Impacts of Lipase Enzyme on the Surface Properties of Marine Aerosols

Schiffer, Jamie M.; Luo, Man; Dommer, Abigail C.; Thoron, G.; Pendergraft, Matthew A.; Santander, Mitchell V.; Lucero, Dolan; Barros, Emília P.; Prather, Kimberly A.; Grassian, Vicki H.; Amaro, Rommie E.

doi:10.1021/acs.jpclett.8b01363

Cited by 23 publications

(33 citation statements)

References 79 publications

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“…[ 24,27 ] Second, molecular dynamics (MD) simulations have been successfully implemented to model physicochemical phenomena such as ice nucleation on sea‐spray aerosols and water coverage mobility on atmospheric aerosols. [ 28–31 ] While these two approaches are paramount to understanding the chemistry of aerosols as it pertains to climate and the environment, recent work has required the use of quantum mechanical (QM) methods to advance our understanding of aerosol phenomena at a molecular level.…”

Section: Introductionmentioning

confidence: 99%

Particle formation and surface processes on atmospheric aerosols: A review of applied quantum chemical calculations

Leonardi

Ricker

Gale

et al. 2020

Int J of Quantum Chemistry

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Aerosols significantly influence atmospheric processes such as cloud nucleation, heterogeneous chemistry, and heavy-metal transport in the troposphere. The chemical and physical complexity of atmospheric aerosols results in large uncertainties in their climate and health effects. In this article, we review recent advances in scientific understanding of aerosol processes achieved by the application of quantum chemical calculations. In particular, we emphasize recent work in two areas: new particle formation and heterogeneous processes. Details in quantum chemical methods are provided, elaborating on computational models for prenucleation, secondary organic aerosol formation, and aerosol interface phenomena. Modeling of relative humidity effects, aerosol surfaces, and chemical kinetics of reaction pathways is discussed. Because of their relevance, quantum chemical calculations and field and laboratory experiments are compared. In addition to describing the atmospheric relevance of the computational models, this article also presents future challenges in quantum chemical calculations applied to aerosols.

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Section: Introductionmentioning

confidence: 99%

Particle formation and surface processes on atmospheric aerosols: A review of applied quantum chemical calculations

Leonardi

Ricker

Gale

et al. 2020

Int J of Quantum Chemistry

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“…[1][2][3][4] Adsorbed proteins at the air/sea water interface play important roles. For example, enzymes at the interface have been suggested to alter the surface properties of sea spray aerosol, 5,6 and surface proteins can also stabilize foams and bubbles. [7][8][9] To provide physical insights into protein adsorption at the air/salt water interface, we combine VSFG with surface pressure measurements to study BSA at low bulk concentrations (2 to 5 ppm) at the air/ salt water interface.…”

Section: Introductionmentioning

confidence: 99%

Salting Up of Proteins at the Air/Water Interface

Shrestha

Luo

et al. 2019

Langmuir

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Vibrational sum frequency generation (VSFG) spectroscopy and surface pressure measurements are used to investigate the adsorption of a globular protein, bovine serum albumin (BSA), at the air/water interface with and without the presence of salts. We find at low (2 to 5 ppm) protein concentrations, which is relevant to environmental conditions, both VSFG and surface pressure measurements of BSA behave drastically different than at higher concentrations. Instead of emerging to the surface immediately, as observed at 1000 ppm, protein adsorption kinetics is on the order of tens of minutes at lower concentrations. Most importantly, salts strongly enhance the presence of BSA at the interface. This "salting up" effect differs from the well-known "salting out" effect as it occurs at protein concentrations wellbelow where "salting out" occurs. The dependence on salt concentration suggests this effect relates to a large extent electrostatic interactions and volume exclusion. Additionally, results from other proteins and the pH dependence of the kinetics indicate that salting up depends on the flexibility of proteins. This initial report demonstrates "salting up" as a new type of salt-driven interfacial phenomenon, which is worthy of continued investigation given the importance of salts in biological and environmental aqueous systems.

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“…Biogenic surfactants have also been explored in more complex systems and have been shown to alter surface features 26 , enhance interactions 19,20,27,28 , and influence the overall film properties. 29 Ex situ analysis of the interfacial regime of native marine systems has been reported, with some studies extending to surface tension measurements, 26 Brewster angle microscopy (BAM), 30,31 and sum frequency generation spectroscopy (SFG).…”

Section: Introductionmentioning

confidence: 99%

The Ocean’s Elevator: Evolution of the Air-Seawater Interface During a Small-Scale Algal Bloom

Rogers¹,

Neal²,

Saha³

et al. 2020

Preprint

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We explore in situ the surface properties of marine algal blooms of diatom monocultures by utilizing surface techniques of Brewster angle microscopy (BAM) imaging, vibrational sum frequency generation spectroscopy (SFG), and infrared reflection absorption spectroscopy (IRRAS). Over the course of the bloom, the marine algae produce surface-active biogenic molecules that temporally partition to the topmost interfacial layers and are selectively probed through surface imaging and spectroscopic measurements. BAM images show morphological structural changes and heterogeneity in the interfacial films with increasing density of surface-active biogenic molecules. Film thickness calculations quantified the average surface thickness over time. The image results reveal an ~5 nm thick surface region in the late stages of the bloom which correlates to typical sea surface nanolayer thicknesses. Our surface-specific SFG spectroscopy results show significant diminishing in the intensity of the dangling OH bond of surface water molecules consistent with organic molecules partitioning and replacing water at the air-seawater interface as the algal bloom progresses. Interestingly, we observe a new broad peak appear between 3500 cm<sup>-1</sup> to 3600 cm<sup>-1</sup> in the late stages of the bloom that is attributed to weak hydrogen bonding interactions of water to the surface-active biogenic matter. IRRAS confirms the presence of organic molecules at the surface as we observe increasing intensity of vibrational alkyl modes and the appearance of a proteinaceous amide band. Our work shows the often overlooked but vast potential of tracking changes in the interfacial regime of small-scale laboratory marine algal blooms. By coupling surface imaging and vibrational spectroscopies to complex, time-evolving, marine-relevant systems, we provide additional insight into unraveling the temporal complexity of sea spray aerosol compositions.

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Impacts of Lipase Enzyme on the Surface Properties of Marine Aerosols

Cited by 23 publications

References 79 publications

Particle formation and surface processes on atmospheric aerosols: A review of applied quantum chemical calculations

Particle formation and surface processes on atmospheric aerosols: A review of applied quantum chemical calculations

Salting Up of Proteins at the Air/Water Interface

The Ocean’s Elevator: Evolution of the Air-Seawater Interface During a Small-Scale Algal Bloom

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