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Electrochemical reduction of NOx - DTU Orbit

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1 Introduction<br />

when a square-wave voltage was applied rather than DC voltage 44 . In a series <strong>of</strong> papers Lucas-<br />

Consuegra et al. reported on an electrochemically assisted NSR catalyst consisting <strong>of</strong> a Pt/K-βAl2O3<br />

cell 46-48 . The Pt/K-βAl2O3 cell investigated by Lucas-Consuegra et al. showed the best performance<br />

at 300 °C, and two different forms <strong>of</strong> nitrate were identified to be formed during the storage<br />

process: a weakly bonded surface nitrate and a bulk nitrate 46 . Furthermore the influence <strong>of</strong> water<br />

in the gas was investigated, and even though the performance <strong>of</strong> the catalyst decreased during<br />

wet conditions, the decrease was not detrimental 46, 47 . Yoshinobu et al. reported recently studies<br />

on electrochemical de<strong>NOx</strong> in combination with electrochemical oxidation <strong>of</strong> particulate matter<br />

(PM); the studies were made both in a disk-electrode set-up and in a honeycomb module tested in<br />

real diesel engine exhaust 49 . The electrodes investigated were composite electrodes <strong>of</strong> Pt or Ag in<br />

combination with YSZ or CGO 49 . The addition <strong>of</strong> BaO to the electrodes was proven to be crucial for<br />

the <strong>NOx</strong> conversion, however in the presence <strong>of</strong> CO2 a performance decrease was observed due to<br />

the formation <strong>of</strong> BaCO3 49 . During the tests in real engine exhaust 97 wt% <strong>of</strong> the PM was removed<br />

and 74% <strong>of</strong> the <strong>NOx</strong> was reduced at a fuel penalty <strong>of</strong> 9%, which are promising results, however a<br />

higher <strong>NOx</strong> conversion and lower fuel penalty must be achieved for the technology to become<br />

commercially attractive 49 .<br />

1.3 Objective and lay-out <strong>of</strong> the thesis<br />

This projects deals with electrochemical de<strong>NOx</strong>, a method under development for <strong>NOx</strong> removal<br />

from automotive diesel engines. The objective <strong>of</strong> the PhD project is to investigate how the <strong>NOx</strong><br />

conversion during electrochemical de<strong>NOx</strong> is affected, when <strong>NOx</strong>-storage compounds are added to<br />

noble metal-free ceramic electrodes. The investigation is centered around three main questions:<br />

1) How much is the activity and selectivity <strong>of</strong> the ceramic electrodes towards <strong>NOx</strong> conversion<br />

affected by the addition <strong>of</strong> a <strong>NOx</strong> storage compound?<br />

2) What are the optimal conditions for <strong>NOx</strong> conversion on ceramic electrodes combined with<br />

<strong>NOx</strong> storage compounds?<br />

3) Which mechanisms/reaction steps are included in the oxidation/storage <strong>of</strong> <strong>NOx</strong> on the<br />

electrodes and the subsequent <strong>reduction</strong>?<br />

8

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