the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
| 02 Feb 2024
Emission Inventory Development for Spatiotemporal Release of Vanadium from Anthropogenic Sources in China
Abstract. Anthropogenic activities contribute primarily to the toxic vanadium presence in the surface environment, but quantitative assessment of its emissions from anthropogenic sources to various environmental receptors is still lacking. This study has developed nationwide vanadium emission inventory in China during 2015–2019, covering five major anthropogenic sources, including coal combustion, stationary oil burning, transportation, industrial production, and waste handling. Cumulative emission flux modelling has shown that 211094 t, 3725 t, and 0.1 t of vanadium were discharged into atmosphere, soil and water during this period. Coal combustion and stationary source of oil burning are the largest vanadium contributors, accounting for 47.5 % and 39.6 % of emission inventory. Shandong, Liaoning, Hebei, Guangdong and Hunan are among the largest provincial emitters. Emissions pertinent to raw coal combustion mainly increase by 719 t and 316 t in the provinces of North China and Northwestern China, respectively. Vanadium output pertinent to steelmaking constitutes 88.2 % emission in industrial production, and continued to increase in all regions. Emissions induced by vanadium mining shows remarkable spatial heterogeneity, with 66.1 % output determined in Southwestern China. Emissions pertinent to raw coal and coke combustion was the main source of uncertainty for the inventory development, resulting in output uncertainty ranging from -47.5 % to 63.7 % and -49.4 % to 53.7 %.
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RC1: 'Comment on egusphere-2024-10', Anonymous Referee #1, 01 Apr 2024
This manuscript investigated the anthropogenic vanadium emission inventory in China during 2015-2019 to various environmental receptors including atmosphere, soil and water. Considering its integrated contents and the scope of Atmospheric Chemistry and Physics, it might be more suitable for an environmental journal rather than ACP.
Some comments are suggested for considering:
The writing like statements should be clarified overall. For instance, Abstract Line 12-13: Is the flux value for the period of five years or a year?
To avoid the limitation of a local investigation, the scientific implications should be strengthened. Such as Abstract Line 14-15, what’s the international or scientific implications for these provinces with largest emissions?
If submitted to ACP, this paper should focus on emissions to atmosphere in detail with depth.
Is year 2015-2019 representative for interannual variation of temporal analysis? Why not longer periods? Is seasonal change more meaningful in this study?
Were their spatial and temporal differences in emission sources? How to consider them in the national emission inventory calculation?
Citation: https://doi.org/10.5194/egusphere-2024-10-RC1 -
AC1: 'Reply on RC1', Baogang Zhang, 08 Apr 2024
A DETAILED LIST OF RESPONSES TO REVIEWERS’ COMMENTS
egusphere-2024-10
Title: "Emission Inventory Development for Spatiotemporal Release of Vanadium from Anthropogenic Sources in China"
Dear Editor,
We hereby re-submit the revised manuscript " Emission Inventory Development for Spatiotemporal Release of Vanadium from Anthropogenic Sources in China " (ID: egusphere-2024-10) for further consideration by ACP.
We are very grateful to the Referee’s comment in the interactive discussion. We have addressed all these comments and revised the manuscript accordingly. The comments from the editor or reviewers are in black, and responses from the authors are in blue. The text revisions of the manuscript are marked in red.
All authors have reviewed the manuscript and approved the submission of the manuscript. Neither the entire manuscript nor any part of its content has been published, accepted or submitted to any other journals. Thank you very much for your attention and consideration.
We are looking forward to receiving your further advice.
Sincerely yours,
Baogang Zhang
Responses to the comments of Referee #1Comment: This manuscript investigated the anthropogenic vanadium emission inventory in China during 2015-2019 to various environmental receptors including atmosphere, soil and water. Considering its integrated contents and the scope of Atmospheric Chemistry and Physics, it might be more suitable for an environmental journal rather than ACP.
Reply: We would like to express our sincere gratitude to the referee for raising this question. The atmosphere pollution is indeed the major focus of our inventory development for vanadium emission. As shown in the result, vanadium emission contributed predominantly to atmospheric pollution (97.3%). However, the emission inventories need to capture the full aspects of each emission source, including direct discharge to other environmental receptors. In addition, vanadium flux released into atmosphere may interact with other environmental media. Therefore, focusing only atmospheric emission may overlook the significance of interconnectedness of different environmental media. With in depth understanding of vanadium emission across different medias, and the patterns of each emission source, more effective and targeted measures will be proposed by policy makers. Lastly, we noticed there are articles (doi.org/10.5194/acp-16-4451-2016; doi.org/10.5194/acp-20-16117-2020) published in ACP, which covered the emission flux directed to environmental media other than atmosphere. Therefore, we believe that our work is relevant to the scope of ACP journal.
Some comments are suggested for considering:
The writing like statements should be clarified overall. For instance, Abstract Line 12-13: Is the flux value for the period of five years or a year?
Reply: Thank you for pointing this out, we have clarified it. The flux values were resulted from five years period (2015-2019).
Line 12-13: Cumulative emission flux modelling has shown that 211094 t, 3725 t, and 0.1 t of vanadium were discharged into atmosphere, soil and water during 2015-2019, respectively.
To avoid the limitation of a local investigation, the scientific implications should be strengthened. Such as Abstract Line 14-15, what’s the international or scientific implications for these provinces with largest emissions?
Reply: All those provinces with largest emissions were densely populated and highly industrialized in China. In addition, the combined emission of vanadium in those provinces also contributed greatly to both national and global vanadium emission inventories. We have incorporated the following statement to strengthen the scientific implication of local results.
Line 14-18: The spatial and temporal of vanadium emission is strongly governed by industrial activity levels across regions. Shandong, Liaoning, Hebei, Guangdong and Hunan, with dense population and great level of industrial activities, are among the largest provincial emitters, contributing 35.8% of national vanadium inventories. Provinces in North China and Northwestern China increase their emission contribution pertinent to raw coal combustion by 719 t and 316 t, respectively, due to their high energy demand.
Line 135-142: In comparison, according to the most up to date research on global vanadium emission (Schlesinger et al., 2017), vanadium released from both stationary and mobile source of oil combustion jointly constituted over 60% of vanadium emission inventory, while coal burning constituted only 26% of total output. To explain the discrepancy, the development of global inventory employed mainly the available data of industrial activities in the United States. Unlike the United States, coal combustion played pivotal roles in China’s energy sector, and vanadium output pertinent to oil extraction was much less. Moreover, vanadium releasing fraction, emission reducing technology, and vanadium content in raw materials varied significantly across regions. To improve the inventory, it is essential to perform local level investigation in different regions.
Line 198-202: In general, a substantial amount of vanadium emission was found in northern, eastern coastal, southern and south western provinces. Shandong, Liaoning, Hebei, Guangdong, and Hunan, the most industrially developed provinces in China, were among the largest provincial emitters with cumulative vanadium discharge over 10000 t (Fig. S3a), accounting for over 35.8% of total national emission in combined.
Line 249-253: The development of vanadium emission inventory at provincial level will serve as key basis to policy making, which would warrant more targeted efforts on major provincial emitters for different emission source. The detailed results on vanadium emission will also provide benchmark for comparing the effectiveness of administrative and technological measures for pollution control. In addition, local results will contribute greatly to the development of global emission inventory, which requires in depth understanding of sources and magnitudes of emission.
If submitted to ACP, this paper should focus on emissions to atmosphere in detail with depth.
Reply: We very much appreciate your comment. The inventory indeed was developed with aim to illustrate the vanadium emission to multiple environment medias, with primary focus on atmospheric emission. Firstly, the inventory provided a quantitative assessment of vanadium emission, including coal combustion, stationary oil burning, transportation, industrial production (steelmaking and glass production), and waste handling (MSW incineration), consisted predominantly vanadium flux to atmosphere (97.3%), as indicated by Figure 1.
Line 114-115: During 2015-2019, 98.3% vanadium generated from anthropogenic processes was directly discharged into the atmosphere, leading to a total emitted vanadium content of 211094 t.
The paper also delineated the temporal evolvement of vanadium emission from major emission sources, highlighting that the major emission contributors are coal combustion and oil burning in combined, both of which were entirely responsibly for atmospheric discharge. In addition, we have drawn parallel with atmospheric vanadium emission on global scale, providing more insight by comparing the difference in contribution fraction by emission sources.
Line 136-143: Investigation on global vanadium emission also accounted the fossil fuel burning as the primary source of atmospheric vanadium discharge (Schlesinger et al., 2017), with stationary and mobile source of oil combustion jointly constituting over 60% of vanadium emission flux, while coal burning made up of only 26% of total output. To explain the discrepancy, the development of global inventory employed mainly the available data of industrial activities in the United States. However, coal combustion played pivotal roles in China’s energy sector, and vanadium output pertinent to oil extraction was much less. The contrast could also be attributed to variation in vanadium releasing fraction, emission reducing technology, and vanadium content in raw materials in different regions. To improve the inventory, it is essential to perform local level investigation in different regions.
For each emission source contributing to atmosphere, and other medias, we have also presented their relative contributions to the emission inventory.
Line 145-149: The relative contribution of coal combustion to the emission inventory slightly decreased by 2.0%.
Line 150: corresponding to a decrease in relative contribution by 8.5%.
Line 155: which led to an increase in relative contribution by 9.7%, 6.4% and 28%, respectively.
Line 165: along with apparent increase in relative contribution to the inventory by 30.6%, -2.0%, and 37.9%.
Furthermore, we have enhanced our discussion on the implications of atmospheric emission results, in conjunction with the impact of the "Clean Air Act". We have explored the roles this policy has played in vanadium emissions and the limitations of the current study, offering insights into future improvements in data acquisition.
Line 146-148: The emission trend of coal combustion was similar to observation in contemporary study, where atmospheric vanadium emission significantly decreased compared to pre-2013 periods as result of introduction of “Clean Air Act”, followed by a relatively constant trend (Bai et al., 2021).
Line 168-176: However, the trend of sulfur content remained flattened in transportation derived emission (Zheng et al., 2018), which implied an increased utilization of vanadium-based catalyzer for exhaust gas treatment (National Bureau of Statistics of China, 2020). Despite the overall increase in industrial activity levels, according to a comprehensive study on anthropogenic emissions trend after the introduction of “Clean Air Act”, energy and industrial manufacturing sectors underwent drastic reduction in pollutant emission (e.g., SO2, NOx) (Zheng et al., 2018), while emission derived from transportation (e.g., NOx, CO, NMVOC) was maintained relatively steady. The result suggested that potential impact of improvement in technological and administrative measures on pollutant emission may counterbalance or even exceed the impact induced by increased activity levels, especially for combustion of coal and petroleum products affiliated with energy and industrial sectors. In comparison, change in activity level more likely affected the trend of transportation derived emission.
Line 292-295: Consequently, the industrial activity level appears to be the primary influencing factor of vanadium emission levels, overshadowing the potential impact of variations in other parameters, such as removal efficiency of pollution control technologies and vanadium content in raw materials, which also varied across regions and processes. To further refine the inventory, acquiring region-specific data and conducting onsite investigations will be essential in our future efforts.
Is year 2015-2019 representative for interannual variation of temporal analysis? Why not longer periods?
Reply: The year of 2015-2019 period is representative considering the following reasons: (1) This time period provided representation in emission trend as result of “Clean Air Act” introduced since the end of 2013. Under the new act, major sectors pertinent to vanadium emission undertook effort to reduce emissions, including power plant, steelmaking, petrochemical, steel and glass production (doi.org/10.5194/acp-18-14095-2018). (2) 2020-2022 marked a period of trough in all industrial activities due to the pandemic, therefore we treated these years as emission anomaly, which is not representative. We have included the following sentences to give more background regarding the study period.
Line 50-52: Moreover, China have adopted “Clean Air Act” since 2014, with aim to reduce the atmospheric emission in wide ranges of industrial activities (Zheng et al., 2018). However, the impact of implementing this act on vanadium emission trend was still underexplored.
Line 62-63: The goal of this study is to establish the bottom-up inventories of vanadium emission from anthropogenic activities, targeting specifically the period from 2015 to 2019 in China post to the introduction of “Clean Air Act”.
Line 395: Zheng, B., Tong, D., Li, M., Liu, F., Hong, C., Geng, G., Li, H., Li, X., Peng, L., Qi, J., Yan, L., Zhang, Y., Zhao, H., Zheng, Y., He, B., Zhang, Q.: Trends in China’s anthropogenic emissions since 2010 as the consequence of clean air actions, Atmos. Chem. Phys., 18, 14095-14111, https://doi.org/10.5194/acp-18-14095-2018, 2018.
Is seasonal change more meaningful in this study?
Reply: Unfortunately, the seasonal variation data is very limited as we performed our study specifically based on yearbook of industrial activities. However, for future effort, we can explore the seasonal spatiotemporal variation in selected regions where seasonal data is available.
Line 295-299: In this study, the spatiotemporal variation pattern of vanadium emission was characterized based on yearly recorded datasets. However, there is still room to improve the accuracy of emission inventory. Seasonal investigation may help in identifying the source specific variation due to altering energy demand (e.g., thermal power plant) or weather influence (e.g., precipitation, strong wind) following seasonal patterns.
Were their spatial and temporal differences in emission sources? How to consider them in the national emission inventory calculation?
Reply: Yes, industrial activity levels pertinent to different emission sources varied in spatial and temporal manner. In the formula of calculating the emission inventories, emission related parameters such as treatment efficiency, vanadium release fraction, and dynamic emission factors, were all obtained from previous literature, and applied into the equation in average values. Therefore, even though our results suggested that the variation in industrial activity level strongly affected the change in vanadium emission, their actual impact may be offset by difference in technological impact (e.g., one region employed better pollution abatement technology) or using cleaner fuel. We have incorporated the following sentence for explanation.
Line 173-176: The result suggested that potential impact of improvement in technological and administrative measures on pollutant emission may counterbalance or even exceed the impact induced by increased activity levels, especially for combustion of coal and petroleum products affiliated with energy and industrial sectors. In comparison, change in activity level more likely affected the trend of transportation derived emission.
Line 298-303: Furthermore, we have utilized average values of reported emission related parameters. Consequently, the industrial activity level appears to be the primary influencing factor of vanadium emission levels, overshadowing the potential impact of variations in other parameters, such as removal efficiency of pollution control technologies and vanadium content in raw materials, which also varied across regions and processes. To further refine the inventory, acquiring region-specific data and conducting onsite investigations will be essential in our future efforts.
Citation: https://doi.org/10.5194/egusphere-2024-10-AC1
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AC1: 'Reply on RC1', Baogang Zhang, 08 Apr 2024
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RC2: 'Comment on egusphere-2024-10', Anonymous Referee #2, 16 Nov 2024
The manuscript presents and discusses, to some extent, the calculated anthropogenic Vanadium emission inventory at China for the period 2015-2019. The emissions are reported in terms of compartments, atmosphere, water and soil over the years and for the 31 Chinese provinces/7 regions. The content is of great relevance considering China as one of the main, perhaps the largest economy in the planet with strong and active industry and energy production sectors. However, in my opinion, the paper lacks in discussing their findings. For example, the authors did not put the findings into a world perspective, did not compare with other studies, etc., which could enhance the importance of such results. Also, the methodology is poorly described. In my opinion, the paper requires substantial improvement in order to be accepted.
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Emission Inventory Development for Spatiotemporal Release of Vanadium from Anthropogenic Sources in China Han Zhang https://doi.org/10.5281/zenodo.10395785
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