Article
Chemistry, Multidisciplinary
Bradley C. C. Dallin, Atharva S. S. Kelkar, Reid C. C. Van Lehn
Summary: The hydrophobicity of chemically heterogeneous interfaces is complex and difficult to predict due to non-additive contributions from polar and nonpolar groups. This study uses molecular dynamics simulations and data-centric analysis to quantitatively relate changes in interfacial water structure to the hydration free energy. By analyzing a large data set of chemically heterogeneous self-assembled monolayers, the study identifies five features of interfacial water structure that accurately predict hydration free energies and reveals mechanistic insights into hydrogen bonding behaviors and highly coordinated water structures that are unique signatures of hydrophobicity.
Article
Chemistry, Multidisciplinary
Xinghui Wu, Jiawei Di, Zhen Yang, Yuanyuan Duan
Summary: This study investigates the dynamic spreading process of mixed droplets on chemically heterogeneous surfaces through molecular dynamic simulations. The research finds that the actual component mole fraction in the triple contact region is consistent with the nominal one for R32/R1234yf mixture droplets, but differs for ethanol/water mixture droplets. By using local properties to modify the molecular kinetic theory, the prediction of dynamic spreading of water/ethanol mixture droplets on chemically heterogeneous surfaces can be significantly improved.
Article
Engineering, Environmental
Liubin Huang, Elianna S. Frank, Mona Shrestha, Saleh Riahi, Douglas J. Tobias, Vicki H. Grassian
Summary: Oxygenated organic compounds (OOCs) are widely present in indoor environments and their adsorption on indoor surfaces, driven by pi hydrogen bonding and O-H hydrogen bonding interactions, plays a significant role in the removal of OOCs. Indoor surfaces can also act as a reservoir of OOCs due to their slower desorption kinetics compared to other indoor relevant organic compounds.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Physical
Atharva S. Kelkar, Bradley C. Dallin, Reid C. Van Lehn
Summary: Hydrophobic interactions play a crucial role in various biological and synthetic processes. This study demonstrates that the hydrophobicity of surfaces with chemically heterogeneous compositions can vary substantially depending on the spatial patterns and chemical identities of polar and nonpolar groups. The clustering of nonpolar groups is a common signature of highly hydrophobic patterns, and molecular dynamics analysis reveals its correlation with the perturbation of interfacial water structure.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Ahmad Boudaghi, Masumeh Foroutan
Summary: This study investigated the wettability of polydimethylsiloxane (PDMS) surfaces using molecular dynamics simulation and found that the constituent atoms and their number influenced the contact angle and droplet radius, with surfaces containing more carbon atoms offering better hydrophobicity. Additionally, rough surfaces rich in carbon increased the surface hydrophobicity.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Optics
Xinzhong Chen, Ziheng Yao, Zhiyuan Sun, Stefan G. Stanciu, D. N. Basov, Rainer Hillenbrand, Mengkun Liu
Summary: The modeling of near-field interaction in scattering-type scanning near-field optical microscope (s-SNOM) is rapidly advancing, but a versatile and accurate modeling framework for various complex situations is still lacking. In this work, a time-efficient numerical scheme in the quasi-electrostatic limit is proposed to capture the tip-sample interaction in the near field. The method considers an extended tip geometry, providing an advantage compared to the previously reported methods. Through investigating anisotropy, experimental parameters, and spatial resolution, the method contributes to the understanding of the contrast mechanism in s-SNOM imaging and spectroscopy and provides a valuable platform for future quantitative analysis of experimental observations.
Article
Engineering, Environmental
Kunkun Wang, Yi Ma, Binbin Sun, Yi Yang, Yinqing Zhang, Lingyan Zhu
Summary: This study investigated the transport and retention of AgNPs capped with PVP of different molecular weights in porous media. It was found that higher molecular weight PVP provided stronger steric effect and electrostatic repulsive forces among PVP-AgNPs, enhancing their mobility. The results shed light on the interplay between capping agents and surface heterogeneity in the transport of AgNPs in porous media.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Environmental Sciences
Kristen Yeh, Li Li, Frank Wania, Jonathan P. D. Abbatt
Summary: Thirdhand smoke (THS) refers to the contamination that remains indoors after smoking. This study reviews the composition and behavior of different types of indoor THS, including from tobacco, e-cigarettes, cannabis, and illicit substances. Modeling results suggest that volatile compounds are inhaled, while water-soluble compounds are absorbed by the skin.
ENVIRONMENT INTERNATIONAL
(2022)
Article
Engineering, Environmental
James M. Mattila, Caleb Arata, Andrew Abeleira, Yong Zhou, Chen Wang, Erin F. Katz, Allen H. Goldstein, Jonathan P. D. Abbatt, Peter F. DeCarlo, Marina E. Vance, Delphine K. Farmer
Summary: The study of indoor Reactive Organic Carbon (ROC) emissions found that cooking significantly impacts indoor ROC concentrations and physicochemical properties, while cleaning has minimal effects. Indoor ROC emissions may play an important role in air quality and secondary pollutant formation outdoors.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Review
Chemistry, Multidisciplinary
Shunyao Wang, Yue Zhao, Arthur W. H. Chan, Min Yao, Zhongming Chen, Jonathan P. D. Abbatt
Summary: Organic peroxides (POs) are important reactive intermediates in atmospheric multiphase processes. They play a key role in the formation, growth, aging, climate, and health impacts of aerosol. This article summarizes the current understanding of atmospheric POs, including their identification, quantification, formation mechanisms, transformation pathways, and environmental and health impacts. The study highlights the need to understand the complex nature and dynamic behavior of POs in order to fully comprehend their origin, fate, and impacts in the atmosphere.
Article
Engineering, Environmental
Spiro D. Jorga, Yutong Wang, Jonathan P. D. Abbatt
Summary: High loadings of biomass burning aerosol particles from wildfire or residential heating sources can deposit onto surfaces and interact with oxidants. Hypochlorous acid (HOCl), emitted during cleaning with chlorine-cleaning agents, can form organochlorine pollutants when exposed to wood smoke aerosol particles. Unsaturated species in wood smoke such as coniferaldehyde and furfural react efficiently with HOCl. The presence of biomass burning emissions suppresses active chlorine recycling in the outdoor environment.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Engineering, Environmental
Emily Reidy, Brandon P. Bottorff, Colleen Marciel F. Rosales, Felipe J. Cardoso-Saldan, Caleb Arata, Shan Zhou, Chen Wang, Andrew Abeleira, Lea Hildebrandt Ruiz, Allen H. Goldstein, Atila Novoselac, Tara F. Kahan, Jonathan P. D. Abbatt, Marina E. Vance, Delphine K. Farmer, Philip S. Stevens
Summary: There have been relatively few measurements of the OH radical in indoor environments despite its importance outdoors. Elevated concentrations of OH were observed near a window during cooking events, in addition to elevated mixing ratios of HONO, VOCs, and NOX. The measured OH concentrations were underestimated by a chemical model, even during periods of direct sunlight, indicating incomplete understanding of oxidation in indoor environments.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Engineering, Environmental
Shunyao Wang, Peter J. Gallimore, Carolyn Liu-Kang, Kirsten Yeung, Steven J. Campbell, Battist Utinger, Tengyu Liu, Hui Peng, Markus Kalberer, Arthur W. H. Chan, Jonathan P. D. Abbatt
Summary: This study reports the unique chemical and toxicological metrics of biomass burning organic aerosols (BBOA) from pine wood smoldering during multiphase aging by gas-phase hydroxyl radicals (OH). Both the fresh and OH-aged BBOA show activity relevant to adverse health outcomes. Short-term aging initiated by OH radicals can produce biomass burning particles with a higher particle-bound reactive oxygen species (ROS) generation capacity, posing a greater exposure hazard for residents in large population centers close to wildfire regions than previously studied fresh biomass burning emissions.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Analytical
Annastacia D. Stubbs, Melodie Lao, Chen Wang, Jonathan P. D. Abbatt, John Hoffnagle, Trevor C. VandenBoer, Tara F. Kahan
Summary: Cleaning surfaces with bleach can release high levels of chlorine gas and hypochlorous acid, which are linked to respiratory issues. A new spectral analysis method using cavity ring-down spectroscopy allows for real-time quantification of hypochlorous acid. The study measured hypochlorous acid levels in a residential bathroom during disinfection, showing higher concentrations near the bathtub and lower concentrations further away. Experimental results also suggested potential human exposure to bleach emissions. This research provides insights into reducing exposure risks from bleach and other cleaning products.
ENVIRONMENTAL SCIENCE-PROCESSES & IMPACTS
(2023)
Article
Chemistry, Analytical
Stephanie R. Schneider, Pascale S. J. Lakey, Manabu Shiraiwa, Jonathan P. D. Abbatt
Summary: This study evaluates the fundamental understanding of the gas-phase iodine emissions resulting from the ozonolysis of iodide. Experimental measurements of I-2(g) formation were compared to predictions made by the kinetic multilayer model for surface and bulk chemistry (KM-SUB). The model successfully predicts the trends observed in the experiments, including the suppression of I-2(g) formation in the presence of chloride ions and biological organic material.
ENVIRONMENTAL SCIENCE-PROCESSES & IMPACTS
(2023)
Article
Engineering, Environmental
Zilin Zhou, Leigh R. Crilley, Jenna C. Ditto, Trevor C. Vandenboer, Jonathan P. D. Abbatt
Summary: Unsaturated triglycerides found in food and skin oils are reactive in ambient air, but their chemical fate in genuine indoor environments is not well understood. This study monitored the aging of oil coatings on glass surfaces and found that ozonolysis is the dominant degradation pathway for oil films in both commercial and office settings. Indoor photooxidation was found to accelerate radical formation on surfaces. The reactive oxygen species (ROS) observed may induce oxidative stress in human bodies and further investigation of their toxicological properties is warranted.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Multidisciplinary Sciences
Chen Wang, John Liggio, Jeremy J. B. Wentzell, Spiro Jorga, Andrew Folkerson, Jonathan P. D. Abbatt
Summary: Monochloramine, dichloramine, and trichloramine were measured in the ambient atmosphere of downtown and suburban Toronto. The results show that chloramines are prevalent in urban areas, with NCl3 exhibiting a diel pattern and a strong correlation between NH2Cl and NHCl2. Photolysis of chloramines contributes to the production of chlorine atoms and is an important source of Cl in urban areas.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Chemistry, Analytical
Jenna C. Ditto, Leigh R. Crilley, Melodie Lao, Trevor C. VandenBoer, Jonathan P. D. Abbatt, Arthur W. H. Chan
Summary: Gas and particulate emissions from commercial kitchens significantly impact urban air quality. This study analyzed volatile organic compounds and particulate matter concentrations in a well-ventilated commercial kitchen during cooking and cleaning operations. The results showed that cooking emissions primarily consist of oxygenated compounds from cooking oil degradation. The high ventilation rate effectively reduces exposure to gas-phase chemicals, but exposure to particulate matter and chlorinated gases increases during evening cleaning. This highlights the importance of careful consideration of ventilation rates and methods in commercial kitchen environments.
ENVIRONMENTAL SCIENCE-PROCESSES & IMPACTS
(2023)
Article
Environmental Sciences
Pascale S. J. Lakey, Andreas Zuend, Glenn C. Morrison, Thomas Berkemeier, Jake Wilson, Caleb Arata, Allen H. Goldstein, Kevin R. Wilson, Nijing Wang, Jonathan Williams, Jonathan P. D. Abbatt, Manabu Shiraiwa
Summary: Studies have shown that the reaction of squalene with ozone can produce various products, and the yield depends on relative humidity. A new mechanism has been developed to simulate these reactions and control the concentrations of different products accordingly. Increasing relative humidity significantly impacts the concentrations of various products.
ENVIRONMENTAL SCIENCE-ATMOSPHERES
(2023)
Article
Environmental Sciences
Carolyn Liu-Kang, Peter J. Gallimore, Tengyu Liu, Jonathan P. D. Abbatt
Summary: This study investigates the short-term aging process of primary BrC particles generated by burning pine wood under UV light exposure. The results show that during the 30-minute exposure, the scattering reflectance of the particles significantly decreases, accompanied by an increase in oxidation. Surprisingly, the decrease in scattering reflectance continues even after the light exposure stops, suggesting the presence of long-lived reactive species.
ENVIRONMENTAL SCIENCE-ATMOSPHERES
(2022)
Article
Environmental Sciences
Rachel Y-W Chang, Jonathan P. D. Abbatt, Matthew C. Boyer, Jai Prakash Chaubey, Douglas B. Collins
Summary: The impact of aerosols on clouds is a significant and still uncertain aspect of the atmospheric system. This study measured cloud condensation nuclei concentrations in the Canadian Arctic and found that ultrafine particles and growth events were mainly composed of slightly hygroscopic organic vapours from the ocean, which could increase background cloud condensation nuclei concentrations at low supersaturation levels.
ATMOSPHERIC CHEMISTRY AND PHYSICS
(2022)
Article
Environmental Sciences
Zoe Brasseur, Dimitri Castarede, Erik S. Thomson, Michael P. Adams, Saskia Drossaart van Dusseldorp, Paavo Heikkila, Kimmo Korhonen, Janne Lampilahti, Mikhail Paramonov, Julia Schneider, Franziska Vogel, Yusheng Wu, Jonathan P. D. Abbatt, Nina S. Atanasova, Dennis H. Bamford, Barbara Bertozzi, Matthew Boyer, David Brus, Martin I. Daily, Romy Foesig, Ellen Gute, Alexander D. Harrison, Paula Hietala, Kristina Hoehler, Zamin A. Kanji, Jorma Keskinen, Larissa Lacher, Markus Lampimaki, Janne Levula, Antti Manninen, Jens Nadolny, Maija Peltola, Grace C. E. Porter, Pyry Poutanen, Ulrike Proske, Tobias Schorr, Nsikanabasi Silas Umo, Janos Stenszky, Annele Virtanen, Dmitri Moisseev, Markku Kulmala, Benjamin J. Murray, Tuukka Petaja, Ottmar Moehler, Jonathan Duplissy
Summary: The formation of ice particles in Earth's atmosphere has a significant impact on the dynamics and optical properties of clouds and their effect on the climate system. This study investigates the emission potential of ice-nucleating particles (INPs) in high-latitude boreal forests during the mixed-phase cloud regime. The research utilizes various instruments to quantify INP concentrations and sources in the boreal environment. The results show consistent findings across the instruments and favorable agreement with an established parameterization.
ATMOSPHERIC CHEMISTRY AND PHYSICS
(2022)