Tracking the history of polycyclic aromatic compounds in London through a River Thames sediment core and ultrahigh resolution mass spectrometry

Journal of Hazardous Materials, Год журнала: 2024, Номер 473, С. 134605 - 134605

Опубликована: Май 14, 2024

Polycyclic aromatic compounds (PACs), including polycyclic hydrocarbons (PAHs) and heteroatom-containing analogues, constitute an important environmental contaminant class. For decades, limited numbers of priority PAHs have been routinely targeted in pollution investigations, however, there is growing awareness for the potential occurrence thousands PACs environment. In this study, untargeted Fourier transform ion cyclotron resonance mass spectrometry was used molecular characterisation a sediment core from Chiswick Ait, River Thames, London, UK. Using complex mixture analysis approaches, aromaticity index calculations, number PAC components determined eight depths, extending back to 1930s. A maximum 1676 compositions representing detected at depth corresponding 1950s, decline observed up core. case linking London's coal consumption history presented, alongside other possible sources, with some data features indicating pyrogenic origins. The overall profile trend components, oxygen, sulfur, nitrogen, chlorine atoms, shown broadly correspond 16 PAH concentration previously These findings implications industry-impacted environments.

Язык: Английский

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Ionization selectivity of electrospray and atmospheric pressure photoionization FT-ICR MS for petroleum refinery wastewater dissolved organic matter

Environmental Science Processes & Impacts, Год журнала: 2021, Номер 23(10), С. 1466 - 1475

Опубликована: Янв. 1, 2021

Dissolved organic matter (DOM) in petroleum refinery wastewater is an extremely complex mixture. A better understanding of chemical compositions DOM at the molecular level necessary for design and optimization treatment processes. In this study, two largely different samples, one from a other Suwannee river water, were characterized by Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) coupled with positive-/negative-ion electrospray ionization (ESI), positive-ion atmospheric pressure photoionization (APPI). For DOM, total 6226 formulae assigned three modes. However, only 1182 common all spectra, indicating that techniques highly complementary types molecules they ionize. Acid Ox (x = 1-9) basic N1Ox 0-2) classes dominant detected negative-ion ESI mode, respectively. And contains considerable amounts polycyclic aromatic hydrocarbons did not respond to but can be ionized selectively APPI. Compared riverine has higher complexity more enriched hydrocarbon, nitrogen- sulfur-containing compounds. The results show major components distinctive those natural matter. Though quantitative, obtained various found complementary, are helpful our selectivity as well DOM.

Язык: Английский

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Exploring Complex Mixtures by Cyclic Ion Mobility High-Resolution Mass Spectrometry: Application Toward Petroleum

Analytical Chemistry, Год журнала: 2021, Номер 93(14), С. 5872 - 5881

Опубликована: Март 30, 2021

The in-depth isomeric and isobaric description of ultra-complex organic mixtures remains one the most challenging analytical tasks. In last two decades, ion mobility coupled to high-performance mass spectrometry added an additional structural dimension. Despite tremendous instrumental improvements, commercial devices are still limited in spectrometric resolving power struggle resolve species complex patterns. To overcome these limitations, we explored capabilities cyclic high-resolution with special emphasis on petrochemical applications. We could show that quadrupole-selected gives closer insights into distribution. combination slicing specific parts dimension, interferences be drastically removed. Collision-induced dissociation (CID) allowed separating groups polycyclic aromatic hydrocarbons heterocycles (PAH/PASH), deploying up 10 passes device. Finally, introduce a data processing workflow 3.4 mDa SH4/C3 split by combining power. Cyclic intelligent design experiments routines will powerful approach addressing complexity mixtures.

Язык: Английский

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Molecular Composition Reveals Unique Rheological Property of Karamay Heavy Crude Oil

Energy & Fuels, Год журнала: 2020, Номер 35(1), С. 473 - 478

Опубликована: Дек. 15, 2020

Heavy oils are commonly found in China; however, the Karamay heavy oil is unique among all. It has very low asphaltene content and an excellent feedstock for producing high-quality lubricant base oils. Physical characteristics of dependent on its chemical composition, which quite difficult to be characterized due complexity. In this work, bulk properties molecular composition crude were compared with those other was that high concentration compounds long side chains naphthenic skeletons makes exhibit a viscosity index. The less temperature at temperatures, technically challenged using thermal enhanced recovery techniques production. However, ideal use as oil. Moreover, total sulfur sulfides/thiophenes ratio provide good oxidation stability. Special biological precursors geological history considered elucidate

Язык: Английский

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Innate Sulfur Compounds as an Internal Standard for Determining Vacuum Gas Oil Compositions by APPI FT-ICR MS

Energy & Fuels, Год журнала: 2020, Номер 34(7), С. 8260 - 8273

Опубликована: Июнь 12, 2020

Innate sulfur components in high boiling petroleum samples were used as an internal standard for the estimation of sample's composition through atmospheric pressure photo ionization (APPI) Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). The first step was recording a representative spectrum aromatic use time-of-flight spectrometer (TOF MS) to tune FT-ICR MS parameters. molecular weight and number atoms per species identified high-resolution measurement, their spectrometric abundance, total content combined calculate fraction each (and by sum all) present. Aromatic hydrocarbon (HC) compound quantification based on equimolar response compared species. Nitrogen treated analogously compounds distributing nitrogen content. balance all yields saturated (saturates), which is not directly accessible APPI process. validity biases this approach evaluated series vacuum distilled fractions with narrow ranges using comprehensive two-dimensional gas chromatography (GCxGC) reference technique. There are clear presented GCxGC analysis, especially underestimation monoaromatic overestimation diaromatic (benzothiophenes); however, results agree surprisingly well and, overall, hydrocarbon- sulfur-containing families. saturates also matched reasonably gravimetrically determined contents, isolated further characterized field desorption/field TOF MS. inclusion carbon distribution, combination data, more complete compositional description studied oil samples. method applied two typical range (derived from Norwegian Arabian crude oil) provide insight into usefulness limitations semiquantitative context, deemed important many industry applications.

Язык: Английский

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Review on Evolved Gas Analysis Mass Spectrometry with Soft Photoionization for the Chemical Description of Petroleum, Petroleum-Derived Materials, and Alternative Feedstocks

Energy & Fuels, Год журнала: 2021, Номер 35(22), С. 18308 - 18332

Опубликована: Ноя. 1, 2021

Modern industry strongly relies on the molecular analysis of fossil petroleum and petroleum-derived materials. In context a circular economy carbon neutrality, chemical description alternative feedstock materials, such as waste plastic biomass pyrolysis oils, increases in importance. Moreover, online monitoring thermochemical catalytic conversion processes has gained rising attention. this framework, evolved gas (EGA) concepts with soft photoionization mass spectrometry (PIMS) were successfully deployed for numerous challenges. On one hand, is highly versatile technique allows "soft" ionization analyte molecule, preserving information. other multiple exist unique benefits, loss information thermogravimetry coupling, high-throughput direct inlet probe concepts, or straightforward reactor monitoring, allowing insights into pyrolytic transformation processes. Hence, review aims to summarize recent work field EGA–PIMS. After technical thermal applied studies are summarized, discussed, evaluated. Besides fuels, alternatives from renewable pyrolysis, recycling processes, reviewed. Finally, future perspectives given, highlighting importance those schemes together state-of-the-art detection by high-resolution energy fuels research.

Язык: Английский

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Semi-quantitative analysis of molecular composition for petroleum fractions using electrospray ionization high-resolution mass spectrometry

Fuel, Год журнала: 2022, Номер 335, С. 127049 - 127049

Опубликована: Дек. 12, 2022

Язык: Английский

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Next Challenges for the Comprehensive Molecular Characterization of Complex Organic Mixtures in the Field of Sustainable Energy

Molecules, Год журнала: 2022, Номер 27(24), С. 8889 - 8889

Опубликована: Дек. 14, 2022

The conversion of lignocellulosic biomass by pyrolysis or hydrothermal liquefaction gives access to a wide variety molecules that can be used as fuel building blocks in the chemical industry. For such purposes, it is necessary obtain their detailed composition adapt process, including upgrading steps. Petroleomics has emerged an integral approach cover missing link investigation bio-oils and linked products. It relies on ultra-high-resolution mass spectrometry attempt unravel contribution many compounds complex samples non-targeted approach. most recent developments petroleomics partially alter discriminating nature analyses. However, peak referring one formula possibly hides forest isomeric compounds, which may present large diversity concerning functions. This identification functions essential context bio-oils. latest dedicated this analytical challenge will reviewed discussed, particularly integrating ion source features incorporating new steps workflow. representativeness data obtained petroleomic still important issue.

Язык: Английский

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Top-Down Protein Analysis by Tandem-Trapped Ion Mobility Spectrometry/Mass Spectrometry (Tandem-TIMS/MS) Coupled with Ultraviolet Photodissociation (UVPD) and Parallel Accumulation/Serial Fragmentation (PASEF) MS/MS Analysis

Journal of the American Society for Mass Spectrometry, Год журнала: 2023, Номер 34(10), С. 2232 - 2246

Опубликована: Авг. 28, 2023

"Top-down" proteomics analyzes intact proteins and identifies proteoforms by their mass as well the observed fragmentation pattern in tandem spectrometry (MS/MS) experiments. Recently, hybrid ion mobility spectrometry–mass (IM/MS) methods have gained traction for top-down experiments, either allowing analysis of individual isomers or alternatively improving signal/noise dynamic range fragment assignment. We recently described construction a tandem-trapped spectrometer/mass spectrometer (tandem-TIMS/MS) coupled with an ultraviolet (UV) laser demonstrated proof-of-principle UV photodissociation (UVPD) at 2–3 mbar. The present work builds on this exploration method that couples tandem-TIMS/MS UVPD parallel-accumulation serial (PASEF) MS/MS analysis. first survey types structures UVPD-specific ions generated mbar pressure regime our instrument. Notably, we observe UVPD-induced multiple conformations differ from those produced absence irradiation. Subsequently, discuss how spectra lend themselves ideally probability-based scoring developed bottom-up field ability to record automated PASEF-MS/MS resolves ambiguities assignment ions. Finally, describe coupling workflows native protein

Язык: Английский

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A Light Touch: Solar Photocatalysis Detoxifies Oil Sands Process-Affected Waters Prior to Significant Treatment of Naphthenic Acids

ACS ES&T Water, Год журнала: 2024, Номер 4(4), С. 1483 - 1497

Опубликована: Фев. 23, 2024

Environmental reclamation of Canada's oil sands tailings ponds is among the single largest water treatment challenges globally. The toxicity process-affected (OSPW) has been associated with its dissolved organics, a complex mixture naphthenic acid fraction components (NAFCs). Here, we evaluated solar buoyant photocatalysts (BPCs) as passive advanced oxidation process (P-AOP) for OSPW remediation. Photocatalysis fully degraded acids (NAs) and extractable organics (AEO) in 3 different samples. However, classical NAs AEO, traditionally considered principal toxicants OSPW, were not correlated herein. Instead, nontarget petroleomic analysis revealed that low-polarity organosulfur compounds, composing <10% total apparently accounted majority waters' to fish, described by model tissue partitioning. These findings have implications release, which less extensive but more selective may be required than previously expected.

Язык: Английский

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