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- ItemMultiphase MCM-CAPRAM modeling of the formation and processing of secondary aerosol constituents observed during the Mt. Tai summer campaign in 2014(Katlenburg-Lindau : EGU, 2020) Zhu, Yanhong; Tilgner, Andreas; Hoffmann, Erik Hans; Herrmann, Hartmut; Kawamura, Kimitaka; Yang, Lingxiao; Xue, Likun; Wang, WenxingDespite the high abundance of secondary aerosols in the atmosphere, their formation mechanisms remain poorly understood. In this study, the Master Chemical Mechanism (MCM) and the Chemical Aqueous-Phase Radical Mechanism (CAPRAM) are used to investigate the multiphase formation and processing of secondary aerosol constituents during the advection of air masses towards the measurement site of Mt. Tai in northern China. Trajectories with and without chemical–cloud interaction are modeled. Modeled radical and non-radical concentrations demonstrate that the summit of Mt. Tai, with an altitude of ∼1.5 km a.m.s.l., is characterized by a suburban oxidants budget. The modeled maximum gas-phase concentrations of the OH radical are 3.2×106 and 3.5×106 molec. cm−3 in simulations with and without cloud passages in the air parcel, respectively. In contrast with previous studies at Mt. Tai, this study has modeled chemical formation processes of secondary aerosol constituents under day vs. night and cloud vs. non-cloud cases along the trajectories towards Mt. Tai in detail. The model studies show that sulfate is mainly produced in simulations where the air parcel is influenced by cloud chemistry. Under the simulated conditions, the aqueous reaction of HSO−3 with H2O2 is the major contributor to sulfate formation, contributing 67 % and 60 % in the simulations with cloud and non-cloud passages, respectively. The modeled nitrate formation is higher at nighttime than during daytime. The major pathway is aqueous-phase N2O5 hydrolysis, with a contribution of 72 % when cloud passages are considered and 70 % when they are not. Secondary organic aerosol (SOA) compounds, e.g., glyoxylic, oxalic, pyruvic and malonic acid, are found to be mostly produced from the aqueous oxidations of hydrated glyoxal, hydrated glyoxylic acid, nitro-2-oxopropanoate and hydrated 3-oxopropanoic acid, respectively. Sensitivity studies reveal that gaseous volatile organic compound (VOC) emissions have a huge impact on the concentrations of modeled secondary aerosol compounds. Increasing the VOC emissions by a factor of 2 leads to linearly increased concentrations of the corresponding SOA compounds. Studies using the relative incremental reactivity (RIR) method have identified isoprene, 1,3-butadiene and toluene as the key precursors for glyoxylic and oxalic acid, but only isoprene is found to be a key precursor for pyruvic acid. Additionally, the model investigations demonstrate that an increased aerosol partitioning of glyoxal can play an important role in the aqueous-phase formation of glyoxylic and oxalic acid. Overall, the present study is the first that provides more detailed insights in the formation pathways of secondary aerosol constituents at Mt. Tai and clearly emphasizes the importance of aqueous-phase chemical processes on the production of multifunctional carboxylic acids.
- ItemInfluence of aerosol copper on HO2 uptake: A novel parameterized equation(Katlenburg-Lindau : EGU, 2020) Song, Huan; Chen, Xiaorui; Lu, Keding; Zou, Qi; Tan, Zhaofeng; Fuchs, Hendrik; Wiedensohler, Alfred; Moon, Daniel R.; Heard, Dwayne E.; Baeza-Romero, María-Teresa; Zheng, Mei; Wahner, Andreas; Kiendler-Scharr, Astrid; Zhang, YuanhangHeterogeneous uptake of hydroperoxyl radicals (HO2) onto aerosols has been proposed to be a significant sink of HOx , hence impacting the atmospheric oxidation capacity. Accurate calculation of the HO2 uptake coefficient HO2 is key to quantifying the potential impact of this atmospheric process. Laboratory studies show that HO2 can vary by orders of magnitude due to changes in aerosol properties, especially aerosol soluble copper (Cu) concentration and aerosol liquid water content (ALWC). In this study we present a state-of-the-art model called MARK to simulate both gas- and aerosol-phase chemistry for the uptake of HO2 onto Cu-doped aerosols. Moreover, a novel parameterization of HO2 uptake was developed that considers changes in relative humidity (RH) and condensed-phase Cu ion concentrations and which is based on a model optimization using previously published and new laboratory data included in this work. This new parameterization will be applicable to wet aerosols, and it will complement current IUPAC recommendations. The new parameterization is as follows (the explanations for symbols are in the Appendix): (Formula presented) All parameters used in the paper are summarized in Table A1. Using this new equation, field data from a field campaign were used to evaluate the impact of the HO2 uptake onto aerosols on the ROx (=OH+HO2 CRO2) budget. Highly variable values for HO2 uptake were obtained for the North China Plain (median value <0.1). © 2020 Copernicus GmbH. All rights reserved.
- ItemMutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility(Katlenburg-Lindau : EGU, 2020) Wang, Yu; Chen, Ying; Wu, Zhijun; Shang, Dongjie; Bian, Yuxuan; Du, Zhuofei; Schmitt, Sebastian H.; Su, Rong; Gkatzelis, Georgios I.; Schlag, Patrick; Hohaus, Thorsten; Voliotis, Aristeidis; Lu, Keding; Zeng, Limin; Zhao, Chunsheng; Alfarra, M. Rami; McFiggans, Gordon; Wiedensohler, Alfred; Kiendler-Scharr, Astrid; Zhang, Yuanhang; Hu, MinAs has been the case in North America and western Europe, the SO2 emissions have substantially reduced in the North China Plain (NCP) in recent years. Differential rates of reduction in SO2 and NOx concentrations result in the frequent occurrence of particulate matter pollution dominated by nitrate (pNO−3) over the NCP. In this study, we observed a polluted episode with the particulate nitrate mass fraction in nonrefractory PM1 (NR-PM1) being up to 44 % during wintertime in Beijing. Based on this typical pNO−3-dominated haze event, the linkage between aerosol water uptake and pNO−3 enhancement, further impacting on visibility degradation, has been investigated based on field observations and theoretical calculations. During haze development, as ambient relative humidity (RH) increased from ∼10 % to 70 %, the aerosol particle liquid water increased from ∼1 µg m−3 at the beginning to ∼75 µg m−3 in the fully developed haze period. The aerosol liquid water further increased the aerosol surface area and volume, enhancing the condensational loss of N2O5 over particles. From the beginning to the fully developed haze, the condensational loss of N2O5 increased by a factor of 20 when only considering aerosol surface area and volume of dry particles, while increasing by a factor of 25 when considering extra surface area and volume due to water uptake. Furthermore, aerosol liquid water favored the thermodynamic equilibrium of HNO3 in the particle phase under the supersaturated HNO3 and NH3 in the atmosphere. All the above results demonstrated that pNO−3 is enhanced by aerosol water uptake with elevated ambient RH during haze development, in turn facilitating the aerosol take-up of water due to the hygroscopicity of particulate nitrate salt. Such mutual promotion between aerosol particle liquid water and particulate nitrate enhancement can rapidly degrade air quality and halve visibility within 1 d. Reduction of nitrogen-containing gaseous precursors, e.g., by control of traffic emissions, is essential in mitigating severe haze events in the NCP.
- ItemNear-real-time monitoring of global CO2 emissions reveals the effects of the COVID-19 pandemic([London] : Nature Publishing Group UK, 2020) Liu, Zhu; Ciais, Philippe; Deng, Zhu; Lei, Ruixue; Davis, Steven J.; Feng, Sha; Zheng, Bo; Cui, Duo; Dou, Xinyu; Zhu, Biqing; Guo, Rui; Ke, Piyu; Sun, Taochun; Lu, Chenxi; He, Pan; Wang, Yuan; Yue, Xu; Wang, Yilong; Lei, Yadong; Zhou, Hao; Cai, Zhaonan; Wu, Yuhui; Guo, Runtao; Han, Tingxuan; Xue, Jinjun; Boucher, Olivier; Boucher, Eulalie; Chevallier, Frédéric; Tanaka, Katsumasa; Wei, Yiming; Zhong, Haiwang; Kang, Chongqing; Zhang, Ning; Chen, Bin; Xi, Fengming; Liu, Miaomiao; Bréon, François-Marie; Lu, Yonglong; Zhang, Qiang; Guan, Dabo; Gong, Peng; Kammen, Daniel M.; He, Kebin; Schellnhuber, Hans JoachimThe COVID-19 pandemic is impacting human activities, and in turn energy use and carbon dioxide (CO2) emissions. Here we present daily estimates of country-level CO2 emissions for different sectors based on near-real-time activity data. The key result is an abrupt 8.8% decrease in global CO2 emissions (−1551 Mt CO2) in the first half of 2020 compared to the same period in 2019. The magnitude of this decrease is larger than during previous economic downturns or World War II. The timing of emissions decreases corresponds to lockdown measures in each country. By July 1st, the pandemic’s effects on global emissions diminished as lockdown restrictions relaxed and some economic activities restarted, especially in China and several European countries, but substantial differences persist between countries, with continuing emission declines in the U.S. where coronavirus cases are still increasing substantially.
- ItemTaking stock of national climate policies to evaluate implementation of the Paris Agreement([London] : Nature Publishing Group UK, 2020) Roelfsema, Mark; van Soest, Heleen L.; Harmsen, Mathijs; van Vuuren, Detlef P.; Bertram, Christoph; den Elzen, Michel; Höhne, Niklas; Iacobuta, Gabriela; Krey, Volker; Kriegler, Elmar; Luderer, Gunnar; Riahi, Keywan; Ueckerdt, Falko; Després, Jacques; Drouet, Laurent; Emmerling, Johannes; Frank, Stefan; Fricko, Oliver; Gidden, Matthew; Humpenöder, Florian; Huppmann, Daniel; Fujimori, Shinichiro; Fragkiadakis, Kostas; Gi, Keii; Keramidas, Kimon; Köberle, Alexandre C.; Aleluia Reis, Lara; Rochedo, Pedro; Schaeffer, Roberto; Oshiro, Ken; Vrontisi, Zoi; Chen, Wenying; Iyer, Gokul C.; Edmonds, Jae; Kannavou, Maria; Jiang, Kejun; Mathur, Ritu; Safonov, George; Vishwanathan, Saritha SudharmmaMany countries have implemented national climate policies to accomplish pledged Nationally Determined Contributions and to contribute to the temperature objectives of the Paris Agreement on climate change. In 2023, the global stocktake will assess the combined effort of countries. Here, based on a public policy database and a multi-model scenario analysis, we show that implementation of current policies leaves a median emission gap of 22.4 to 28.2 GtCO2eq by 2030 with the optimal pathways to implement the well below 2 °C and 1.5 °C Paris goals. If Nationally Determined Contributions would be fully implemented, this gap would be reduced by a third. Interestingly, the countries evaluated were found to not achieve their pledged contributions with implemented policies (implementation gap), or to have an ambition gap with optimal pathways towards well below 2 °C. This shows that all countries would need to accelerate the implementation of policies for renewable technologies, while efficiency improvements are especially important in emerging countries and fossil-fuel-dependent countries.
- ItemQuantifying Water Scarcity in Northern China Within the Context of Climatic and Societal Changes and South-to-North Water Diversion(Hoboken, NJ : Wiley-Blackwell, 2020) Yin, Yuanyuan; Wang, Lei; Wang, Zhongjing; Tang, Qiuhong; Piao, Shilong; Chen, Deliang; Xia, Jun; Conradt, Tobias; Liu, Junguo; Wada, Yoshihide; Cai, Ximing; Xie, Zhenghui; Duan, Qingyun; Li, Xiuping; Zhou, Jing; Zhang, JianyunWith the increasing pressure from population growth and economic development, northern China (NC) faces a grand challenge of water scarcity, which can be further exacerbated by climatic and societal changes. The South-to-North Water Diversion (SNWD) project is designed to mitigate the water scarcity in NC. However, few studies have quantified the impact of the SNWD on water scarcity within the context of climatic and societal changes and its potential effects on economic and agricultural food in the region. We used water supply stress index (WaSSI) to quantify water scarcity within the context of environmental change in NC and developed a method to estimate the economic and agricultural impacts of the SNWD. Focuses were put on alleviating the water supply shortage and economic and agricultural benefits for the water-receiving NC. We find that societal changes, especially economic growth, are the major contributors to water scarcity in NC during 2009–2099. To completely mitigate the water scarcity of NC, at least an additional water supply of 13 billion m3/year (comparable to the annual diversion water by SNWD Central Route) will be necessary. Although SNWD alone cannot provide the full solution to NC's water shortage in next few decades, it can significantly alleviate the water supply stress in NC (particularly Beijing), considerably increasing the agricultural production (more than 115 Tcal/year) and bringing economic benefits (more than 51 billion RMB/year) through supplying industrial and domestic water use. Additionally, the transfer project could have impacts on the ecological environment in the exporting regions. ©2020. The Authors.
- ItemEarly transformation of the Chinese power sector to avoid additional coal lock-in(Bristol : IOP Publ., 2020) Wang, Huan; Chen, Wenying; Bertram, Christoph; Malik, Aman; Kriegler, Elmar; Luderer, Gunnar; Després, Jacques; Jiang, Kejun; Krey, VolkerEmission reduction from the coal-dominated power sector is vital for achieving China's carbon mitigation targets. Although the coal expansion has been slowed down due to the cancellation of and delay in new construction, coal-based power was responsible for over one third of China's energy-related CO2 emissions by 2018. Moreover, with a technical lifetime of over 30 years, current investment in coal-based power could hinder CO2 mitigation until 2050. Therefore, it is important to examine whether the current coal-based power planning aligns with the long-term climate targets. This paper introduces China's Nationally Determined Contribution (NDC) goals and an ambitious carbon budget along with global pathways well-below 2 degrees that are divided into five integrated assessment models, which are two national and three global models. We compare the models' results with bottom-up data on current capacity additions and expansion plans to examine if the NDC targets are in line with 2-degree pathways. The key findings are: 1. NDC goals alone are unlikely to lead to significant reductions in coal-based power generation. On the contrary, more plants may be built before 2030; 2. this would require an average of 187–261 TWh of annual coal-based power capacity reduction between 2030 and 2050 to achieve a 2 °C compatible trajectory, which would lead to the stranding of large-scale coal-based power plants; 3. if the reduction in coal power can be brought forward to 2020, the average annual coal-based power reduction required would be 104–155 TWh from 2020 to 2050 and the emissions could peak earlier; 4. early regulations in coal-based power would require accelerated promotion of alternatives between 2020 and 2030, with nuclear, wind and solar power expected to be the most promising alternatives. By presenting the stranding risk and viability of alternatives, we suggest that both the government and enterprises should remain cautious about making new investment in coal-based power sector.
- ItemThe evolution of cloud and aerosol microphysics at the summit of Mt. Tai, China(Katlenburg-Lindau : EGU, 2020) Li, Jiarong; Zhu, Chao; Chen, Hui; Zhao, Defeng; Xue, Likun; Wang, Xinfeng; Li, Hongyong; Liu, Pengfei; Liu, Junfeng; Zhang, Chenglong; Mu, Yujing; Zhang, Wenjin; Zhang, Luming; Herrmann, Hartmut; Li, Kai; Liu, Min; Chen, JianminThe influence of aerosols, both natural and anthropogenic, remains a major area of uncertainty when predicting the properties and the behaviours of clouds and their influence on climate. In an attempt to better understand the microphysical properties of cloud droplets, the simultaneous variations in aerosol microphysics and their potential interactions during cloud life cycles in the North China Plain, an intensive observation took place from 17 June to 30 July 2018 at the summit of Mt. Tai. Cloud microphysical parameters were monitored simultaneously with number concentrations of cloud condensation nuclei (NCCN) at different supersaturations, PM2:5 mass concentrations, particle size distributions and meteorological parameters. Number concentrations of cloud droplets (NC), liquid water content (LWC) and effective radius of cloud droplets (reff) show large variations among 40 cloud events observed during the campaign. The low values of reff and LWC observed at Mt. Tai are comparable with urban fog. Clouds on clean days are more susceptible to the change in concentrations of particle number (NP), while clouds formed on polluted days might be more sensitive to meteorological parameters, such as updraft velocity and cloud base height. Through studying the size distributions of aerosol particles and cloud droplets, we find that particles larger than 150 nm play important roles in forming cloud droplets with the size of 5-10 μm. In general, LWC consistently varies with reff. As NC increases, reff changes from a trimodal distribution to a unimodal distribution and shifts to smaller size mode. By assuming a constant cloud thickness and ignoring any lifetime effects, increase in NC and decrease in reff would increase cloud albedo, which may induce a cooling effect on the local climate system. Our results contribute valuable information to enhance the understanding of cloud and aerosol properties, along with their potential interactions on the North China plain. © Author(s) 2020.
- ItemChemical characteristics of cloud water and the impacts on aerosol properties at a subtropical mountain site in Hong Kong SAR(Katlenburg-Lindau : EGU, 2020) Li, Tao; Wang, Zhe; Wang, Yaru; Wu, Chen; Liang, Yiheng; Xia, Men; Yu, Chuan; Yun, Hui; Wang, Weihao; Wang, Yan; Guo, Jia; Herrmann, Hartmut; Wang, TaoTo investigate the cloud water chemistry and the effects of cloud processing on aerosol properties, comprehensive field observations of cloud water, aerosols, and gasphase species were conducted at a mountaintop site in Hong Kong SAR in October and November 2016. The chemical composition of cloud water including water-soluble ions, dissolved organic matter (DOM), carbonyl compounds (refer to aldehydes and acetone), carboxylic acids, and trace metals was quantified. The measured cloud water was very acidic with a mean pH of 3.63, as the ammonium (174 μeq L-1) was insufficient for neutralizing the dominant sulfate (231 μeq L-1) and nitrate (160 μeq L-1). Substantial DOM (9.3 mgC L-1) was found in cloud water, with carbonyl compounds and carboxylic acids accounting for 18% and 6% in carbon molar concentrations, respectively. Different from previous observations, concentrations of methylglyoxal (19.1 μM; μM is equal to μmol L-1) and glyoxal (6.72 μM) were higher than that of formaldehyde (1.59 μM). The partitioning of carbonyls between cloud water and the gas phase was also investigated. The measured aqueous fractions of dicarbonyls were comparable to the theoretical estimations, while significant aqueous-phase supersaturation was found for less soluble monocarbonyls. Both organics and sulfate were significantly produced in cloud water, and the aqueous formation of organics was more enhanced by photochemistry and under less acidic conditions. Moreover, elevated sulfate and organics were measured in the cloudprocessed aerosols, and they were expected to contribute largely to the increase in droplet-mode aerosol mass fraction. This study demonstrates the significant role of clouds in altering the chemical compositions and physical properties of aerosols via scavenging and aqueous chemical processing, providing valuable information about gas-cloud-aerosol interactions in subtropical and coastal regions. © 2020 Author(s). This work is distributed under the Creative Commons Attribution 4.0 License.