Airborne formaldehyde and volatile organic compound measurements over the Daesan petrochemical complex on Korea's northwest coast during the Korea-United States Air Quality study

Creators: Fried, Alan; Walega, James; Weibring, Petter; Richter, Dirk; Simpson, Isobel J.; Blake, Donald R.; Blake, Nicola J.; Meinardi, Simone; Barletta, Barbara; Hughes, Stacey C.; Crawford, James H.; Diskin, G.; Barrick, John; Hair, Johnathan; Fenn, Marta; Wisthaler, Armin; Mikoviny, Tomas; Woo, Jung-Hun; Park, Minwoo; Kim, Jinseok; Min, Kyung-Eun; Jeong, Seokhan; Wennberg, Paul O.; Kim, Michelle J.; Crounse, John D.; Teng, Alex P.; Bennett, Ryan; Yang-Martin, Melissa; Shook, Michael A.; Huey, Greg; Tanner, David; Knote, Christoph; Kim, JongHo; Park, Rokjin; Brune, William

Abstract

The U.S. National Aeronautics and Space Administration in partnership with Korea's National Institute of Environmental Research embarked on the Korea-United States Air Quality (KORUS-AQ) study to address air quality issues over the Korean peninsula. Underestimation of volatile organic compound (VOC) emissions from various large facilities on South Korea's northwest coast may contribute to this problem, and this study focuses on quantifying top-down emissions of formaldehyde (CH₂O) and VOCs from the largest of these facilities, the Daesan petrochemical complex, and comparisons with the latest emission inventories. To accomplish this and additional goals discussed herein, this study employed a number of measurements acquired during KORUS-AQ onboard the NASA DC-8 aircraft during three Daesan overflights on June 2, 3, and 5, 2016, in conjunction with a mass balance approach. The measurements included fast airborne measurements of CH₂O and ethane from an infrared spectrometer, additional fast measurements from other instruments, and a suite of 33 VOC measurements acquired by the whole air sampler. The mass balance approach resulted in consistent top-down yearly Daesan VOC emission flux estimates, which averaged (61 ± 14) × 10³ MT/year for the 33 VOC compounds, a factor of 2.9 ± 0.6 (±1.0) higher than the bottom-up inventory value. The top-down Daesan emission estimate for CH₂O and its four primary precursors averaged a factor of 4.3 ± 1.5 (± 1.9) times higher than the bottom-up inventory value. The uncertainty values in parentheses reflect upper limits for total uncertainty estimates. The resulting averaged top-down Daesan emission estimate for sulfur dioxide (SO₂) yielded a ratio of 0.81–1.0 times the bottom-up SO₂ inventory, and this provides an important cross-check on the accuracy of our mass balance analysis.

Additional Information

© 2020 The Author(s). This is an open-access article distributed under the terms of the Creative Commons Attribution 4.0 International License (CC-BY 4.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. See http://creativecommons.org/licenses/by/4.0/. Received: August 14 2020; Accepted: November 10 2020. We acknowledge Andy Weinheimer and Denise Montzka of NCAR for their oxides of nitrogen measurements and the entire NASA DC-8 ground crew, aircraft crew, and pilots, which enabled the acquisition of in the situ aircraft data. The instrument team of P. Eichler, L. Kaser, and M. Müller as well as Ionicon Analytik is acknowledged for their support of this instrument in the field and during the mission preparation phase. Funding to the University of Colorado for AF and his group was supported by Grant Number NNX15AV02G from the NASA Tropospheric Chemistry Program. The KORUS-AQ mission was jointly funded by the NASA Tropospheric Chemistry Program and the Korean National Institute of Environmental Research (NIER). The PTR-ToF-MS measurements were supported by the Austrian Federal Ministry for Transport, Innovation and Technology (BMVIT) through the Austrian Space Applications Programme (ASAP) of the Austrian Research Promotion Agency (FFG). Competing interests: The authors declare no competing interests. However, two of the authors, Isobel Simpson and Armin Wisthaler are Associate Editors of Elementa. Author contributions: Acquired and interpreted all the CAMS CH₂O and C₂H₆ data on the NASA DC-8 and wrote the manuscript: AF. Responsible for preparing the instrument for airborne measurements and helping in the data quality control, final data submission, and manuscript editing: JW, PW, DR. Provided significant critical input on the data analysis and interpretation: IJS (of the WAS team) and JHC (at NASA Langley). Responsible for the high quality WAS VOC measurement acquisition, follow-up laboratory analysis, data management, and final data quality control and submittal: The entire WAS team at Irvine, led by DRB, of IJS, NJB, SM, BB, and SCH. Provided DC-8 aircraft data and critical input on DC-8 measurements of wind speed and direction: JB at NASA Langley and RB, MY-M, and MAS at NSRC Bay Area Environmental Research Institute. Acquired HSRL data and provided critical input in the analysis of the mixed layer heights: JH and MF from the NASA Langley LIDAR group. Provided PTR-ToF-MS measurements of benzene and toluene: AW and TM at the Universities of Oslo and Innsbruck. Provided measurements of CO and CH4: G. Diskin and his group at NASA Langley. Oversaw the KORUSv5 emission inventory and provided data for this article: JHW, MP, JK. Provided support in the analysis: JK at the Konkuk University and K-EM and SJ at the Gwangju Institute of Science and Technology. Provided measurements and analysis of alkene-hydroxynitrates employed in determining photochemically produced CH₂O: POW, MJK, JDC, and APT of the California Institute of Technology. Provided the FLEXPART back trajectories: CK of the Meteorological Institute in Germany. Provided critical measurements of SO₂: GH and DT at the GIT. Provided measurements of OH: WB at PSU. Provided critical supporting measurements: JHK at Hanseo University and RP at Seoul National University. Revised the manuscript and approved the submitted version for publication: All coauthors. Data accessibility statement: All observational data from the KORUS-AQ mission, including the CAMS and WAS VOC data, are archived at http://doi.org/10.5067/Suborbital/KORUSAQ/DATA01.

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