE_eBC used in MAAP was aligning with EC determined by VDI part 1 protocol (Petzold and Schonlinner, 2004). How MAE_eBC was derived was not clear in the current manuscript.

The use of the delta-C approach for BB-derived eBC was questionable. A study in the UK has shown that the delta-C approach derived BC_bb is unreliable (Harrison et al., 2013). The Aethalometer AAE model has its limitations for resolving BC from BB, which is only valid when the variability of AAE is dominated by primary brown carbon. The study by Lack and Langridge (2013) had shown that a transparent coating on BC can also lead to an increase of AAE of BC up to 1.5. As a result, the Aethalometer model/delta-C method is only valid when the primary brown carbon contribution is much higher than the lensing effect. The BC_bb/eBC ratio found in this study was lowest in winter, which is unreasonable. Since BB emissions were active during winter, BC_bb/eBC ratio is expected to be higher than other seasons. The authors should provide more evidence (e.g. a good correlation between delta-C and levoglucosan or potassium) to prove that this method is suitable for the samples used in this study.

References
Coen, M. C., Weingartner, E., Apituley, A., Ceburnis, D., Fierz-Schmidhauser, R., Flentje, H., Henzing, J. S., Jennings, S. G., Moerman, M., Petzold, A., Schmid, O., and Baltensperger, U.: Minimizing light absorption measurement artifacts of the Aethalometer: evaluation of five correction algorithms, Atmos. Meas. Tech., 3, 457-474, doi: https://doi.org/10.5194/amt-3-457-2010, 2010.
Gundel, L. A., Dod, R. L., Rosen, H., and Novakov, T.: The Relationship between Optical Attenuation and Black Carbon Concentration for Ambient and Source Particles, Sci. Total. Environ., 36, 197-202, doi: https://doi.org/10.1016/0048-9697(84)90266-3, 1984.
Harrison, R. M., Beddows, D. C. S., Jones, A. M., Calvo, A., Alves, C., and Pio, C.: An evaluation of some issues regarding the use of aethalometers to measure woodsmoke concentrations, Atmos. Environ., 80, 540-548, doi: https://doi.org/10.1016/j.atmosenv.2013.08.026, 2013.
Lack, D. A. and Langridge, J. M.: On the attribution of black and brown carbon light absorption using the Ångström exponent, Atmos. Chem. Phys., 13, 10535-10543, doi: https://doi.org/10.5194/acp-13-10535-2013, 2013.
Manohar, M., Atanacio, A., Button, D., and Cohen, D.: MABI - A multi-wavelength absorption black carbon instrument for the measurement of fine light absorbing carbon particles, Atmospheric Pollut. Res., 12, 133-140, doi: https://doi.org/10.1016/j.apr.2021.02.009, 2021.
Pandey, A., Shetty, N. J., and Chakrabarty, R. K.: Aerosol light absorption from optical measurements of PTFE membrane filter samples: sensitivity analysis of optical depth measures, Atmos. Meas. Tech., 12, 1365-1373, doi: https://doi.org/10.5194/amt-12-1365-2019, 2019.
Petzold, A. and Schonlinner, M.: Multi-angle absorption photometry - a new method for the measurement of aerosol light absorption and atmospheric black carbon, J. Aerosol. Sci., 35, 421-441, doi: https://doi.org/10.1016/j.jaerosci.2003.09.005, 2004.
Presler-Jur, P., Doraiswamy, P., Hammond, O., and Rice, J.: An Evaluation of Mass Absorption Cross-Section for Optical Carbon Analysis on Teflon Filter Media, J. Air Waste Manage. Assoc., 67, 1213-1228 doi: https://doi.org/10.1080/10962247.2017.1310148, 2017.
Citation: https://doi.org/10.5194/acp-2021-766-CC1
- AC1:
  'Reply on CC1', Lucyna Samek, 14 Nov 2021
  This study (acp-2021-766) reported a one-year eBC measurement study in Poland using a multiwavelength absorption black carbon instrument (MABI). MABI is a newly developed offline filter-based absorption photometer that provides more wavelengths (7λ) than the existing OT-21 (2λ) and MWAA (3λ). The application of MABI could provide more information to study the spectral characteristics of light-absorbing aerosols. However, the following concerns need to be addressed.
  Reply: We would like to thank for valuable feedback. Please see attached for our response to comments.
  Line 105. The assumption of the multi-scattering correction factor C_ref =1 is arbitrary. C_ref is not only filter type specific (Presler-Jur et al., 2017), but also site specific (Coen et al., 2010). Teflon filter usually has a C_ref value smaller than the quartz filter (Pandey et al., 2019). The exact value of C_ref can only be determined through co-located field comparisons with a reference instrument (e.g. photo-acoustic spectrometry).
  
  Reply: Based on “Summary of Light Absorbing Carbon and Visibility Measurements and Terms” (Cohen, 2020), the authors assumed C_ref = 1. This paper (Cohen, 2020) provides deeply discussion about C_ref for different type of filters and sizes of particulate matter, among other on page 10. Moreover very similar research, to the present in current manuscript, was conducted during a comparble period in Poland (Zioła et al., 2021) The condition and type of location were very similar, but measurement was conducted by different instrument (a modern Aethalometer AE33). This study presents comparable results with shown in the manuscript, which was expected. They have annual average of eBC concentration equal to 3.22±2.81µg/m³ compared with our study 3.5±1.5µg/m³. As of today, our research group does not have possible to performe co-located field comparisons with reference instrument .
  The MAE_eBC used in this study (6.036 m²g^-1 @ 639 nm) lacks scientific evidence. Neither the MABI manual nor the recent MABI paper (Manohar et al., 2021) had shown how MAE_eBC was derived. The key question is that for the MAE_eBC used in MABI, which EC protocol is aligning with? For example, the MAE_eBC used in the aethalometer was aligning with EC determined by Lawrence Berkeley Laboratory evolved gas analysis (EGA) protocol (Gundel et al., 1984). The MAE_eBC used in MAAP was aligning with EC determined by VDI part 1 protocol (Petzold and Schonlinner, 2004). How MAE_eBC was derived was not clear in the current manuscript.
  
  Reply: The MAE_eBC used in this study was recommended by the Australian Nuclear Science and Technology Organisation (ANSTO) in ANSTO External Report ER-790 (Cohen, 2020). In this report -“Summary of Light Absorbing Carbon and Visibility Measurements and Terms”, you can find discussion about results of research and analysis which have done over the years. The aspect raised in this point described among other on page 11, and 15 – 17. The comparison of the results of MABI measurements and Aethalometer was presented by Manohar (Manohar et al., 2021).
  
  The article aimed to present the method of calculating the results obtained by MABI based on the paper provided particular by ANSTO. Moreover, authors wanted to show the result for BC by MABI, which can show general BC situation in Krakow and give opportunity to compare BC result in the future.
  The use of the delta-C approach for BB-derived eBC was questionable. A study in the UK has shown that the delta-C approach derived BC_bb is unreliable (Harrison et al., 2013). The Aethalometer AAE model has its limitations for resolving BC from BB, which is only valid when the variability of AAE is dominated by primary brown carbon. The study by Lack and Langridge (2013) had shown that a transparent coating on BC can also lead to an increase of AAE of BC up to 1.5. As a result, the Aethalometer model/delta-C method is only valid when the primary brown carbon contribution is much higher than the lensing effect. The BC_bb/eBC ratio found in this study was lowest in winter, which is unreasonable. Since BB emissions were active during winter, BC_bb/eBC ratio is expected to be higher than other seasons. The authors should provide more evidence (e.g. a good correlation between delta-C and levoglucosan or potassium) to prove that this method is suitable for the samples used in this study.
  
  Reply: Our comprehensive study provides that potassium is the highest in winter, and the lowest in summer. Please take a look, on Table 1, that the values for BC_BB shows similar relation, the highest value is in winter (0.4±0.3 µg/m³) and the lowest is in summer (0.2±0.1 µg/m³). Moreover, the values for eBC are also the highest in winter (5.3±1.8 µg/m³), what is expected. The relative contribution of biomass (BC_BB) to eBC, present in this table for winter, shows that the higher excess of eBC contribution from fossil fuels than biomass burning was observed during winter. Our results for BC_BB annual average concentration is 0.25±0.15 µg/m³ and it is lower than in Zabrze (Poland) (0.93±0.76. µg/m³) (Ziola et al., 2021). It can probably be connected with introduction in September 2019 of ban of burning wood and coal in Krakow.
  
  Period
  
  K (ng m^-3)
  
  u(K) (ng m^-3)
  
  Spring
  
  117
  
  2
  
  Summer
  
  65
  
  1
  
  Autumn
  
  159
  
  4
  
  Winter
  
  197
  
  3
  
  Reply: Bibliography:
  Cohen, D. D.: Summary of Light Absorbing Carbon and Visibility Measurements and Terms. ANSTO External Report ER-790, ISBN – 1 921268 32 8, October 2020., 2020.
  Manohar, M., Atanacio, A., Button, D. and Cohen, D.: MABI - A multi-wavelength absorption black carbon instrument for the measurement of fine light absorbing carbon particles, Atmos. Pollut. Res., 12(4), 133–140, https://doi.org/https://doi.org/10.1016/j.apr.2021.02.009, 2021.
  Zioła, N., Błaszczak, B. and Klejnowski, K.: Temporal Variability of Equivalent Black Carbon Components in Atmospheric Air in Southern Poland, Atmosphere (Basel)., 12(1), https://doi.org/10.3390/atmos12010119, 2021.
  
  References
  Coen, M. C., Weingartner, E., Apituley, A., Ceburnis, D., Fierz-Schmidhauser, R., Flentje, H., Henzing, J. S., Jennings, S. G., Moerman, M., Petzold, A., Schmid, O., and Baltensperger, U.: Minimizing light absorption measurement artifacts of the Aethalometer: evaluation of five correction algorithms, Atmos. Meas. Tech., 3, 457-474, doi: https://doi.org/10.5194/amt-3-457-2010, 2010.
  Gundel, L. A., Dod, R. L., Rosen, H., and Novakov, T.: The Relationship between Optical Attenuation and Black Carbon Concentration for Ambient and Source Particles, Sci. Total. Environ., 36, 197-202, doi: https://doi.org/10.1016/0048-9697(84)90266-3, 1984.
  Harrison, R. M., Beddows, D. C. S., Jones, A. M., Calvo, A., Alves, C., and Pio, C.: An evaluation of some issues regarding the use of aethalometers to measure woodsmoke concentrations, Atmos. Environ., 80, 540-548, doi: https://doi.org/10.1016/j.atmosenv.2013.08.026, 2013.
  Lack, D. A. and Langridge, J. M.: On the attribution of black and brown carbon light absorption using the Ångström exponent, Atmos. Chem. Phys., 13, 10535-10543, doi: https://doi.org/10.5194/acp-13-10535-2013, 2013.
  Manohar, M., Atanacio, A., Button, D., and Cohen, D.: MABI - A multi-wavelength absorption black carbon instrument for the measurement of fine light absorbing carbon particles, Atmospheric Pollut. Res., 12, 133-140, doi: https://doi.org/10.1016/j.apr.2021.02.009, 2021.
  Pandey, A., Shetty, N. J., and Chakrabarty, R. K.: Aerosol light absorption from optical measurements of PTFE membrane filter samples: sensitivity analysis of optical depth measures, Atmos. Meas. Tech., 12, 1365-1373, doi: https://doi.org/10.5194/amt-12-1365-2019, 2019.
  Petzold, A. and Schonlinner, M.: Multi-angle absorption photometry - a new method for the measurement of aerosol light absorption and atmospheric black carbon, J. Aerosol. Sci., 35, 421-441, doi: https://doi.org/10.1016/j.jaerosci.2003.09.005, 2004.
  Presler-Jur, P., Doraiswamy, P., Hammond, O., and Rice, J.: An Evaluation of Mass Absorption Cross-Section for Optical Carbon Analysis on Teflon Filter Media, J. Air Waste Manage. Assoc., 67, 1213-1228 doi: https://doi.org/10.1080/10962247.2017.1310148, 2017.
  
  Citation: https://doi.org/10.5194/acp-2021-766-AC1
RC1: 'Comment on acp-2021-766', Anonymous Referee #1, 15 Nov 2021

The comment was uploaded in the form of a supplement: https://acp.copernicus.org/preprints/acp-2021-766/acp-2021-766-RC1-supplement.pdf

Citation: https://doi.org/10.5194/acp-2021-766-RC1
RC2: 'Comment on acp-2021-766', Anonymous Referee #2, 15 Nov 2021

REVIEW of Rys and Samek

Measurement report: Determination of Black Carbon concentration in PM2.5 fraction by Multi-wavelength absorption black carbon instrument (MABI), Atmos. Chem. Phys. 2021-766

https://doi.org/10.5194/acp-2021-766

The authors present results of a more than 1 year measurement campaign in Krakow, Poland, with a new instrument – the Multi-wavelength absorption black carbon instrument (MABI). While the manuscript is a “measurement report”, it still lacks vital information to warrant its publication in ACP. The topic is treated superficially. The manuscript does not meet the standard of publication, and I recommend its rejection.

There have been numerous publications on the state-of-the-art absorption filter photometers, ranging from the characterization of new instrumentation (Bond et al., 1999; Drinovec et al., 2015; Ogren et al., 2017), the methodologies to post-process the data (Park et al., 2010; Virkkula et al., 2007; Weingartner et al., 2003), to the measurements, quantifying the limitations of filter photometers (Bernardoni et al., 2021; Yus-Diez et al., 2021). The interpretation of the data from the presented measurement campaign should address the issues described in the literature. I specify the most blatant omissions below.

The sampling of the filters was performed for 24 hours. With the concentrations reported, there are significant loading effects present (see for example, Bond et al., 1999; Drinovec et al., 2015; Park et al., 2010; Weingartner et al., 2003). These need to be addresses. The loading effects are wavelength dependent and the reported Angstrom exponent alpha=0.6 (the authors should avoid an excessive number of digits beyond any reasonable measurement uncertainty) will increase once this is addressed. The assumption of C=R=1 is probably wrong, but we do not know how this correction is parametrized as there are no links to the MABI manual in the manuscript, and this shall remain an open question.

It is unclear if the epsilon is the absorption coefficient (units m^-1) or the mass absorption cross-section (units m²g^-1). If this is MAC, then the explanation on the measurement of mass is lacking in the manuscript.

The wavelength difference method is a very simplistic and non-quantitative way to perform source apportionment and much more sophisticated methods are available in the literature (starting with Sandradewi et al., 2008). The 11.3% BC apportioned to biomass burning should be reported to the nearest 1% and its uncertainty should be determined.

The source apportionment methods using filter photometers use the PM optical properties to determine the contribution of sources to BC. The presented results do not take into account that coal combustion could also result in PM absorbing strongly at low wavelengths. More sophisticated studies in Krakow (Tobler et al., 2021) have opted to use “solid fuel” rather than specifying the fuel type due to this possibility.

References

Bernardoni, V., Ferrero, L., Bolzacchini, E., Forello, A. C., GregoriÄ, A., Massabò, D., MoÄnik, G., Prati, P., Rigler, M., Santagostini, L., Soldan, F., Valentini, S., Valli, G., and Vecchi, R.: Determination of Aethalometer multiple-scattering enhancement parameters and impact on source apportionment during the winter 2017/18 EMEP/ACTRIS/COLOSSAL campaign in Milan, Atmos. Meas. Tech., 14, 2919–2940, https://doi.org/10.5194/amt-14-2919-2021, 2021.

Bond, T. C., Anderson, T. L., and Campbell, D.: Calibration and intercomparison of filter-based measurements of visible light absorption by aerosols, Aerosol Sci. Tech., 30, 582–600, 1999.

Drinovec, L., MoÄnik, G., Zotter, P., Prévôt, A. S. H., Ruckstuhl, C., Coz, E., Rupakheti, M., Sciare, J., Müller, T., Wiedensohler, A., and Hansen, A. D. A.: The "dual-spot" Aethalometer: an improved measurement of aerosol black carbon with real-time loading compensation, Atmos. Meas. Tech., 8, 1965–1979, https://doi.org/10.5194/amt-8-1965-2015, 2015.

Ogren, J. A., Wendell, J., Andrews, E., and Sheridan, P. J.: Continuous light absorption photometer for long-term studies, Atmos. Meas. Tech., 10, 4805–4818, https://doi.org/10.5194/amt-10-4805-2017, 2017.

Park, S. S., Hansen, A. D. A., and Cho, Y.: Measurement of real time black carbon for investigating spot loading effects of Aethalometer data, Atmos. Environ., 11, 1449–1455, doi:10.1016/j.atmosenv.2010.01.025, 2010.

Sandradewi, J., Prévôt, A. S. H., Szidat, S., Perron, N., Alfarra, M. R., Lanz, V. A., Weingartner, E., and Baltensperger, U.: Using aerosol light absorption measurements for the quantitative determination of wood burning and traffic emission contributions to particulate matter, Environ. Sci. Technol., 42, 3316–3323, https://doi.org/10.1021/es702253m, 2008.

Tobler, A. K., Skiba, A., Canonaco, F., MoÄnik, G., Rai, P., Chen, G., Bartyzel, J., Zimnoch, M., Styszko, K., NÄcki, J., Furger, M., RóÅ¼aÅski, K., Baltensperger, U., Slowik, J. G., and Prevot, A. S. H.: Characterization of non-refractory (NR) PM1 and source apportionment of organic aerosol in Kraków, Poland, Atmos. Chem. Phys., 21, 14893–14906, https://doi.org/10.5194/acp-21-14893-2021, 2021.

Virkkula, A., Mäkelä, T., Hillamo, R., Yli-Tuomi, T., Hirsikko, A., Hämeri, K., and Koponen, I. K.: A simple procedure for correcting loading effects of aethalometer data, J. Air Waste Manage., 57, 1214–1222, doi:10.3155/1047-3289.57.10.1214, 2007.

Weingartner, E., Saathoff, H., Schnaiter, M., Streit, N., Bitnar, B., and Baltensperger, U.: Absorption of light by soot particles: determination of the absorption coefficient by means of aethalometers, J. Aerosol Sci., 34, 1445–1463, doi:10.1016/S0021-8502(03)00359-8, 2003.

Yus-Díez, J., Bernardoni, V., MoÄnik, G., Alastuey, A., Ciniglia, D., IvanÄiÄ, M., Querol, X., Perez, N., Reche, C., Rigler, M., Vecchi, R., Valentini, S., and Pandolfi, M.: Determination of the multiple-scattering correction factor and its cross-sensitivity to scattering and wavelength dependence for different AE33 Aethalometer filter tapes: a multi-instrumental approach, Atmos. Meas. Tech., 14, 6335–6355, https://doi.org/10.5194/amt-14-6335-2021, 2021.

Citation: https://doi.org/10.5194/acp-2021-766-RC2

Interactive discussion

Status: closed

CC1:
'Comment on acp-2021-766', Cheng Wu, 01 Nov 2021
This study (acp-2021-766) reported a one-year eBC measurement study in Poland using a multiwavelength absorption black carbon instrument (MABI). MABI is a newly developed offline filter-based absorption photometer that provides more wavelengths (7λ) than the existing OT-21 (2λ) and MWAA (3λ). The application of MABI could provide more information to study the spectral characteristics of light-absorbing aerosols. However, the following concerns need to be addressed.
Line 105. The assumption of the multi-scattering correction factor C_ref =1 is arbitrary. C_ref is not only filter type specific (Presler-Jur et al., 2017), but also site specific (Coen et al., 2010). Teflon filter usually has a C_ref value smaller than the quartz filter (Pandey et al., 2019). The exact value of C_ref can only be determined through co-located field comparisons with a reference instrument (e.g. photo-acoustic spectrometry).

The MAE_eBC used in this study (6.036 m²g^-1 @ 639 nm) lacks scientific evidence. Neither the MABI manual nor the recent MABI paper (Manohar et al., 2021) had shown how MAE_eBC was derived. The key question is that for the MAE_eBC used in MABI, which EC protocol is aligning with? For example, the MAE_eBC used in the aethalometer was aligning with EC determined by Lawrence Berkeley Laboratory evolved gas analysis (EGA) protocol (Gundel et al., 1984). The MAE_eBC used in MAAP was aligning with EC determined by VDI part 1 protocol (Petzold and Schonlinner, 2004). How MAE_eBC was derived was not clear in the current manuscript.

The use of the delta-C approach for BB-derived eBC was questionable. A study in the UK has shown that the delta-C approach derived BC_bb is unreliable (Harrison et al., 2013). The Aethalometer AAE model has its limitations for resolving BC from BB, which is only valid when the variability of AAE is dominated by primary brown carbon. The study by Lack and Langridge (2013) had shown that a transparent coating on BC can also lead to an increase of AAE of BC up to 1.5. As a result, the Aethalometer model/delta-C method is only valid when the primary brown carbon contribution is much higher than the lensing effect. The BC_bb/eBC ratio found in this study was lowest in winter, which is unreasonable. Since BB emissions were active during winter, BC_bb/eBC ratio is expected to be higher than other seasons. The authors should provide more evidence (e.g. a good correlation between delta-C and levoglucosan or potassium) to prove that this method is suitable for the samples used in this study.

References
Coen, M. C., Weingartner, E., Apituley, A., Ceburnis, D., Fierz-Schmidhauser, R., Flentje, H., Henzing, J. S., Jennings, S. G., Moerman, M., Petzold, A., Schmid, O., and Baltensperger, U.: Minimizing light absorption measurement artifacts of the Aethalometer: evaluation of five correction algorithms, Atmos. Meas. Tech., 3, 457-474, doi: https://doi.org/10.5194/amt-3-457-2010, 2010.
Gundel, L. A., Dod, R. L., Rosen, H., and Novakov, T.: The Relationship between Optical Attenuation and Black Carbon Concentration for Ambient and Source Particles, Sci. Total. Environ., 36, 197-202, doi: https://doi.org/10.1016/0048-9697(84)90266-3, 1984.
Harrison, R. M., Beddows, D. C. S., Jones, A. M., Calvo, A., Alves, C., and Pio, C.: An evaluation of some issues regarding the use of aethalometers to measure woodsmoke concentrations, Atmos. Environ., 80, 540-548, doi: https://doi.org/10.1016/j.atmosenv.2013.08.026, 2013.
Lack, D. A. and Langridge, J. M.: On the attribution of black and brown carbon light absorption using the Ångström exponent, Atmos. Chem. Phys., 13, 10535-10543, doi: https://doi.org/10.5194/acp-13-10535-2013, 2013.
Manohar, M., Atanacio, A., Button, D., and Cohen, D.: MABI - A multi-wavelength absorption black carbon instrument for the measurement of fine light absorbing carbon particles, Atmospheric Pollut. Res., 12, 133-140, doi: https://doi.org/10.1016/j.apr.2021.02.009, 2021.
Pandey, A., Shetty, N. J., and Chakrabarty, R. K.: Aerosol light absorption from optical measurements of PTFE membrane filter samples: sensitivity analysis of optical depth measures, Atmos. Meas. Tech., 12, 1365-1373, doi: https://doi.org/10.5194/amt-12-1365-2019, 2019.
Petzold, A. and Schonlinner, M.: Multi-angle absorption photometry - a new method for the measurement of aerosol light absorption and atmospheric black carbon, J. Aerosol. Sci., 35, 421-441, doi: https://doi.org/10.1016/j.jaerosci.2003.09.005, 2004.
Presler-Jur, P., Doraiswamy, P., Hammond, O., and Rice, J.: An Evaluation of Mass Absorption Cross-Section for Optical Carbon Analysis on Teflon Filter Media, J. Air Waste Manage. Assoc., 67, 1213-1228 doi: https://doi.org/10.1080/10962247.2017.1310148, 2017.
Citation: https://doi.org/10.5194/acp-2021-766-CC1
- AC1:
  'Reply on CC1', Lucyna Samek, 14 Nov 2021
  This study (acp-2021-766) reported a one-year eBC measurement study in Poland using a multiwavelength absorption black carbon instrument (MABI). MABI is a newly developed offline filter-based absorption photometer that provides more wavelengths (7λ) than the existing OT-21 (2λ) and MWAA (3λ). The application of MABI could provide more information to study the spectral characteristics of light-absorbing aerosols. However, the following concerns need to be addressed.
  Reply: We would like to thank for valuable feedback. Please see attached for our response to comments.
  Line 105. The assumption of the multi-scattering correction factor C_ref =1 is arbitrary. C_ref is not only filter type specific (Presler-Jur et al., 2017), but also site specific (Coen et al., 2010). Teflon filter usually has a C_ref value smaller than the quartz filter (Pandey et al., 2019). The exact value of C_ref can only be determined through co-located field comparisons with a reference instrument (e.g. photo-acoustic spectrometry).
  
  Reply: Based on “Summary of Light Absorbing Carbon and Visibility Measurements and Terms” (Cohen, 2020), the authors assumed C_ref = 1. This paper (Cohen, 2020) provides deeply discussion about C_ref for different type of filters and sizes of particulate matter, among other on page 10. Moreover very similar research, to the present in current manuscript, was conducted during a comparble period in Poland (Zioła et al., 2021) The condition and type of location were very similar, but measurement was conducted by different instrument (a modern Aethalometer AE33). This study presents comparable results with shown in the manuscript, which was expected. They have annual average of eBC concentration equal to 3.22±2.81µg/m³ compared with our study 3.5±1.5µg/m³. As of today, our research group does not have possible to performe co-located field comparisons with reference instrument .
  The MAE_eBC used in this study (6.036 m²g^-1 @ 639 nm) lacks scientific evidence. Neither the MABI manual nor the recent MABI paper (Manohar et al., 2021) had shown how MAE_eBC was derived. The key question is that for the MAE_eBC used in MABI, which EC protocol is aligning with? For example, the MAE_eBC used in the aethalometer was aligning with EC determined by Lawrence Berkeley Laboratory evolved gas analysis (EGA) protocol (Gundel et al., 1984). The MAE_eBC used in MAAP was aligning with EC determined by VDI part 1 protocol (Petzold and Schonlinner, 2004). How MAE_eBC was derived was not clear in the current manuscript.
  
  Reply: The MAE_eBC used in this study was recommended by the Australian Nuclear Science and Technology Organisation (ANSTO) in ANSTO External Report ER-790 (Cohen, 2020). In this report -“Summary of Light Absorbing Carbon and Visibility Measurements and Terms”, you can find discussion about results of research and analysis which have done over the years. The aspect raised in this point described among other on page 11, and 15 – 17. The comparison of the results of MABI measurements and Aethalometer was presented by Manohar (Manohar et al., 2021).
  
  The article aimed to present the method of calculating the results obtained by MABI based on the paper provided particular by ANSTO. Moreover, authors wanted to show the result for BC by MABI, which can show general BC situation in Krakow and give opportunity to compare BC result in the future.
  The use of the delta-C approach for BB-derived eBC was questionable. A study in the UK has shown that the delta-C approach derived BC_bb is unreliable (Harrison et al., 2013). The Aethalometer AAE model has its limitations for resolving BC from BB, which is only valid when the variability of AAE is dominated by primary brown carbon. The study by Lack and Langridge (2013) had shown that a transparent coating on BC can also lead to an increase of AAE of BC up to 1.5. As a result, the Aethalometer model/delta-C method is only valid when the primary brown carbon contribution is much higher than the lensing effect. The BC_bb/eBC ratio found in this study was lowest in winter, which is unreasonable. Since BB emissions were active during winter, BC_bb/eBC ratio is expected to be higher than other seasons. The authors should provide more evidence (e.g. a good correlation between delta-C and levoglucosan or potassium) to prove that this method is suitable for the samples used in this study.
  
  Reply: Our comprehensive study provides that potassium is the highest in winter, and the lowest in summer. Please take a look, on Table 1, that the values for BC_BB shows similar relation, the highest value is in winter (0.4±0.3 µg/m³) and the lowest is in summer (0.2±0.1 µg/m³). Moreover, the values for eBC are also the highest in winter (5.3±1.8 µg/m³), what is expected. The relative contribution of biomass (BC_BB) to eBC, present in this table for winter, shows that the higher excess of eBC contribution from fossil fuels than biomass burning was observed during winter. Our results for BC_BB annual average concentration is 0.25±0.15 µg/m³ and it is lower than in Zabrze (Poland) (0.93±0.76. µg/m³) (Ziola et al., 2021). It can probably be connected with introduction in September 2019 of ban of burning wood and coal in Krakow.
  
  Period
  
  K (ng m^-3)
  
  u(K) (ng m^-3)
  
  Spring
  
  117
  
  2
  
  Summer
  
  65
  
  1
  
  Autumn
  
  159
  
  4
  
  Winter
  
  197
  
  3
  
  Reply: Bibliography:
  Cohen, D. D.: Summary of Light Absorbing Carbon and Visibility Measurements and Terms. ANSTO External Report ER-790, ISBN – 1 921268 32 8, October 2020., 2020.
  Manohar, M., Atanacio, A., Button, D. and Cohen, D.: MABI - A multi-wavelength absorption black carbon instrument for the measurement of fine light absorbing carbon particles, Atmos. Pollut. Res., 12(4), 133–140, https://doi.org/https://doi.org/10.1016/j.apr.2021.02.009, 2021.
  Zioła, N., Błaszczak, B. and Klejnowski, K.: Temporal Variability of Equivalent Black Carbon Components in Atmospheric Air in Southern Poland, Atmosphere (Basel)., 12(1), https://doi.org/10.3390/atmos12010119, 2021.
  
  References
  Coen, M. C., Weingartner, E., Apituley, A., Ceburnis, D., Fierz-Schmidhauser, R., Flentje, H., Henzing, J. S., Jennings, S. G., Moerman, M., Petzold, A., Schmid, O., and Baltensperger, U.: Minimizing light absorption measurement artifacts of the Aethalometer: evaluation of five correction algorithms, Atmos. Meas. Tech., 3, 457-474, doi: https://doi.org/10.5194/amt-3-457-2010, 2010.
  Gundel, L. A., Dod, R. L., Rosen, H., and Novakov, T.: The Relationship between Optical Attenuation and Black Carbon Concentration for Ambient and Source Particles, Sci. Total. Environ., 36, 197-202, doi: https://doi.org/10.1016/0048-9697(84)90266-3, 1984.
  Harrison, R. M., Beddows, D. C. S., Jones, A. M., Calvo, A., Alves, C., and Pio, C.: An evaluation of some issues regarding the use of aethalometers to measure woodsmoke concentrations, Atmos. Environ., 80, 540-548, doi: https://doi.org/10.1016/j.atmosenv.2013.08.026, 2013.
  Lack, D. A. and Langridge, J. M.: On the attribution of black and brown carbon light absorption using the Ångström exponent, Atmos. Chem. Phys., 13, 10535-10543, doi: https://doi.org/10.5194/acp-13-10535-2013, 2013.
  Manohar, M., Atanacio, A., Button, D., and Cohen, D.: MABI - A multi-wavelength absorption black carbon instrument for the measurement of fine light absorbing carbon particles, Atmospheric Pollut. Res., 12, 133-140, doi: https://doi.org/10.1016/j.apr.2021.02.009, 2021.
  Pandey, A., Shetty, N. J., and Chakrabarty, R. K.: Aerosol light absorption from optical measurements of PTFE membrane filter samples: sensitivity analysis of optical depth measures, Atmos. Meas. Tech., 12, 1365-1373, doi: https://doi.org/10.5194/amt-12-1365-2019, 2019.
  Petzold, A. and Schonlinner, M.: Multi-angle absorption photometry - a new method for the measurement of aerosol light absorption and atmospheric black carbon, J. Aerosol. Sci., 35, 421-441, doi: https://doi.org/10.1016/j.jaerosci.2003.09.005, 2004.
  Presler-Jur, P., Doraiswamy, P., Hammond, O., and Rice, J.: An Evaluation of Mass Absorption Cross-Section for Optical Carbon Analysis on Teflon Filter Media, J. Air Waste Manage. Assoc., 67, 1213-1228 doi: https://doi.org/10.1080/10962247.2017.1310148, 2017.
  
  Citation: https://doi.org/10.5194/acp-2021-766-AC1
RC1: 'Comment on acp-2021-766', Anonymous Referee #1, 15 Nov 2021

The comment was uploaded in the form of a supplement: https://acp.copernicus.org/preprints/acp-2021-766/acp-2021-766-RC1-supplement.pdf

Citation: https://doi.org/10.5194/acp-2021-766-RC1
RC2: 'Comment on acp-2021-766', Anonymous Referee #2, 15 Nov 2021

REVIEW of Rys and Samek

Measurement report: Determination of Black Carbon concentration in PM2.5 fraction by Multi-wavelength absorption black carbon instrument (MABI), Atmos. Chem. Phys. 2021-766

https://doi.org/10.5194/acp-2021-766

The authors present results of a more than 1 year measurement campaign in Krakow, Poland, with a new instrument – the Multi-wavelength absorption black carbon instrument (MABI). While the manuscript is a “measurement report”, it still lacks vital information to warrant its publication in ACP. The topic is treated superficially. The manuscript does not meet the standard of publication, and I recommend its rejection.

There have been numerous publications on the state-of-the-art absorption filter photometers, ranging from the characterization of new instrumentation (Bond et al., 1999; Drinovec et al., 2015; Ogren et al., 2017), the methodologies to post-process the data (Park et al., 2010; Virkkula et al., 2007; Weingartner et al., 2003), to the measurements, quantifying the limitations of filter photometers (Bernardoni et al., 2021; Yus-Diez et al., 2021). The interpretation of the data from the presented measurement campaign should address the issues described in the literature. I specify the most blatant omissions below.

The sampling of the filters was performed for 24 hours. With the concentrations reported, there are significant loading effects present (see for example, Bond et al., 1999; Drinovec et al., 2015; Park et al., 2010; Weingartner et al., 2003). These need to be addresses. The loading effects are wavelength dependent and the reported Angstrom exponent alpha=0.6 (the authors should avoid an excessive number of digits beyond any reasonable measurement uncertainty) will increase once this is addressed. The assumption of C=R=1 is probably wrong, but we do not know how this correction is parametrized as there are no links to the MABI manual in the manuscript, and this shall remain an open question.

It is unclear if the epsilon is the absorption coefficient (units m^-1) or the mass absorption cross-section (units m²g^-1). If this is MAC, then the explanation on the measurement of mass is lacking in the manuscript.

The wavelength difference method is a very simplistic and non-quantitative way to perform source apportionment and much more sophisticated methods are available in the literature (starting with Sandradewi et al., 2008). The 11.3% BC apportioned to biomass burning should be reported to the nearest 1% and its uncertainty should be determined.

The source apportionment methods using filter photometers use the PM optical properties to determine the contribution of sources to BC. The presented results do not take into account that coal combustion could also result in PM absorbing strongly at low wavelengths. More sophisticated studies in Krakow (Tobler et al., 2021) have opted to use “solid fuel” rather than specifying the fuel type due to this possibility.

References

Bernardoni, V., Ferrero, L., Bolzacchini, E., Forello, A. C., GregoriÄ, A., Massabò, D., MoÄnik, G., Prati, P., Rigler, M., Santagostini, L., Soldan, F., Valentini, S., Valli, G., and Vecchi, R.: Determination of Aethalometer multiple-scattering enhancement parameters and impact on source apportionment during the winter 2017/18 EMEP/ACTRIS/COLOSSAL campaign in Milan, Atmos. Meas. Tech., 14, 2919–2940, https://doi.org/10.5194/amt-14-2919-2021, 2021.

Bond, T. C., Anderson, T. L., and Campbell, D.: Calibration and intercomparison of filter-based measurements of visible light absorption by aerosols, Aerosol Sci. Tech., 30, 582–600, 1999.

Drinovec, L., MoÄnik, G., Zotter, P., Prévôt, A. S. H., Ruckstuhl, C., Coz, E., Rupakheti, M., Sciare, J., Müller, T., Wiedensohler, A., and Hansen, A. D. A.: The "dual-spot" Aethalometer: an improved measurement of aerosol black carbon with real-time loading compensation, Atmos. Meas. Tech., 8, 1965–1979, https://doi.org/10.5194/amt-8-1965-2015, 2015.

Ogren, J. A., Wendell, J., Andrews, E., and Sheridan, P. J.: Continuous light absorption photometer for long-term studies, Atmos. Meas. Tech., 10, 4805–4818, https://doi.org/10.5194/amt-10-4805-2017, 2017.

Park, S. S., Hansen, A. D. A., and Cho, Y.: Measurement of real time black carbon for investigating spot loading effects of Aethalometer data, Atmos. Environ., 11, 1449–1455, doi:10.1016/j.atmosenv.2010.01.025, 2010.

Sandradewi, J., Prévôt, A. S. H., Szidat, S., Perron, N., Alfarra, M. R., Lanz, V. A., Weingartner, E., and Baltensperger, U.: Using aerosol light absorption measurements for the quantitative determination of wood burning and traffic emission contributions to particulate matter, Environ. Sci. Technol., 42, 3316–3323, https://doi.org/10.1021/es702253m, 2008.

Tobler, A. K., Skiba, A., Canonaco, F., MoÄnik, G., Rai, P., Chen, G., Bartyzel, J., Zimnoch, M., Styszko, K., NÄcki, J., Furger, M., RóÅ¼aÅski, K., Baltensperger, U., Slowik, J. G., and Prevot, A. S. H.: Characterization of non-refractory (NR) PM1 and source apportionment of organic aerosol in Kraków, Poland, Atmos. Chem. Phys., 21, 14893–14906, https://doi.org/10.5194/acp-21-14893-2021, 2021.

Virkkula, A., Mäkelä, T., Hillamo, R., Yli-Tuomi, T., Hirsikko, A., Hämeri, K., and Koponen, I. K.: A simple procedure for correcting loading effects of aethalometer data, J. Air Waste Manage., 57, 1214–1222, doi:10.3155/1047-3289.57.10.1214, 2007.

Weingartner, E., Saathoff, H., Schnaiter, M., Streit, N., Bitnar, B., and Baltensperger, U.: Absorption of light by soot particles: determination of the absorption coefficient by means of aethalometers, J. Aerosol Sci., 34, 1445–1463, doi:10.1016/S0021-8502(03)00359-8, 2003.

Yus-Díez, J., Bernardoni, V., MoÄnik, G., Alastuey, A., Ciniglia, D., IvanÄiÄ, M., Querol, X., Perez, N., Reche, C., Rigler, M., Vecchi, R., Valentini, S., and Pandolfi, M.: Determination of the multiple-scattering correction factor and its cross-sensitivity to scattering and wavelength dependence for different AE33 Aethalometer filter tapes: a multi-instrumental approach, Atmos. Meas. Tech., 14, 6335–6355, https://doi.org/10.5194/amt-14-6335-2021, 2021.

Citation: https://doi.org/10.5194/acp-2021-766-RC2

Anna Ryś and Lucyna Samek

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This study shows how the contributions of biomass burning and fossil fuel/traffic to PM_2.5 mass can be assessed. The samples of PM_2.5 fraction were collected from February 1, 2020 to March 27, 2021 every third day. About 18 % of PM_2.5 mass belongs to eBC. The eBC contribution is the significant part of PM_2.5 mass and we observed seasonal variation of the eBC concentration during the year with the peak in winter.

Period	K (ng m^-3)	u(K) (ng m^-3)
Spring	117	2
Summer	65	1
Autumn	159	4
Winter	197	3


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Measurement report: Determination of Black Carbon concentration in PM2.5 fraction by Multi-wavelength absorption black carbon instrument (MABI)

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Measurement report: Determination of Black Carbon concentration in PM_2.5 fraction by Multi-wavelength absorption black carbon instrument (MABI)