On the microscopic mechanism of carbon gasification: A theoretical study

被引：75

作者：

Frankcombe, TJ ^{[1
]}

Smith, SC ^{[1
]}

机构：

[1] Univ Queensland, Ctr Computat Mol Sci, Brisbane, Qld 4072, Australia

来源：

CARBON | 2004年 / 42卷 / 14期

基金：

澳大利亚研究理事会;

关键词：

graphitic carbon; gasification; computational chemistry; modeling; reaction kinetics;

D O I：

10.1016/j.carbon.2004.07.002

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 [物理化学]; 081704 [应用化学];

摘要：

In this paper we report the results of ab initio calculations on the energetics and kinetics of oxygen-driven carbon gasification reactions using a small model cluster, with full characterisation of the stationary points on the reaction paths. We show that previously unconsidered pathways present significantly reduced barriers to reaction and must be considered as alternative viable paths. At least two electronic spin states of the model cluster must be considered for a complete description. (C) 2004 Elsevier Ltd. All rights reserved.

引用

页码：2921 / 2928

页数：8

共 37 条

[1]

DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE [J].

BECKE, AD .

JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) :5648-5652

[2]

Electrical conductivity of anthracites as a function of heat treatment temperature [J].

Celzard, A ;

Marêché, JF ;

Payot, F ;

Bégin, D ;

Furdin, G .

CARBON, 2000, 38 (08) :1207-1215

[3]

Ab initio molecular orbital calculation on graphite: Selection of molecular system and model chemistry [J].

Chen, N ;

Yang, RT .

CARBON, 1998, 36 (7-8) :1061-1070

[4]

Ab initio molecular orbital study of the unified mechanism and pathways for gas-carbon reactions [J].

Chen, N ;

Yang, RT .

JOURNAL OF PHYSICAL CHEMISTRY A, 1998, 102 (31) :6348-6356

[5]

Unified mechanism of alkali and alkaline earth catalyzed gasification reactions of carbon by CO2 and H2O [J].

Chen, SG ;

Yang, RT .

ENERGY & FUELS, 1997, 11 (02) :421-427

[6]

A NEW SURFACE OXYGEN COMPLEX ON CARBON - TOWARD A UNIFIED MECHANISM FOR CARBON GASIFICATION REACTIONS [J].

CHEN, SG ;

YANG, RT ;

KAPTEIJN, F ;

MOULIJN, JA .

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1993, 32 (11) :2835-2840

[7]

SELF-CONSISTENT MOLECULAR-ORBITAL METHODS .23. A POLARIZATION-TYPE BASIS SET FOR 2ND-ROW ELEMENTS [J].

FRANCL, MM ;

PIETRO, WJ ;

HEHRE, WJ ;

BINKLEY, JS ;

GORDON, MS ;

DEFREES, DJ ;

POPLE, JA .

JOURNAL OF CHEMICAL PHYSICS, 1982, 77 (07) :3654-3665

[8]

Ab initio modelling of basal plane oxidation of graphenes and implications for modelling char combustion [J].

Frankcombe, TJ ;

Bhatia, SK ;

Smith, SC .

CARBON, 2002, 40 (13) :2341-2349

[9]

Frisch M.J., 2004, Gaussian 03

[10]

Revision C.02

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