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Full-Text Articles in Physical Sciences and Mathematics

Potentially Massive And Global Non-Pyrogenic Production Of Condensed "Black" Carbon Through Biomass Oxidation, Aleksandar I. Goranov, Hongmei Chen, Jianshu Duan, Satish C. B. Myneni, Patrick G. Hatcher Jan 2024

Potentially Massive And Global Non-Pyrogenic Production Of Condensed "Black" Carbon Through Biomass Oxidation, Aleksandar I. Goranov, Hongmei Chen, Jianshu Duan, Satish C. B. Myneni, Patrick G. Hatcher

Chemistry & Biochemistry Faculty Publications

With the increased occurrences of wildfires worldwide, there has been an increase in scientific interest surrounding the chemistry of fire-derived "black" carbon (BC). Traditionally, wildfire research has assumed that condensed aromatic carbon (ConAC) is exclusively produced via combustion, and thus, ConAC is equated to BC. However, the lack of correlations between ConAC in soils or rivers and wildfire history suggests that ConAC may be produced non-pyrogenically. Here, we show quantitative evidence that this occurs during the oxidation of biomass with environmentally ubiquitous hydroxyl radicals. Pine wood boards exposed to iron nails and natural weather conditions for 12 years yielded a …


Biolability Of Fresh And Photodegraded Pyrogenic Dissolved Organic Matter From Laboratory-Prepared Chars, K. W. Bostick, A. R. Zimmerman, A. I. Goranov, S. Mitra, P. G. Hatcher, A. S. Wozniak Jan 2021

Biolability Of Fresh And Photodegraded Pyrogenic Dissolved Organic Matter From Laboratory-Prepared Chars, K. W. Bostick, A. R. Zimmerman, A. I. Goranov, S. Mitra, P. G. Hatcher, A. S. Wozniak

Chemistry & Biochemistry Faculty Publications

Pyrogenic dissolved organic matter (pyDOM) is known to be an important biogeochemical constituent of aquatic ecosystems and the carbon cycle. While recent studies have examined how pyDOM production, composition, and photolability varies with parent pyrogenic solid material type, we lack an understanding of potential microbial mineralization and transformation of pyDOM in the biogeosphere. Thus, leachates of oak, charred at 400 °C and 650 °C, as well as their photodegraded counterparts were incubated with a soil‐extracted microbial consortium over 96 days. During the incubation, significantly more carbon was biomineralized from the lower versus higher temperature char leachate (45% vs. 37% lost, …


Production And Composition Of Pyrogenic Dissolved Organic Matter From A Logical Series Of Laboratory-Generated Chars, Kyle W. Bostick, Andrew R. Zimmerman, Andrew S. Wozniak, Siddhartha Mitra, Patrick G. Hatcher Apr 2018

Production And Composition Of Pyrogenic Dissolved Organic Matter From A Logical Series Of Laboratory-Generated Chars, Kyle W. Bostick, Andrew R. Zimmerman, Andrew S. Wozniak, Siddhartha Mitra, Patrick G. Hatcher

Chemistry & Biochemistry Faculty Publications

Though pyrogenic carbon (pyC) has been assumed to be predominantly stable, degradation and transfers of pyC between various pools have been found to influence its cycling and longevity in the environment. Dissolution via leaching may be the main control on loss processes such as microbial or abiotic oxidation, mineral sorption, or export to aquatic systems. Yet, little is known about the controls on pyrogenic dissolved organic matter (pyDOM) generation or composition. Here, the yield and composition of pyDOM generated through batch leaching of a thermal series of oak and grass biochars, as well as several non-pyrogenic reference materials, was compared …


Detailed Source-Specific Molecular Composition Of Ambient Aerosol Organic Matter Using Ultrahigh Resolution Mass Spectrometry And H Nmr, Amanda S. Willoughby, Andrew S. Wozniak, Patrick G. Hatcher Jan 2016

Detailed Source-Specific Molecular Composition Of Ambient Aerosol Organic Matter Using Ultrahigh Resolution Mass Spectrometry And H Nmr, Amanda S. Willoughby, Andrew S. Wozniak, Patrick G. Hatcher

Chemistry & Biochemistry Faculty Publications

Organic aerosols (OA) are universally regarded as an important component of the atmosphere that have far-ranging impacts on climate forcing and human health. Many of these impacts are related to OA molecular characteristics. Despite the acknowledged importance, current uncertainties related to the source apportionment of molecular properties and environmental impacts make it difficult to confidently predict the net impacts of OA. Here we evaluate the specific molecular compounds as well as bulk structural properties of total suspended particulates in ambient OA collected from key emission sources (marine, biomass burning, and urban) using ultrahigh resolution mass spectrometry (UHR-MS) and proton nuclear …


Use Of Esi-Fticr-Ms To Characterize Dissolved Organic Matter In Headwater Streams Draining Forest-Dominated And Pasture-Dominated Watersheds, Yuehan Lu, Xiaping Li, Rajaa Mesfioui, James E. Bauer, R. M. Chambers, Elizabeth A. Canuel, Patrick G. Hatcher Jan 2015

Use Of Esi-Fticr-Ms To Characterize Dissolved Organic Matter In Headwater Streams Draining Forest-Dominated And Pasture-Dominated Watersheds, Yuehan Lu, Xiaping Li, Rajaa Mesfioui, James E. Bauer, R. M. Chambers, Elizabeth A. Canuel, Patrick G. Hatcher

Chemistry & Biochemistry Faculty Publications

Electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI-FTICR-MS) has proven to be a powerful technique revealing complexity and diversity of natural DOM molecules, but its application to DOM analysis in grazing-impacted agricultural systems remains scarce. In the present study, we presented a case study of using ESI-FTICR-MS in analyzing DOM from four headwater streams draining forest-or pasture-dominated watersheds in Virginia, USA. In all samples, most formulas were CHO compounds (71.8-87.9%), with other molecular series (CHOS, CHON, CHONS, and CHOP (N, S)) accounting for only minor fractions. All samples were dominated by molecules falling in the lignin-like region (H/C …


A Molecular-Level Approach For Characterizing Water-Insoluble Components Of Ambient Organic Aerosol Particulates Using Ultrahigh-Resolution Mass Spectrometry, A. S. Willoughby, A. S. Wozniak, Patrick G. Hatcher Jan 2014

A Molecular-Level Approach For Characterizing Water-Insoluble Components Of Ambient Organic Aerosol Particulates Using Ultrahigh-Resolution Mass Spectrometry, A. S. Willoughby, A. S. Wozniak, Patrick G. Hatcher

Chemistry & Biochemistry Faculty Publications

The chemical composition of organic aerosols in the atmosphere is strongly influenced by human emissions. The effect these have on the environment, human health, and climate change is determined by the molecular nature of these chemical species. The complexity of organic aerosol samples limits the ability to study the chemical composition, and therefore the associated properties and the impacts they have. Many studies have addressed the watersoluble fraction of organic aerosols and have had much success in identifying specific molecular formulas for thousands of compounds present. However, little attention is given to the water-insoluble portion, which can contain most of …


Distinguishing Molecular Characteristics Of Aerosol Water Soluble Organic Matter From The 2011 Trans-North Atlantic Us Geotraces Cruise, A. S. Wozniak, A. S. Willoughby, S. C. Gurganus, Patrick G. Hatcher Jan 2014

Distinguishing Molecular Characteristics Of Aerosol Water Soluble Organic Matter From The 2011 Trans-North Atlantic Us Geotraces Cruise, A. S. Wozniak, A. S. Willoughby, S. C. Gurganus, Patrick G. Hatcher

Chemistry & Biochemistry Faculty Publications

The molecular characteristics of aerosol organic matter (OM) determines to a large extent its impacts on the atmospheric radiative budget and ecosystem function in terrestrial and aquatic environments, yet the OM molecular details of aerosols from different sources are not well established. Aerosol particulate samples with North American-influenced, North African-influenced, and marine (minimal recent continental influence) air mass back trajectories were collected as part of the 2011 trans-North Atlantic US GEOTRACES cruise and analyzed for their water soluble OM (WSOM) molecular characteristics using electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Principal component analysis (PCA) separated the samples into …


Fossil And Contemporary Aerosol Particulate Organic Carbon In The Eastern United States: Implications For Deposition And Inputs To Watersheds, Andrew S. Wozniak, James E. Bauer, Rebecca M. Dickhut Jan 2011

Fossil And Contemporary Aerosol Particulate Organic Carbon In The Eastern United States: Implications For Deposition And Inputs To Watersheds, Andrew S. Wozniak, James E. Bauer, Rebecca M. Dickhut

Chemistry & Biochemistry Faculty Publications

Atmospheric particulate matter samples were collected from mid-Atlantic and northeastern U. S. (Virginia and New York, respectively) sites to assess the fossil versus contemporary sources contributing to aerosol organic carbon (OC) and the implications for its deposition to watersheds. Mean particulate matter total OC (TOC) deposition rates (wet + dry deposition) were calculated to be 1.6 and 2.4 mg C m-2 d-1 for the Virginia and New York sites, respectively. Wet deposition of particulate TOC was determined to be the dominant depositional mode, accounting for >65% (Virginia) and >80% (New York) of total aerosol TOC deposition. Isotopic mass …


Technical Note: Molecular Characterization Of Aerosol-Derived Water Soluble Organic Carbon Using Ultrahigh Resolution Electrospray Ionization Fourier Transform Ion Cyclotron Resonance Mass Spectrometry, A. S. Wozniak, J. E. Bauer, R. L. Sleighter, R. M. Dickhut, Patrick Hatcher Jan 2008

Technical Note: Molecular Characterization Of Aerosol-Derived Water Soluble Organic Carbon Using Ultrahigh Resolution Electrospray Ionization Fourier Transform Ion Cyclotron Resonance Mass Spectrometry, A. S. Wozniak, J. E. Bauer, R. L. Sleighter, R. M. Dickhut, Patrick Hatcher

Chemistry & Biochemistry Faculty Publications

Despite the acknowledged relevance of aerosol-derived water-soluble organic carbon (WSOC) to climate and biogeochemical cycling, characterization of aerosol WSOC has been limited. Electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI FT-ICR MS) was utilized in this study to provide detailed molecular level characterization of the hi(,h molecular weight (HMW; m/z>223) component of aerosol-derived WSOC collected from rural sites in Virginia and New York, USA. More than 3000 peaks were detected by ESI FT-ICR MS within a m/z range of 223-600 for each sample. Approximately 86% (Virginia) and 78% (New York) of these peaks were assigned molecular formulas …


Naturally Present Fatty Acids As Internal Calibrants For Fourier Transform Mass Spectra Of Dissolved Organic Matter, Rachel L. Sleighter, Georgina A. Mckee, Zhanfei Liu, Patrick G. Hatcher Jan 2008

Naturally Present Fatty Acids As Internal Calibrants For Fourier Transform Mass Spectra Of Dissolved Organic Matter, Rachel L. Sleighter, Georgina A. Mckee, Zhanfei Liu, Patrick G. Hatcher

Chemistry & Biochemistry Faculty Publications

The analysis of dissolved organic matter ( DOM) by Fourier transform ion cyclotron resonance mass spectrometry ( FTICR- MS) has gained wide interest recently, driven primarily by its ultrahigh resolving power and mass accuracy. Accurate calibration of mass spectra is a key step to successfully decipher the DOM components. We propose a simple and accurate method to internally calibrate the peaks in the complex spectra without the need to add a calibrant. Mass spectra of DOM samples from the Dismal Swamp, Virginia, and the lower Chesapeake Bay display the presence of naturally occurring fatty acids which can be readily recognized …