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At least 433 records · Page 24

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DOE OSTI2017

Effect of autohydrolysis pretreatment on biomass structure and the resulting bio-oil from a pyrolysis process

Pyrolysis is a promising method for converting biomass to biofuels. However, some of pyrolysis oil's physiochemical properties still limit its commercial applications. Here, the autohydrolysis pretreatment at 175 ± 3 °C for 40 min was conducted to improve the resulting pine pyrolysis oil’s properties as a fuel. During autohydrolysis, deacetylation and decomposition of hemicellulose was observed by ion-exchange chromatography and Fourier transform infrared spectroscopy (FT-IR). Additionally, the cleavage of lignin ether bonds was clearly determined by 13 C cross-polarization/magic angle spinning (CP/MAS) nuclear magnetic resonance (NMR). Phosphitylation followed by 31 P NMR analysis of the heavy oils gave detailed structural information of the hydroxyl groups; the results revealed that autohydrolysis pretreatment led to a reduction of carboxyl acids in the heavy oils generated at all three pyrolysis temperatures (400, 500, and 600 °C). The 31 P NMR analysis also revealed that autohydrolysis pretreatment led to a reduction of condensed phenolic hydroxyl groups in the heavy oils produced at 600 °C. 1 H- 13 C heteronuclear single-quantum correlation (HSQC) NMR analysis showed that at a pyrolysis temperature of 600 °C, the pretreated pine produced lower methoxy group constituents. In both 31 P and HSQC NMR results indicated that autohydrolysis pretreatment increased levoglucosan yields in the bio-oils.

09 BIOMASS FUELS↗

DOE OSTI2016

Altering wettability to recover more oil from tight formations

We describe here a method for chemically modifying fracturing fluids and overflushes to chemically increase oil recovery from tight formations. Oil wetting of tight formations is usually controlled by adhesion to illite, kerogen, or both; adhesion to carbonate minerals may also play a role. Oil-illite adhesion is sensitive to salinity, dissolved divalent cation content, and pH. We measure oil-rock adhesion with middle Bakken formation oil and core to verify a surface complexation model of reservoir wettability. The agreement between the model and experiments suggests that wettability trends in tight formations can be quantitatively predicted and that fracturing fluid and overflush compositions can be individually tailored to increase oil recovery.

04 OIL SHALES AND TAR SANDS↗

DOE OSTI2015

Characterization of raw and burnt oil shale from Dotternhausen: Petrographical and mineralogical evolution with temperature

The Toarcian Posidonia shale from Dotternhausen, Germany, is quarried and burnt in a fluidized bed reactor to produce electricity. The combustion residue, namely burnt oil shale (BOS), is used in the adjacent cement work as an additive in blended cements. The starting material is a typical laminated oil shale with an organic matter content ranging from 6 to 18%. Mineral matter consists principally of quartz, feldspar, pyrite and clays. After calcination in the range, the resulting product, burnt oil shale, keeps the macroscopic layered texture however with different mineralogy (anhydrite, lime, iron oxides) and the formation of an amorphous phase. This one, studied under STEM, reveals a typical texture of incipient partial melting due to a long retention time (ca. 30 min) and quenching. An in-situ high temperature X-ray diffraction (HTXRD) allowed studying precisely the mineralogical changes associated with the temperature increase. - Highlights: • We present oil shale/burnt oil shale characterization. • The Posidonia Shale is burnt in a fluidized bed. • Mineralogical evolution with temperature is complex. • The burnt oil shale is used in composite cements.

36 MATERIALS SCIENCE↗

DOE OSTI2019

A comprehensive state-of-technology review for upgrading bio-oil to renewable or blended hydrocarbon fuels

Bioenergy sources are being advanced as a meaningful environmental solution and a substitute for conventional energy sources. Bioenergy from biomass feedstocks currently comprises the largest portion of renewables in the United States. Thus, more effective process-level solutions can result in scaling-up biomass-derived energy production (e.g., biofuels). Pyrolysis, a thermochemical conversion technology, offers a commercially viable pathway to produce bio-oil from a wide range of biomass feedstocks (e.g., algae and terrestrial). Bio-oil requires further upgrading for producing final bio-products (e.g., transportation fuels and biochemicals). This article focuses on upgrading bio-oil to transportation fuels (liquid hydrocarbons), highlights the critical challenges of existing upgrading technologies, and identifies the potential research directions to meet the market needs. A comprehensive overview and classification of bio-oil upgrading pathways and their competencies are presented through both comparative and systematic literature reviews. It is concluded that the biofuel production cost is highly dependent on post-conversion pathways, particularly their hydrogenation and deoxygenation capacity. Thermochemical treatments are effective, but less cost-competitive due to the intensive process requirements (e.g., heat or pressure). Physicochemical treatments are less effective, however, they operate under mild process conditions and could be integrated with other treatments. Biochemical treatments are inadequate as a standalone process for upgrading bio-oil. It is further concluded that the electrochemical approach can be effective due to the retention of hydrogen from bio-oil water content during deoxygenation.

09 BIOMASS FUELS↗

DOE OSTI2024

Proof-of-concept chemometric approach for environmental forensic sourcing of crude oil samples using SPME-GC-MS

Environmental exposure to crude oil through seepage and spillage poses risks to the immediate environment and the broader ecosystem as areas along the oil distribution path are affected by the influx of crude petroleum as well as the environmental, economic, and civil unrest that accompanies it. There is a large financial burden associated with the lost resources, including the cost of rehabilitation, and the affected sources of revenue for communities affected by oil spills. As such, it is crucial to determine the responsible parties. This work outlines an environmental forensics approach to determining the source of an un-weathered crude oil sample. The researchers employed solid phase microextraction coupled with gas chromatography mass spectrometry (SPME-GC-MS) to capture and analyze the gaseous components emitted by crude oil samples sourced from five locations. Samples were analyzed using Spearman's rank correlation and 3D covariance analysis. Both chemometric approaches yielded optimal performance results with no misclassifications, true positive rate (TPR) = 100 % and false positive rate (FPR) = 0 %. The similarity metrics calculated by each test noted clear delineations between the values of same-source and differently sourced samples. The Spearman's rank correlation test and 3D covariance calculations both demonstrated the ability to correctly identify sample source origin in this dataset. Finally, the authors outline an approach to the future application of these tests and suggest their joint use in future crude oil sourcing endeavors.

3D covariance mapping↗

DOE OSTI2014

Quality improvement of pyrolysis oil from waste rubber by adding sawdust

Highlights: • Rubber-pyrolysis oil is difficult to be fuel due to high proportion of PAHs. • The efficiency of pyrolysis was increased as the percentage of sawdust increased. • The adding of sawdust improved pyrolysis oil quality by reducing the PAHs content. • Adding sawdust reduced nitrogen/sulfur in oil and was easier to convert to diesel. - Abstract: This work was aimed at improving the pyrolysis oil quality of waste rubber by adding larch sawdust. Using a 1 kg/h stainless pyrolysis reactor, the contents of sawdust in rubber were gradually increased from 0%, 50%, 100% and 200% (wt%) during the pyrolysis process. Using a thermo-gravimetric (TG) analyzer coupled with Fourier transform infrared (FTIR) analysis of evolving products (TG–FTIR), the weight loss characteristics of the heat under different mixtures of sawdust/rubber were observed. Using the pyrolysis–gas chromatography (GC)–mass spectrometry (Py–GC/MS), the vapors from the pyrolysis processes were collected and the compositions of the vapors were examined. During the pyrolysis process, the recovery of the pyrolysis gas and its composition were measured in-situ at a reaction temperature of 450 °C and a retaining time of 1.2 s. The results indicated that the efficiency of pyrolysis was increased and the residual carbon was reduced as the percentage of sawdust increased. The adding of sawdust significantly improved the pyrolysis oil quality by reducing the polycyclic aromatic hydrocarbons (PAHs) and nitrogen and sulfur compounds contents, resulting in an improvement in the combustion efficiency of the pyrolysis oil.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Determination of Carbonyl Groups in Pyrolysis Bio-oils Using Potentiometric Titration: Review and Comparison of Methods

Carbonyl compounds present in bio-oils are known to be responsible for bio-oil property changes upon storage and during upgrading. As such, carbonyl content has previously been used as a method of tracking bio-oil aging and condensation reactions with less variability than viscosity measurements. Given the importance of carbonyls in bio-oils, accurate analytical methods for their quantification are very important for the bio-oil community. Potentiometric titration methods based on carbonyl oximation have long been used for the determination of carbonyl content in pyrolysis bio-oils. Here in this study, we present a modification of the traditional carbonyl oximation procedures that results in less reaction time, smaller sample size, higher precision, and more accurate carbonyl determinations. Some compounds such as carbohydrates are not measured by the traditional method (modified Nicolaides method), resulting in low estimations of the carbonyl content. Furthermore, we have shown that reaction completion for the traditional method can take up to 300 hours. The new method presented here (the modified Faix method) reduces the reaction time to 2 hours, uses triethanolamine (TEA) in the place of pyridine, and requires a smaller sample size for the analysis. Carbonyl contents determined using this new method are consistently higher than when using the traditional titration methods.

09 BIOMASS FUELS↗

DOE OSTI2017

Compatibility Assessment of Fuel System Infrastructure Plastics with Bio-oil and Diesel Fuel

We report that bio-oil derived via fast pyrolysis is being developed as a renewable fuel option for petroleum distillates. The compatibility of neat bio-oil with 18 plastic types was evaluated using neat diesel fuel as the baseline. The plastic materials included polyphenylene sulfide (PPS), polyethylene terephthalate (PET), polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PVDF), polyoxymethylene (POM), POM copolymer, high density polyethylene (HDPE), polybutylene terephthalate (PBT), polypropylene (PP), polyethylene terephthalate glycol (PETG), polythiourea (PTU), four nylon grades, and four thermosetting resins. Specimens of each material were immersed in the test fuels for a period of 16 weeks to achieve full saturation. Except for PP and HDPE, the plastic materials underwent higher volume expansion in bio-oil than in the baseline diesel (which was negligible in most cases). This volume increase corresponds to the higher polarity of the bio-oil. PPS, PET, and PTFE were unaffected by bio-oil exposure, but modest swelling (between 2 and 5%) occurred for the two acetals (POM and POM copolymer), Nylon-12, PBT, PETG, and the four resin grades. More moderate swelling (8–15%) was noted for Nylon-6, Nylon-6/6, and Nylon-11, and excessive swell (>40%) occurred for PTU. The nonpolar nature of PP and HDPE matches that of diesel, leading to higher solubility (swell) in this fuel type. Finally, the relatively low volume expansion following exposure indicates that many of the existing infrastructure plastics (excluding PTU) should be suitable for use with bio-oil.

09 BIOMASS FUELS↗

DOE OSTI2020

Isotopic Studies for Tracking Biogenic Carbon during Co-processing of Biomass and Vacuum Gas Oil

Co-processing bio-oils with petroleum-derived feeds in the existing multitrillion dollar refining and distribution infrastructure is an attractive option for introducing renewable energy into the fuels marketplace. Considerable research on co-processing bio-oils and vacuum gas oil (VGO) in fluid catalytic cracking units (FCC) using equilibrium catalysts (E-Cats) demonstrated that biomass-derived molecules decreased activity of and increased carbon laydown on E-Cat. In this work, 13 C-labeled biomass was co-processed with VGO using either an E-Cat or a proprietary zeolite Johnson Matthey catalyst (CP758), which is optimzed for upgrading biomass vapors in a riser reactor, to evaluate the fate of biogenic carbon in FCC products. The results from both catalysts indicate that biogenic carbon was incorporated into alkenes and aromatic hydrocarbons. While no biogenic carbon was found in linear alkanes, it was observed in cycloalkanes during experiments with E-Cat but not with CP758. All produced CO2 was biogenic as was most of the carbon laydown on the catalysts. Several partially deoxygenated biomass compounds, such as alkylphenols and benzofurans, unexpectedly contained small amounts of carbon from VGO. Although this study was conducted with labeled biomass and not bio-oil, it provides insights to reaction mechanisms for co-processing bio-oil and VGO in an FCC, which is required to develop catalysts that efficiently convert bio-oil components during FCC co-processing. This work also demonstrates that comprehensive catalyst development utilizing both biomass- and fossil-derived feeds is required to maximize the incorporation of biogenic carbon into transportation fuels.

09 BIOMASS FUELS↗

DOE OSTI2015

Modeling the Kinetics of Deactivation of Catalysts during the Upgrading of Bio-Oil

The fouling of catalysts for the upgrading of bio-oils appears to be very different from the fouling of catalysts for the hydroprocessing of petroleum-derived streams. There are two reasons for the differences: a) bio-oil contains polarizable components and phases that can stabilize reaction intermediates exhibiting charge separation and b) bio-oil components contain functional groups that contain O, notably carbonyls (>C=O). Aldol condensation of carbonyls affords very different pathways for the production of oligomeric, refractory deposits than does dehydrogenation/polymerization of petroleum-derived hydrocarbons. Colloquially, we refer to the bio-oil derived deposits as “gunk” to discriminate them from coke, the carbonaceous deposits encountered in petroleum refining. Classical gelation, appears to be a suitable model for the “gunking” reaction. Our work has helped explain the temperature range at which bio-oil should be pre-processed (“stabilized”) to confer longer lifetimes on the catalysts used for more severe processing. Stochastic modeling (kinetic Monte Carlo simulations) appears suitable to capture the rates of oligomerization of bio-oil. This work was supported by the US Department of Energy, Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated for DOE by Battelle.

bio-oil upgrading↗

DOE OSTI2021

Controlling Bacterial Contamination During Fuel Ethanol Fermentation Using Thermochemically Depolymerized Lignin Bio-Oils

Lactic acid bacteria (LAB) contamination during fuel ethanol fermentation can lead to significant economic loses. To circumvent this, fuel ethanol plants add antibiotics prophylactically, but their overuse has resulted in the emergence of antibiotic-resistant LAB strains. Lignin is a sustainable biopolymer that can be found as a waste product from lignocellulosic biorefineries. Technical lignins and their smaller phenolic subunits have been shown to exhibit broad-spectrum antimicrobial properties, but there is a lack of demonstrations of lignin derivatives with highly selective properties in the literature. Here, corn stover lignin from a biorefinery was oxidatively depolymerized using an environmentally benign organic oxidant, peracetic acid, into a bio-oil that has selective antimicrobial properties against LAB and not yeasts. The resulting bio-oil demonstrated up to 90% inhibition of commercially sampled LAB (including antibiotic-resistant strains) at 4 mg ml-1 with no inhibition against an industrial yeast strain. These antimicrobial properties of the bio-oil are attributed to larger unidentified lignin oligomers, compared to monolignols, that have a membrane damaging mode of action. Using the bio-oil (4 mg ml-1) during simultaneous saccharification and fermentation (SSF) of raw corn starch showed no inhibition of enzymatic activity, and in LAB contaminated fermentations the bio-oil treatments showed an 8% increase in ethanol yields at higher bacterial contamination ratios (l : 100 yeast to LAB, CFU per ml). This study illustrates the efficacy of using lignin bio-oil as an antibiotic replacement during fuel ethanol fermentation and demonstrates the highly selective antimicrobial properties of lignin oligomers, which creates a viable lignin valorization strategy for biorefineries.

bio-oil↗

DOE OSTI2015

Space charge inhibition effect of nano-Fe{sub 3}O{sub 4} on improvement of impulse breakdown voltage of transformer oil based on improved Kerr optic measurements

Transformer oil-based nanofluids (NFs) with 0.03 g/L Fe{sub 3}O{sub 4} nanoparticle content exhibit 11.2% higher positive impulse breakdown voltage levels than pure transformer oils. To study the effects of the Fe{sub 3}O{sub 4} nanoparticles on the space charge in transformer oil and to explain why the nano-modified transformer oil exhibits improved impulse breakdown voltage characteristics, the traditional Kerr electro-optic field mapping technique is improved by increasing the length of the parallel-plate electrodes and by using a photodetector array as a high light sensitivity device. The space charge distributions of pure transformer oil and of NFs containing Fe{sub 3}O{sub 4} nanoparticles can be measured using the improved Kerr electro-optic field mapping technique. Test results indicate a significant reduction in space charge density in the transformer oil-based NFs with the Fe{sub 3}O{sub 4} nanoparticles. The fast electrons are captured by the nanoparticles and are converted into slow-charged particles in the NFs, which then reduce the space charge density and result in a more uniform electric field distribution. Streamer propagation in the NFs is also obstructed, and the breakdown strengths of the NFs under impulse voltage conditions are also improved.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Properties of bio-oil generated by a pyrolysis of forest cedar residuals with the movable Auger-type reactor

Our research project has developed the new movable reactor for bio-oil production in 2013 on the basis of Auger-type system. This package would be a great impact due to the concept of local production for local consumption in the hilly and mountainous area in not only Japan but also in the world. Herein, we would like to report the properties of the bio-oil generated by the developing Auger-type movable reactor. The synthesized bio-oil possessed C: 46.2 wt%, H: 6.5 wt%, N: wt%, S: <0.1 wt%, O: 46.8 wt% and H{sub 2}O: 18.4 wt%, and served a good calorific value of 18.1 MJ/kg. The spectroscopic and mass analyses such as FT-IR, GC-MS, {sup 13}C-NMR and FT-ICR MS supported that the bio-oil was composed by the fine mixtures of methoxy phenols and variety of alcohol or carboxylic acid functional groups. Thus, it is suggested that the bio-oil generated by the new movable Auger-type reactor has a significant potential as well as the existing bio-oil reported previously.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Dielectric, ferroelectric, and thermodynamic properties of silicone oil modified PVDF films for energy storage application

Silicone oil modified poly(vinylidene fluoride-co-hexafluoropropylene) (P(VDF-HFP)) films were fabricated by the blending, casting, and hot-molding methods. The dielectric constant was increased for the 7.4 wt. % and 17.0 wt. % silicone oil modified P(VDF-HFP) films, while the dielectric loss for all blend films are decreased. D-E loops of 7.4 wt. % and 17.0 wt. % silicone oil modified P(VDF-HFP) films become slimmer than the pristine P(VDF-HFP) films. The maximum discharged energy density of 10.3 J/cm{sup 3} was obtained in 7.4 wt. % silicone oil modified P(VDF-HFP) films at the external electric field of 398 kV/mm. The Gibbs energy, miscibility, and phase behavior of binary mixture of P(VDF-HFP) silicone oil were investigated using molecular simulations and the extended Flory–Huggins model revealing favorable interactions and compatibility between P(VDF-HFP) and silicone oil.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2017

Simulation of Deepwater Horizon oil plume reveals substrate specialization within a complex community of hydrocarbon degraders

The Deepwater Horizon (DWH) accident released an estimated 4.1 million barrels of oil and 10 1 0 mol of natural gas into the Gulf of Mexico, forming deep-sea plumes of dispersed oil droplets and dissolved gases that were largely degraded by bacteria. During the course of this 3-mo disaster a series of different bacterial taxa were enriched in succession within deep plumes, but the metabolic capabilities of the different populations that controlled degradation rates of crude oil components are poorly understood. We experimentally reproduced dispersed plumes of fine oil droplets in Gulf of Mexico seawater and successfully replicated the enrichment and succession of the principal oil-degrading bacteria observed during the DWH event. We recovered near-complete genomes, whose phylogeny matched those of the principal biodegrading taxa observed in the field, including the DWH Oceanospirillales (now identified as a Bermanella species), multiple species of Colwellia, Cycloclasticus, and other members of Gammaproteobacteria, Flavobacteria, and Rhodobacteria. Metabolic pathway analysis, combined with hydrocarbon compositional analysis and species abundance data, revealed substrate specialization that explained the successional pattern of oil-degrading bacteria. The fastest-growing bacteria used short-chain alkanes. The analyses also uncovered potential cooperative and competitive relationships, even among close relatives. We conclude that patterns of microbial succession following deep ocean hydrocarbon blowouts are predictable and primarily driven by the availability of liquid petroleum hydrocarbons rather than natural gases.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Metabolic capability and in situ activity of microorganisms in an oil reservoir

Background: Microorganisms have long been associated with oxic and anoxic degradation of hydrocarbons in oil reservoirs and oil production facilities. While we can readily determine the abundance of microorganisms in the reservoir and study their activity in the laboratory, it has been challenging to resolve what microbes are actively participating in crude oil degradation in situ and to gain insight into what metabolic pathways they deploy. Results: Here, we describe the metabolic potential and in situ activity of microbial communities obtained from the Jiangsu Oil Reservoir (China) by an integrated metagenomics and metatranscriptomics approach. Almost complete genome sequences obtained by differential binning highlight the distinct capability of different community members to degrade hydrocarbons under oxic or anoxic condition. Transcriptomic data delineate active members of the community and give insights that Acinetobacter species completely oxidize alkanes into carbon dioxide with the involvement of oxygen, and Archaeoglobus species mainly ferment alkanes to generate acetate which could be consumed by Methanosaeta species. Furthermore, nutritional requirements based on amino acid and vitamin auxotrophies suggest a complex network of interactions and dependencies among active community members that go beyond classical syntrophic exchanges; this network defines community composition and microbial ecology in oil reservoirs undergoing secondary recovery. Conclusion: Our data expand current knowledge of the metabolic potential and role in hydrocarbon metabolism of individual members of thermophilic microbial communities from an oil reservoir. The study also reveals potential metabolic exchanges based on vitamin and amino acid auxotrophies indicating the presence of complex network of interactions between microbial taxa within the community.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Hydrogenation of Pyrolysis Oil from Loblolly Pine Residue

Loblolly pine residue prepared with and without zeolite ZSM-5 was pyrolyzed at 60°C and the pyrolysis oil was hydrogenated using formic acid as a hydrogen source, in the presence of a Ru/activated carbon catalyst. As indicated by the pyrolysis yield, addition of the zeolite ZSM-5 increased the yield of light oil but decreased the yield of heavy oil. The pyrolysis oils were analyzed by 13 C, 31 P, 19 F, and heteronuclear single quantum coherence or heteronuclear single quantum correlation nuclear magnetic resonance (HSQC-NMR), demonstrating that the zeolite ZSM-5 can efficiently induce decarboxylation reactions and decrease the content of aliphatic hydroxyl groups in the heavy oil by 57%. After hydrogenation of the pyrolysis oil, the aromatic carbon content decreased by 78%, with a significant increase in the aliphatic carbon content.

hydrogenation↗

DOE OSTI2022

Offshore Oil and Gas Infrastructure Reuse for CCS: Opportunities and Challenges in the U.S. Gulf of Mexico

The United States Gulf of Mexico has historically been a significant oil and gas producing region and continues to produce hydrocarbons today. As such, significant investments have been made to install oil and gas infrastructure such as pipelines, platforms, and wells. As these assets reach the end of their useful life or production associated with the assets is curtailed, the assets become a liability for both the owner/operators and the U.S. and state governments responsible for regulating the assets. There are costs and risks associated with safely decommissioning the assets, and in some cases, the assets may be abandoned (e.g., the owner is no longer a going concern). In parallel, carbon capture and storage (CCS) technology has developed in the United States and interest and incentives for CCS projects have accelerated in recent years, with many public announcements of CCS projects in development in the U.S. Gulf of Mexico region. The region is particularly well-suited to CCS due to the high density of industry on the coastline (i.e., CO 2 sources) and favorable geology in the near-offshore region. CCS also requires the use of many of the same assets required for oil and gas production (pipelines, platforms, wells) and the oil and gas industry has direct experience with CO 2 transport and injection (i.e., EOR). Therefore, the combination of existing infrastructure in close proximity to potential CCS project sites appears to provide a potential “win-win” solution for re-use of existing oil and gas assets. This paper presents a high-level evaluation of oil and gas infrastructure in the Gulf of Mexico with the goals of identifying the scale of the opportunity (e.g., how much existing infrastructure is realistically re-usable), identifying gaps in knowledge/policy/information required to evaluate existing infrastructure for re-use, and proposing key actions that could be pursued to further the assessment of existing infrastructure re-use for CCS.

Infrastructure, reuse, re-purpose, oil and gas, pi↗