the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
| 26 Nov 2024
Downward and upward revisions of Chinese emissions of black carbon and CO in bottom-up inventories are still required: an integrated analysis of WRF/CMAQ model and EMeRGe observations in East Asia in spring 2018
Abstract. Accurate estimates of short-lived climate forcers (SLCFs) emissions are required to allow efficient strategies that mitigate climate change to be developed. However, there remain large uncertainties about emissions of SLCFs from Asia. We identified and improved the constraints of combustion-related emissions of black carbon (BC) and CO using the WRF/CMAQ model (v5.0.2) and the EMeRGe airborne observation data for East Asia in spring 2018. We performed case studies of air masses containing emissions from fires near Thailand and emissions from urban areas in the Philippines and China. Chinese emissions were analysed in depth. Unlike observations at ground-based stations, the observations from aircraft used here would not have been strongly influenced by local emissions and near-surface processes. We confirmed that the GFEDv4.1s inventory provided accurate data for emissions from fires near Thailand. However, anthropogenic BC and CO emissions from the Philippines (REASv2.1) were negatively biased. Marked positive and negative differences were found for BC (+1.62 µg m−3) and CO (−400 ppbv) from the HTAPv2.2z emission inventory for Chinese air masses, consistent with the results of previous ground-based studies. The Chinese BC/CO emission ratio, 3.5±0.1 ng m−3 ppb−1, calculated using data from airborne observations in the altitude range ~0.3–1 km also agreed with the ground-based results. Linearly scaling BC emissions using an observation/model ratio (E(BC) = 0.48±0.13) gave our best estimate of 0.65±0.25 (Tg BC) yr-1. The calculated BC/CO and CO/CO2 ratios led us to estimate that emissions from China are 166±65 (Tg CO) yr-1 and 12.4±4.8 (Pg CO2) yr-1. The results suggested that downward and upward revisions of Chinese emissions of BC (−50 %) and CO (+20 %), respectively, are required in HTAPv2.2z emission inventory.
Competing interests: At least one of the (co-)authors is a member of the editorial board of Atmospheric Chemistry and Physics.
Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims made in the text, published maps, institutional affiliations, or any other geographical representation in this paper. While Copernicus Publications makes every effort to include appropriate place names, the final responsibility lies with the authors. Views expressed in the text are those of the authors and do not necessarily reflect the views of the publisher.-
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The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
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The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
- Preprint
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Supplement
(1691 KB) - BibTeX
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- Final revised paper
Journal article(s) based on this preprint
Interactive discussion
Status: closed
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RC1: 'Comment on egusphere-2024-2064', Anonymous Referee #1, 02 Jan 2025
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AC1: 'Reply on RC1', Phuc Ha, 21 Jul 2025
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-2064/egusphere-2024-2064-AC1-supplement.pdf
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AC1: 'Reply on RC1', Phuc Ha, 21 Jul 2025
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RC2: 'Comment on egusphere-2024-2064', Anonymous Referee #2, 26 May 2025
Comments on manuscript egusphere-2024-2064: "Downward and upward revisions of Chinese emissions of black carbon and CO in bottom-up inventories are still required: an integrated analysis of WRF/CMAQ model and EMeRGe observations in East Asia in spring 2018” by Phuc Thi Minh Ha et al.
General remarks and questions
This preprint reports aircraft measurements of black carbon (BC), CO, and CO2 measured in the lower troposphere eastward along the Asian continent over the sea and around Japan and the Philippines. Pollution plumes with elevated levels of CO and BC are investigated and the observed concentrations are compared with predictions from the WRF-CMAQ model. Observed to modeled concentration ratios derived from this are proposed as correction factors for emission inventories used in the model. Such an investigation of emission inventories is useful to achieve improved air quality predictions in the regions studied, and the aircraft measurements presented here provide a rare and good opportunity to extend analyses from ground based measurements.
Unfortunately, the presentation of the scientific approach and results in this paper is somewhat confusing and difficult to understand in places. The following aspects are not addressed clearly enough for general understanding and require a more detailed discussion. Major revisions are required before the paper is suitable for publication in ACP.
(1) To what extent can CO, CO2, and BC be considered as inert tracers that are essentially only subject to transport and deposition after emission on a 5d time scale, as considered in the backward trajectory calculations. To what extent could other chemical or physical processes influence their concentrations observed on the aircraft?
(2) Which source regions were exactly investigated using the approach with model calculations and flight measurements? Line 108 states: “Pollution plumes from major population centers in Asia were detected during parts of flights.” Which major population centers are specifically meant? Asia is a very large continent. Generalized statements such as “The results suggested that downward and upward revisions of Chinese emissions ... are required” (see abstract) is VERY general and should be formulated more cautiously and refer specifically to the regions or areas investigated. The authors should also consider making the title of the paper more specific. Also, to what extent could the findings be limited in time, e.g., only for the season or year investigated? How representative were the environmental conditions (fire activity, traffic, meteorology) prevailing during the flight campaign for the years before and after?
(3) The title of the paper states “Downward and upward revisions … are still required…”. Is this statement still valid approximately seven years after the aircraft campaign? Have there been any developments in East Asia since then with regard to biomass burning, industrial emissions, or traffic that would warrant a new investigation?
(4) There is only very limited information given on the EMERGE campaign and the aircraft measurements. A brief overview should therefore be provided in Section 2.1. The following information would be of interest. Why was springtime chosen for the campaign? What altitude range was covered during the measurement flights and what altitude range was specifically evaluated? Which measuring instruments were used (manufacturer, model) and what are their total measurement errors (precision, accuracy)? Which particle sizes were detected by the BC measuring device and how was the photometer signal converted into mass concentration? For which reference conditions (T, p) do the specified mass concentrations apply? Were other compounds (e.g., NOx, VOCs) measured and used in this work, e.g., for the identification of plumes, apart from BC, CO, and CO2? A PTR-MS instrument is mentioned in line 112. What was measured by this instrument and were the corresponding data used in any way?
(5) Section 2.2: which processes (apart from emission, transport, and deposition) play a role for the simulation of BC, CO, and CO2 on the 5d time scale of the backward trajectories investigated? Table 1 lists various types of emissions. Apart from direct emissions of BC, CO, and CO2, do other emitted substances, for example biogenic VOCs mentioned in the table, play a role? If so, which chemical processes were involved? Which processes represented in the AERO 6 aerosol module are relevant for the modeled results of BC in this study? What role do the volcanic emissions listed in Table 1 potentially play?
(6) For each model component listed in Table 1, references should be provided where a description or corresponding data can be found.
(7) In Section 2.4, the general description of the concept of "residual ratios" and "baseline values" is hard to understand and should be rephrased for clarity.
Minor Comments
Abbreviations (EMERGE, WRF-CMAQ, GFED, HTAPv2.2z, etc.) should be defined at the beginning of the paper when they are first used.
Line 42: Typo “nanometre-sized”
Lines 96-97: The sentence is unclear. Which other pollutants (apart from CO, CO2, BC) were investigated?
Line 105: Typo “Deutches”
What is the meaning of the given quantities (e.g., max = 1.3 mm) for APT3 in lines 340 and 575?
Table S3 appears to have no use in the paper and should be deleted.
Citation: https://doi.org/10.5194/egusphere-2024-2064-RC2 -
AC2: 'Reply on RC2', Phuc Ha, 21 Jul 2025
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-2064/egusphere-2024-2064-AC2-supplement.pdf
-
AC2: 'Reply on RC2', Phuc Ha, 21 Jul 2025
Interactive discussion
Status: closed
-
RC1: 'Comment on egusphere-2024-2064', Anonymous Referee #1, 02 Jan 2025
-
AC1: 'Reply on RC1', Phuc Ha, 21 Jul 2025
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-2064/egusphere-2024-2064-AC1-supplement.pdf
-
AC1: 'Reply on RC1', Phuc Ha, 21 Jul 2025
-
RC2: 'Comment on egusphere-2024-2064', Anonymous Referee #2, 26 May 2025
Comments on manuscript egusphere-2024-2064: "Downward and upward revisions of Chinese emissions of black carbon and CO in bottom-up inventories are still required: an integrated analysis of WRF/CMAQ model and EMeRGe observations in East Asia in spring 2018” by Phuc Thi Minh Ha et al.
General remarks and questions
This preprint reports aircraft measurements of black carbon (BC), CO, and CO2 measured in the lower troposphere eastward along the Asian continent over the sea and around Japan and the Philippines. Pollution plumes with elevated levels of CO and BC are investigated and the observed concentrations are compared with predictions from the WRF-CMAQ model. Observed to modeled concentration ratios derived from this are proposed as correction factors for emission inventories used in the model. Such an investigation of emission inventories is useful to achieve improved air quality predictions in the regions studied, and the aircraft measurements presented here provide a rare and good opportunity to extend analyses from ground based measurements.
Unfortunately, the presentation of the scientific approach and results in this paper is somewhat confusing and difficult to understand in places. The following aspects are not addressed clearly enough for general understanding and require a more detailed discussion. Major revisions are required before the paper is suitable for publication in ACP.
(1) To what extent can CO, CO2, and BC be considered as inert tracers that are essentially only subject to transport and deposition after emission on a 5d time scale, as considered in the backward trajectory calculations. To what extent could other chemical or physical processes influence their concentrations observed on the aircraft?
(2) Which source regions were exactly investigated using the approach with model calculations and flight measurements? Line 108 states: “Pollution plumes from major population centers in Asia were detected during parts of flights.” Which major population centers are specifically meant? Asia is a very large continent. Generalized statements such as “The results suggested that downward and upward revisions of Chinese emissions ... are required” (see abstract) is VERY general and should be formulated more cautiously and refer specifically to the regions or areas investigated. The authors should also consider making the title of the paper more specific. Also, to what extent could the findings be limited in time, e.g., only for the season or year investigated? How representative were the environmental conditions (fire activity, traffic, meteorology) prevailing during the flight campaign for the years before and after?
(3) The title of the paper states “Downward and upward revisions … are still required…”. Is this statement still valid approximately seven years after the aircraft campaign? Have there been any developments in East Asia since then with regard to biomass burning, industrial emissions, or traffic that would warrant a new investigation?
(4) There is only very limited information given on the EMERGE campaign and the aircraft measurements. A brief overview should therefore be provided in Section 2.1. The following information would be of interest. Why was springtime chosen for the campaign? What altitude range was covered during the measurement flights and what altitude range was specifically evaluated? Which measuring instruments were used (manufacturer, model) and what are their total measurement errors (precision, accuracy)? Which particle sizes were detected by the BC measuring device and how was the photometer signal converted into mass concentration? For which reference conditions (T, p) do the specified mass concentrations apply? Were other compounds (e.g., NOx, VOCs) measured and used in this work, e.g., for the identification of plumes, apart from BC, CO, and CO2? A PTR-MS instrument is mentioned in line 112. What was measured by this instrument and were the corresponding data used in any way?
(5) Section 2.2: which processes (apart from emission, transport, and deposition) play a role for the simulation of BC, CO, and CO2 on the 5d time scale of the backward trajectories investigated? Table 1 lists various types of emissions. Apart from direct emissions of BC, CO, and CO2, do other emitted substances, for example biogenic VOCs mentioned in the table, play a role? If so, which chemical processes were involved? Which processes represented in the AERO 6 aerosol module are relevant for the modeled results of BC in this study? What role do the volcanic emissions listed in Table 1 potentially play?
(6) For each model component listed in Table 1, references should be provided where a description or corresponding data can be found.
(7) In Section 2.4, the general description of the concept of "residual ratios" and "baseline values" is hard to understand and should be rephrased for clarity.
Minor Comments
Abbreviations (EMERGE, WRF-CMAQ, GFED, HTAPv2.2z, etc.) should be defined at the beginning of the paper when they are first used.
Line 42: Typo “nanometre-sized”
Lines 96-97: The sentence is unclear. Which other pollutants (apart from CO, CO2, BC) were investigated?
Line 105: Typo “Deutches”
What is the meaning of the given quantities (e.g., max = 1.3 mm) for APT3 in lines 340 and 575?
Table S3 appears to have no use in the paper and should be deleted.
Citation: https://doi.org/10.5194/egusphere-2024-2064-RC2 -
AC2: 'Reply on RC2', Phuc Ha, 21 Jul 2025
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-2064/egusphere-2024-2064-AC2-supplement.pdf
-
AC2: 'Reply on RC2', Phuc Ha, 21 Jul 2025
Peer review completion
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Phuc Thi Minh Ha
Yugo Kanaya
Kazuyo Yamaji
Syuichi Itahashi
Satoru Chatani
Takashi Sekiya
Maria Dolores Andrés Hernández
John Philip Burrows
Hans Schlager
Michael Lichtenstern
Mira Poehlker
Bruna Holanda
The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
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