TY - JOUR
T1 - Evolution and impact of acidic oxygen functional groups on activated carbon fiber cloth during NO oxidation
AU - Atkinson, John D.
AU - Zhang, Zhanquan
AU - Yan, Zifeng
AU - Rood, Mark J.
N1 - Funding Information:
This material is based upon work supported by the National Science Foundation under NSF Grants CBET 10-34470 and OISE 10-6378 . Support for Zhanquan Zhang from the Chinese Scholarship Council ( 2011645015 ) is acknowledged. XPS was carried out in part in the Frederick Seitz Materials Research Laboratory Central Facilities, University of Illinois , which are partially supported by the US Department of Energy under grants DE-FG02-07ER46453 and DE-FG02-07ER46471 .
PY - 2013/4
Y1 - 2013/4
N2 - Fundamental studies describing the impact of carbon's physical and chemical properties on NO oxidation allow for the development of catalysts tailored specifically for abating emissions of nitrogen oxides. Here, we show that acidic oxygen functional groups are developed on activated carbon fiber cloth during carbon-catalyzed NO oxidation. Reaction and thermal desorption cycle experiments demonstrate the continuous addition of oxygen to carbon as carbonyl and carboxyl functional groups. After four cycles, the oxygen content of carbon increased by 280%. There is also a 65% reduction in the time required to release NO2 from the carbon surface, allowing the reaction to achieve steady-state NO conversion 45% faster. The steady-state NO oxidation rate remains constant during the four cycles (48.5 ± 1.6 μmol/h), which is attributed to stable physical properties of carbon during the cycles. Oxygen groups added during the cycles, therefore, have no detectable impact on the overall conversion of NO over carbon, but control the pathway to achieving stable conditions. Carbon catalysts prepared with acidic oxygen functionalities are promising as NO oxidation catalysts, as confirmed with NO2 and nitric acid treatments. It is proposed that carbon's chemical properties impact NO oxidation kinetics while carbon's physical properties impact the steady-state NO oxidation rate.
AB - Fundamental studies describing the impact of carbon's physical and chemical properties on NO oxidation allow for the development of catalysts tailored specifically for abating emissions of nitrogen oxides. Here, we show that acidic oxygen functional groups are developed on activated carbon fiber cloth during carbon-catalyzed NO oxidation. Reaction and thermal desorption cycle experiments demonstrate the continuous addition of oxygen to carbon as carbonyl and carboxyl functional groups. After four cycles, the oxygen content of carbon increased by 280%. There is also a 65% reduction in the time required to release NO2 from the carbon surface, allowing the reaction to achieve steady-state NO conversion 45% faster. The steady-state NO oxidation rate remains constant during the four cycles (48.5 ± 1.6 μmol/h), which is attributed to stable physical properties of carbon during the cycles. Oxygen groups added during the cycles, therefore, have no detectable impact on the overall conversion of NO over carbon, but control the pathway to achieving stable conditions. Carbon catalysts prepared with acidic oxygen functionalities are promising as NO oxidation catalysts, as confirmed with NO2 and nitric acid treatments. It is proposed that carbon's chemical properties impact NO oxidation kinetics while carbon's physical properties impact the steady-state NO oxidation rate.
UR - http://www.scopus.com/inward/record.url?scp=84872832374&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84872832374&partnerID=8YFLogxK
U2 - 10.1016/j.carbon.2012.11.060
DO - 10.1016/j.carbon.2012.11.060
M3 - Article
AN - SCOPUS:84872832374
SN - 0008-6223
VL - 54
SP - 444
EP - 453
JO - Carbon
JF - Carbon
ER -