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All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Cooling Strategies for Vane Leading Edges in a Syngas Environment Including Effects of Deposition and Turbulence

The Department of Energy has goals to move land based gas turbine systems to alternate fuels including coal derived synthetic gas and hydrogen. Coal is the most abundant energy resource in the US and in the world and it is economically advantageous to develop power systems which can use coal. Integrated gasification combined cycles are (IGCC) expected to allow the clean use of coal derived fuels while improving the ability to capture and sequester carbon dioxide. These cycles will need to maintain or increase turbine entry temperatures to develop competitive efficiencies. The use of coal derived syngas introduces a range of potential contaminants into the hot section of the gas turbine including sulfur, iron, calcium, and various alkali metals. Depending on the effectiveness of the gas clean up processes, there exists significant likelihood that the remaining materials will become molten in the combustion process and potentially deposit on downstream turbine surfaces. Past evidence suggests that deposition will be a strong function of increasing temperature. Currently, even with the best gas cleanup processes a small level of particulate matter in the syngas is expected. Consequently, particulate deposition is expected to be an important consideration in the design of turbine components. The leading edge region of first stage vanes most often have higher deposition rates than other areas due to strong fluid acceleration and streamline curvature in the vicinity of the surface. This region remains one of the most difficult areas in a turbine nozzle to cool due to high inlet temperatures and only a small pressure ratio for cooling. The leading edge of a vane often has relatively high heat transfer coefficients and is often cooled using showerhead film cooling arrays. The throat of the first stage nozzle is another area where deposition potentially has a strongly adverse effect on turbine performance as this region meters the turbine inlet flow. Based on roughness levels found on in service vanes (Bons, et al., 2001, up to 300 microns) flow blockage in first stage turbine nozzles can easily reach 1 to 2 percent in conventional turbines. Deposition levels in syngas fueled gas turbines are expected to be even more problematic. The likelihood of significant deposition to the leading edge of vanes in a syngas environment indicates the need to examine this effect on the leading edge cooling problem. It is critical to understand the influence of leading edge geometry and turbulence on deposition rates for both internally and showerhead cooled leading edge regions. The expected level of deposition in a vane stagnation region not only significantly changes the heat transfer problem but also suggests that cooling arrays may clog. Addressing the cooling issue suggests a need to better understand stagnation region heat transfer with realistic roughness as well as the other variables affecting transport near the leading edge. Also, the question of whether leading edge regions can be cooled internally with modern cooling approaches should also be raised, thus avoiding the clogging issue. Addressing deposition in the pressure side throat region of the nozzle is another critical issue for this environment. Issues such as examining the protective effect of slot and full coverage discrete-hole film cooling on limiting deposition as well as the influence of roughness and turbulence on effectiveness should be raised. The objective of this present study is to address these technical challenges to help enable the development of high efficiency syngas tolerant gas turbine engines.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2015

Low Cost High-H 2 Syngas Production for Power and Liquid Fuels

This report summarizes the technical progress made of the research project entitled “Low Cost High-H2 Syngas Production for Power and Liquid Fuels,” under DOE Contract No. DE-FE-0011958. The period of performance was October 1, 2013 through July 30, 2015. The overall objectives of this project was to determine the technical and economic feasibility of a systems approach for producing high hydrogen syngas from coal with the potential to reduce significantly the cost of producing power, chemical-grade hydrogen or liquid fuels, with carbon capture to reduce the environmental impact of gasification. The project encompasses several areas of study and the results are summarized here. (1) Experimental work to determine the technical feasibility of a novel hybrid polymer/metal H2-membrane to recover pure H2 from a coal-derived syngas was done. This task was not successful. Membranes were synthesized and show impermeability of any gases at required conditions. The cause of this impermeability was most likely due to the densification of the porous polymer membrane support made from polybenzimidazole (PBI) at test temperatures above 250 °C. (2) Bench-scale experimental work was performed to extend GTI's current database on the University of California Sulfur Recovery Process-High Pressure (UCSRP-HP) and recently renamed Sulfur Removal and Recovery (SR2) process for syngas cleanup including removal of sulfur and other trace contaminants, such as, chlorides and ammonia. The SR2 process tests show >90% H2S conversion with outlet H2S concentrations less than 4 ppmv, and 80-90% ammonia and chloride removal with high mass transfer rates. (3) Techno-economic analyses (TEA) were done for the production of electric power, chemical-grade hydrogen and diesel fuels, from a mixture of coal- plus natural gas-derived syngas using the Aerojet Rocketdyne (AR) Advanced Compact coal gasifier and a natural gas partial oxidation reactor (POX) with SR2 technology. Due to the unsuccessful experimental results with the hybrid polymer/metal H2 membrane, a conventional CO2 capture (single-stage Selexol) and hydrogen purification (PSA) technologies were used in the appropriate cases. In all cases, the integrated system of Advanced Compact coal gasifier, non-catalytic natural gas partial oxidation, and SR2 multicontaminant removal with state-of-the-art auxiliary system provided a 5-25% cost advantage over the base line plants using GEE coal gasifier with conventional Selexol/Claus sulfur removal and recovery. These plants also produce 18-30% less CO2 than with the conventional coal gasification plants.

08 HYDROGEN↗
DOE OSTI2017

Hybrid Molten Bed Gasifier for High Hydrogen Syngas Production

The techno-economic analyses of the hybrid molten bed gasification technology and laboratory testing of the HMB process were carried out in this project by the Gas Technology Institute and partner Nexant, Inc. under contract with the US Department of Energy’s National Energy Technology Laboratory. This report includes the results of two complete IGCC and Fischer-Tropsch TEA analyses comparing HMB gasification with the Shell slagging gasification process as a base case. Also included are the results of the laboratory simulation tests of the HMB process using Illinois #6 coal fed along with natural gas, two different syngases, and steam. Work in this 18-month project was carried out in three main Tasks. Task 2 was completed first and involved modeling, mass and energy balances, and gasification process design. The results of this work were provided to Nexant as input to the TEA IGCC and FT configurations studied in detail in Task 3. The results of Task 2 were also used to guide the design of the laboratory-scale testing of the HMB concept in the submerged combustion melting test facility in GTI’s industrial combustion laboratory. All project work was completed on time and budget. A project close-out meeting reviewing project results was conducted on April 1, 2015 at GTI in Des Plaines, IL. The hybrid molten bed gasification process techno-economic analyses found that the HMB process is both technically and economically attractive compared with the Shell entrained flow gasification process. In IGCC configuration, HMB gasification provides both efficiency and cost benefits. In Fischer-Tropsch configuration, HMB shows small benefits, primarily because even at current low natural gas prices, natural gas is more expensive than coal on an energy cost basis. HMB gasification was found in the TEA to improve the overall IGCC economics as compared to the coal only Shell gasification process. Operationally, the HMB process proved to be robust and easy to operate. The burner was stable over the full oxygen to fuel firing range (0.8 to 1.05 of fuel gas stoichiometry) and with all fuel gases (natural gas and two syngas compositions), with steam, and without steam. The lower Btu content of the syngases presented no combustion difficulties. The molten bed was stable throughout testing. The molten bed was easily established as a bed of molten glass. As the composition changed from glass cullet to cullet with slag, no instabilities were encountered. The bed temperature and product syngas temperature remained stable throughout testing, demonstrating that the bed serves as a good heat sink for the gasification process. Product syngas temperature measured above the bed was stable at ~1600ºF. Testing found that syngas quality measured as H 2 /CO ratio increased with decreasing oxygen to fuel gas stoichiometric ratio, higher steam to inlet carbon ratio, higher temperature, and syngas compared with natural gas. The highest H 2 /CO ratios achieved were in the range of 0.70 to 0.78. These values are well below the targets of 1.5 to 2.0 that were expected and were predicted by modeling. The team, however, is encouraged that the HMB process can and will achieve H 2 /CO ratios up to 2.0. Changes needed include direct injection of coal into the molten bed of slag to prevent coal particle bypass into the product gas stream, elevation of the molten bed temperature to approximately 2500ºF, and further decrease of the oxygen to fuel gas ratio to well below the 0.85 minimum ratio used in the testing in this project.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2021

Nano-Engineered Catalyst Supported on Ceramic Hollow Fibers for the Utilization of CO 2 in Dry Reforming to Produce Syngas

The objective of this project was to develop a novel catalytic reactor containing nano-engineered catalysts for the utilization of CO 2 (captured from coal-fired power plants and other CO 2 emitting sources) in dry methane reforming (DMR) (CO 2 + CH 4 → 2 H 2 + 2 CO) to produce synthesis gas (syngas). The technology aims to reduce CO2 emissions by developing beneficial uses for CO 2 from coal-fired power plants. It also offers an alternative to mitigate CO 2 emissions in areas where geologic storage may not be an optimal solution and/or utilization could significantly offset the costs of carbon capture and sequestration. The nano-engineered Ni-based catalyst was prepared by atomic layer deposition (ALD). The Ni particles were as small as ~2-4 nm. The nano-engineered catalyst showed CH 4 conversion >95%, H 2 /CO ratio in the range of 0.7-1.0, and CH 4 reforming rate as high as 2,500 L/h/gNi at 850 ºC and pressure of 15-25 psia. The Ni-based ALD catalyst also showed good stability in DMR reaction during a 200-h continuous operation at 850 °C. This is due to strong bonding between the nanoparticles and substrates since the Ni nanoparticles were chemically bonded to the substrate during the ALD process. The high thermal stability maintains the high dispersion of Ni nanoparticles, which can inhibit coke formation because their step edges are small enough to limit carbon nucleation and growth. Technoeconomic analysis (TEA) indicates the levelized cost of syngas (LCOS) is $172/ton with our technology, which is lower than the equivalent (molar) cost of hydrogen produced by steam methane reforming (SMR) or autothermal reforming (ATR). The major operating cost is natural gas feed and fuel, and the levelized cost is highly sensitive to the price of natural gas and relatively insensitive to the CAPEX. Revenues from syngas could have a significant impact on the net cost of electricity (COE), depending on the cost of natural gas and the selling price of syngas, estimated at $36 per MWh if the syngas were sold at $195 per ton. Following DOE NETL’s guidance, a lifecycle analysis (LCA) was conducted to compare with SMR. The functional unit for the basis of comparison was defined as 1kg carbon monoxide in the product stream. The global warming potential (GWP) of our process was found to be 40% lower than the state-of-the-art SMR process. The sensitivity analysis confirms the emissions are most sensitive to the natural gas fuel requirements to deliver heat to the process.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2019

Effects of organic silicon compounds on syngas auto-ignition behavior

Siloxanes are a significant impurity in syngas feedstocks and an important source of silicon in combustion synthesis applications. However, little is known regarding the fundamental combustion chemistry of siloxane compounds. The impact of two organic silicon species with different but related chemical structures, trimethylsilanol (TMSO) and hexamethyldisiloxane (HMDSO), on syngas auto-ignition behavior was investigated in this study using physical and computational experiments. A rapid compression facility (RCF) was used to create temperatures of 1010–1070 K and pressures of 8–10.3 atm for auto-ignition experiments. Experiments with trace concentrations of TMSO (100 ppm, mole basis) or HMDSO (100 ppm) were added to a surrogate syngas blend (CO and H 2 with a molar ratio of 2.34:1, air levels of dilution, with molar equivalence ratios of Φ = 0.1). The measured ignition delay times showed both siloxane species promote ignition behavior with TMSO yielding faster ignition delay times by approximately 37% and HMDSO yielding faster times by approximately 50% compared with the reference syngas mixture which contained no siloxanes. A computational study was conducted to interpret the results of the ignition experiments. Due to the fact that detailed chemistry does not exist for these organo-silicon compounds, the effects of the addition of CH 3 , H, and OH radicals to H 2 and CO mixtures were explored to simulate the potential rapid decomposition of the siloxanes in the H 2 and CO system. Addition of the radicals decreased the predicted ignition delay times when compared with the H 2 and CO mixture simulations without the radical species, but the simulations did not fully capture the behavior observed in the experiments, indicating the siloxane chemistry is more complex than providing a rapid source of radicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Process Intensification for Direct Conversion of Biomass-Based Syngas to High Octane Gasoline

The conversion of lignocellulosic-derived carbon sources via the creation of a CO2 rich syngas stream provides means to produce liquid hydrocarbon fuels, with advancements intended to create a cost-competitive method of sequential conversion via methanol and dimethyl ether intermediates. Previously developed methods with Cu/Beta zeolites enabled the conversion of dimethyl ether to linear and branched hydrocarbons, with high selectivities towards products with high-octane fuel properties. Through process intensification, use of a single reactor to convert syngas to methanol and DME, then further to hydrocarbons, allows for reduced capitol and operation cost for the same chemistries that typically use 3 reactors instead of one. Utilization of commercially available methanol synthesis catalyst (Megamax 800, Clariant, CZA) and methanol dehydration catalyst with the Cu/Beta catalyst allowed for conversion into hydrocarbon products in this single reactor set up. Reactor configuration with CZA and alumina catalysts mixed with or stacked in a bed physically above the Cu/Beta catalyst provided a system for the direct conversion of the syngas to hydrocarbons with improved yields and selectivities with higher net C1 conversions for stacked bed configurations. Through control of the process conditions, greater conversion of C1 oxygenate intermediates (i.e., methanol and dimethyl ether) was achieved with concomitant increase in selectivities towards gasoline and jet fuel range olefin and paraffin products. Lower hydrocarbon number products and less naphthenes were observed for the conversion of syngas compared to DME conversion on only the Cu/Beta system with prominent selectivities observed for C4, C5, and C7 hydrocarbons. The DME and methanol formation rates, with understanding of the equilibria for both processes, were determined as important factors to allow for improved performance of the Cu/Beta. Determination of the factors which allow for tuning of selectivities and yields created an intensified process which allows for a "market-responsive" biorefinery design, which can produce high octane gasoline or jet fuel range hydrocarbons to meet demands for a more sustainable route to liquid fuels.

BIOMASS FUELS↗
DOE OSTI2021

Kinetics of Direct Olefin Synthesis from Syngas over Mixed Beds of Zn–Zr Oxides and SAPO-34

A packed bed containing a physical mixture of both Zn–Zr mixed oxide catalyst and SAPO-34 converts syngas directly into a mixture of C 2 –C 5 olefins and paraffins. Specifically, the mixed oxide catalyst is responsible for intermediate oxygenate synthesis from syngas while the molecular sieve catalyzes olefin synthesis from the oxygenate intermediates. Kinetic measurements with cofed propylene over each catalyst independently confirm olefin hydrogenation activity over both components of the composite bed. The addition of either water or CO to the feed drops the activity of propylene hydrogenation over the Zn–Zr oxide. In sum, under reaction conditions of syngas feed and produced water, olefin hydrogenation predominantly occurs over the SAPO-34 catalyst, rather than over the catalyst responsible for hydrogenating CO into oxygenate intermediates. Here, a developed kinetic model consistent with this conclusion describes measurements at differing feed compositions, temperatures, space velocities, and bed catalyst mixing ratios. Technoeconomic analysis of the process indicates that the olefin-to-paraffin ratio is a key performance metric for commercial scale syngas conversion and highlights the importance of considering olefin hydrogenation rates over the molecular sieve component.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

CO Laser Absorption Measurements During Syngas Combustion at High Pressure

Abstract Syngas is a desirable fuel for combustion in the Allam-Fetvedt cycle, which involves combustion under supercritical-CO2 conditions. While some work has been conducted in collecting ignition delay times (IDT) at the extreme pressures required by these systems, significant model deficiencies remain. Additionally, considerable barriers in terms of nonideal gas dynamic effects have been shown for these experiments in shock tubes. Further investigation into the fundamental combustion kinetics of H2/CO/CO2 mixtures is required. Time-resolved speciation measurements for target species have been shown to better aid in improving the understanding of underlying chemical kinetics than global ignition delay time measurements. Therefore, laser absorption measurements of CO were measured behind reflected shock waves during combustion of syngas at 5 and 10 bar and temperatures between 1080 and 2100 K. The mixtures investigated utilized H2-to-CO ratios of 1:1 and 1:4, respectively, each at stoichiometric conditions, allowing for discussions of the effect of initial fuel composition. A ratio of fuel to CO2 of 1:2 was also utilized to represent commercially available syngas. The mixtures were diluted in helium and argon (20% He, 76.5% Ar) to minimize thermal effects and to expedite CO thermal relaxation during the experiment. The resulting CO time histories were then compared to modern chemical kinetics mechanisms, and disagreement is seen for this system, which is assumed to be fairly well known. This study elucidates particular chemistry that needs improvement in moving toward a better understanding of syngas combustion at elevated pressures.

Engineering↗
NASA NTRS1979

A study of industrial hydrogen and syngas supply systems

The potential and incentives required for supplying hydrogen and syngas feedstocks to the U.S. chemical industry from coal gasification systems were evaluated. Future hydrogen and syngas demand for chemical manufacture was estimated by geographic area and projected economics for hydrogen and syngas manufacture was estimated with geographic area of manufacture and plant size as parameters. Natural gas, oil and coal feedstocks were considered. Problem areas presently affecting the commercial feasibility of coal gasification discussed include the impact of potential process improvements, factors involved in financing coal gasification plants, regulatory barriers affecting coal gasification, coal mining/transportation, air quality regulations, and competitive feedstock pricing barriers. The potential for making coal gasification the least costly H2 and syngas supply option. Options to stimulate coal gasification system development are discussed.

Amos, W. J.↗
DOE OSTI2016

Catalysts for converting syngas into liquid hydrocarbons and methods thereof

The presently-disclosed subject matter includes methods for producing liquid hydrocarbons from syngas. In some embodiments the syngas is obtained from biomass and/or comprises a relatively high amount of nitrogen and/or carbon dioxide. In some embodiments the present methods can convert syngas into liquid hydrocarbons through a one-stage process. Also provided are catalysts for producing liquid hydrocarbons from syngas, wherein the catalysts include a base material, a transition metal, and a promoter. In some embodiments the base material includes a zeolite-iron material or a cobalt-molybdenum carbide material. In still further embodiments the promoter can include an alkali metal.

09 BIOMASS FUELS↗
DOE OSTI2019

Subtask 2.5 – Syngas Testing of NETL's Advanced Precombustion CO2 Capture Solvent

U.S. Department of Energy (DOE) National Energy Technology Laboratory (NETL) on-site researchers have been examining and developing a novel solvent for precombustion capture that has the potential for improved performance and lower costs compared to Selexol™ and Rectisol®. In Subtask 2.5, the Energy & Environmental Research Center (EERC) conducted actual comparison tests on actual coal-derived syngas of a PEGDME (polyethylene glycol dimethyl ether) Selexol-type solvent and three other solvents provided by NETL. One was a new hybrid PEG–PDMS (poly[dimethylsiloxane]) solvent engineered by NETL. In addition, two commercially available chemicals that are projected to have good CO2 capture abilities were also selected for testing on actual coal-derived syngas. These tests were conducted in the EERC high-pressure fluid-bed gasifier (HPFBG) system utilizing an existing gas-sweetening absorption system (GSAS) to test the solvents. The four solvents tested were Solvent 1 – AGR II from Coastal Chemical Co., LLC, NETL Solvent 2 – XG-3229 Bis(methoxytriethyleneoxypropyl)hexamethyltrisiloxane, as manufactured by Gelast, Inc.; Solvent 3 – CASSH-1 (diethyl sebacate), procured from Sigma Aldrich; and Solvent 4 – TBP (tributyl phosphate), purchased from ThermoFisher Scientific. The solvents were all tested at a consistent syngas flow and composition at approximately 50 bar to make direct comparisons easier; two solvent flow rates which would bracket 90% CO2 capture; and, temperatures of 10°, 25°, 40°, and 55°C to determine the effects of temperature on CO2 uptake and CO2 to H2 selectivity. Figure E-1 shows the results for CO2 uptake and selectivity for the various solvents. These data show that the CO2 uptake for the Selexol-type solvent for the PEG-PDMS-3 and CASHH-1 solvents at higher operating temperatures around 40°C was better than the Selexol-type solvent was able to achieve at the lower operating temperature of 10°C. Selectivity of CO2 over H2 was at least as good as Selexol for the PEG-PDMS-3 solvent and even better than Selexol for the CASSH-1 solvent. The TBP solvent also displayed good CO2 uptake; however, CO2/H2 selectivity was worse than for the Selexol-type solvent. Operation of precombustion CO2 solvents at temperatures above ambient can provide a 2% process efficiency improvement along with a significant capital cost reduction since refrigeration and solvent dehydration equipment is not required. The excellent results from these tests warrant further longer-duration testing with one or both superior NETL-provided solvents to determine if longer-term exposure to any coal-derived syngas trace species may have an adverse impact on solvent performance. This project was funded through the EERC–DOE Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FE0024233.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2026

Co‐Electrolysis of CO 2 and H 2 O to Syngas on Bimetallic Pd x Cu 1‐ x Catalysts for Tandem Thermochemical Conversion to Carbon Nanofibers

Electrification of chemical production using renewable energy and abundant feedstocks offers a promising pathway for decarbonizing the chemical industry. Current efforts on CO 2 valorization largely focus on making chemicals and fuels. Here, to help achieve net-negative emissions through long-term carbon storage, this study aims to develop efficient electrocatalysts for a tandem electrochemical-thermochemical process to convert CO 2 into carbon nanofibers (CNFs). CO 2 and water are first electrochemically reduced in a membrane electrode assembly (MEA) electrolyzer to produce syngas (CO + H 2 ), which is subsequently fed into a thermochemical packed bed reactor to facilitate CNF growth. This work systematically evaluated Pd x Cu 1-x bimetallic electrocatalysts to assess the effect of Pd–Cu alloying on enhancing syngas production while reducing Pd loading. Transmission electron microscopy and Raman spectroscopy confirmed the formation of high-purity, crystalline CNFs, regardless of the syngas composition from the MEA. In situ X-ray absorption spectroscopy and X-ray diffraction measurements revealed that increasing Cu content in the Pd x Cu 1-x alloy progressively inhibited palladium hydride formation, consistent with DFT calculations on the stability of Pd x Cu 1-x under reducing electrochemical potentials.

58 GEOSCIENCES↗
DOE OSTI2019

Directing Clostridium ljungdahlii fermentation products via hydrogen to carbon monoxide ratio in syngas

Clostridium ljungdahlii was grown on syngas of varying composition to investigate how syngas blends used in fermentation can be tailored toward desired product formation. Experiments were conducted with liquid batch cultures exposed to the same volume of gas with varying ratios of hydrogen to carbon monoxide (H 2 /CO). Formation of acetate was favored by higher concentrations of hydrogen in the headspace. The maximum acetate concentration of 35.21 +/- 0.84 mM was obtained using an H 2 /CO ratio of 2.0. Generation of more reduced metabolites was favored by greater carbon monoxide concentrations in the headspace. Maximum ethanol (7.53 +/- 0.58 mM) and 2,3-Butanediol (5.20 +/- 0.79 mM) concentrations were achieved under an H 2 /CO ratio of 0.5. Linear relationships were obtained in that describe the effect of the syngas H 2 /CO ratios on acetate, ethanol, and 2,3-BD formation, respectively.

09 BIOMASS FUELS↗
DOE OSTI2020

A new approach of reduction of carbon dioxide emission and optimal use of carbon and hydrogen content for the desired syngas production from coal

We report this research is designed to make progress in overcoming the challenges through the development of a two-stage coal processing. Specifically, a two-stage process was used to maximize the use of the carbon in coal or increase the carbon monoxide yield or lower carbon dioxide and methane yields. Carbon dioxide-char gasification in the absence of water can generate carbon monoxide with near-zero methane, which is desired to produce high-carbon and low-hydrogen chemicals such as oxalic acid through catalytic carbon monoxide coupling and hydrolysis. The technology is applicable to any coal, although Power River Basin (PRB) coal is used as an example feedstock in this research Also, the sodium-iron catalyst can accelerate not only the reaction kinetics in both stages but also increase the hydrogen/carbon monoxide ratio in the syngas produced in the second stage. In other words, the catalyst is a multifunctional agent, which can not only intensify the overall coal process efficiency but also improve the qualities of the desired syngas products and reduce carbon dioxide emission. Thus, In the 1st stage, the catalysts can significantly reduce the CO 2 -char gasification by as high as 75.00%. In the 2nd stage, the H 2 /CO ratio of ideal syngas is ~2:1 with near-0 CH 4 generation and the CH4 production can be reduced as high as 61.29% for the CO 2 –H 2 O-Char coal gasification. The activation energy for the 2nd stage is reduced by as high as 35.43% than that of raw coal without use Na–Fe catalyst. The overall carbon footprint reduction for the study is reduced by 87.33% in the 1st stage and 96.77% compared to the direct coal combustion.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2020

Intensified Co-electrolysis Process for Syngas Production from Captured CO 2

CO 2 reduction to syngas provides a way of ameliorating carbon footprint and storing energy in high-energy-density and versatile feedstock. This current work explores the isothermal integration of CO2 capture with an intensified unit operation for the reduction of CO2 and capture media regeneration. Intensified captured CO2 co-electrolysis (ICC) to syngas (H2:CO ratio of 2) with low CO2 content (<10%) was demonstrated with over 70% CO2 conversion at a current density up to 0.20 A/cm2 for 14 hours of operation. Integration of the co-electrolysis unit with CO2 capture was performed feeding pure and diluted CO2, for which CO2 conversions >65% were observed. Performance of the capture unit becomes critical to maintain syngas ratios (SR). Technology feasibility was assessed through comparative techno-economic and life cycle analysis showing that process intensification enables competitive performance, even at the higher energy consumption featured at the current state of the technology. This because several unit operations can be avoided. LCA also showed that based on the current US electricity mix the reduction of life cycle CO2 emissions is possible at scenarios observed with 0.15 A/cm2 to accomplish a carbon-negative technology.

08 HYDROGEN↗
DOE OSTI2016

Integrated process for the catalytic conversion of biomass-derived syngas into transportation fuels

Efficient synthesis of renewable fuels that will enable cost competitiveness with petroleum-derived fuels remains a grand challenge for U.S. scientists. In this paper, we report on an integrated catalytic approach for producing transportation fuels from biomass-derived syngas. The composition of the resulting hydrocarbon fuel can be modulated to meet specified requirements. Biomass-derived syngas is first converted over an Rh-based catalyst into a complex aqueous mixture of condensable C2+ oxygenated compounds (predominantly ethanol, acetic acid, acetaldehyde, ethyl acetate). This multi-component aqueous mixture then is fed to a second reactor loaded with a ZnxZryOz mixed oxide catalyst, which has tailored acid-base sites, to produce an olefin mixture rich in isobutene. The olefins then are oligomerized using a solid acid catalyst (e.g., Amberlyst-36) to form condensable olefins with molecular weights that can be targeted for gasoline, jet, and/or diesel fuel applications. The product rich in long-chain olefins (C7+) is finally sent to a fourth reactor that is needed for hydrogenation of the olefins into paraffin fuels. Simulated distillation of the hydrotreated oligomerized liquid product indicates that ~75% of the hydrocarbons present are in the jet-fuel range. Process optimization for the oligomerization step could further improve yield to the jet-fuel range. All of these catalytic steps have been demonstrated in sequence, thus providing proof-of-concept for a new integrated process for the production of drop-in biofuels. This unique and flexible process does not require external hydrogen and also could be applied to non-syngas derived feedstock, such as fermentation products (e.g., ethanol, acetic acid, etc.), other oxygenates, and mixtures thereof containing alcohols, acids, aldehydes and/or esters.

biofuel↗
DOE OSTI2016

Effects of thermal pretreatment and catalyst on biomass gasification efficiency and syngas composition

This work explores the combined effects of thermal pretreatment and using a catalyst in situ on gasification carbon conversion efficiency, as well as product gas and tar content and compositions. To compare the effects of thermal pretreatment, pelletized and ground oak with three different levels of thermal pretreatment were gasified in a fluidized bed reactor. The pretreatments applied to the oak were (1) pelletization, (2) drying at 180 °C in air, and (3) torrefaction at 270 °C in nitrogen. The oak dried at 180 °C produced syngas of similar quality and approximately the same amount of char as untreated oak. Torrefaction at 270 °C resulted in syngas with a higher hydrogen to CO ratio, lower methane, and less than half of the total tar -- all of which are desirable properties in terms of product gas quality. However, the oak torrefied at 270 °C also produced more than two times the amount of char as the untreated, pelletized oak. To determine the effect of catalyst, a series of experiments were conducted using olivine impregnated with nickel and cerium as the fluidized bed material in the gasifier. These tests showed that modified olivine can improve hydrogen production and reduce methane and tar levels in the syngas. The result was observed for both treated and untreated oak; although the effect was more substantial for untreated oak, for which the use of modified olivine reduced tar concentrations in the product gas by 60%, with a larger reduction in heavier tars than lighter tars. Furthermore, this result is important because reduction in heavier tar plays a more important role in benefitting downstream operations.

09 BIOMASS FUELS↗
DOE OSTI2020

Hybrid Ceramic-CMC Vane with EBC for Future Coal Derived Syngas Fired 65% Efficient Turbine Combined Cycle

The efficiency of both simple cycle and combined cycle power generation systems scale with the peak temperature at which the gas exits the combustor to drive the turbine. In conventional systems, a substantial fraction of the total turbine core flow exiting the compressor is diverted downstream to cool metallic turbine hardware rather than power the turbine, much of which is used to cool the first-stage turbine vane. The use of coal derived syngas fuels provides an additional challenge to the lifetime of materials utilized in the turbine, as particulate byproducts created in the coal gasification process melt in the combustion gas, and can subsequently deposit and interact with the turbine hardware. The development of durable hot-section materials capable of operating at temperature well above that of single crystal superalloy airfoil/zirconia based thermal barrier coatings is critical to realizing 65% efficient coal derived syngas fired gas turbine based power systems. To enable higher turbine inlet temperatures while lowering cooling air requirements, United Technologies Research Center (UTRC), the central R&D laboratory supporting UT Pratt & Whitney, led the conceptual design of a new type of ceramic composite turbine hot section materials system. The design focused on a novel hybrid monolithic ceramic-fiber reinforced ceramic matrix composite (CMC) first stage turbine vane having an environmental barrier coating. By utilizing ceramic construction in the turbine hot-section, the core flow normally used to cool metallic components will be substantially reduced, increasing efficiency and reducing emissions. To provide the framework for future demonstration testing, UTRC partnered with University of North Dakota Energy and Environmental Research Center (UNDEERC) to provide a conceptual design for a gasified coal fed high-pressure turbine combustor system designed to mimic the conditions expected in a future 65% fuel to busbar efficient syngas fueled gas turbine based combined cycle. The UNDEERC and UTRC collaborated on characterizing dusts from coal gasifier filtration systems.

10 SYNTHETIC FUELS↗