Microwave-Fluidized Catalytic Reactor for the Direct Conversion of Methane to Higher Hydrocarbons (Final Report)
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03 NATURAL GAS↗
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Phase I Final Technical Report Award Number: DE-SC0017227 Microwave-Fluidized Catalytic Reactor for the Direct Conversion of Methane to Higher Hydrocarbons
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03 NATURAL GAS↗
Nanowire-based hydrodesulfurization catalysts for hydrocarbon fuels
The present development is a metal particle coated nanowire catalyst for use in the hydrodesulfurization of fuels and a process for the production of the catalyst. The catalyst comprises titanium(IV) oxide nanowires wherein the nanowires are produced by exposure of a TiO2—KOH paste to microwave radiation. Metal particles selected from the group consisting of molybdenum, nickel, cobalt, tungsten, or a combination thereof, are impregnated on the metal oxide nanowire surface. The metal impregnated nanowires are sulfided to produce catalytically-active metal particles on the surface of the nanowires The catalysts of the present invention are intended for use in the removal of thiophenic sulfur from liquid fuels through a hydrodesulfurization (HDS) process in a fixed bed reactor. The presence of nanowires improves the HDS activity and reduces the sintering effect, therefore, the sulfur removal efficiency increases.
Sunkara, Mahendra Kumar↗
Turbulent transport and reactions of plant-emitted hydrocarbons in an Amazonian rain forest
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54 ENVIRONMENTAL SCIENCES↗
Nanowire-based hydrodesulfurization catalysts for hydrocarbon fuels
The present development is a metal particle coated nanowire catalyst for use in the hydrodesulfurization of fuels and a process for the production of the catalyst. The catalyst comprises titanium(IV) oxide nanowires wherein the nanowires are produced by exposure of a TiO2—KOH paste to microwave radiation. Metal particles selected from the group consisting of molybdenum, nickel, cobalt, tungsten, or a combination thereof, are impregnated on the metal oxide nanowire surface. The metal impregnated nanowires are sulfided to produce catalytically-active metal particles on the surface of the nanowires The catalysts of the present invention are intended for use in the removal of thiophenic sulfur from liquid fuels through a hydrodesulfurization (HDS) process in a fixed bed reactor. The presence of nanowires improves the HDS activity and reduces the sintering effect, therefore, the sulfur removal efficiency increases.
Sunkara, Mahendra K.↗
Simultaneous measurement of visible energy and momentum transfer in anti-electron neutrino interactions on hydrocarbon
Precise knowledge of neutrino interaction cross sections is required for current and future accelerator-based neutrino oscillation experiments. Precision neutrino oscillation measurements require inference of the neutrino energy and flavor from the visible particles in the neutrino interaction in the detector. This inference is different for the true neutrino flavors measured, electron and muon neutrinos, and can be studied by observation of neutrino interactions in an experiment’s near detector. However, anti-electron neutrinos make up only a few percent of an anti-muon neutrino beam and pose a challenge in making cross section measurements and predictions. The reported measurements were made using data from MINERvA, a neutrino-nucleus scattering experiment, with an anti-neutrino beam configuration of mean energy ~ 6 GeV. This thesis provides two double-differential cross sections of anti-electron neutrino inclusive charged-current reactions using the kinematics of visible energy, three-momentum transfer, and transverse momentum. The analysis is carried out at low three-momentum transfer, making it sensitive to regions with multi-nucleon effects.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
CHARGED-CURRENT DOUBLE-DIFFERENTIAL CROSS SECTION MEASUREMENT OF ELECTRON NEUTRINOS IN LOW RECOIL REGION ON HYDROCARBON AT ∼7 GEV
Measuring neutrino mixing angles, especially the CP violation phase and mass hierarchy, is one of the priorities of the neutrino community and long baseline neutrino oscillation programs, such as T2K and NOvA, provided the most precise measurements to date. One of the dominating uncertainties of the measurements is the neutrino interaction model due to the difficulty of modeling the nuclear effects from first principles. As a result, neutrino scattering experiments such as MINERvA were conducted to provide data as input to reduce this uncertainty. This thesis presents a charged-current double-differential cross section measurement of electron neutrinos using the MINERvA detector in terms of available energy (a proxy of energy transfer), three-momentum transfer, and/or transverse momentum of the final state electron. This measurement focuses on the transition region between quasi-elastic and resonance processes, where the multi-nucleon knockout process dominates. The result is compared to a modified GENIE model and similar measurements using muon neutrino samples. In addition, this measurement reproduces the photon-like excess seen by previous MINERvA electron neutrino measurements.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Thermally stable hydrocarbon-based anion exchange membrane and ionomers
An anion exchange membrane is composed of a copolymer of 1,1-diphenylethylene and one or more styrene monomers, such as 4-tert-butylstyrene. The copolymer includes a backbone substituted with a plurality of ionic groups coupled to phenyl groups on the backbone via hydrocarbyl tethers between about 1 and about 7 carbons in length. High-temperature conditions enabled by these copolymers enhance conductivity performance, making them particularly suitable for use in anion exchange membranes in fuel cells, electrolyzers employing hydrogen, ion separations, etc. The properties of the membranes can be tuned via the degree of functionalization of the phenyl groups and selection of the functional groups, such as quaternary ammonium groups. Several processes can be used to incorporate the desired ionic functional groups into the polymers, such as chloromethylation, radical bromination, Friedel-Crafts acylation and alkylation, sulfonation followed by amination, or combinations thereof.
Lee, Sangwoo↗
Transfer hydrogenation of heavy hydrocarbons with hydrogen-donor solvents
Processes for converting the coal-derived heavy-oil fraction of syncrude to polyols are described. The processes involve mixing a feed stream comprising the coal-derived heavy-oil fraction with an alcohol and aqueous sulfuric acid, heating the mixture, reacting the coal-derived heavy-oil fraction with ozone, and reacting the ozonated heavy-oil fraction with glycerin to form the polyol. In some cases, the ozonated heavy-oil fraction can be neutralized before reacting the ozonated heavy-oil fraction with the glycerin.
Chauhan, Satya P.↗
Internal combustion engine as a chemical reactor to produce synthesis gas from hydrocarbon feeds
An internal combustion engine is operated at fuel-rich conditions by adjusting one or more operating parameters such as, for example, a throttle, an ignition timing, a load coupled to the engine, a fuel pressure, power to a supercharger, and power to a preheater to maintain a specified engine speed and a temperature of an exhaust gas. Operating the engine under these conditions allows the engine to function as a reformer producing a synthesis gas comprising hydrogen and carbon monoxide.
Carpenter, III, John Reeves↗
Method for optimization of huff-n-puff gas injection in hydrocarbon reservoirs
Methods for optimization of liquid oil production by huff-n-puff in shale reservoirs to achieve an improved (and optimal) oil recovery factor. The process determines and utilizes the optimum huff and puff times, number of cycles and soaking time under practical operation and reservoir conditions. The huff time in the process is a period so long that the pressure near the wellbore reaches the set maximum injection pressure during the huff period. The puff time in the process is the time required for the pressure near the wellbore to reach the set minimum production pressure during the puff period. Soaking is typically not necessary during the huff-n-puff gas injection in shale oil reservoirs. The number of huff-n-puff cycles is determinable by the time in which the economic rate cut-off is reached.
Sheng, James J.↗
Hydrocarbon polymers containing ammonium functionality
Described herein are cationic polymers having a plurality of quaternary amino groups, methods of making such polymers, and uses of such polymers as ion exchange membranes in electrochemical devices.
Laskowski, Carl A.↗
Highly Conductive Hydrocarbon Membranes for Fuel Cells and Electrolyzers
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08 HYDROGEN↗
Thermally stable hydrocarbon-based anion exchange membrane and ionomers
An anion exchange membrane is composed of a copolymer of 1,1-diphenylethylene and one or more styrene monomers, such as 4-tert-butylstyrene. The copolymer includes a backbone substituted with a plurality of ionic groups coupled to phenyl groups on the backbone via hydrocarbyl tethers between about 1 and about 7 carbons in length. High-temperature conditions enabled by these copolymers enhance conductivity performance, making them particularly suitable for use in anion exchange membranes in fuel cells, electrolyzers employing hydrogen, ion separations, etc. The properties of the membranes can be tuned via the degree of functionalization of the phenyl groups and selection of the functional groups, such as quaternary ammonium groups. Several processes can be used to incorporate the desired ionic functional groups into the polymers, such as chloromethylation, radical bromination, Friedel-Crafts acylation and alkylation, sulfonation followed by amination, or combinations thereof.
Lee, Sangwoo↗
Comparisons of triple-differential cross sections for quasielastic-like $ν_μ$-hydrocarbon interactions using $\langle E_ν\rangle \sim$ 3~GeV versus $\sim$ 6~GeV beams in MINERvA
Neutrino charged-current quasielastic-like scattering, a reaction category extensively used in neutrino oscillation measurements, receives contributions from single nucleon knockout processes, multinucleon processes, and inelastic scattering with subsequent rescattering or absorption in the nucleus to produce only nucleons in the final state. In this article, comparisons are presented of the same measurement in two different wideband neutrino beams: one beam peaks near 3 GeV with few neutrinos above 6 GeV; the other peaks near 6 GeV with few neutrinos above 10 GeV. Comparisons of differential cross sections in muon and proton kinematics for these two exposures probe deviations from free-neutron scattering that arise from the processes involving the nuclear medium, and provide a test of neutrino interaction models used to infer neutrino energies in oscillation experiments. Discrepancies are observed between the data and predictions that point to overestimates of the final state interactions of both protons and charged pions in quasielastic-like events.
Ruterbories, D. [Rochester U.]↗
Effect of Composition and Pressure on Diamond Formation Timescales from Hydrocarbon Demixing at Icy Planetary Interior Conditions
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FROST, MUNGO [SLAC National Accelerator Laboratory↗
Towards cost-competitive middle distillate fuels from ethanol within a market-flexible C2 platform-based biorefinery concept
Ethanol to middle distillates (ETMD) is a promising pathway to produce sustainable liquid fuels to decarbonize the hard-to-electrify transportation sectors due to (1) the abundant sugar/starch and lignocellulosic biomass, (2) the existing deployment scale of fuel ethanol production (similar to 29 billion gallons per year globally), and (3) emerging opportunities in C2+ alcohol synthesis from CO2. Here we report a conceptual market-responsive biorefinery centered around a new ETMD pathway based on one-step ethanol to butene-rich olefins (ETO) over a Cu-Zn-Y/Beta catalyst. Specifically, this ethanol conversion pathway comprises one-step ETO, oligomerization, and hydrotreating. This ETO is distinct from that in the conventional ethanol-to-jet process which is based on two-step ethanol to ethylene and ethylene oligomerization to butenes. Butene-rich olefins can be shifted to butadiene-rich products by simply changing the reaction atmosphere from hydrogen to inert gas over the same ETO catalyst. Leveraging the experimental results, baseline techno-economic analysis (TEA) and sensitivity analysis indicate that the ethanol conversion cost is $0.60 per gallon gasoline equivalent (GGE), with opportunities for further cost reduction via improving the liquid hydrocarbon yield and space velocities, and process optimization on balancing dewatering of ethanol feed prior to the ETO step. The minimum fuel selling price (MFSP) of liquid hydrocarbons derived from corn starch ethanol with butadiene as coproduct is $1.64 per GGE, in the range that is cost competitive with petroleum kerosene-type jet fuel. Projected MFSP for cellulosic ethanol (corn stover) derived hydrocarbons is below $3.00 per GGE and co-production of butadiene further reduces the MFSP to $1.70 per GGE. The Well-to-Wake life-cycle analysis indicates that 85% greenhouse gas emission reduction can be achieved when using corn stover compared to petroleum reference and the associated carbon credits will provide significant economic incentives to favor the cellulosic ethanol-derived hydrocarbon fuels. This study demonstrates a low-cost pathway to middle distillate fuels leveraging existing ethanol infrastructure, where catalysis innovation drives the reduction of process complexity and flexible coproduction of a value-added chemical product.
Zhang, Junyan↗
A Hybrid Pathway to Biojet Fuel via 2,3-Butanediol
Production of biomass-derived sustainable alternative jet fuels (SAJF) has been considered as an important approach to decarbonize the aviation industry but still possesses various challenges in technology advancement, particularly in achieving high carbon efficiency. Here we report a hybrid pathway to SAJF from 2,3-butanediol (2,3-BDO), integrating biologically converting biomass to 2,3-BDO with catalytically upgrading of 2,3-BDO to jet-range hydrocarbons. This pathway is demonstrated to have a high carbon recovery to liquid hydrocarbons from corn stover (25–28%) (74–82% of the theoretical maximum efficiency). The catalytic conversion steps involve 2,3-BDO to C3+ olefins, oligomerization, and hydrogenation where the first two steps are the focus of this study. Under optimum reaction conditions (523 K, 115 kPa, 1.0 h-1 weight hourly space velocity), 2,3-BDO conversion and C3+ olefin selectivity are >97% and 94–98% during 40 h time on stream, respectively. To demonstrate the adaptability of this technology with bio-derived 2,3-BDO, we also investigated the impact of water and other organic coproducts (acetoin and acetic acid) inherited from the fermentation broth on the catalyst performance and product selectivities. We have shown that the catalyst can handle a significant amount of water in the liquid feed (40 wt% water/60 wt% 2,3-BDO) and maintain catalyst stability for ~40 h. Acetoin can be converted to similar C3+ olefins as 2,3-BDO with complete conversion of acetoin. Co-feeding 10 wt% acetoin with 2,3-BDO is found to have no impact on 2,3-BDO conversion, C3+ olefin selectivity, and catalyst stability. The utilization of organic coproduct like acetoin can help to improve overall carbon conversion efficiency when using real biomass-derived 2,3-BDO. On the other hand, the presence of 10 wt% acetic acid is shown to drastically inhibit methyl ethyl ketone (MEK) hydrogenation and butene oligomerization as revealed by the increased MEK and butene selectivities, implying the importance of separating organic acids when feeding bio-derived 2,3-BDO. The formed C3–C6 olefins from 2,3-BDO are further oligomerized over Amberlyst-36 catalyst to longer-chain hydrocarbons with >70 wt% jet-range hydrocarbons including predominantly iso-olefins/iso-paraffins. The overall carbon efficiency for the jet-range hydrocarbons is 19–22%, exceeding most of the reported biojet pathways, which makes it a promising approach for SAJF production.
29 ENERGY PLANNING, POLICY, AND ECONOMY↗