The role of different nitrogen functional groups on the removal of SO2 from flue gases by N-doped activated carbon powders and fibres

被引:212
作者
Raymundo-Piñero, E [1 ]
Cazorla-Amorós, D [1 ]
Linares-Solano, A [1 ]
机构
[1] Univ Alicante, Dept Quim Inorgan, E-03080 Alicante, Spain
关键词
activated carbon; X-ray photoelectron spectroscopy; adsorption properties; catalytic properties; functional groups;
D O I
10.1016/S0008-6223(03)00180-5
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
SO2 removal from flue gases by carbonaceous materials is determined by their behaviour as catalysts for SO2 oxidation into SO3 or H2SO4 in the presence of O-2 or O-2 and steam, respectively. Previous studies have demonstrated that nitrogen (N) functional groups are active sites for the adsorption and oxidation of SO2, although the nature of the N groups with the higher activity had not been established yet. For this reason, in the present work a number of activated carbons (AC) and activated carbon fibres (ACF) doped with N atoms have been prepared using different methods. The number and nature of these N groups have been assessed by XPS. The materials prepared have a wide range of nitrogen content, which is distributed into different chemical species. In this way, we were able to determine the effect of the N content and the role of the different N-containing functional groups on the catalytic activity for SO2 oxidation. The results confirm that, although the pore volume and the pore size distribution strongly influence the catalytic activity, the presence of N species at the surface increases the catalytic activity. They also demonstrate that, among the different N functional groups, pyridinic nitrogen is the most active for this reaction. (C) 2003 Elsevier Ltd. All rights reserved.
引用
收藏
页码:1925 / 1932
页数:8
相关论文
共 30 条
[1]   Modified active carbons from precursors enriched with nitrogen functions: sulfur removal capabilities [J].
Bimer, J ;
Satbut, PD ;
Bertozecki, S ;
Boudou, JP ;
Broniek, E ;
Siemieniewska, T .
FUEL, 1998, 77 (06) :519-525
[2]   SOME ASPECTS OF THE SURFACE-CHEMISTRY OF CARBON-BLACKS AND OTHER CARBONS [J].
BOEHM, HP .
CARBON, 1994, 32 (05) :759-769
[3]   3,5,11,13-TETRAAZACYCL[3.3.3]AZINE - THEORETICAL (ABINITIO) AND EXPERIMENTAL (X-RAY AND ULTRAVIOLET PHOTOELECTRON-SPECTROSCOPY) STUDIES OF THE ELECTRONIC-STRUCTURE [J].
BOUTIQUE, JP ;
VERBIST, JJ ;
FRIPIAT, JG ;
DELHALLE, J ;
PFISTERGUILLOUZO, G ;
ASHWELL, GJ .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1984, 106 (16) :4374-4378
[4]   NITROGEN FUNCTIONALITY IN COALS AND COAL-TAR PITCH DETERMINED BY X-RAY PHOTOELECTRON-SPECTROSCOPY [J].
BUCKLEY, AN .
FUEL PROCESSING TECHNOLOGY, 1994, 38 (03) :165-179
[5]   Adsorption of SO2 onto oxidized and heat-treated activated carbon fibers (ACFS) [J].
Daley, MA ;
Mangun, CL ;
DeBarr, JA ;
Riha, S ;
Lizzio, AA ;
Donnals, GL ;
Economy, J .
CARBON, 1997, 35 (03) :411-417
[6]   NITROGEN RELEASE IN THE GASIFICATION OF CARBONS [J].
GRANT, KA ;
ZHU, Q ;
THOMAS, KM .
CARBON, 1994, 32 (05) :883-895
[7]   Chemical vapor deposition of heterocyclic compounds over active carbon fiber to control its porosity and surface function [J].
Kawabuchi, Y ;
Sotowa, C ;
Kishino, M ;
Kawano, S ;
Whitehurst, DD ;
Mochida, I .
LANGMUIR, 1997, 13 (08) :2314-2317
[8]   Thermal chemistry of nitrogen in kerogen and low-rank coal [J].
Kelemen, SR ;
Freund, H ;
Gorbaty, ML ;
Kwiatek, PJ .
ENERGY & FUELS, 1999, 13 (02) :529-538
[9]   OXIDATIVE REMOVAL OF SO2 AND RECOVERY OF H2SO4 OVER POLY(ACRYLONITRILE)-BASED ACTIVE-CARBON FIBER [J].
KISAMORI, S ;
KURODA, K ;
KAWANO, S ;
MOCHIDA, I ;
MATSUMURA, Y ;
YOSHIKAWA, M .
ENERGY & FUELS, 1994, 8 (06) :1337-1340
[10]   ROLES OF SURFACE OXYGEN GROUPS ON POLY(ACRYLONITRILE)-BASED ACTIVE-CARBON FIBERS IN SO2 ADSORPTION [J].
KISAMORI, S ;
MOCHIDA, I ;
FUJITSU, H .
LANGMUIR, 1994, 10 (04) :1241-1245