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Steam Methane Reforming (SMR) operations with carbon capture (CCS)
This entry from the NETL Unit Process Library covers Steam Methane Reforming (SMR) operations with carbon capture (CCS), including hydrogen production through conventional steam methane reforming, with carbon capture.
Steam Methane Reforming (SMR) operations
Hydrogen production through conventional steam methane reforming. To access the model referenced in the report, please visit https://www.netl.doe.gov/energy-analysis/details?id=bbb35592-8589-4187-be70-f6a2466762b4
Dynamic Tracking of NiFe Smart Catalysts using In Situ X-Ray Absorption Spectroscopy for the Dry Methane Reforming Reaction
The exsolution of nanoparticles from perovskite precursors has been explored as a route to synthesize catalysts with sinter or coke resistance. The characteristics of these exsolved nanoparticles are highly dynamic depending on the redox nature of the environment to which they are subjected. To develop their properties for thermo- and electrocatalytic applications, it is necessary to track the states and behavior of exsolved catalysts with in situ and ex situ characterization. In this study, we conduct in situ X-ray absorption spectroscopy (XAS) along with ex situ scanning transmission electron microscopy high-angle annular dark-field (STEM-HAADF) and energy-dispersive X-ray spectroscopy analysis of the parent perovskite oxide precursor, LaFe 0.8 Ni 0.2 O 3 , as its structure forms bimetallic NiFe nanoparticles and evolves in oxidative, reductive, and dry methane reforming environments. We develop a theory that NiFe exsolution is a function of the reduction potential where LaFe 0.8 Ni 0.2 O 3 transforms to NiFe alloy supported on LaO x -LaFeO x . The Ni starts to exsolve at 268 °C, while most Fe exsolves at 700 °C. During dry methane reforming conditions, most of the Fe is oxidized by CO 2 during the reaction and re-enters the perovskite as LaFeO 3 , while Ni remains on the surface as nanoparticles in the metallic state. During the oxidative regeneration phase, most of the Fe re-enters the bulk perovskite phase, while Ni is partially regenerated with a small percentage oxidized to large NiO nanoparticles. Finally, this study sheds light on the exsolution and regeneration of bimetallic alloy nanoparticles and the influence of the reaction conditions on their catalyst performance.
Non-thermal plasma-assisted steam methane reforming for electrically-driven hydrogen production
Plasma-assisted steam methane reforming (SMR) has become a promising approach for low temperature and small-scale hydrogen production. To increase H 2 yields, water-gas-shift reactions are needed to drive the formed CO to CO 2 and H 2 . In this study, bulk gas temperature, plasma power and water feed rate strongly impacted the CO and CO 2 product selectivity at high methane conversions of 60–80% in the presence of a Ni-based catalyst. CO 2 -enriched hydrogen could be formed directly with H 2 O/methane ratios > 4. To further increase the CO 2 /CO product selectivity, a “one-pot” cascade design with a Cu/ZnO/Al 2 O 3 /MgO catalyst bed placed downstream of the plasma zone achieved substantially higher CO 2 /CO selectivity (>15) in the effluent gas at 60% methane conversion and 300°C. Comparably, placing the Cu-based catalyst in the plasma zone does not alter the CO 2 /CO selectivity. Further, this study highlights the use of plasma reactor systems to directly tune the catalytic SMR performance and lead to an electrified route for hydrogen production.
Research goals for minimizing the cost of CO 2 capture when using steam methane reforming for hydrogen production
This paper presents a techno-economic assessment of adding state-of-the-art solvent-based CO 2 capture technologies to greenfield steam methane reforming (SMR)-based H 2 production plants and quantifies the impacts of improvements in CO 2 capture technology. Current conventional capture technologies are reviewed, and future technologies in intermediate and long-term scenarios are analyzed. The results show that adding significantly more efficient solvent-based capture technologies leads to an equivalent rate of natural gas consumption as that of a conventional SMR plant without capture, despite capturing most of the CO 2 and producing the same amount of H 2 . Overall, improvements in reboiler duty and reductions in capital costs can significantly reduce the cost of H 2 production and cost of capture. Particularly, the reboiler duty of pre-combustion capture and the capital cost of post-combustion capture have the greatest impact. Based on the results, research goals are suggested. Solvent development is recommended—particularly pre-combustion solvents—for reducing the reboiler duties, and process schemes to reduce the capital costs. Costlier but more efficient solvents can be considered. A sensitivity analysis using natural gas price shows that technological improvements can reduce the impacts of high natural gas prices. The degree of economic feasibility of CO 2 capture increases with improvements to the capture technology.
Engineering Study of Svante’s Solid Sorbent Post-Combustion CO 2 Capture Technology at a Linde Steam Methane Reforming H 2 Plant
An initial engineering design study was performed for an advanced post combustion CO 2 capture (PCC) technology to be installed at a commercial-scale steam methane reforming (SMR) hydrogen plant located in the US Gulf Coast. The PCC process integrated the VeloxoTherm™ structured adsorbent technology from Svante for the CO 2 separation and CO 2 compression and purification and balance of plant systems provided by Linde. This pre-FEED equivalent study included following: (1) design basis, (2) basic engineering, including development of process flow diagrams and heat & material balances, (3) inside the battery limit (ISBL) equipment and systems specification, (4) balance of plant outside the battery limit (OSBL) equipment and systems specifications, (5) technology maturation plan, (6) hazard identification (HAZID) review, (7) environmental, health and safety (EH&S) assessment and environmental permitting analysis, (8) constructability review, (9) ISBL and OSBL EPC cost estimation, and (10) commercial-scale techno-economic analysis including capital expenditures (CAPEX) and operating expenditures (OPEX) and CO 2 capture cost estimates.
Engineering Design of a Linde-BASF Advanced Post-Combustion CO 2 Capture Technology at a Linde Steam Methane Reforming H 2 Plant
Linde carried out an initial engineering design study for a Linde-BASF advanced post combustion CO 2 capture technology to be installed at a commercial-scale steam methane reforming (SMR) hydrogen plant located in the US Gulf Coast. This pre-FEED equivalent study included following: (1) basic design, including specific project scope definition and design basis, (2) basic engineering, including development of process flow diagrams and heat & material balances, (3) inside the battery limit (ISBL) equipment and systems specification, (4) balance of plant outside the battery limit (OSBL) equipment and systems specifications, (5) technology maturation plan, (6) hazard and operability (HAZOP) review, (7) environmental, health and safety (EH&S) assessment and environmental permitting analysis, (8) constructability review, (9) ISBL and OSBL EPC cost estimation, and (10) commercial-scale techno-economic analysis including capital expenditures (CAPEX) and operating expenditures (OPEX) and CO 2 capture cost estimates.
Nanowire-Based Materials as Coke-Resistant Catalyst Supports for Dry Methane Reforming
In this paper, nanowire-supported catalysts loaded with nickel are shown to be coke resistant compared to nanoparticle-supported catalysts. Specifically, Ni-loaded titania-based nanowire catalysts were tested with the dry methane reforming process in a laboratory-scale continuous packed-bed atmospheric reactor. The CO 2 conversion rate stayed above 90% for over 30 h on stream under coke-promoting conditions, such as high flow rates, low temperatures, and a high ratio of CH 4 to CO 2 . The coke (C x H y , x>>y) on the spent catalyst surface for both nanowire- and nanoparticle-supported catalysts was characterized by TGA, temperature-programmed reduction (TPR), and electron microscopy (SEM/TEM/EDS), and it was revealed that the types of carbon species present and their distribution over the morphology-enhanced materials played a major role in the deactivation. The CO 2 conversion activity of Ni supported on titania nanoparticles was reduced from ~80% to less than 72% in 30 h due to the formation of a graphitic coke formation. On the other hand, Ni particles supported on nanowires exhibited cube-octahedral morphologies, with a high density of non- (111) surface sites responsible for the increased activity and reduced graphitic coke deposition, giving a sustained and stable catalytic activity during a long time-on-stream experiment.
Carbon Capture on Air Liquide United States Gulf Coast Steam Methane Reformer using the Cryocap TM Flue Gases Process
The objective of this DOE-funded project is to execute and complete a Front-End Engineering and Design (FEED) study for a commercial-scale carbon capture project for Air Liquide’s Steam Methane Reformer (SMR) located at La Porte, near Houston, Texas. The Host Site is one of Air Liquide’s largest SMR assets, and supplies hydrogen to the Air Liquide Gulf Coast Hydrogen System, which serves refiners and petrochemical manufacturers through an existing H2 pipeline spanning roughly 200 miles from Port Arthur, TX to Bay City, TX. The Host Site produces up to 116.5 million standard cubic feet per day (MMSCFD) of gaseous hydrogen and emits approximately 950 ktpy CO 2 at the nameplate capacity. The evolving importance of decarbonized H2 for both existing customers and new markets, as well as the availability and intent of prominent third-party partners to transport and sequester captured CO 2 in locally abundant geological sites for 45Q credits, make the AL US Gulf Coast SMR an ideal site for the proposed FEED study. The envisioned carbon capture system is based on Air Liquide’s proprietary Cryocap™ Flue Gas (FG) process. The integration of the Cryocap™ FG technology to the existing SMR would enable the capture of 900 ktpy of CO 2 , with a net carbon capture rate of >95% and with minimum impact on the levelized cost of hydrogen produced at 99.97% purity.
Comprehensive process and environmental impact analysis of integrated DBD plasma steam methane reforming
Utilization of electricity generated from renewable sources to obtain hydrogen, H 2 , is of critical importance to decrease the overall carbon footprint. Here in this work, integration of a dielectric discharge barrier (DBD) plasma reactor to convert low calorific value gas, such as landfill gas or coal mine gas into hydrogen, into the existing steam methane reforming (SMR) technology was evaluated using process design considerations. In particular, a DBD-enhanced catalytic SMR reactor was modeled to operate at near atmospheric pressure and 500 °C sequentially with the conventional reformer to obtain ~ 65 kmol/hr H2 for distributed production. This allowed decreasing the size of the conventional reformer albeit at the increased overall electricity consumption. Calculated process economics showed that only at an electricity cost of less than $0.004/kWh does the hybrid DBD plasma process derived H 2 price become competitive with that of the conventional SMR. A Life Cycle Assessment framework was used to compare environmental impacts from the conventional SMR, hybrid DBD SMR and hybrid DBD SMR utilizing only onshore wind-derived electricity. Larger environmental impacts in the plasma reformer were obtained due to the use of electricity for the plasma reforming operation, which was modeled as coming from the typical U.S. grid mix. Utilizing only 100% wind-derived electricity provided certain environmental benefits, except for the ecotoxicity impact where the wind power scenario modeled here only reduced ecotoxicity impacts associated with electricity by 30%.
Accelerated Steam Methane Reforming by Dynamically Applied Charges
Catalyst design has traditionally focused on tuning active site properties to optimally bind reaction intermediates and balance the kinetic requirements of multiple competing chemical processes, as necessitated by the Sabatier principle. It has recently been proposed that for reactions following certain potential energy landscapes, the activity limit imposed by the Sabatier principle may be overcome by using programmed oscillations of surface electron density at the timescales of surface reactions (i.e., “catalytic resonance”). Here, we use a combination of density functional theory (DFT) simulations and transient kinetic models (TKMs) to simulate the kinetics of steam methane reforming (SMR) on Ru(211) surfaces under statically and dynamically applied charges. DFT-calculated binding energies of SMR intermediates and transition states exhibit strong sensitivity to positively applied charges and follow unique scaling relationships that deviate from linear periodic trends across transition metals. Our simulations demonstrate that applying a small positive charge to Ru dramatically enhances the steady-state turnover frequency (TOF) of SMR by up to 5 orders of magnitude above the TOF observed over neutral Ru. Thus, statically charging Ru catalysts may be an effective strategy to lower the temperature requirements for SMR. Dynamic square-wave oscillations in charge resulted in SMR catalytic resonance with an onset frequency f ∼ 106 Hz and the corresponding average TOFs exceeding the statically charged Ru surface by an additional 15%. Here, based on sensitivity analyses performed for the two end points of oscillation, we propose that dynamic TOF improvement beyond the Sabatier maximum can be expected when the system oscillates between two kinetic regimes that are uniquely controlled by distinct elementary steps.
Intensifying steam methane reforming and water-gas shift in tandem via rapid pulsed Joule heating
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Feedback control of an experimental electrically-heated steam methane reformer
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Model predictive control of an electrically-heated steam methane reformer
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Estimation-based model predictive control of an electrically-heated steam methane reforming process
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Automation and control of an experimental protonic membrane steam methane reforming system
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A Novel Sorbent-assisted Steam Methane Reforming Process for Production of Blue Hydrogen
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