Density Functional Theory Based Micro- and Macro-Kinetic Studies of Ni-Catalyzed Methanol Steam Reforming
The intrinsic mechanism of Ni-catalyzed methanol steam reforming (MSR) is examined by considering 54 elementary reaction steps involved in MSR over Ni(111). Density functional theory computations and transition state theory analyses are performed on the elementary reaction network. A microkinetic mo...
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MDPI AG
2020-03-01
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| Series: | Catalysts |
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| Online Access: | https://www.mdpi.com/2073-4344/10/3/349 |
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doaj-028106a4aad94e0e89f6c94e2fc7d4562020-11-25T02:01:58ZengMDPI AGCatalysts2073-43442020-03-0110334910.3390/catal10030349catal10030349Density Functional Theory Based Micro- and Macro-Kinetic Studies of Ni-Catalyzed Methanol Steam ReformingChangming Ke0Zijing Lin1Department of Physics, University of Science and Technology of China, Hefei 230026, ChinaHefei National Laboratory for Physical Sciences at Microscales & CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Department of Physics, University of Science and Technology of China, Hefei 230026, ChinaThe intrinsic mechanism of Ni-catalyzed methanol steam reforming (MSR) is examined by considering 54 elementary reaction steps involved in MSR over Ni(111). Density functional theory computations and transition state theory analyses are performed on the elementary reaction network. A microkinetic model is constructed by combining the quantum chemical results with a continuous stirring tank reactor model. MSR rates deduced from the microkinetic model agree with the available experimental data. The microkinetic model is used to identify the main reaction pathway, the rate determining step, and the coverages of surface species. An analytical expression of MSR rate is derived based on the dominant reaction pathway and the coverages of surface species. The analytical rate equation is easy to use and should be very helpful for the design and optimization of the operating conditions of MSR.https://www.mdpi.com/2073-4344/10/3/349reaction mechanismquantum chemical calculationtransition state theoryreaction pathwayrate-determining stepanalytical rate equation |
| collection |
DOAJ |
| language |
English |
| format |
Article |
| sources |
DOAJ |
| author |
Changming Ke Zijing Lin |
| spellingShingle |
Changming Ke Zijing Lin Density Functional Theory Based Micro- and Macro-Kinetic Studies of Ni-Catalyzed Methanol Steam Reforming Catalysts reaction mechanism quantum chemical calculation transition state theory reaction pathway rate-determining step analytical rate equation |
| author_facet |
Changming Ke Zijing Lin |
| author_sort |
Changming Ke |
| title |
Density Functional Theory Based Micro- and Macro-Kinetic Studies of Ni-Catalyzed Methanol Steam Reforming |
| title_short |
Density Functional Theory Based Micro- and Macro-Kinetic Studies of Ni-Catalyzed Methanol Steam Reforming |
| title_full |
Density Functional Theory Based Micro- and Macro-Kinetic Studies of Ni-Catalyzed Methanol Steam Reforming |
| title_fullStr |
Density Functional Theory Based Micro- and Macro-Kinetic Studies of Ni-Catalyzed Methanol Steam Reforming |
| title_full_unstemmed |
Density Functional Theory Based Micro- and Macro-Kinetic Studies of Ni-Catalyzed Methanol Steam Reforming |
| title_sort |
density functional theory based micro- and macro-kinetic studies of ni-catalyzed methanol steam reforming |
| publisher |
MDPI AG |
| series |
Catalysts |
| issn |
2073-4344 |
| publishDate |
2020-03-01 |
| description |
The intrinsic mechanism of Ni-catalyzed methanol steam reforming (MSR) is examined by considering 54 elementary reaction steps involved in MSR over Ni(111). Density functional theory computations and transition state theory analyses are performed on the elementary reaction network. A microkinetic model is constructed by combining the quantum chemical results with a continuous stirring tank reactor model. MSR rates deduced from the microkinetic model agree with the available experimental data. The microkinetic model is used to identify the main reaction pathway, the rate determining step, and the coverages of surface species. An analytical expression of MSR rate is derived based on the dominant reaction pathway and the coverages of surface species. The analytical rate equation is easy to use and should be very helpful for the design and optimization of the operating conditions of MSR. |
| topic |
reaction mechanism quantum chemical calculation transition state theory reaction pathway rate-determining step analytical rate equation |
| url |
https://www.mdpi.com/2073-4344/10/3/349 |
| work_keys_str_mv |
AT changmingke densityfunctionaltheorybasedmicroandmacrokineticstudiesofnicatalyzedmethanolsteamreforming AT zijinglin densityfunctionaltheorybasedmicroandmacrokineticstudiesofnicatalyzedmethanolsteamreforming |
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