Beaudry Ellie, Jacob Daniel J, Bates Kelvin H, Zhai Shixian, Yang Laura H, Pendergrass Drew C, Colombi Nadia, Simpson Isobel J, Wisthaler Armin, Hopkins James R, Li Ke, Liao Hong
Harvard University, John A. Paulson School of Engineering and Applied Sciences, Cambridge, Massachusetts 02138, United States.
Harvard University, Department of Earth and Planetary Sciences, Cambridge, Massachusetts 01238, United States.
ACS EST Air. 2025 Mar 27;2(4):456-465. doi: 10.1021/acsestair.4c00210. eCollection 2025 Apr 11.
Observations during the KORUS-AQ, MAPS-Seoul, and APHH-Beijing field campaigns of 2015-2017 reveal high concentrations of ethanol and methanol in urban air over South Korea and China, with median concentrations of 2-4 ppb for ethanol and 12-18 ppb for methanol. Simulations with the GEOS-Chem model show that these values cannot be captured by current emission inventories. They could originate from volatile chemical products (VCPs). Fitting observed ethanol concentrations with GEOS-Chem would imply per capita VCP emissions 2.4 times higher in South Korea and 1.5 times higher in China than in the U.S. The strong ethanol-methanol correlation suggests a major methanol component in VCP emissions, unlike in the U.S. where methanol use is largely banned. Including these emissions in GEOS-Chem increases the level of surface ozone over South Korea and China by 1-3 ppb. KORUS-AQ aircraft profiles also indicate a high free tropospheric methanol background of 3.2 ppb, which appears to be of terrestrial biospheric origin but cannot be reproduced by GEOS-Chem.
2015 - 2017年“美韩空气质量研究(KORUS - AQ)”“首尔多尺度空气质量观测与模拟研究(MAPS - Seoul)”以及“北京大气污染及气候效应综合观测研究(APHH - Beijing)”实地考察期间的观测结果显示,韩国和中国城市空气中乙醇和甲醇浓度很高,乙醇中位数浓度为2 - 4 ppb,甲醇为12 - 18 ppb。运用GEOS - Chem模型进行的模拟表明,当前的排放清单无法体现这些数值。它们可能源自挥发性化学产品(VCP)。用GEOS - Chem模型拟合观测到的乙醇浓度意味着,韩国人均VCP排放量比美国高2.4倍,中国比美国高1.5倍。乙醇与甲醇之间的强相关性表明,VCP排放中甲醇占主要成分,这与美国不同,美国在很大程度上已禁止使用甲醇。在GEOS - Chem模型中纳入这些排放会使韩国和中国的地表臭氧水平升高1 - 3 ppb。“美韩空气质量研究”的飞机探测数据还表明,对流层自由大气中甲醇背景浓度较高,为3.2 ppb,这似乎源自陆地生物圈,但GEOS - Chem模型无法再现这一情况。