Measurement Report: Rapid changes of chemical characteristics and health risks for high time-resolved trace elements in PM<sub>2.5</sub> in a typical industrial city response to stringent clean air actions

Li, Rui; Peng, Meng; Zhao, Weidong; Wang, Gehui; Hao, Jiming

doi:https://doi.org/10.5194/egusphere-2022-848

Preprints

https://doi.org/10.5194/egusphere-2022-848

Preprints

17 Oct 2022

| 17 Oct 2022

Measurement Report: Rapid changes of chemical characteristics and health risks for high time-resolved trace elements in PM_2.5 in a typical industrial city response to stringent clean air actions

Rui Li, Meng Peng, Weidong Zhao, Gehui Wang, and Jiming Hao

Abstract. Atmospheric trace metals entail significant damages in human health and ecosystem safety, and thus a series of clean air actions have been implemented to decrease the ambient element concentrations. Unfortunately, the impact of these emission control measures on element concentrations in fine particles remained poorly understood. In our study, the random forest (RF) model was applied to distinguish the effects of emission and meteorology to trace elements in PM_2.5 in a typical industrial city named Tangshan based on a three-year (2017–2020) hourly field observation. The result suggested that the clean air actions have facilitated the dramatic decreases of the deweathered concentrations of Ga, Co, Pb, Zn, and As by 72 %, 67 %, 62 %, 59 %, and 54 %, respectively. It is attributable to the strict implementation of “coal to gas” strategies and optimization of industrial structure and layout. However, the deweathered levels of Ca (8.3 %), Cr (18.5 %), and Fe (23 %) only displayed minor decreases, indicating that the emission control measures for ferrous metal smelting and vehicle emission were not very effective. The positive matrix factorization (PMF) results suggested that the contribution ratios of biomass burning, non-ferrous metal smelting, coal combustion, ferrous metal smelting, heavy oil combustion, and traffic-related dust changed from 5 %, 17 %, 20 %, 15 %, 9 %, and 34 % to 7 %, 13 %, 15 %, 14 %, 10 %, and 41 %, respectively. To date, no significant noncarcinogenic and carcinogenic risks were observed for all of the elements, while both of As and Pb still showed relatively high health damages. It was proposed to further cut down the combustion-related emissions (e.g., As and Pb) because it showed the highest marginal health benefits. Besides, the control of traffic-related emissions might be a key abatement strategy to facilitate the reduction of elements in fine particles.

Received: 28 Aug 2022 – Discussion started: 17 Oct 2022

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20 Apr 2023

Measurement report: Rapid changes of chemical characteristics and health risks for highly time resolved trace elements in PM_2.5 in a typical industrial city in response to stringent clean air actions

Rui Li, Yining Gao, Yubao Chen, Meng Peng, Weidong Zhao, Gehui Wang, and Jiming Hao

Atmos. Chem. Phys., 23, 4709–4726, https://doi.org/10.5194/acp-23-4709-2023,https://doi.org/10.5194/acp-23-4709-2023, 2023

Short summary

Rui Li, Meng Peng, Weidong Zhao, Gehui Wang, and Jiming Hao

Interactive discussion

Status: closed

RC1:
'Comment on egusphere-2022-848', Anonymous Referee #1, 08 Nov 2022
The authors study the changes of chemical characteristics and health risks for high time-resolved trace elements in PM2.5 in a typical industrial city of China and the changes during three years due to clean air actions. They separated the effects due to meteorology from those due to the

control measures by the use of a random forest (RF) model. The subject is interesting and the use of 1-hour resolution data is not still widespread. However the article can be published only after major revisions.

Comments:

- All the work is based on the analysis of the elemental concentration with 1-h resolution. At least in the supplementary material some graphs presenting the trend of the concentration of some elements over the three years should be presented

Lines 58-59. More references should be added; many articles dealing with elemental concentrations also in Europe or USA can be found in the literature

L 77: Dall’Osto et al. (2013) is a good example of application of PIXE, but it was not the first one (see. e.g. P.Prati et al, Source apportionment near a steel plant in Genoa (Italy) by continuous aerosol sampling and PIXE analysis, , 2000, 34(19), pp. 3149–3157 or A. D'Alessandro et al., Hourly elemental composition and sources identification of fine and coarse PM10 particulate matter in four Italian towns, , 2003, 34(2), pp. 243–259)

L 173: please use the extended name before introducing the acronym (RMSE, MAE)

L 203: The authors should add in the supplementary material the percentage of the elements reconstructed by PMF; it is necessary to assess the quality of the PMF analysis

L 228: How was the total mass measured? The value 5.7% is the average of the hourly or daily values or something else?

L 332: “Such a small change can produce the observed effects?

L 338-340: What about WD? It should be even more important than WS

Paragraph 3.4 The impact of clean air policy on source apportionment of trace elements:

Do the authors believe that the source profiles change over the years? From the data (fig. S4-S6) it does not seem so. The absolute source contribution both to the elements or to the total mass change because the emissions are reduced. I don't understand why the authors don't perform PMF analysis putting all the years together. This would immediately allow to see how the contribution of the different sources is reduced over the years even without having the total PM2.5mass and how the absolute contribution of the different sources to the elements vary. Instead, it is difficult to assess the influence of clean air policies only by looking at fig.7, where the average contributions of the six sources to the total mass concentrations of metals in PM2.5 is reported, which means a percentage contribution. The reduction of the percentage contribution of one source can produce an apparent increase in the percentage contribution of another source, even if the absolute contribution of that source is decreasing! Therefore, in my opinion, it would be more interesting to look at the source trend along the 3 years. The deweathering procedure can be performed also to these data.

L 345: The use of the proper experimental error is mandatory in PMF analysis. How were the experimental uncertainties on deweathered concentrations calculated?

L 368-371(but the same is true for other sources). The identification of the origin of the sources based only on back-trajectories is too qualitative. Since the authors have wind data, they should produce element/source wind polar plots like the ones e.g. reported in fig 3 c of Y. Chen et al.: Simultaneous measurements of urban and rural particles in Beijing, Atmos. Chem. Phys., 20, 9231–9247, 2020

400.402: ref. Moreno et al, says something more complex. At the end they say “Thus there is considerable overlap between V/Ni values in natural mineral dusts and those in emissions from the combustion of refinery-produced materials, and this hinders use of this ratio in pollution source identification.” Therefore the authors can keep the sentence, but they should be more cautious. Furthermore, is 1.2 the V/Ni ratio within the identified source (which can be easily obtained by the PMF analysis) or the ratio between the average concentrations during the sampling period? It is the former one which must be presented

L411-412: The authors must show in the supplementary material the average day (average concentration for each hour of the day like the ones e.g. reported in fig 3 b of Y. Chen et al.: Simultaneous measurements of urban and rural particles in Beijing, Atmos. Chem. Phys., 20, 9231–9247, 2020) at least for Ca, Fe, Zn, to see the rush hour peaks.

L 422-423: I would not define the decreases as dramatic. The experimental uncertainties in source contribution should be also taken into account

L 426: A change of 1% is within the experimental uncertainties due to the fitting procedure, I would not use the word “increase”

L 437-443: I agree with the authors that hourly data can give more valuable information regarding the health risk. However, I do not understand how they calculate the risk from the hourly data without averaging their data at least on a daily scale. EF represents the annual exposure frequency (d y−1), ADD is the daily intake (mg/kg/day) of trace metals, all these are quantities averaged at least on a daily base.
Citation: https://doi.org/10.5194/egusphere-2022-848-RC1
- AC1: 'Reply on RC1', Rui Li, 15 Dec 2022
  
  The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2022/egusphere-2022-848/egusphere-2022-848-AC1-supplement.pdf
  
  Citation: https://doi.org/10.5194/egusphere-2022-848-AC1
RC2:
'Comment on egusphere-2022-848', Anonymous Referee #2, 16 Nov 2022
This paper reports occurrence levels of elements in PM_2.5 in Tangshan China, analyzes the temporal variations and evolution of PM_2.5-associated elements, assesses the contributions of emission and meteorology to these species, apportions sources of elements during the whole period and evaluated influence of pollution control measures on the changes of carcinogenic and non-carcinogenic risks. This manuscript tries to represent the observation results and address relevant scientific questions. The scientific methods and assumptions are almost valid and outlined so that conclusions are reached. The description of experiments and calculations are shown. Observed phenomena as presented in the text and SIs have been described in detail. However, there are some hypotheses in the manuscript lacking of crucial evidential data to support. The link between the observed data and suggested implications is not strong. I do not recommend the publication of this article in its current form except some points.

The authors should go beyond reporting the measurements, present informative interpretations of the data and provide worldwide implication rather than local attention.

Please introduce clean air actions and pollution control measures in detail. Which control measures are used to improve air quality?

Atmospheric trace metals include nutrient elements and hazard elements. The nutrient elements are beneficial for ecosystem safety.

A comparative analysis was performed on the concentration of the trace metals in PM₅ observed in different cities. A scientific summary is necessary. Moreover, considering that the analytical methods and sampling duration were probably different for the available data set from the measurement and the literature review and uncertainty existed, the difference in the concentration of trace elements should be obtained based on statistical analysis.

Uncertainty on results of the random forest (RF) model (deweather) should be further shown in detail. Detailed input should be introduced into the model in detail.

Sufficient information was not provided by authors to validate the quality of the data. Being a field/experimental study, I am surprised by the lack of details on the data quality assessment and/or quality control methods, instrument calibration, how uncertainties are estimated. How to obtain meteorological parameters and PM₅?

No legends in some figures were given. Figure s has too crowded X-axe. Please modify them.

Why As had relatively high contribution in factor 1? Why was no vehicular emission identified in the results of source apportionment? As well known, dust (fugitive dust, dust storm, soil dust and road dust) have high or moderate loading of Ca, Cu and Fe.

The overall carcinogenic properties of mass PM itself should be taken into account. Emissions from gasoline and diesel engines and metal smelting and refining are considered Class 1A carcinogens by IARC; numerous populations studies have demonstrated increased (lung) cancer risk in communities with high urban PM exposures. Thus, the overall cancer risk from mass-based PM is likely to outweigh the risk of a limited set of elements. The authors seem to overinterpret their own risk assessment. If a realistic assessment of the actual health risks was involved, the results would be more meaningful.

Since RfD and HQ typically have (considerable) uncertainty/safety factors included, a HQ> 1 does not indicate “occurrence of adverse n-c effects” as claimed.

Open biomass burning has been banned in China after the execution of clean air act since 2013, in particular after 2018. How authors judged that biomass burning or open waste incineration in NCP contributed to the concentrations of trace elements in Tangshan?
Citation: https://doi.org/10.5194/egusphere-2022-848-RC2
- AC2: 'Reply on RC2', Rui Li, 15 Dec 2022
  
  The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2022/egusphere-2022-848/egusphere-2022-848-AC2-supplement.pdf
  
  Citation: https://doi.org/10.5194/egusphere-2022-848-AC2

Interactive discussion

Status: closed

RC1:
'Comment on egusphere-2022-848', Anonymous Referee #1, 08 Nov 2022
The authors study the changes of chemical characteristics and health risks for high time-resolved trace elements in PM2.5 in a typical industrial city of China and the changes during three years due to clean air actions. They separated the effects due to meteorology from those due to the

control measures by the use of a random forest (RF) model. The subject is interesting and the use of 1-hour resolution data is not still widespread. However the article can be published only after major revisions.

Comments:

- All the work is based on the analysis of the elemental concentration with 1-h resolution. At least in the supplementary material some graphs presenting the trend of the concentration of some elements over the three years should be presented

Lines 58-59. More references should be added; many articles dealing with elemental concentrations also in Europe or USA can be found in the literature

L 77: Dall’Osto et al. (2013) is a good example of application of PIXE, but it was not the first one (see. e.g. P.Prati et al, Source apportionment near a steel plant in Genoa (Italy) by continuous aerosol sampling and PIXE analysis, , 2000, 34(19), pp. 3149–3157 or A. D'Alessandro et al., Hourly elemental composition and sources identification of fine and coarse PM10 particulate matter in four Italian towns, , 2003, 34(2), pp. 243–259)

L 173: please use the extended name before introducing the acronym (RMSE, MAE)

L 203: The authors should add in the supplementary material the percentage of the elements reconstructed by PMF; it is necessary to assess the quality of the PMF analysis

L 228: How was the total mass measured? The value 5.7% is the average of the hourly or daily values or something else?

L 332: “Such a small change can produce the observed effects?

L 338-340: What about WD? It should be even more important than WS

Paragraph 3.4 The impact of clean air policy on source apportionment of trace elements:

Do the authors believe that the source profiles change over the years? From the data (fig. S4-S6) it does not seem so. The absolute source contribution both to the elements or to the total mass change because the emissions are reduced. I don't understand why the authors don't perform PMF analysis putting all the years together. This would immediately allow to see how the contribution of the different sources is reduced over the years even without having the total PM2.5mass and how the absolute contribution of the different sources to the elements vary. Instead, it is difficult to assess the influence of clean air policies only by looking at fig.7, where the average contributions of the six sources to the total mass concentrations of metals in PM2.5 is reported, which means a percentage contribution. The reduction of the percentage contribution of one source can produce an apparent increase in the percentage contribution of another source, even if the absolute contribution of that source is decreasing! Therefore, in my opinion, it would be more interesting to look at the source trend along the 3 years. The deweathering procedure can be performed also to these data.

L 345: The use of the proper experimental error is mandatory in PMF analysis. How were the experimental uncertainties on deweathered concentrations calculated?

L 368-371(but the same is true for other sources). The identification of the origin of the sources based only on back-trajectories is too qualitative. Since the authors have wind data, they should produce element/source wind polar plots like the ones e.g. reported in fig 3 c of Y. Chen et al.: Simultaneous measurements of urban and rural particles in Beijing, Atmos. Chem. Phys., 20, 9231–9247, 2020

400.402: ref. Moreno et al, says something more complex. At the end they say “Thus there is considerable overlap between V/Ni values in natural mineral dusts and those in emissions from the combustion of refinery-produced materials, and this hinders use of this ratio in pollution source identification.” Therefore the authors can keep the sentence, but they should be more cautious. Furthermore, is 1.2 the V/Ni ratio within the identified source (which can be easily obtained by the PMF analysis) or the ratio between the average concentrations during the sampling period? It is the former one which must be presented

L411-412: The authors must show in the supplementary material the average day (average concentration for each hour of the day like the ones e.g. reported in fig 3 b of Y. Chen et al.: Simultaneous measurements of urban and rural particles in Beijing, Atmos. Chem. Phys., 20, 9231–9247, 2020) at least for Ca, Fe, Zn, to see the rush hour peaks.

L 422-423: I would not define the decreases as dramatic. The experimental uncertainties in source contribution should be also taken into account

L 426: A change of 1% is within the experimental uncertainties due to the fitting procedure, I would not use the word “increase”

L 437-443: I agree with the authors that hourly data can give more valuable information regarding the health risk. However, I do not understand how they calculate the risk from the hourly data without averaging their data at least on a daily scale. EF represents the annual exposure frequency (d y−1), ADD is the daily intake (mg/kg/day) of trace metals, all these are quantities averaged at least on a daily base.
Citation: https://doi.org/10.5194/egusphere-2022-848-RC1
- AC1: 'Reply on RC1', Rui Li, 15 Dec 2022
  
  The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2022/egusphere-2022-848/egusphere-2022-848-AC1-supplement.pdf
  
  Citation: https://doi.org/10.5194/egusphere-2022-848-AC1
RC2:
'Comment on egusphere-2022-848', Anonymous Referee #2, 16 Nov 2022
This paper reports occurrence levels of elements in PM_2.5 in Tangshan China, analyzes the temporal variations and evolution of PM_2.5-associated elements, assesses the contributions of emission and meteorology to these species, apportions sources of elements during the whole period and evaluated influence of pollution control measures on the changes of carcinogenic and non-carcinogenic risks. This manuscript tries to represent the observation results and address relevant scientific questions. The scientific methods and assumptions are almost valid and outlined so that conclusions are reached. The description of experiments and calculations are shown. Observed phenomena as presented in the text and SIs have been described in detail. However, there are some hypotheses in the manuscript lacking of crucial evidential data to support. The link between the observed data and suggested implications is not strong. I do not recommend the publication of this article in its current form except some points.

The authors should go beyond reporting the measurements, present informative interpretations of the data and provide worldwide implication rather than local attention.

Please introduce clean air actions and pollution control measures in detail. Which control measures are used to improve air quality?

Atmospheric trace metals include nutrient elements and hazard elements. The nutrient elements are beneficial for ecosystem safety.

A comparative analysis was performed on the concentration of the trace metals in PM₅ observed in different cities. A scientific summary is necessary. Moreover, considering that the analytical methods and sampling duration were probably different for the available data set from the measurement and the literature review and uncertainty existed, the difference in the concentration of trace elements should be obtained based on statistical analysis.

Uncertainty on results of the random forest (RF) model (deweather) should be further shown in detail. Detailed input should be introduced into the model in detail.

Sufficient information was not provided by authors to validate the quality of the data. Being a field/experimental study, I am surprised by the lack of details on the data quality assessment and/or quality control methods, instrument calibration, how uncertainties are estimated. How to obtain meteorological parameters and PM₅?

No legends in some figures were given. Figure s has too crowded X-axe. Please modify them.

Why As had relatively high contribution in factor 1? Why was no vehicular emission identified in the results of source apportionment? As well known, dust (fugitive dust, dust storm, soil dust and road dust) have high or moderate loading of Ca, Cu and Fe.

The overall carcinogenic properties of mass PM itself should be taken into account. Emissions from gasoline and diesel engines and metal smelting and refining are considered Class 1A carcinogens by IARC; numerous populations studies have demonstrated increased (lung) cancer risk in communities with high urban PM exposures. Thus, the overall cancer risk from mass-based PM is likely to outweigh the risk of a limited set of elements. The authors seem to overinterpret their own risk assessment. If a realistic assessment of the actual health risks was involved, the results would be more meaningful.

Since RfD and HQ typically have (considerable) uncertainty/safety factors included, a HQ> 1 does not indicate “occurrence of adverse n-c effects” as claimed.

Open biomass burning has been banned in China after the execution of clean air act since 2013, in particular after 2018. How authors judged that biomass burning or open waste incineration in NCP contributed to the concentrations of trace elements in Tangshan?
Citation: https://doi.org/10.5194/egusphere-2022-848-RC2
- AC2: 'Reply on RC2', Rui Li, 15 Dec 2022
  
  The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2022/egusphere-2022-848/egusphere-2022-848-AC2-supplement.pdf
  
  Citation: https://doi.org/10.5194/egusphere-2022-848-AC2

Peer review completion

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

AR by Rui Li on behalf of the Authors (15 Dec 2022) Author's response Author's tracked changes Manuscript

ED: Reconsider after major revisions (10 Jan 2023) by Willy Maenhaut

The authors have reasonably addressed the comments of the two anonymous referees. However, the manuscript has major shortcomings. It suffers from poor language and grammar. I tried to improve on this, see under Alterations and Corrections below, but additional improvement is desirable. Furthermore, the manuscript is on various occasions unclear. Moreover, verbs are often used with the past tense where the present tense would be more appropriate. Major revision is definitely needed before this manuscript could become acceptable for publication.

Alterations, Corrections and Comments for the Main text:
Line 9: Replace "energy conservation and environmental protection" by "Energy Conservation and Environmental Protection".
Line 18: Just one example of using improper tense, replace "remained" by "remains".
Line 38: Replace "the persistent" by "persistent".
Line 39: Replace "the massive" by "massive".
Lines 41, 254, and 466: Replace "threaten" by "threat".
Line 42: Replace "physiochemical" by "physicochemical".
Lines 55 and 529: Replace "controls measures" by "control measures".
Line 60: Replace "mountain" by "mountainous" and replace "the filter sampling" by "filter sampling".
Line 61: Replace "technique coupled" by "coupled".
Line 64: Replace "many valuable" by "much valuable".
Line 70: Replace "the receptor models" by "receptor models".
Line 78: Replace "analyze hourly" by "measure hourly" and replace "work, A." by "work,".
Line 81: Replace "used Xact" by "used the Xact".
Line 83: Replace "performed in" by "employed in".
Line 85: Replace "found traffic" by "found that traffic".
Line 87: Replace "1-year atmospheric elements" by "atmospheric elements during a full year".
Line 88: Replace "considered as the" by "the".
Line 93: Replace "Chinese government proposed" by "the Chinese government proposed a".
Line 94: Replace "suffered from" by "showed".
Line 96: Replace "the rapid changes response" by "rapid changes due".
Lines 99-100: It is unclear what is meant by "population-weighted mean concentrations".
Line 101: Replace "respectively during" by "respectively, during".
Line 105: Replace "of clean" by "of the clean".
Line 113: Replace "in North" by "in the North".
Line 120: Replace "for coal-fired" by "for the coal-fired".
Line 121: Replace "coal to" by "the coal to".
Line 122: Replace "suffered from" by "underwent".
Line 126: Replace "China during" by "China, during".
Line 136: Replace "including Airport" by "including the Airport".
Line 139: Replace "Beihu" by "the Beihu".
Line 142: Replace "of large" by "of the large".
Line 143: Replace "focus on" by "focus on the".
Lines 146-148: I understand from line 515 that the measurement was done continuously; therefore, replace "were determined" by "were determined continuously".
Line 151: Replace "detect the" by "determine the".
Line 154: Replace "of online" by "of the online".
Line 161: Replace "the particulate" by "a particulate".
Line 173: Replace "All of trace" by "All trace".
Line 178: Replace "the remained" by "the remaining".
Line 179: Replace "of trace" by "of the trace".
Line 181: Replace "of original element concentrations and deweathered" by "between the original element concentrations and the deweathered".
Line 185: Replace "be the unconvincing" by "be an unconvincing".
Line 191: Replace "PMF 5.0" by "the PMF 5.0"; furthermore, a literature reference is needed here; an appropriate one is: Norris, G., Duvall, R., Brown, S., and Bai, S.: EPA positive matrix factorization (PMF) 5.0 fundamentals and user guide. U.S. Environmental Protection Agency Office of Research and Development, Washington, DC, 20460 (i-124, EPA/600/R-14/108, April), 2014.
Line 192: Replace "of atmospheric" by "of the atmospheric".
Line 194: Replace "between measured" by "between the measured".
Line 195: Replace "contribution and factor profile" by "contributions and factor profiles".
Line 196: Replace "for individual" by "for an individual".
Line 202: Replace "of jth" by "of the jth".
Line 203: Replace "of kth source to ith sample, fkj represents the ratio of jth element in kth" by "of the kth source to the ith sample, fkj represents the ratio of the jth element in the kth".
Line 204: Replace "of jth element in the i sample" by "of the jth element in the ith sample".
Line 205: Replace "including bootstraps" by "including the bootstrap".
Line 218: Replace "by International" by "by the International".
Line 219: Replace "of IARC" by "of the IARC".
Line 220: Replace "meatal" by "metal".
Lines 226-230: The units should be indicated for InhR, ED, BW, AT, ADD, RfD, the reference concentrations, and CSF.
Line 237: A median value does not have a single associated uncertainty; is it perhaps the mean value and associated standard deviation here?
Lines 241-245, and further on: When data with associated uncertainties are give, what are they? Perhaps the mean value and associated standard deviation? In any case, it should be specified.
Line 245: Replace "were most" by "were the most".
Line 247: Replace "to the previous" by "to in previous".
Line 252: Replace "However, the" by "Moreover, the".
Line 260: Replace "Europe" by "European".
Line 262: Replace "of CAAQS" by "of the CAAQS".
Line 264: Replace "of original concentrations of" by "of the original concentrations of the".
Line 265: Replace "Figure 3 and S2-S3. The original concentrations of all the trace elements exhibited the" by "Figures 3 and S2-S3. The original concentrations of all the trace elements exhibited".
Line 266: Replace "Cu, Co, Zn, Pb, As, and Ga concentrations suffered from" by "The Cu, Co, Zn, Pb, As, and Ga concentrations showed".
Line 268: Replace "observed K" by "the K".
Line 273: Replace "of trace" by "of the trace".
Line 274: Replace "on element" by "on the element".
Line 276: Replace "of element concentrations to" by "of the element concentrations to the".
Line 277: Replace "by RF" by "by the RF".
Line 281: Replace "on RF" by "on the RF".
Line 286: Replace "has estimated" by "have estimated".
Line 288: Replace "of industrial" by "of the industrial".
Line 291: Replace "However," by "In contrast,".
Line 295: Replace "of deweathered" by "of the deweathered".
Line 297: Replace "future work" by "future".
Line 300: Replace "suffered from" by "showed".
Line 302: Replace "industrial layout" by "the industrial layout".
Line 303: Replace "in high-pollution" by "in the high-pollution".
Line 304: Replace "suffered from" by "exhibited".
Line 307: Replace "in harvest" by "in the harvest".
Line 317: Replace "the higher decreasing ratios at the weekends than those" by "higher decreasing ratios at the weekends than on".
Line 318: Replace "(2020) has" by "(2020) have".
Line 331: Replace "show regular" by "show a regular".
Line 332: Replace "increase from" by "increased from".
Line 334: Replace "Vi and Ni" by "V and Ni".
Line 337: Replace "of original and" by "between the original and the".
Line 339: Replace "on trace" by "on the trace".
Line 348: Replace "used RF" by "used the RF"; also, it is unclear what is meant by "variable importance".
Line 352: Replace "to the higher" by "to a higher".
Line 356: Replace "displayed slight" by "displayed a slight".
Line 360: Replace "(Figure S6-8). As shown in Figure S8, both of V and Ni showed the" by "(Figures S6-S8). As shown in Figure S8, both V and Ni showed".
Line 364: Replace "on source apportionment of" by "on the source apportionment of the".
Line 366: Replace "of major" by "of the major".
Line 367: Replace "(PMF 5.0) version" by "(version PMF 5.0)".
Line 368: Replace "elements in PM2.5 during 2017-2020 based on" by "the elements in PM2.5 during 2017-2020 based on the".
Line 371: Replace "of PMF analysis and error diagnostics are" by "of the PMF analysis and error diagnostics is".
Line 372: Replace "Table S4-6" by "Tables S4-S6".
Line 373: Replace "similar cluster" by "similar".
Line 376: Replace "showed the higher" by "showed higher".
Line 378: Replace "Except the domestic heating, we found some episodes during" by "Except for the domestic heating, we found some episodes during the".
Lines 379, 435, and 519, and in Table 1: Some numeric data are given with too many significant figures; 2 significant figures suffice and 3 can be used when the first significant figure is "1"; thus, in line 379, replace "2450" by "2500" and replace "2630" by "2600", and in line 435 replace "1458, 479, 636, and 569 ng/m3 to 901, 225, 230, and 345" by "1460, 480, 640, and 570 ng/m3 to 900, 230, 230, and 350".
Line 381: Replace "Figure S6-8" by "Figures S6-S8".
Line 382: Replace "in NCP" by "in the NCP".
Line 386: Replace "such Ag in nonferrous metal ores could be vaporized as the" by "such as Ag in nonferrous metal ores could be vaporized as a"
Line 387: Replace "Therefore, the" by "Therefore,".
Line 391: Replace "suffered from" by "showed".
Line 392: Replace "as the important" by "as important".
Line 393: Replace "of burning" by "of the burning".
Line 397: Replace "in NCP. In our study, As, Co and Pb showed the" by "in the NCP. In our study, As, Co and Pb showed".
Line 402: Replace "were mainly sourced from" by "mainly originated from the".
Line 403: Replace "occupied more" by "was responsible for more".
Line 404: Replace "world steel production in 2017 (approximate 830 million tons), and 60%" by "the world steel production in 2017 (approximate 830 million tons), and 60% of the".
Line 411: Replace "However, Ni" by "Ni".
Line 413: Replace "Figure S6-S8" by "Figures S6-S8".
Line 416: Replace "of V and Ni concentrations displayed the" by "the V and Ni concentrations displayed".
Line 422: Replace "Ni the" by "Ni in the".
Line 424: Replace "that both of Cu" by "that Cu".
Lines 426-427: Replace "was probably sourced from" by "probably originated from".
Line 428: Replace "continents (Alves et al., 2015; Liu et al., 2018a). Moreover, we have found" by "soil (Alves et al., 2015; Liu et al., 2018a). Moreover, we have found that".
Line 430: Replace "of traffic volume. Thus, the" by "of the traffic volume. Thus,".
Line 433: Replace "Figure 7" by "Figures 7".
Line 437: Replace "displayed slight" by "displayed a slight".
Line 438: Replace "all of the sources to trace elements suffered from" by "all sources to the trace elements showed".
Line 440: Replace "to trace" by "to the trace".
Line 441: Replace "of traffic-related" by "of the traffic-related".
Line 442: Replace "However," by "In contrast,".
Line 446: Replace "of clean" by "of the clean".
Line 447: Replace "the cleaner technologies have been upgraded" by "cleaner technologies were implemented".
Line 451: Replace "to trace" by "to the trace".
Line 456: Replace "to trace elements also showed" by "to the trace elements also showed a".
Line 457: Replace "the marked" by "marked".
Line 458: Replace "suffered from" by "displayed".
Line 465: Replace "for minor fraction of" by "for a minor fraction of the".
Line 468: Replace "the filter sampling" by "filter sampling".
Line 470: Replace "the online" by "online".
Line 473: Replace "Table S7 and Table S8" by "Tables S7 and S8".
Line 474: Replace "of major" by "of the major".
Line 475: Replace "on element concentrations, both of" by "on the element concentrations, both".
Line 476: Replace "original element levels and" by "the original element levels and the".
Line 477: Replace "on original" by "on the original".
Line 481: Replace "from slight" by "from a slight".
Line 483: Replace "both of Pb" by "both Pb".
Line 484: Replace "of trace" by "of the trace".
Line 485: Replace "showed the higher" by "showed higher".
Line 486: Replace "all of the elements" by "all elements".
Line 487: Replace "because HQ" by "because the HQ".
Line 488: Replace "were also" by "was also".
Line 489: Replace "show significant" by "show a significant".
Line 490: Replace "of meteorological conditions, we can isolate the impact of clean" by "of the meteorological conditions, we can isolate the impact of the clean".
Lines 491 and 493: Replace "decrease ratios of" by "decreased ratios of the".
Line 493: Replace "on original" by "on the original".
Line 495: Replace "decrease ratios of HQ values for" by "decreased ratios of the HQ values for the".
Line 496: Replace "much less than those for" by "lower than those for the".
Line 497: Replace "show the similar" by "show similar".
Lines 497-498: Replace "show the similar characteristics. For instance, the decrease ratios of HQ values for original Cr (21%) and Fe (27%) were even slightly higher than those for" by "show similar characteristics. For instance, the decreased ratios of the HQ values for the original Cr (21%) and Fe (27%) were even slightly higher than those for the".
Line 501: Replace "of elements" by "of the elements".
Line 502: Replace "in the section" by "in section".
Line 516: Replace "air clean policy on" by "the clean air policy on the".
Line 517: Replace "were quantified. The main conclusions were drawn" by "was quantified. The main conclusions were".
Line 518: Replace "showed the rapid" by "showed rapid".
Line 520: Replace "Clean air" by "The clean air".
Line 524: Replace "might be not" by "might not be".
Line 528: Replace "offset the" by "offsets the".
Line 535: Replace "All of the" by "All".
Line 536: Replace "of As" by "As".
Line 539: Replace "enlightenment for" by "insights for the".
Line 543: Replace "these elements" by "the elements" and replace "Sunset" by "a Sunset".
Line 544: Replace "Monitoring" by "a Monitoring".
Line 556: Replace "author has" by "authors have".
Pages 21-26, Reference list:
- for authors with more than 1 initial, there should be a space between two subsequent initials;
- there should be a comma instead of a period before the abbreviated journal name;
- abbreviated journal names (and correct abbreviated journal names) should be used; for example, instead of "J. Aero. Sci." it should be "J. Aerosol Sci.".
Lines 558-560: This reference should be moved down; it should come before "Dall'Osto et al., 2013".
Line 585: Replace "matter. Atmospheric Environment,89" by "matter, Atmos. Environ., 89".
Line 623: Replace "Greece." by "Greece, ".
Line 643: Replace "metals. J" by "metals, J.".
Line 685: Replace " 191" by ", 191".
Lines 714-716: The page numbers are missing.
Line 720: Replace " 5" by ", 5".
Lines 789-790: This reference should be moved up; it should come after "Shi et al., 2015".
Line 792: Replace " 621" by ", 621".
Page 27, caption of Figure 1: Replace "The topographic map of China indicating the location of Tangshan (a), sampling" by "Topographic map of China indicating the location of Tangshan (a), the sampling".
Page 28, caption of Figure 2: Replace "The bar" by "Bar"; furthermore, it should be indicated what the data in the figure represent; are they mean values and associated standard deviations?
Page 29, caption of Figure 3: Replace "of original" by "of the original"; furthermore, it should be indicated what the data in the figure represent; are they mean values and associated standard deviations?
Page 30, caption of Figure 4: Replace "The original" by "Original"; furthermore, it should be indicated what the data points and shaded areas in the figure represent.
Page 31, caption of Figure 5: Replace "of original" by "of the original" in lines 1 and 2; furthermore, it should be indicated what the data in the figure represent; are they mean values and are the error bars associated standard deviations?
Page 32, caption of Figure 6, line 2: Replace "in RF models for" by "in the RF models for the".
Page 33, caption of Figure 7: Replace "The deweathered concentrations of" by "Deweathered concentrations of the"; furthermore, it should be indicated what the data in the figure represent; are they mean values?
Page 34, caption of Figure 8: Replace "of six sources to the deweathered concentrations of elements in PM2.5 based on PMF" by "of the six sources to the deweathered concentrations of the elements in PM2.5 based on the PMF",
Page 35, heading of Table 1: Replace "The comparison of" by "Comparison of the"; also it should be indicated what the unit is for the numeric data.
Page 36, heading of Table 2: Replace "The non-carcinogenic" by "Non-carcinogenic"; also it should be indicated what the unit is for the numeric data.
Page 38, heading of Table 3: Replace "The non-carcinogenic" by "Non-carcinogenic"; also it should be indicated what the unit is for the numeric data.

Alterations, Corrections and Comments for the Supplement:
Page 1, for affiliation "c": Replace "energy conservation and environmental protection" by "Energy Conservation and Environmental Protection".
Page 2: I found no reference to this section in the Main text, whereas such reference is needed.
Page 2, line 1: Replace "the detailed" by "Detailed".
Page 2, line 2: Replace "Chinese government imposed many emission controls to alleviate" by "the Chinese government imposed many emission controls to alleviate the".
Page 2, line 3: Replace "enhanced comprehensive" by "enhanced a comprehensive".
Page 2, line 4: Replace "Second" by "Secondly".
Page 2, line 5: Replace "upgrade industrial" by "upgrade their industrial".
Page 2, line 6: Replace "Third" by "Thirdly".
Page 2, line 8: Replace "the energy efficiency were tried to improve" by "it was tried to improve the energy efficiency".
Page 2, line 9: Replace "Chinese governments tried to optimize industrial layout. Chinese" by "The Chinese governments tried to optimize the industrial layout. The Chinese".
Page 4, caption of Figure S2: Replace "The time-series varies variations of" by "Time series for"; also it should be indicated what the unit is for the data in the figure.
Page 5, caption of Figure S3: Replace "The time-series varies variations of" by "Time series for"; also it should be indicated what the unit is for the data in the figure.
Page 6, caption of Figure S4: line 1, replace "The performance" by "Performance"; line 2, replace "original" by "of the original; line 3, replace "applied to" by "used to"; also it should be indicated what the unit is for the data in the figure.
Page 7, caption of Figure S5: Replace "The changes" by Changes".
Page 8, caption of Figure S6: Replace "The 72-h" by "72-h"; also it should be indicated what the unit is for the K data in figure (b).
Page 9, caption of Figure S7, line 1: Replace "The 72-h air masses" by "72-h air mass".
Page 9, caption of Figure S7, line 2: Replace "of total air masses" by "of the total air mass trajectories".
Page 10, caption of Figure S8: Replace "The polar" by "Polar"; also it should be indicated what the unit is for the V and Ni data in figures (a) and (b).
Page 11, caption of Figure S9: Replace "The source" by "Source".
Page 12, caption of Figure S10: Replace "The diurnal" by "Diurnal".
Page 13, heading of Table S1: Replace "The basic" by "Basic".
Page 14, heading of Table S2: Replace "by Model" by "by the Model".
Page 15, heading of Table S3: Replace "The sampling duration, analytic method, and average element" by "Sampling duration, analytical method, and average"; also the unit for the numeric data in the table should be given.
Page 15, Table S3: Replace "Visser et al. (2015)" by "(Visser et al., 2015)"; also, this reference is missing in the Reference list.
Page 15, Table S3, column 1: Replace "Analytic method" by "Analytical technique"; also the abbreviated analytical techniques should be explained (written full-out) in a footnote.
Page 20, Table S8: The units for the numeric data in the table should be indicated.
Page 21, Reference list: the references are not in the proper format:
- the publication year should come at the end of the reference;
- for authors with more than 1 initial, there should be a space between two subsequent initials;
- there should be "and" before the last name of the last author;
- titles of journal articles should be in lower case instead of in Title Case;
- there should be a comma instead of a period before the abbreviated journal name;
- abbreviated journal names (and correct abbreviated journal names) should be used.

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AR by Rui Li on behalf of the Authors (14 Jan 2023) Author's response Author's tracked changes Manuscript

ED: Publish subject to minor revisions (review by editor) (09 Feb 2023) by Willy Maenhaut

Unfortunately, in contrast to what the authors claim in their response document, many alterations, corrections and comments that I indicated were not taken into consideration; therefore, these alterations, corrections and comments are repeated below and also a few new ones are given. I urge the authors to be more careful in their next revision.

Alterations, Corrections and Comments for the Main text:
Line 9: Replace "Energy conservation" by "Energy Conservation".
Line 96: Replace "the rapid changes" by "rapid changes".
Line 174: Replace "All of the trace" by "All trace".
Line 179: Replace "the remained" by "the remaining".
Line 182: Replace "theoriginal" by "the original".
Line 206: Replace "the i sample" by "the ith sample".
Line 228: The unit should be indicated for InhR.
Line 243: Replace "concentrations of" by "average concentrations (± standard deviation) of".
Line 267: Replace "of trace elements" by "of the trace elements".
Line 269: Replace "Cu, Co," by "The Cu, Co,
Line 340: Replace "and deweathered" by "and the deweathered".
Lines 363-364: Replace "both of V and Ni showed the higher" by "both V and Ni showed higher".
Line 367: Replace "of trace elements" by "of the trace elements".
Line 376: Replace "Table S4-S6" by "Tables S4-S6".
Line 400: Replace "showed the higher" by "showed higher".
Line 405: Replace "from metallurgical" by "from the metallurgical".
Line 420: Replace "displayed the gradual" by "displayed gradual".
Line 432: Replace "found Fe" by "found that Fe".
Line 442: Replace "to trace elements suffered from" by "to the trace elements showed".
Line 451: Replace "have been upgraded" by "were implemented".
Line 460: Replace "showed slight" by "showed a slight".
Line 479: Replace "original element levels" by "the original element levels".
Lines 494 and 496: Replace "decrease ratios" by "decreased ratios".
Line 498: Replace "decrease ratios of HQ" by "decreased ratios of the HQ".
Line 499: Replace "much less than" by "lower than".
Line 520: Replace "were drawn as" by "were as".
Pages 21-26, Reference list:
- for authors with more than 1 initial, there should be a space between two subsequent initials; for example, in line 565 replace "A.I." by "A. I.";
- abbreviated journal names (and correct abbreviated journal names) should be used; see corrections below.
Lines 615 and 791: Replace "Int. J. Env. Res. Pub. He." by "Int. J. Environ. Res. Public Health".
Line 628: Replace "Res.,18" by "Res., 18".
Line 706: Replace "Air Qual. Atmos. Heal." by "Air Qual. Atmos. Health".
Line 713: Replace "Interna. J." by "Intern. J.".
Line 721: The reference starting with "Oldani" should start on a new line.
Lines 734 and 789: Replace "Environ. Interna." by "Environ. Int.".
Line 752: Replace "China 38" by "China, 38".
Line 755: Replace "Food and Chemical Toxicology 46" by "Food Chem. Toxicol., 46"
Page 28, caption of Figure 2: Replace "The bar and black line" by "The bars and black lines".
Page 29, caption of Figure 3: Replace "The bar and black line" by "The bars and black lines".
Page 30, caption of Figure 4: Replace "The point and shaded area" by "The points and shaded areas".
Page 31, caption of Figure 5: Replace "of original" by "of the original" in lines 1 and 2; furthermore, replace "The bar and black line" by "The bars and black lines".
Page 33, caption of Figure 7: It should be indicated what the data in the figure represent; are they mean values? If so, replace "Deweathered concentrations" by "Deweathered mean concentrations".
Page 34, caption of Figure 8: Replace "of elements in" by "of the elements in",
Pages 35-39, Tables 1, 2, and 3: Several numeric data are given with too many significant figures; 2 significant figures suffice and 3 can be used when the first significant figure is "1"; for example, in Table 1 for V, replace " 3.98±3.57" by "4.0±3.6".
Page 36, heading of Table 2: It should be indicated in the heading what the unit is for the numeric data; incidentally, the unit cannot be "1"; could it be fraction of 1?.
Page 38, heading of Table 3: It should be indicated in the heading what the unit is for the numeric data; incidentally, the unit cannot be "1"; could it be fraction of 1?.

Alterations, Corrections and Comments for the Supplement:
Page 1, for affiliation "c": Replace "Energy conservation " by "Energy Conservation".
Page 2: I found no reference to this section in the Main text, whereas such reference is needed.
Page 8, caption of Figure S6, line 3: Replace "colorbar" by "color bar".
Page 9, caption of Figure S7, line 2: Replace "of total air" by "of the total air".
Page 10, caption of Figure S8, line 1: Replace "colorbar" by "color bar".
Page 15, Table S3, column 1: Replace "Analytic method" by "Analytical technique"; in the footnote, replace "energy-dispersive" by "energy dispersive" and replace "X‐ray fluorescence spectrometer" by "X‐ray fluorescence analysis".
Page 21, for "Salameh et al.": Replace "Res. 155" by "Res., 155".
Page 21, for "Visser et al.": Replace "Dressler" by "and Dressler".

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AR by Rui Li on behalf of the Authors (12 Feb 2023) Author's response Author's tracked changes Manuscript

ED: Publish subject to minor revisions (review by editor) (10 Mar 2023) by Willy Maenhaut

AR by Rui Li on behalf of the Authors (11 Mar 2023) Author's response Author's tracked changes Manuscript

ED: Publish as is (02 Apr 2023) by Willy Maenhaut

AR by Rui Li on behalf of the Authors (02 Apr 2023) Manuscript

Journal article(s) based on this preprint

20 Apr 2023

Rui Li, Yining Gao, Yubao Chen, Meng Peng, Weidong Zhao, Gehui Wang, and Jiming Hao

Atmos. Chem. Phys., 23, 4709–4726, https://doi.org/10.5194/acp-23-4709-2023,https://doi.org/10.5194/acp-23-4709-2023, 2023

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Rui Li, Meng Peng, Weidong Zhao, Gehui Wang, and Jiming Hao

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https://doi.org/10.5194/egusphere-2022-848-supplement

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Data for “Measurement Report: Rapid changes of chemical characteristics and health risks for high time-resolved trace elements in PM2.5 in a typical industrial city in response to stringent clean air actions” Li, R., Peng, M., Zhao, W. D., Wang, G. H., and Hao, J. M. https://zenodo.org/record/7031975#.Ywys8cjfmfU

Rui Li, Meng Peng, Weidong Zhao, Gehui Wang, and Jiming Hao

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RF model was used to isolate the effects of emission and meteorology to trace elements in PM_2.5 in Tangshan. The result suggested that the control measures facilitated the decreases of Ga, Co, Pb, Zn, and As. It is due to the strict implementation of “coal to gas” strategies and optimization of industrial structure and layout. However, the deweathered levels of Ca, Cr, and Fe only displayed minor decreases, indicating that ferrous metal smelting and vehicle emission controls should be enhanced.


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Measurement Report: Rapid changes of chemical characteristics and health risks for high time-resolved trace elements in PM2.5 in a typical industrial city response to stringent clean air actions

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Measurement Report: Rapid changes of chemical characteristics and health risks for high time-resolved trace elements in PM_2.5 in a typical industrial city response to stringent clean air actions