Impacts of elevated anthropogenic emissions on physicochemical characteristics of BC-containing particles over the Tibetan Plateau

Wang, Jinbo; Wang, Jiaping; Zhang, Yuxuan; Liu, Tengyu; Chi, Xuguang; Huang, Xin; Ge, Dafeng; Lai, Shiyi; Zhu, Caijun; Wang, Lei; Zha, Qiaozhi; Qi, Ximeng; Nie, Wei; Fu, Congbin; Ding, Aijun

doi:https://doi.org/10.5194/egusphere-2024-879

Preprints

https://doi.org/10.5194/egusphere-2024-879

Preprints

08 Apr 2024

| 08 Apr 2024

Impacts of elevated anthropogenic emissions on physicochemical characteristics of BC-containing particles over the Tibetan Plateau

Jinbo Wang, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Xuguang Chi, Xin Huang, Dafeng Ge, Shiyi Lai, Caijun Zhu, Lei Wang, Qiaozhi Zha, Ximeng Qi, Wei Nie, Congbin Fu, and Aijun Ding

Abstract. Black carbon (BC) in the Tibetan Plateau (TP) region has distinct climate effect, which strongly depends on its mixing state. The aging processes of BC in TP are subject to emissions from various regions, resulting in considerable variability of its mixing state and physicochemical properties. However, the mechanism and magnitude of this effect are not yet clear. In this study, filed observations on physicochemical properties of BC-containing particles (PM_BC) were conducted in the northeast (Xihai) and southeast (Lulang) regions of the TP to investigate the impacts of transported emissions from lower-altitude areas on BC characteristics in the TP. Large spatial discrepancies were found in the chemical composition of PM_BC. Both sites showed higher concentrations of PM_BC when they were affected by transported airmasses outside the TP, but with diverse chemical composition. Source apportionment for organic aerosol (OA) suggested that primary OA in the northeastern TP was attributed to hydrocarbon OA (HOA) from anthropogenic emissions, while it was dominated by biomass burning OA (BBOA) in the southeastern TP. Regarding secondary aerosol, a marked enhancement in nitrate fraction was observed on aged BC coating in Xihai when the airmasses were brought by updrafts and easterly winds from lower-altitude areas. With the development of boundary layer, the enhanced turbulent mixing promoted the elevation of anthropogenic pollutants. In contrast to Xihai, the thickly coated BC in Lulang was mainly caused by self-elevated biomass burning plume from the South Asia, showing a large contribution of secondary organic aerosol (SOA). The distinct transported emissions lead to substantial variations of both chemical composition and light absorption ability of BC across the TP. The thicker coating and higher mass absorption cross-section (MAC) of PM_BC in airmasses elevated from lower-altitude regions reveals the promoted BC aging processes and their impacts on the mixing state and light absorption of BC in TP. These findings emphasize the vulnerability of plateau regions to influences of elevated emissions, leading to significant changes in BC concentration, mixing states and light absorption across the TP, which needs to be considered in the evaluation of BC radiative effects for the TP region.

Received: 24 Mar 2024 – Discussion started: 08 Apr 2024

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Journal article(s) based on this preprint

02 Oct 2024

Impacts of elevated anthropogenic emissions on physicochemical characteristics of black-carbon-containing particles over the Tibetan Plateau

Jinbo Wang, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Xuguang Chi, Xin Huang, Dafeng Ge, Shiyi Lai, Caijun Zhu, Lei Wang, Qiaozhi Zha, Ximeng Qi, Wei Nie, Congbin Fu, and Aijun Ding

Atmos. Chem. Phys., 24, 11063–11080, https://doi.org/10.5194/acp-24-11063-2024,https://doi.org/10.5194/acp-24-11063-2024, 2024

Short summary

Jinbo Wang, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Xuguang Chi, Xin Huang, Dafeng Ge, Shiyi Lai, Caijun Zhu, Lei Wang, Qiaozhi Zha, Ximeng Qi, Wei Nie, Congbin Fu, and Aijun Ding

Interactive discussion

Status: closed

RC1:
'Comment on egusphere-2024-879', Anonymous Referee #3, 24 Apr 2024
The manuscript by Wang et al. provides a comprehensive analysis of the physicochemical properties of black carbon (BC)-containing particles over the Tibetan Plateau, with an emphasis on the impacts of anthropogenic emissions. The authors conduct detailed field observations, which contribute valuable data to this field of study. Their findings represent a noteworthy advancement in elucidating the impact of anthropogenic emissions on the properties of BC, especially within the environmentally sensitive Tibetan Plateau region. See my detailed comments below.
Major Comments:
Addressing Seasonality and Expanding Temporal Scope: The manuscript effectively outlines how regional transport influences the BC characteristics over the plateau. This is particularly evident in the comparison between the northeast and southeast regions. Yet, the study seems to focus predominantly on the spring season (Table 1). It would be valuable if the authors could discuss the potential seasonality of these findings or provide reasons for the focus on this particular season, including how the results might vary in other seasons.

Lack of Detailed Model Evaluation：The manuscript utilizes the WRF-Chem model to simulate the atmospheric processes and black carbon (BC) characteristics over the Tibetan Plateau. However, there seems to be a lack of detailed evaluation or validation of the model simulations against observational data. Without proper validation, the reliability of the model results and the subsequent conclusions drawn from them may be questionable.

Minor Comments:
Line 155: According to my understanding, the study by Cui et al. (2022) only provides BC concentrations in urban areas of Shanghai, and does not directly provide the number 25%. Please directly provide the BC concentrations mentioned in Cui et al. (2022)'s study and explain how the calculation for obtaining 25% is done. In addition, although EC is sometimes used as a substitute for BC in some cases due to the lack of BC observations, it should not be said that they are equivalent

Line 158: The sentence suggests that the intermediate position of the concentration within the TP region may be due to anthropogenic emissions in the surrounding area. However, it does not explain why it is not in a high concentration position.

Line 175: Is this difference statistically significant? Are there any indicators for testing the significance of differences that can be reported?

Line 192: The sentence could be improved by providing citations to support the claim that C2H3O+ is a typical biomass burning (BB) tracer.

Line 222: 17.3% cannot be reflected in Fig. 5b, but only in Fig. 5a, and there is no particular reason to switch from two decimal places to one decimal place in the figure.

Line 240: The statement "The abundant NO3- was closely associated with anthropogenic sources" is mentioned here, but it should be referenced in line 222 to support the conclusion that "indicating that anthropogenic..."
Citation: https://doi.org/10.5194/egusphere-2024-879-RC1
- AC1: 'Reply on RC1', Jiaping Wang, 19 Jun 2024
  
  The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-879/egusphere-2024-879-AC1-supplement.pdf
  
  Citation: https://doi.org/10.5194/egusphere-2024-879-AC1
RC2:
'Comment on egusphere-2024-879', Anonymous Referee #1, 03 May 2024

The manuscript provides observational evidence of the spatial discrepancies in the physicochemical properties of black carbon (BC)-containing particles within the Tibetan Plateau region. It emphases the significant impacts of elevated anthropogenic emissions from surrounding low-altitude areas on BC, altering its concentration and chemical composition, as well as enhancing its light absorption ability. The manuscript is well written, and the topic is of interest and fits the scope of ACP. I recommend a minor revision before publication. The detailed comments or suggestions are shown below:
1. In this study, there are three factors identified using PMF, which is a little less than the usual number (normally 4 or 5 factors can be resolved by PMF for HR-AMS data). It is better to provide the explanation of why the 3-factor result is chosen in the main text or SI.
2. Line 131: what refractive index did you use for the core-shell Mie model? Please add the numbers you adopted and reference here.
3. Line 154: It is suggested to clarify the different measuring instruments corresponding to different BC definitions before comparing BC concentrations in Table 1.
4. In Table 1, the description “BC (EC)” is not very precise here. Please revise them.
5. Table 1: Please add a note illustrating the meaning of the numbers in “BC concentration” column, i.e., is it a mean or median value? What does the range stand for in the parenthesis?
6. Line 106: please add abbreviation of light absorption coefficients (b_abs) here.
7. Figure 7: the color of CL2 in subplot (b) overlaps with the background map. It is better to change it to ensure the visibility.
8. Please check and ensure that the number of significant digits are consistent throughout the manuscript.

Citation: https://doi.org/10.5194/egusphere-2024-879-RC2
- AC2: 'Reply on RC2', Jiaping Wang, 19 Jun 2024
  
  The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-879/egusphere-2024-879-AC2-supplement.pdf
  
  Citation: https://doi.org/10.5194/egusphere-2024-879-AC2
RC3:
'Comment on egusphere-2024-879', Anonymous Referee #2, 06 May 2024

Black carbon (BC) is one of the most important aerosol species affecting climate, glaciers and hydrology in Tibetan Plateau (TP). However, large uncertainties still exist in the estimation of BC DRF over the TP, which is related to the mixing states of BC. This study presents multi-point observations of BC mixing states, especially the chemical composition of BC-containing particles, and combines model simulation to reveal the causes of spatial differences and the impacts of transported emission sources. It provides valuable results which may support the future evaluation of BC climate and environmental effects over the TP region. The coupling mechanism between the planetary boundary layer, topography, and pollution mentioned in the text is also interesting. Overall, it is a well-organized manuscript. Thus, I suggest publishing after minor revisions. The detail comments are shown below:

1. My main suggestion is that the model configuration and validation need to be more detailed, which can be described in 2.3 part. Additional figures of model validation can be added into the SI (e.g. meteorological parameters, gaseous pollutants). Furthermore, a brief setup of the chemical transport model should be elucidated within the main text, in addition to its inclusion in the Supplementary Information.

2. As I commented earlier in the discussion process, the authors should pay careful attention to the use of significant figures in both the main text and figures. For instance, in Figure 5, the fractions should be reported with 2 significant digits, not 4. Additionally, it is important that the number of significant figures is consistent across all panels in Figures 3 and 7.

3. Line 27: the term “self-elevated” is typically associated with plume uplift due to the absorption of solar radiation by black carbon. However, as the uplift in question may not be solely attributed to this mechanism, it is recommended to replace the term.

4. Line 36: The expression “2,500,000 km2” appears twice in a sentence. Please remove one instance to ensure clarity and conciseness.

5. Line 150, too many digitals for wind speed and gaseous pollutant concentrations

6. Line 175, a t-test is needed when comparing RBC between Xinhan and Lulang

7. Line 199-200, “MO-OOA had very high O:C (0.84), while the O:C of LO-OOA was only 0.49.”

It is better to be rephrased to in Xinhai “MO-OOA exhibited higher O:C ratio (0.84) than LO-OOA (0.49) ”

8. Line 201 “Therefore, this POA factor was identified as biomass burning OA (BBOA) in Lulang.”

Since f60 from this factor is not as high as those from biomass burning source test, likely caused by aging process, it is better to state that this factor is likely associated with biomass burning activities.

9. Figure 6, in the figure caption, it is better to explain how the grid of x-axis is calculated since RBC equals 0 meaning externally mixed BC.

10. Line 191: “The POA factor had higher signal of C4H7+ and C4H9+ in its mass spectrum…”. Please explain the major sources of C4H7+ and C4H9+ and add proper references here.

11. Line 214: “OA was the dominant component of BC coating (Fig. 5b) at both sites”. Here it should refer to Fig. 5a rather than Fig. 5b.

12. Line 219: “The dominance of MO-OOA in BC coating was resulted from strong atmospheric oxidizing capacity in TP and fast aging process during transport.”. Based on Fig. 5, I don’t think there is information about the atmospheric oxidation capacity and aging rates during transport. If this discussion is located in the latter part of the article, it is suggested to place this sentence in a more appropriate location.

13. Line 305: is there any observed MAC in TP region? If yes, it is recommended to compare the results in this study with previous observations (references need to be added accordingly).

14. The abbreviations of CL 1,2,3 should be defined in the main text.

Citation: https://doi.org/10.5194/egusphere-2024-879-RC3
- AC3: 'Reply on RC3', Jiaping Wang, 19 Jun 2024
  
  The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-879/egusphere-2024-879-AC3-supplement.pdf
  
  Citation: https://doi.org/10.5194/egusphere-2024-879-AC3

Interactive discussion

Status: closed

RC1:
'Comment on egusphere-2024-879', Anonymous Referee #3, 24 Apr 2024
The manuscript by Wang et al. provides a comprehensive analysis of the physicochemical properties of black carbon (BC)-containing particles over the Tibetan Plateau, with an emphasis on the impacts of anthropogenic emissions. The authors conduct detailed field observations, which contribute valuable data to this field of study. Their findings represent a noteworthy advancement in elucidating the impact of anthropogenic emissions on the properties of BC, especially within the environmentally sensitive Tibetan Plateau region. See my detailed comments below.
Major Comments:
Addressing Seasonality and Expanding Temporal Scope: The manuscript effectively outlines how regional transport influences the BC characteristics over the plateau. This is particularly evident in the comparison between the northeast and southeast regions. Yet, the study seems to focus predominantly on the spring season (Table 1). It would be valuable if the authors could discuss the potential seasonality of these findings or provide reasons for the focus on this particular season, including how the results might vary in other seasons.

Lack of Detailed Model Evaluation：The manuscript utilizes the WRF-Chem model to simulate the atmospheric processes and black carbon (BC) characteristics over the Tibetan Plateau. However, there seems to be a lack of detailed evaluation or validation of the model simulations against observational data. Without proper validation, the reliability of the model results and the subsequent conclusions drawn from them may be questionable.

Minor Comments:
Line 155: According to my understanding, the study by Cui et al. (2022) only provides BC concentrations in urban areas of Shanghai, and does not directly provide the number 25%. Please directly provide the BC concentrations mentioned in Cui et al. (2022)'s study and explain how the calculation for obtaining 25% is done. In addition, although EC is sometimes used as a substitute for BC in some cases due to the lack of BC observations, it should not be said that they are equivalent

Line 158: The sentence suggests that the intermediate position of the concentration within the TP region may be due to anthropogenic emissions in the surrounding area. However, it does not explain why it is not in a high concentration position.

Line 175: Is this difference statistically significant? Are there any indicators for testing the significance of differences that can be reported?

Line 192: The sentence could be improved by providing citations to support the claim that C2H3O+ is a typical biomass burning (BB) tracer.

Line 222: 17.3% cannot be reflected in Fig. 5b, but only in Fig. 5a, and there is no particular reason to switch from two decimal places to one decimal place in the figure.

Line 240: The statement "The abundant NO3- was closely associated with anthropogenic sources" is mentioned here, but it should be referenced in line 222 to support the conclusion that "indicating that anthropogenic..."
Citation: https://doi.org/10.5194/egusphere-2024-879-RC1
- AC1: 'Reply on RC1', Jiaping Wang, 19 Jun 2024
  
  The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-879/egusphere-2024-879-AC1-supplement.pdf
  
  Citation: https://doi.org/10.5194/egusphere-2024-879-AC1
RC2:
'Comment on egusphere-2024-879', Anonymous Referee #1, 03 May 2024

The manuscript provides observational evidence of the spatial discrepancies in the physicochemical properties of black carbon (BC)-containing particles within the Tibetan Plateau region. It emphases the significant impacts of elevated anthropogenic emissions from surrounding low-altitude areas on BC, altering its concentration and chemical composition, as well as enhancing its light absorption ability. The manuscript is well written, and the topic is of interest and fits the scope of ACP. I recommend a minor revision before publication. The detailed comments or suggestions are shown below:
1. In this study, there are three factors identified using PMF, which is a little less than the usual number (normally 4 or 5 factors can be resolved by PMF for HR-AMS data). It is better to provide the explanation of why the 3-factor result is chosen in the main text or SI.
2. Line 131: what refractive index did you use for the core-shell Mie model? Please add the numbers you adopted and reference here.
3. Line 154: It is suggested to clarify the different measuring instruments corresponding to different BC definitions before comparing BC concentrations in Table 1.
4. In Table 1, the description “BC (EC)” is not very precise here. Please revise them.
5. Table 1: Please add a note illustrating the meaning of the numbers in “BC concentration” column, i.e., is it a mean or median value? What does the range stand for in the parenthesis?
6. Line 106: please add abbreviation of light absorption coefficients (b_abs) here.
7. Figure 7: the color of CL2 in subplot (b) overlaps with the background map. It is better to change it to ensure the visibility.
8. Please check and ensure that the number of significant digits are consistent throughout the manuscript.

Citation: https://doi.org/10.5194/egusphere-2024-879-RC2
- AC2: 'Reply on RC2', Jiaping Wang, 19 Jun 2024
  
  The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-879/egusphere-2024-879-AC2-supplement.pdf
  
  Citation: https://doi.org/10.5194/egusphere-2024-879-AC2
RC3:
'Comment on egusphere-2024-879', Anonymous Referee #2, 06 May 2024

Black carbon (BC) is one of the most important aerosol species affecting climate, glaciers and hydrology in Tibetan Plateau (TP). However, large uncertainties still exist in the estimation of BC DRF over the TP, which is related to the mixing states of BC. This study presents multi-point observations of BC mixing states, especially the chemical composition of BC-containing particles, and combines model simulation to reveal the causes of spatial differences and the impacts of transported emission sources. It provides valuable results which may support the future evaluation of BC climate and environmental effects over the TP region. The coupling mechanism between the planetary boundary layer, topography, and pollution mentioned in the text is also interesting. Overall, it is a well-organized manuscript. Thus, I suggest publishing after minor revisions. The detail comments are shown below:

1. My main suggestion is that the model configuration and validation need to be more detailed, which can be described in 2.3 part. Additional figures of model validation can be added into the SI (e.g. meteorological parameters, gaseous pollutants). Furthermore, a brief setup of the chemical transport model should be elucidated within the main text, in addition to its inclusion in the Supplementary Information.

2. As I commented earlier in the discussion process, the authors should pay careful attention to the use of significant figures in both the main text and figures. For instance, in Figure 5, the fractions should be reported with 2 significant digits, not 4. Additionally, it is important that the number of significant figures is consistent across all panels in Figures 3 and 7.

3. Line 27: the term “self-elevated” is typically associated with plume uplift due to the absorption of solar radiation by black carbon. However, as the uplift in question may not be solely attributed to this mechanism, it is recommended to replace the term.

4. Line 36: The expression “2,500,000 km2” appears twice in a sentence. Please remove one instance to ensure clarity and conciseness.

5. Line 150, too many digitals for wind speed and gaseous pollutant concentrations

6. Line 175, a t-test is needed when comparing RBC between Xinhan and Lulang

7. Line 199-200, “MO-OOA had very high O:C (0.84), while the O:C of LO-OOA was only 0.49.”

It is better to be rephrased to in Xinhai “MO-OOA exhibited higher O:C ratio (0.84) than LO-OOA (0.49) ”

8. Line 201 “Therefore, this POA factor was identified as biomass burning OA (BBOA) in Lulang.”

Since f60 from this factor is not as high as those from biomass burning source test, likely caused by aging process, it is better to state that this factor is likely associated with biomass burning activities.

9. Figure 6, in the figure caption, it is better to explain how the grid of x-axis is calculated since RBC equals 0 meaning externally mixed BC.

10. Line 191: “The POA factor had higher signal of C4H7+ and C4H9+ in its mass spectrum…”. Please explain the major sources of C4H7+ and C4H9+ and add proper references here.

11. Line 214: “OA was the dominant component of BC coating (Fig. 5b) at both sites”. Here it should refer to Fig. 5a rather than Fig. 5b.

12. Line 219: “The dominance of MO-OOA in BC coating was resulted from strong atmospheric oxidizing capacity in TP and fast aging process during transport.”. Based on Fig. 5, I don’t think there is information about the atmospheric oxidation capacity and aging rates during transport. If this discussion is located in the latter part of the article, it is suggested to place this sentence in a more appropriate location.

13. Line 305: is there any observed MAC in TP region? If yes, it is recommended to compare the results in this study with previous observations (references need to be added accordingly).

14. The abbreviations of CL 1,2,3 should be defined in the main text.

Citation: https://doi.org/10.5194/egusphere-2024-879-RC3
- AC3: 'Reply on RC3', Jiaping Wang, 19 Jun 2024
  
  The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-879/egusphere-2024-879-AC3-supplement.pdf
  
  Citation: https://doi.org/10.5194/egusphere-2024-879-AC3

Peer review completion

AR: Author's response | RR: Referee report | ED: Editor decision | EF: Editorial file upload

AR by Jiaping Wang on behalf of the Authors (19 Jun 2024) Author's response Author's tracked changes Manuscript

ED: Referee Nomination & Report Request started (24 Jun 2024) by Zhibin Wang

RR by Anonymous Referee #1 (24 Jun 2024)

RR by Anonymous Referee #2 (10 Jul 2024)

ED: Publish as is (19 Jul 2024) by Zhibin Wang

AR by Jiaping Wang on behalf of the Authors (26 Jul 2024) Author's response Manuscript

Journal article(s) based on this preprint

02 Oct 2024

Impacts of elevated anthropogenic emissions on physicochemical characteristics of black-carbon-containing particles over the Tibetan Plateau

Jinbo Wang, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Xuguang Chi, Xin Huang, Dafeng Ge, Shiyi Lai, Caijun Zhu, Lei Wang, Qiaozhi Zha, Ximeng Qi, Wei Nie, Congbin Fu, and Aijun Ding

Atmos. Chem. Phys., 24, 11063–11080, https://doi.org/10.5194/acp-24-11063-2024,https://doi.org/10.5194/acp-24-11063-2024, 2024

Short summary

Jinbo Wang, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Xuguang Chi, Xin Huang, Dafeng Ge, Shiyi Lai, Caijun Zhu, Lei Wang, Qiaozhi Zha, Ximeng Qi, Wei Nie, Congbin Fu, and Aijun Ding

Supplement

https://doi.org/10.5194/egusphere-2024-879-supplement

Jinbo Wang, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Xuguang Chi, Xin Huang, Dafeng Ge, Shiyi Lai, Caijun Zhu, Lei Wang, Qiaozhi Zha, Ximeng Qi, Wei Nie, Congbin Fu, and Aijun Ding

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In this study, we found large spatial discrepancies in the physical and chemical properties of black carbon over the Tibetan Plateau (TP). Elevated anthropogenic emissions from low-altitude regions can significantly change the mass concentration, mixing state and chemical composition of black carbon -containing aerosol in TP region, further altering its light absorption ability. Our study emphasizes the vulnerability of remote plateau regions to intense anthropogenic influences.


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