scholarly journals Direct Simultaneous Measurement of Particulate Matter and Ammonia Storage on Combined Selective Catalytic Reduction Filter Systems Using Radio Frequency Sensors

Author(s):  
Paul A. Ragaller ◽  
Alexander Sappok ◽  
Jie Qiao ◽  
Xiaojin Liu ◽  
Jonathan Aguilar

Tightening global emissions regulations are motivating interest in the development and implementation of Selective Catalytic Reduction + Filtration (SCRF) systems, which are designed to reduce the concentration of tailpipe particulate matter (PM) and NOx emissions. These systems allow designers to combine the NOx reduction capability of an SCR with the filtration capability of a particulate filter on a single unit. Practical implementation of these systems requires reliable measurement and diagnosis of their state — both with respect to trapped particulate matter as well as adsorbed ammonia. Currently, these systems rely on a variety of gas sensors, mounted upstream or downstream of the system, that only provide an indirect inference of the operation state. In this study, a single radio frequency (RF) sensor was used to perform simultaneous measurements of soot loading and ammonia inventory on an SCRF. Several SCRF core samples were tested at varying soot and ash loads in a catalyst reactor bench. Soot levels were measured by monitoring changes in the bulk dielectric properties within the catalyst using the sensor, while ammonia levels were determined by feeding selected regions of the RF spectrum into a pretrained generalized regression neural network model. Results show the RF sensor is able to directly measure the instantaneous ammonia inventory, while simultaneously providing soot loading measurements within 0.5 g/L. These results confirm that simultaneous measurements of both the PM and ammonia loading state of an SCRF are possible using a single RF sensor via analysis of specific features in the full RF spectrum. The results indicate significant potential to remove the control barriers typically associated with the implementation of advanced SCRF systems.

Author(s):  
Oana Mihai ◽  
Stefanie Tamm ◽  
Marie Stenfeldt ◽  
Louise Olsson

A selective catalytic reduction (SCR)-coated particulate filter was evaluated by means of dynamic tests performed using NH 3 , NO 2 , O 2 and H 2 O. The reactions were examined both prior to and after soot removal in order to study the effect of soot on ammonium nitrate formation and decomposition, ammonia storage and NO 2 SCR. A slightly larger ammonia storage capacity was observed when soot was present in the sample, which indicated that small amounts of ammonia can adsorb on the soot. Feeding of NO 2 and NH 3 in the presence of O 2 and H 2 O at low temperature (150, 175 and 200°C) leads to a large formation of ammonium nitrate species and during the subsequent temperature ramp using H 2 O and argon, a production of nitrous oxides was observed. The N 2 O formation is often related to ammonium nitrate decomposition, and our results showed that the N 2 O formation was clearly decreased by the presence of soot. We therefore propose that in the presence of soot, there are fewer ammonium nitrate species on the surface due to the interactions with the soot. Indeed, we do observe CO 2 production during the reaction conditions also at 150°C, which shows that there is a reaction with these species and soot. In addition, the conversion of NO x due to NO 2 SCR was significantly enhanced in the presence of soot; we attribute this to the smaller amount of ammonium nitrate species present in the experiments where soot is available since it is well known that ammonium nitrate formation is a major problem at low temperature due to the blocking of the catalytic sites. Further, a scanning electron microscopy analysis of the soot particles shows that they are about 30–40 nm and are therefore too large to enter the pores of the zeolites. There are likely Cu x O y or other copper species available on the outside of the zeolite crystallites, which could have been enhanced due to the hydrothermal treatment at 850°C of the SCR-coated filter prior to the soot loading. We therefore propose that soot is interacting with the ammonium nitrate species on the Cu x O y or other copper species on the surface of the zeolite particles, which reduces the ammonium nitrate blocking of the catalyst and thereby results in higher NO 2 SCR activity.


2018 ◽  
Author(s):  
Z. Gerald Liu ◽  
Devin R. Berg ◽  
Thaddeus A. Swor ◽  
James J. Schauer‡

Two methods, diesel particulate filter (DPF) and selective catalytic reduction (SCR) systems, for controlling diesel emissions have become widely used, either independently or together, for meeting increasingly stringent emissions regulations world-wide. Each of these systems is designed for the reduction of primary pollutant emissions including particulate matter (PM) for the DPF and nitrogen oxides (NOx) for the SCR. However, there have been growing concerns regarding the secondary reactions that these aftertreatment systems may promote involving unregulated species emissions. This study was performed to gain an understanding of the effects that these aftertreatment systems may have on the emission levels of a wide spectrum of chemical species found in diesel engine exhaust. Samples were extracted using a source dilution sampling system designed to collect exhaust samples representative of real-world emissions. Testing was conducted on a heavy-duty diesel engine with no aftertreatment devices to establish a baseline measurement and also on the same engine equipped first with a DPF system and then a SCR system. Each of the samples was analyzed for a wide variety of chemical species, including elemental and organic carbon, metals, ions, n-alkanes, aldehydes, and polycyclic aromatic hydrocarbons, in addition to the primary pollutants, due to the potential risks they pose to the environment and public health. The results show that the DPF and SCR systems were capable of substantially reducing PM and NOx emissions, respectively. Further, each of the systems significantly reduced the emission levels of the unregulated chemical species, while the notable formation of new chemical species was not observed. It is expected that a combination of the two systems in some future engine applications would reduce both primary and secondary emissions significantly.


Author(s):  
Paul Ragaller ◽  
Josh Mandelbaum ◽  
Luc Lapenta ◽  
Alexander Sappok ◽  
Josh Pihl ◽  
...  

Abstract Lean gasoline engine operation provides clear efficiency benefits relative to conventional stoichiometric combustion approaches. One of the key hurdles to the widespread, practical implementation of lean gasoline combustion remains the challenge of lean NOx control. One of the potential approaches for controlling NOx emission from lean gasoline engines is the so-called passive selective catalytic reduction (SCR) system. In such systems, periods of rich operation generate ammonia over a three-way catalyst (TWC), which is then adsorbed on the downstream SCR and consumed during lean operation. Brief periods of rich operation must occur in response to the depletion of stored ammonia on the SCR, which requires reliable measurements of the SCR ammonia inventory. Presently, lean exhaust system controls rely on a variety of gas sensors mounted up- and downstream of the catalysts, and which only provide an indirect inference of the operation state. In this study, a radio frequency (RF) sensor was used to provide a direction measurement of the amount of ammonia adsorbed on the SCR in real-time. The RF sensor was calibrated and deployed on a BMW N43B20 4-cylinder lean gasoline engine equipped with a passive SCR system. Brief periods of rich operation performed at lambda values between 0.98 and 0.99 generated the ammonia, subsequently stored on the SCR for consumption during periods of lean operation. The experiments compared real-time measurements of SCR ammonia inventory from the RF sensor with estimates of ammonia coverage derived from exhaust gas composition measurements upstream and downstream of the catalyst. The results showed a high degree of correlation between the RF measurements and SCR ammonia storage inventory, and demonstrated NOx conversion efficiencies above 98%, confirming the feasibility of the concept. Relative to stoichiometric operation, lean-gasoline operation resulted in fuel efficiency gains of up to 10%, which may be further improved through direct feedback control from the RF sensor to optimize lean–rich cycling based on actual, measured SCR ammonia levels.


Materials ◽  
2018 ◽  
Vol 11 (8) ◽  
pp. 1307 ◽  
Author(s):  
Yaping Zhang ◽  
Xiupeng Yue ◽  
Tianjiao Huang ◽  
Kai Shen ◽  
Bin Lu

TiO2-ZrO2 (Ti-Zr) carrier was prepared by a co-precipitation method and 1 wt. % V2O5 and 0.2 CeO2 (the Mole ratio of Ce to Ti-Zr) was impregnated to obtain the V2O5-CeO2/TiO2-ZrO2 catalyst for the selective catalytic reduction of NOx by NH3. The transient activity tests and the in situ DRIFTS (diffuse reflectance infrared Fourier transform spectroscopy) analyses were employed to explore the NH3-SCR (selective catalytic reduction) mechanism systematically, and by designing various conditions of single or mixing feeding gas and pre-treatment ways, a possible pathway of NOx reduction was proposed. It was found that NH3 exhibited a competitive advantage over NO in its adsorption on the catalyst surface, and could form an active intermediate substance of -NH2. More acid sites and intermediate reaction species (-NH2), at lower temperatures, significantly promoted the SCR activity of the V2O5-0.2CeO2/TiO2-ZrO2 catalyst. The presence of O2 could promote the conversion of NO to NO2, while NO2 was easier to reduce. The co-existence of NH3 and O2 resulted in the NH3 adsorption strength being lower, as compared to tests without O2, since O2 could occupy a part of the active site. Due to CeO2’s excellent oxygen storage-release capacity, NH3 adsorption was weakened, in comparison to the 1 wt. % V2O5-0.2CeO2/TiO2-ZrO2 catalyst. If NOx were to be pre-adsorbed in the catalyst, the formation of nitrate and nitro species would be difficult to desorb, which would greatly hinder the SCR reaction. All the findings concluded that NH3-SCR worked mainly through the Eley-Rideal (E-R) mechanism.


Author(s):  
S-C Jung ◽  
W-S Yoon

Nitrogen oxide (NO x) reduction by the selective catalytic reduction (SCR) system assisted by an oxidation precatalyst is modelled and analytically investigated. The Langmuir—Hinshelwood SCR kinetic scheme with vanadium-based catalyst and ammonia (NH3) reductant in conjunction with the NO—NO2 conversion reaction over a platinum-based catalyst is used. The effects of the ratio of the oxidation precatalyst to the SCR monolith volume, the gas temperature, the space velocity, and the NH3-to-NO x concentration ratio on the de-NO x performance are parametrically examined. The oxidation precatalyst promotes NO x conversion at low temperatures. At intermediate temperatures, the NO x reduction is either activated or deactivated with increase in the space velocity. A higher oxidation precatalyst-to-SCR monolith volume ratio tends to promote the NO x reduction of higher space velocities. At high temperatures, the de-NO x efficiency is very high and insensitive to the space velocity. The NO x conversion efficiency depends on the NH3-to-NO x ratio at low temperatures.


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