“…An issue that is becoming increasingly recognized is the unwanted formation of N 2 O during SCR where small pore Cu- and Fe-zeolites are used as catalysts. − A similar phenomenon has also been observed when Mn-Fe spinels, V 2 O 5 -WO 3 /TiO 2 , and Mn/Ti-Si are used as the catalyzing agent. Although historically exempt from emissions regulations due to their believed lack of toxicity, harmful indications following long-term exposure and a global warming potential almost 300 times that of CO 2 mean that N 2 O will inevitably become the subject of increasingly exacting legislation beyond emissions standards.…”
Unwanted N2O formation is a problem that has been noted
in selective catalytic reduction (SCR) where copper zeolite catalysts
are utilized. With its immense global warming potential and long-term
stability, elevated atmospheric N2O has already been identified
as a future challenge in the war on climate change. This paper explores
the phenomenon of N2O formation during NH3-SCR
over Cu-SSZ-13 catalysts, which are currently commercialized in automotive
emissions control systems, and proposes a link between N2O production and the local copper environment found within the zeolite.
To achieve this, a comparison is made between two Cu-SSZ-13 samples
with different copper co-ordinations produced via different synthesis
methods. A combination of synchrotron X-ray absorption near-edge spectroscopy,
UV–vis, Raman, and density functional theory (DFT) is used
to characterize the nature of copper species present within each sample.
Synchrotron IR microspectroscopy is then used to compare their behavior
during SCR under operando conditions and monitor
the evolution of nitrate intermediates, which, along with further
DFT, informs a mechanistic model for nitrate decomposition pathways.
Increased N2O production is seen in the Cu-SSZ-13 sample
postulated to contain a linear Cu species, providing an important
correlation between the catalytic behavior of Cu-zeolites and the
nature of their metal ion loading and speciation.
“…An issue that is becoming increasingly recognized is the unwanted formation of N 2 O during SCR where small pore Cu- and Fe-zeolites are used as catalysts. − A similar phenomenon has also been observed when Mn-Fe spinels, V 2 O 5 -WO 3 /TiO 2 , and Mn/Ti-Si are used as the catalyzing agent. Although historically exempt from emissions regulations due to their believed lack of toxicity, harmful indications following long-term exposure and a global warming potential almost 300 times that of CO 2 mean that N 2 O will inevitably become the subject of increasingly exacting legislation beyond emissions standards.…”
Unwanted N2O formation is a problem that has been noted
in selective catalytic reduction (SCR) where copper zeolite catalysts
are utilized. With its immense global warming potential and long-term
stability, elevated atmospheric N2O has already been identified
as a future challenge in the war on climate change. This paper explores
the phenomenon of N2O formation during NH3-SCR
over Cu-SSZ-13 catalysts, which are currently commercialized in automotive
emissions control systems, and proposes a link between N2O production and the local copper environment found within the zeolite.
To achieve this, a comparison is made between two Cu-SSZ-13 samples
with different copper co-ordinations produced via different synthesis
methods. A combination of synchrotron X-ray absorption near-edge spectroscopy,
UV–vis, Raman, and density functional theory (DFT) is used
to characterize the nature of copper species present within each sample.
Synchrotron IR microspectroscopy is then used to compare their behavior
during SCR under operando conditions and monitor
the evolution of nitrate intermediates, which, along with further
DFT, informs a mechanistic model for nitrate decomposition pathways.
Increased N2O production is seen in the Cu-SSZ-13 sample
postulated to contain a linear Cu species, providing an important
correlation between the catalytic behavior of Cu-zeolites and the
nature of their metal ion loading and speciation.
“…Meanwhile, NH 3 may react with NO 2 alone. This is the slow reaction rate of SCR ( r slw ) because the reaction occurs very slowly, slower than the major SCR reactions 41…”
This work presents an optimized ammonia injection strategy for the Worldwide Harmonized Light Vehicles Test Cycle and its potential benefits in terms of NO x emissions and ammonia consumption in selective catalytic reduction. An optimization tool based on optimal control was used to improve the ammonia injection in the selective catalytic reduction with different NO x emission limits. This optimal control can be used in two ways: one to minimize NO x emission and another to reduce the ammonia consumption in the selective catalytic reduction. The optimized strategy and the standard ammonia injection strategy were tested and compared on a fully instrumented engine test bench when applied in a Worldwide Harmonized Light Vehicles Test Cycle. The results showed a considerable improvement in the use of the optimization tool. When compared to the standard calibration, the new injection strategy for the same amount of ammonia injection reduced NO x emissions by 13.7%, and for the same NO x concentration emissions 33.5% of ammonia consumption was saved.
“…NO X emission in internal combustion engines is mainly NO and a small amount of NO 2. 1 Exhaust gas recirculation (EGR) is often introduced to reduce NO X emission in the actual combustion of internal combustion engines. At the same time, due to the dilution and oxidation in the fresh intake air, NO in EGR gas is oxidized to NO 2.…”
Summary
Based on the shock tube experiments, the influence of NO2 on the ignition characteristics of methanol fuel was systematically studied. The ignition delay time of the CH3OH/NO2/O2/Ar mixture with equivalence ratios of 0.5, 1, and 1.5 was measured at the reflected shock temperatures of 1100 ~ 1650 K and the reflected shock pressure of 0.20 MPa. The methanol–NO2 mechanism was newly constructed based on previously developed mechanisms for methanol and NO2 reaction pathways. The new combined reduced mechanism could well predict the ignition delay time of the CH3OH/NO2/O2/Ar mixture. Based on the newly constructed methanol–NO2 mechanism, the reaction path, sensitivity, and important elementary reactions of the stoichiometric mixture were analyzed, and the reasons why NO2 promoted the ignition of methanol fuel were found out: the increase of OH radicals generation and rapid accumulation in the early ignition stage enhanced the activity of the reaction system, interfered the ignition process of CH3OH/NO2/O2/Ar mixture in advance, and promoted the ignition of methanol fuel.
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