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molecular composition of low-temperature oxidation products of the heavy oil

Petroleum Science 2023年第5期20卷 3264-3271页

作者： Shuai Ma Yun-Yun Li Ri-Gu Su Xu-Sheng Wang Jing-Jun Pan Quan Shi Guang-Zhi Liao Chun-Ming Xu State Key Laboratory of Heavy Oil Processing Petroleum Molecular Engineering Center(PMEC)China University of PetroleumBeijing102249China Engineering Technology Research Institute of PetroChina Xinjiang Oilfield Company Karamay834000XinjiangChina CAS Lanzhou Institute of Chemical Physics Lanzhou730000GansuChina PetroChina Exploration&Production Company Beijing100007China

Low-temperature oxidation(LTO)is the main reaction that affects fuel formation in the in-situ combustion process,which has important significance for the subsequent combustion propulsion and the successful extraction of crude *** this study,heavy oil was subjected to LTO reactions at different *** types of reaction products with varying oxidation depths were characterized in terms of the number of oxygen atoms and the polarity of the molecule to reveal the low-temperature oxidation process of the heavy *** compounds and acid polyoxides in the oil phase and deep oxidation products with a higher number of oxygen atoms in the coke were identified with increasing oxidation *** experimental results showed that the oxidation reaction of the heavy oil changed from kinetic-controlled to diffusion-controlled in the open oxidation system of the heavy oil as the oxidation depth *** oxidation reaction of the oil phase reached a maximum and stable value in oxygen *** molecular compositions of the ketone compound and acid polyoxide did not change significantly with further increase in reaction *** molecular compositions of the deep oxidation products with a higher number of oxygen atoms in the coke phase changed *** coke precursor molecules with a lower oxygen content and condensation degree participated in the coke formation,and the oxidation reaction pathway and the complexity of the oxidation product component also increased.

关键词： Low-temperature oxidation In-situ combustion Heavy oil Coke precursor molecular composition

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Revealing the characteristics of dissolved organic matter in urban runoff at three typical regions via optical indices and molecular composition

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Journal of Environmental Sciences 2021年第10期33卷 8-21页

作者： Zhenliang Liao Jiangyong Chu Chongjia Luo Hao Chen College of Civil Engineering and Architecture Xinjiang UniversityUrumqi 830046China UNEP-Tongji Institute of Environment for Sustainable Development College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Key Laboratory of Yangtze River Water Environment Ministry of EducationTongji UniversityShanghai 200092China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China Shanghai Academy of Environmental Sciences Shanghai 200233China

Dissolved organic matter(DOM)plays a major role in ecological systems and influences the fate and transportation of many *** the significance of DOM,understanding of how environmental and anthropogenic factors influence its composition and characteristics is limited,especially in urban stormwater *** this article,the chemical properties(pollutant loads,molecular weight,aromaticity,sources,and molecular composition)of DOM in stormwater extracted from three typical end-members(traffic,residential,and campus regions)were characterized by UV–visible(UV–vis)spectroscopy,excitationemission matrix spectroscopy combined with parallel factor analysis(EEM-PARAFAC),and ultra-performance liquid chromatography quadrupole time-of-flight mass spectrometry(UPLC-Q-TOF-MS).There are three findings:(1)The basic properties of DOM in stormwater runoff varied obviously from three urban fields,and the effect of initial flush was also apparent.(2)The DOM in residential areas mainly came from autochthonous sources,while allochthonous sources primarily contributed to the DOM in traffic and campus ***,it was mainly composed of terrestrial humic-like components with CHO and CHON element composition and HULO and aliphatic formulas.(3)The parameters characterizing DOM were primarily related to terrestrial source and aromaticity,but their correlations *** the combination of optical methods and UPLC-Q-TOF spectrometry,the optical and molecular characteristics of rainwater are effectively revealed,which may provide a solid foundation for the classification management of stormwater runoff in different urban regions.

关键词： Urban stormwater runoff Dissolved organic matter(DOM) Optical properties molecular composition characteristics

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Characterization of chemical composition of high viscosity heavy oils:Macroscopic properties, and semi-quantitative analysis of molecular composition using high-resolution mass spectrometry

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Petroleum Science 2024年第5期21卷 3612-3620页

作者： Jian-Xun Wu Shuo-Fan Li Qi-Fu Li Feng Yan Qi-Lin Zhou Shuai Ma Ya-He Zhang Suo-Qi Zhao Quan Shi State Key Laboratory of Heavy Oil Processing Petroleum Molecular Engineering Center(PMEC)China University of PetroleumBeijing102249China PipeChina Institute of Science and Technology Tianjin300457China

Heavy oil is an important resource in current petroleum exploitation, and the chemical composition information of heavy oil is crucial for revealing its viscosity-inducing mechanism and solving practical exploitation issues. In this study, the techniques of high-temperature gas chromatography and high-resolution mass spectrometry equipped with an electrospray ionization source were applied to reveal the chemical composition of typical heavy oils from western, central, and eastern China. The results indicate that these heavy oils display significant variations in their bulk properties, with initial boiling points all above 200℃. Utilizing pre-treatment and ESI high-resolution mass spectrometry, an analysis of the molecular composition of saturated hydrocarbons, aromatic hydrocarbons, acidic oxygen compounds, sulfur compounds, basic nitrogen compounds, and neutral nitrogen compounds within the heavy oil was conducted. Ultimately, a semi-quantitative analysis of the molecular composition of the heavy oil was achieved by integrating the elemental content. The semi-quantitative analysis results of Shengli-J8 heavy oil and a conventional Shengli crude oil show that Shengli-J8 heavy oil lacks alkanes and low molecular weight aromatic hydrocarbons, which contributes to its high viscosity. Additionally,characteristic molecular sets for different heavy oils were identified based on the semi-quantitative analysis of molecular composition. The semi-quantitative analysis of molecular composition in heavy oils may provide valuable reference data for establishing theoretical models on the viscosity-inducing mechanism in heavy oils and designing viscosity-reducing agents for heavy oil exploitation.

关键词： Heavy oil HRMS molecular composition Semi-quantitative analysis Viscosity

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Bioactivity profile of dissolved organic matter and its relation to molecular composition

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Natural Products and Bioprospecting 2023年第1期13卷 425-440页

作者： Teresa S.Catalá Linn G.Speidel Arlette Wenzel-Storjohann Thorsten Dittmar Deniz Tasdemir Global Society Institute WälderhausHamburgGermany Organization for Science Education and Global Society gGmbHStuttgartGermany ICBM-MPI Bridging Group for Marine Geochemistry Institute for Chemistry and Biology of the Marine Environment(ICBM)University of OldenburgOldenburgGermany Geological Institute Department of Earth SciencesETH Zurich8092 ZurichSwitzerland GEOMAR Centre for Marine Biotechnology Research Unit Marine Natural Products ChemistryGEOMAR Helmholtz Centre for Ocean Research KielAm Kiel-Kanal 4424106 KielGermany Helmholtz Institute for Functional Marine Biodiversity University of OldenburgOldenburgGermany Kiel University Christian-Albrechts-Platz 424118 KielGermany

Dissolved organic matter(DOM)occupies a huge and uncharted molecular *** its properties,DOM can be presented as a promising biotechnological ***,research into bioactivities of DOM is still in early *** this study,the biotechnological potential of terrestrial and marine DOM,its molecular composition and their relationships are *** were screened for their in vitro antibacterial,antifungal,anticancer and antioxidant *** activity was detected against Staphylococcus aureus in almost all DOM samples,with freshwater DOM showing the lowest IC50 *** samples also inhibited Staphylococcus epidermidis,and four DOM extracts showed up to fourfold higher potency than the reference *** activity was limited to only porewater DOM towards human dermatophyte Trichophyton *** significant in vitro anticancer activity was *** antioxidant potential was *** molecular characterization by FT-ICR MS allowed a broad compositional *** main distinguished groups have been identified by PCoA *** activities are related to high aromaticity content and highly-unsaturated molecular formulae(O-poor).Antifungal effect is correlated with highly-unsaturated molecular formulae(O-rich).Antioxidant activity is positively related to the presence of double bonds and *** study evidenced for the first time antibacterial and antifungal activity in DOM with potential applications in cosmeceutical,pharmaceutical and aquaculture *** lack of cytotoxicity and the almost unlimited presence of this organic material may open new avenues in future marine bioprospect-ing efforts.

关键词： Dissolved organic matter Antibacterial activity Antifungal activity Antioxidant activity molecular composition

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Effects of experimental conditions on the molecular composition of maltenes and asphaltenes derived from oilsands bitumen: Characterized by negative-ion ESI FT-ICR MS

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Science China Chemistry 2013年第7期56卷 863-873页

作者： WANG LiTao HE Chen LIU Yang ZHAO SuoQi ZHANG YaHe XU ChunMing CHUNG Keng H. SHI Quan State Key Laboratory of Heavy Oil Processing China University of Petroleum Well Resources Inc.

A vacuum topped Canadian oilsands bitumen （VTB） was subjected to solvent precipitation and subsequently characterized by elemental analysis, gel permeation chromatograph （GPC）, IH-NMR spectroscopy and negative-ion electrospray ionization （ESI） Fourier transform ion cyclotron resonance mass spectrometry （FT-ICR MS）. Effects of experimental conditions such as solvent types （n-Cs, n-C6, and n-C7）, solvent purity, and solvent washing time on asphaltenes yields, bulk composition, and molecular composition of detectable heteroatom compounds in ESI source were determined. Elemental nitrogen and sulfur were enriched in asphaltenes while elemental oxygen had comparable content in maltenes and asphaltenes. molecular compo- sition of asphaltenes varies with separation conditions. The N1 and O1 species identified by ESI FT-ICR MS were enriched in maltenes. The 02 species exhibited two different double bond equivalents （DBE） distributions and solubility in normal paraffin solvents, indicating two types of molecular structures. Multi oxygen atom containing compounds mainly detected in asphal- tenes. Compound class distributions are similar for maltenes derived from n-Cs, n-C6, and n-C7 , as well as for asphaltenes. The cyclic paraffin impurities in normal paraffin solvents had a significant influence on asphaltenes yields and heteroatom molecu- lar composition. A portion of neutral N1 species and acidic 02 species adsorbed on asphaltenes could be dissolved by increas- ing washing time. Cautions should be exercised when interpreting the properties and composition of asphaltenes obtained with different experimental conditions.

关键词： asphaltene precipitation experimental conditions bulk properties molecular composition ESI FT-ICR MS

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The molecular composition and mass-size distribution of biogenic secondary organic aerosol from Xi’an

The molecular composition and mass-size distribution of biog...

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十一届全国气溶胶会议暨第十届海峡两岸气溶胶技术研讨会

作者： SUN Tao WANG Ge-hui LI Jian-jun State Key Laboratory of Loess and Quaternary Geology Institute of Earth and EnvironmentChinese Academy of Sciences

In this study, concentration and size distribution of biogenic secondary organic aerosols（i.e., isoprene, pinene and sesquiterpene photooxidation products） in the summertime atmosphere of Xi’an city, China was characterized using a GC/MS technique after a conversion to TMS derivatives. Our results showed that BSOA in Xi’an are dominated by isoprene oxidation products, which accounted for around 80% of the total quantified BSOA. Biogenic secondary organic carbon derived from isoprene, α-/β-pinene and sesquiterpene were 0.39μg C/m3, 0.13μg C/m3, 0.10μg C/m3, respectively. Size distributions of the nine determined compounds suggest that BSOA in the city are enriched in fine particles. Compared to that in other cities and mountain areas the relatively lower ratio of MBTCA/CPA ratio of Xi’an BSOA indicates that BSOA in the city are mostly derived from local sources and more fresh.

关键词： biogenic secondary organic aerosol isoprene α-/β-pinene sesquiterpene molecular composition size distribution

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molecular compositions and sources of organic aerosols at a rural site on the Guanzhong Plain,Northwest China:The importance of biomass burning

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Particuology 2024年第6期89卷 44-56页

作者： Yali Liu Minxia Shen Haijiao Liu Wenting Dai Weining Qi Yifan Zhang Lu Li Yue Cao Xin Wang Xiao Guo Yingkun Jiang Jianjun Li State Key Laboratory of Loess and Quaternary Geology Key Lab of Aerosol Chemistry and PhysicsInstitute of Earth EnvironmentChinese Academy of SciencesXi'an 710061China Xi'an Institute for Innovative Earth Environment Research Xi'an 710061China National Observation and Research Station of Regional Ecological Environment Change and Comprehensive Management in the Guanzhong Plain ShaanxiChina

The concentration of PM_(2.5)has considerably reduced in recent years,but remains relatively high in *** particular,the increasing contribution of organic compounds to PM_(2.5)generates popular pressure for further reductions,resulting in an urgent need to study organic aerosol(OA).To investigate the molecular composition and source contribution of OA in the rural area of the Guanzhong Plain,Northwest China,PM_(2.5)samples were collected during 3–23 August 2016 and 5–20 January 2017 and studied for more than 100 organic tracer *** mean concentration of total measured organic compounds is 662±296 ng/m^(3)in summer and 3258±1925 ng/m^(3)in *** is the most abundant single compound found throughout the sampling period,which is a crucial tracer for biomass burning emissions,preliminary suggesting that biomass burning is an essential source of *** summer,organic compounds such as lipid compounds,sugar compounds,and polycyclic aromatic hydrocarbons(PAHs),more come from higher plants,wood burning,vehicle exhausts,plastic waste,and other direct emission *** PAHs(OPAHs),nitrophenols,and phthalic acids more come from the atmosphere through the oxidation reaction of aromatic precursors,especially photochemical ***,in winter,most of the increases in concentrations of organic compounds are attributed to biomass *** analysis of a haze event(14–19 January 2017)during the winter sampling period shows that the increases in the concentration of organic compounds are unaccompanied by strong secondary formation under lower relative humidity(49.1%±13.5%).The main reason for the growth of OA in this haze event is the accumulation of primary OA(POA).The source apportionment by the positive matrix factorization(PMF)model shows that biomass burning(37.1%)is the primary source of OA in the rural regions of the Guanzhong Plain,especially in winter(40.6%).The contribution of secondary formation decreases from 26.0%in summer t

关键词： Organic aerosol molecular composition Seasonal variation Source apportionment Guanzhong Plain

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The optical and molecular signatures of DOM under the eutrophication status in a shallow,semi-enclosed coastal bay in southeast China

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Science China Earth Sciences 2021年第7期64卷 1090-1104页

作者： Chen ZHAO Yuping ZHOU Yu PANG Yanzhen ZHANG Wei HUANG Yuntao WANG Ding HE Key Laboratory of Geoscience Big Data and Deep Resource of Zhejiang Province School of Earth SciencesZhejiang UniversityHangzhou 310027China State Key Laboratory of Satellite Ocean Environment Dynamics Second Institute of OceanographyMinistry of Natural ResourcesHangzhou 310027China

We applied stable carbon isotopes,ultraviolet-visible absorption(UV-Vis),fluorescence excitation-emission matrices spectroscopy(EEMs),and Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR-MS)to investigate the chemical composition and sources of the dissolved organic matter(DOM)in both the water column and pore water in Xiangshan Bay,a representative semi-enclosed and eutrophic bay in Zhejiang Province,*** protein-like fluorescent component(C1)and two humic-like fluorescent components(C2 and C3)were identified by PARAFAC *** concentration of dissolved organic carbon(DOC),the relative intensities of C2,C3,and black carbon-like compounds are all negatively correlated with salinity,indicating that there is a dilution effect of terrestrial signals by seawater in Xiangshan *** differences in light penetration ability of Xiangshan Bay cause different degrees of photo-degradation,which may play an important role in the transformation of organic matter in Xiangshan *** weak correlation between the C1 fluorescent component and salinity indicates that autochthonous sources cannot dominate the protein-like FDOM in the Xiangshan Bay drainage *** sources(such as anthropogenic inputs and release of pore water)also affect the distribution of the protein-like fluorescent component under eutrophication *** relative proportion of the protein-like fluorescent component in Xiangshan Bay is on a medium level in China and anthropogenic inputs may be a significant source of DOM in coastal bays.

关键词： Xiangshan Bay Dissolved organic matter Optical properties molecular composition Transporting and processing

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Mechanism investigation of steam flooding heavy oil by comprehensive molecular characterization

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Petroleum Science 2023年第4期20卷 2554-2563页

作者： Bo Zhang Chun-Ming Xu Zhe-Yu Liu Qing-Hui Zhao Hai-Qing Cheng Yi-Qiang Li Quan Shi State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing102249China College of Petroleum Engineering China University of PetroleumBeijing102249China Research Institute of Exploration and Development Liaohe Oilfield CompanyPetroChinaPanjinLiaoning124010China

Steam flooding is a widely used technique to enhance oil recovery of heavy *** viscosity reduction and distillation effect are considered as two main displacement mechanisms in steam flooding ***,the molecular composition understanding and contribution for oil production are still *** this study,the composition analysis of the heavy oil was investigated in the core scale steam flooding process with the temperature from 120 to 280℃.The crude oil,produced oils and residual oils were characterized comprehensively by gas chromatography and high-resolution mass *** is found that steam flooding preferentially extracts aromatics and remains more resins in the residual *** reduction is the dominant mechanism when steam is injected at a low *** molecular heteroatoms with high carbon number and high double bond equivalent(DBE)are eluted into the produced oil,while compounds with low carbon number and low DBE are remained in the residual *** the steam temperature rises,the increased distillation effect results in the extraction of light hydrocarbons from the residual oil to the produced *** small heteroatoms with low carbon number and low DBE enter into the produced oil,especially in the none water cut *** compositional difference of produced oils is characterized in DBE versus carbon number distribution of the N and O containing compound *** work uses a variety of composition analysis methods to clarify the steam flooding mechanism and provides a novel understanding of steam flooding mechanisms with various temperatures and production stages from the molecular perspective.

关键词： Steam flooding mechanism molecular composition High-resolution mass spectrometry Heavy oil Enhance oil recovery

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Application of Fourier transform ion cyclotron resonance mass spectrometry in molecular characterization of dissolved organic matter

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Science China Earth Sciences 2022年第12期65卷 2219-2236页

作者： Chen HE Ding HE Chunmao CHEN Quan SHI State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing 102249China Department of Ocean Science and Hong Kong Branch of the Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou) The Hong Kong University of Science and TechnologyHong Kong 999077China

Dissolved organic matter(DOM)plays an important role in the global carbon cycle,and an in-depth analysis of its chemical composition is fundamental to the study of its environmental and biogeochemical behavior and *** is a complex mixture of organic substances,and determining its molecular composition is a long-standing challenge in the field of analytical *** development and application of Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR MS)has enabled the identification of the chemical composition of DOM at the molecular *** paper summarizes progress made in the molecular characterization of DOM based on the FT-ICR MS technique,including DOM sample pretreatment methods,mass spectrometry ionization techniques,data acquisition,data processing and presentation,and molecular structure *** on the work done by the instrument at the State Key Laboratory of Heavy Oil Processing in the China University of Petroleum,Beijing,we introduce applications of FT-ICR MS in the fields of earth science,environmental science and engineering,and look ahead to further research directions in the future.

关键词： Dissolved organic matter FT-ICR MS molecular composition Recalcitrant dissolved organic matter High resolution mass spectrometry

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