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24 records · Page 2

The advanced low-emissions catalytic-combuster program. Phase 1: Description and status

An overview of the ongoing program is presented. Objectives, plan, schedule, pollution and performance goals, catalyst advantages, present problems, and the present status of identified combustor concepts are discussed. The possible increase in upper atmosphere oxides of nitrogen (NOx) levels due to aircraft number density increases was predicted to adversely decrease ozone concentration levels. A technique for achieving low NOx emission levels was experimentally demonstrated with a lean, premixing prevaporizing flame-tube combustor.

Szaniszlo, A. J.↗

Integrated Capture and Conversion of CO 2 to Methanol in a Post‐Combustion Capture Solvent: Heterogeneous Catalysts for Selective CN Bond Cleavage

Abstract An efficient and selective heterogeneous catalyst is identified for the condensed‐phase hydrogenation of captured CO 2 in the presence of an advanced water‐lean post‐combustion capture solvent, ( N ‐(2‐EthoxyEthyl)‐3‐MorpholinoPropan‐1‐Amine), 2‐EEMPA. The catalysts commonly used for gas‐phase CO 2 hydrogenation (e.g., Cu/Zn/Al 2 O 3 ) cause deactivation of amine promoters via N ‐methylation by CO cleavage of formamide intermediates. A heterogeneous catalyst system that suppresses N ‐methylation of amine solvents is identified, demonstrating how Pt, supported by reducible metal oxides CeO 2 or TiO 2 , can be selective for CN cleavage to produce methanol. This is the first known demonstration of integrated low‐temperature thermocatalytic capture and conversion of CO 2 to methanol in an economically viable CO 2 capture solvent. Technoeconomic analyses performed on the state‐of‐technology suggest that methanol can be produced with a minimum selling price of $4.4/gallon ($1,460/metric ton) when using CO 2 captured from a 650 MW natural gas combined cycle plant. Ultimately, a road map of how realistic and achievable improvements to space velocity and methanol selectivity of this integrated process can enable near cost parity to fossil‐derived methanol, with a selling price of ≈$1.4/gal ($470/metric ton), is presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Simultaneous Control of Unburned NH 3 and NO x Emissions From High Load Dual-Fuel Ammonia Operation on a High-Speed Diesel Engine Using a Cu-SCR System

Dual-fuel ammonia strategies are being investigated as a promising way to utilize NH 3 as an alternative fuel for internal combustion engines in the maritime sector. One of the remaining barriers to implementing dual-fuel NH 3 combustion strategies is understanding ways to minimize unburned NH 3 and nitrogen oxide (NO x ) emissions from these engines, both of which are elevated relative to a conventional diesel baseline. Selective catalytic reduction (SCR) systems are widely used for lean NO x emission controls for engines across transportation and stationary energy applications. SCR systems use a reducing agent, such as NH 3 , to react with NO x in the exhaust, converting it into nitrogen and water. Typically, NH 3 is injected into the exhaust as a urea solution. In dual-fuel NH 3 engines, where unburned NH 3 is present in the exhaust, an SCR system could be used to mitigate both NH 3 and NO x emissions. The presented work evaluates a commercial copper-zeolite SCR and ammonia slip catalyst system, designed for on-road diesel engine applications, for controlling unburned NH 3 and NO x emissions from a dual-fuel NH 3 combustion engine. The aftertreatment system was installed downstream of a single-cylinder four-stroke diesel engine that has been modified for dual-fuel ammonia use. Furthermore, the emissions were characterized by using a Fourier transform infrared spectrometer for both late- and early-injection diesel pilot strategies over three air–fuel equivalence ratios spanning from 1.6 to 1.0 at 1200 rpm and 12.6 bar IMEP g condition (with greater than 95% ammonia energy fraction). Initial findings indicate that the SCR achieves more than 99% NO x conversion with less than 50 ppm NH 3 slip at air–fuel equivalence ratios greater than 1.4 at the operating conditions investigated. However, these benefits are accompanied by additional N 2 O emissions that are formed over the Cu-SCR.

Catalysts↗

Optimizing feed modulation for coupled methane and NO x conversion over Pd-Pt/Mn 0.5 Fe 2.5 O 4 /Al 2 O 3 monolith catalyst

Here the impacts of feed modulation (frequency, amplitude) and catalyst design (composition and architecture) parameters are reported for the conversion of methane and NO x over a dual-layer Pt+Pd/Al 2 O 3 + Mn 0.5 Fe 2.5 O 4 /Al 2 O 3 monolith. CH 4 and NO x conversion data show that the dual-layer catalyst outperforms single-layer samples having the same catalyst loadings, with and without spinel. Close proximity of the PGM and MFO functions in the mixed-layer catalyst lowers the CH 4 conversion at high temperature while separating the PGM and spinel layers with an intermediate Al 2 O 3 layer does not. Methane conversion enhancement is linked to its nonmonotonic dependence on O 2 . The performance gains are tied to a transient activity spike that occurs during the lean-to-rich feed transition when water is present in the feed. The transient spike is attributed to the removal of CO and H 2 products via reactions with stored O 2 in the spinel, eliminating inhibition of methane steam reforming.

03 NATURAL GAS↗

Catalytic Microtube Rocket Igniter

Devices that generate both high energy and high temperature are required to ignite reliably the propellant mixtures in combustion chambers like those present in rockets and other combustion systems. This catalytic microtube rocket igniter generates these conditions with a small, catalysis-based torch. While traditional spark plug systems can require anywhere from 50 W to multiple kW of power in different applications, this system has demonstrated ignition at less than 25 W. Reactants are fed to the igniter from the same tanks that feed the reactants to the rest of the rocket or combustion system. While this specific igniter was originally designed for liquid methane and liquid oxygen rockets, it can be easily operated with gaseous propellants or modified for hydrogen use in commercial combustion devices. For the present cryogenic propellant rocket case, the main propellant tanks liquid oxygen and liquid methane, respectively are regulated and split into different systems for the individual stages of the rocket and igniter. As the catalyst requires a gas phase for reaction, either the stored boil-off of the tanks can be used directly or one stream each of fuel and oxidizer can go through a heat exchanger/vaporizer that turns the liquid propellants into a gaseous form. For commercial applications, where the reactants are stored as gases, the system is simplified. The resulting gas-phase streams of fuel and oxidizer are then further divided for the individual components of the igniter. One stream each of the fuel and oxidizer is introduced to a mixing bottle/apparatus where they are mixed to a fuel-rich composition with an O/F mass-based mixture ratio of under 1.0. This premixed flow then feeds into the catalytic microtube device. The total flow is on the order of 0.01 g/s. The microtube device is composed of a pair of sub-millimeter diameter platinum tubes connected only at the outlet so that the two outlet flows are parallel to each other. The tubes are each approximately 10 cm long and are heated via direct electric resistive heating. This heating brings the gasses to their minimum required ignition temperature, which is lower than the auto-thermal ignition temperature, and causes the onset of both surface and gas phase ignition producing hot temperatures and a highly reacting flame. The combustion products from the catalytic tubes, which are below the melting point of platinum, are injected into the center of another combustion stage, called the primary augmenter. The reactants for this combustion stage come from the same source but the flows of non-premixed methane and oxygen gas are split off to a secondary mixing apparatus and can be mixed in a near-stoichiometric to highly lean mixture ratio. The primary augmenter is a component that has channels venting this mixed gas to impinge on each other in the center of the augmenter, perpendicular to the flow from the catalyst. The total crosssectional area of these channels is on a similar order as that of the catalyst. The augmenter has internal channels that act as a manifold to distribute equally the gas to the inward-venting channels. This stage creates a stable flame kernel as its flows, which are on the order of 0.01 g/s, are ignited by the combustion products of the catalyst. This stage is designed to produce combustion products in the flame kernel that exceed the autothermal ignition temperature of oxygen and methane.

Schneider, Steven J.↗

Two dimensional, transient catalytic combustion of CO-air on platinum

The light off transient of catalytic combustion of lean CO-air mixtures in a platinum coated channel of a honeycomb monolith is studied with a model that resolves transient radial and axial gradients in both the gas and the solid. For the conditions studied it is concluded that: the initial heat release occurs near the entrance at the gas-solid interface and is controlled by heterogeneous reactions; large spatial and temporal temperature gradients occur in the solid near the entrance controlled mostly by the availability of fuel; the temperature of the solid near the entrance achieves almost its steady state value before significant heating of the back; heterogeneous reactions and the gas heated up front and flowing downstream heat the back of the solid; the overall transient time is controlled by the thermal inertia of the solid and by forced convection; radiation significantly influences both transient and steady state particularly near the entrance; the oxidation of CO occurs mostly on the catalyst and becomes diffusion controlled soon into the transient.

Sinha, N.↗