Metalloporphyrin-derived carbons:: models for investigating NOx release from coal char combustion

被引:29
作者
Jones, JM [1 ]
Zhu, Q
Thomas, KM
机构
[1] Univ Leeds, Dept Fuel & Energy, Leeds LS2 9JT, W Yorkshire, England
[2] Univ Newcastle Upon Tyne, Dept Chem, No Carbon Res Labs, Newcastle Upon Tyne NE1 7RU, Tyne & Wear, England
关键词
char; combustion; X-ray Absorption Near-Edge Structure (XANES); reactivity; catalytic properties;
D O I
10.1016/S0008-6223(98)00304-2
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Nitrogen-containing carbons prepared by the co-carbonisation of tetraphenylporphine and acenaphthylene have been used as models to study NO, release during coal char combustion. In addition, carbons prepared from metalloporphyrins have been studied in an attempt to examine the role of well-dispersed metal catalysts on nitrogen release during combustion. The nitrogen functionality in some of the carbons was investigated by nitrogen X-ray Absorption Near-Edge Structure Spectroscopy (XANES), and thermogravimetric analysis-mass spectrometry was used as a means of studying the combustion properties. The nitrogen species present in the carbon are similar to those observed in coals and carbons, and there is some indication of a portion of chelated metal still being present for a lower (873 K) heat-treated carbon prepared from tetraphenylporphine cobalt (II). Even so, the effect of nitrogen functionality on NO emission is secondary to the effect of carbon structure on NO reduction. A model is presented which discusses NO emission in terms of the steady-state surface oxygen concentration on the carbon. In the case of catalysed carbon combustion, the NO reduction reaction is also catalysed. Carbons prepared from these types of metal-containing precursors show larger catalytic effects in combustion than transition metal-impregnated carbons. (C) 1999 Elsevier Science Ltd. All rights reserved.
引用
收藏
页码:1123 / 1131
页数:9
相关论文
共 28 条
[1]   A review of the kinetics of the nitric oxide carbon reaction [J].
Aarna, I ;
Suuberg, EM .
FUEL, 1997, 76 (06) :475-491
[2]   A KINETIC-MODEL FOR THE LOW-TEMPERATURE OXIDATION OF CARBON .1. [J].
AHMED, S ;
BACK, MH ;
ROSCOE, JM .
COMBUSTION AND FLAME, 1987, 70 (01) :1-16
[3]   SURFACE-CHEMISTRY OF CARBON - ACTIVATION OF MOLECULAR-OXYGEN [J].
ATAMNY, F ;
BLOCKER, J ;
DUBOTZKY, A ;
KURT, H ;
TIMPE, O ;
LOOSE, G ;
MAHDI, W ;
SCHLOGL, R .
MOLECULAR PHYSICS, 1992, 76 (04) :851-886
[4]  
CHAMBRION P, 1998, IN PRESS P 27 S INT
[5]   KINETIC MEASUREMENT AND MODELING OF CARBON OXIDATION [J].
DU, ZY ;
SAROFIM, AF ;
LONGWELL, JP ;
MIMS, CA .
ENERGY & FUELS, 1991, 5 (01) :214-221
[6]   NITRIC-OXIDE REDUCTION BY CHAR AND CARBON-MONOXIDE - FUNDAMENTAL KINETICS OF NITRIC-OXIDE REDUCTION IN FLUIDIZED-BED COMBUSTION OF COAL [J].
FURUSAWA, T ;
TSUNODA, M ;
TSUJIMURA, M ;
ADSCHIRI, T .
FUEL, 1985, 64 (09) :1306-1309
[7]  
HUCHAMPS C, 1966, CARBON, V4, P243
[8]   NO reduction by activated carbons .7. Some mechanistic aspects of uncatalyzed and catalyzed reaction [J].
IllanGomez, MJ ;
LinaresSolano, A ;
Radovic, LR ;
deLecea, CSM .
ENERGY & FUELS, 1996, 10 (01) :158-168
[9]   DETECTION OF REACTIVE INTERMEDIATE NITROGEN AND SULFUR SPECIES IN THE COMBUSTION OF CARBONS THAT ARE MODELS FOR COAL CHARS [J].
JONES, JM ;
HARDING, AW ;
BROWN, SD ;
THOMAS, KM .
CARBON, 1995, 33 (06) :833-843
[10]   C-13 MATERIALS AS MODELS FOR NOX AND N2O RELEASE DURING COAL CHAR COMBUSTION [J].
JONES, JM ;
THOMAS, KM .
CARBON, 1995, 33 (08) :1129-1139