Kinetic studies of CH4 oxidation over Pt-NiO/δ-Al2O3 in a fluidised bed reactor

被引:28
作者
Opoku-Gyamfi, K [1 ]
Adesina, AA [1 ]
机构
[1] Univ New S Wales, Reactor Engn & Technol Grp, Sch Chem Engn & Ind Chem, Sydney, NSW 2052, Australia
基金
澳大利亚研究理事会;
关键词
CH4; oxidation; Pt-NiO/delta-Al2O3; fluidised bed reactor;
D O I
10.1016/S0926-860X(98)00340-8
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
The oxidation of CH4 over Pt-NiO/delta-Al2O3 has been studied in a fluidised bed reactor as part of a major project on an autothermal (combined oxidation-steam reforming) system for CH4 conversion. The kinetic data were collected between 773 and 893 K and 101 kPa total pressure using CH4 and O-2 compositions of 10-35% and 8-30%, respectively. Rate-temperature data were also obtained over alumina-supported monometallic catalysts, Pt and NiO. The bimetallic Pt-NiO system has a lower activation energy (80.8 kJ mol(-1)) than either Pt (86.45 kJ mol(-1)) and NiO (103.73 kJ mol(-1)). The superior performance of the bimetallic catalyst was attributed to chemical synergy. The reaction rate over the Pt-NiO catalyst increased monotonically with CH4 partial pressure but was inhibited by O-2 At low partial pressures (<30 kPa), H2O has a detrimental effect on CH4 conversion, whilst above 30 kPa, the rate increased dramatically with water content. (C) 1999 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:113 / 122
页数:10
相关论文
共 25 条
[1]  
ANDERSON JB, 1963, CHEM ENG SCI, V18, P147
[2]   SYNTHESIS GAS-FORMATION BY CATALYTIC-OXIDATION OF METHANE IN FLUIDIZED-BED REACTORS [J].
BHARADWAJ, SS ;
SCHMIDT, LD .
JOURNAL OF CATALYSIS, 1994, 146 (01) :11-21
[3]   PARTIAL OXIDATION OF METHANE TO SYNGAS OVER CO/MGO CATALYSTS - IS IT LOW-TEMPERATURE [J].
CHANG, YF ;
HEINEMANN, H .
CATALYSIS LETTERS, 1993, 21 (3-4) :215-224
[4]   PARTIAL OXIDATION OF METHANE USING FERRIC MOLYBDATE CATALYST [J].
CHELLAPPA, AS ;
VISWANATH, DS .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1995, 34 (06) :1933-1940
[5]   Partial oxidation of methane to carbon monoxide and hydrogen over NiO/La2O3/gamma-Al2O3 catalyst [J].
Chu, YL ;
Li, SB ;
Lin, JZ ;
Gu, JF ;
Yang, YL .
APPLIED CATALYSIS A-GENERAL, 1996, 134 (01) :67-80
[6]   Simulation of the catalytic partial oxidation of methane to synthesis gas [J].
DeGroote, AM ;
Froment, GF .
APPLIED CATALYSIS A-GENERAL, 1996, 138 (02) :245-264
[7]   Synthesis gas production from natural gas in a fixed bed reactor with reversed flow [J].
DeGroote, AM ;
Froment, GF ;
Kobylinski, T .
CANADIAN JOURNAL OF CHEMICAL ENGINEERING, 1996, 74 (05) :735-742
[8]   PARTIAL OXIDATION OF METHANE TO CARBON-MONOXIDE AND HYDROGEN OVER A NI/AL2O3 CATALYST [J].
DISSANAYAKE, D ;
ROSYNEK, MP ;
KHARAS, KCC ;
LUNSFORD, JH .
JOURNAL OF CATALYSIS, 1991, 132 (01) :117-127
[9]   COMPARATIVE-STUDY OF THE ACTIVITY OF AL-PD AND AL-PT CATALYSTS IN DEEP OXIDATION OF HYDROCARBONS [J].
DROZDOV, VA ;
TSYRULNIKOV, PG ;
POPOVSKII, VV ;
BULGAKOV, NN ;
MOROZ, EM ;
GALEEV, TG .
REACTION KINETICS AND CATALYSIS LETTERS, 1985, 27 (02) :425-427
[10]  
DZRADZIL M, 1988, CATAL TODAY, V3, P269