Abstract
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.
Highlights
Fuel cell is an attractive environmentally friendly energy conversion technology, but its application is very limited due to the difficulties associated with the transportation and storage of hydrogen [1,2,3].A promising route for the broad adoption of fuel cells is through the so-called onboard fuel cell technology where H2 is obtained via real-time steam reforming of hydrocarbon, such as methanol, which is liquid at room temperature and normal pressure [3,4].Cu is the most commonly used commercial catalyst for the methanol steam reforming (MSR), CH3 OH + H2 O CO2 + 3H2
A microkinetic model is built based on the density functional theory (DFT) results and the transition state theory (TST) theory
The microkinetic model is in good agreement with the available experimental data
Summary
Fuel cell is an attractive environmentally friendly energy conversion technology, but its application is very limited due to the difficulties associated with the transportation and storage of hydrogen [1,2,3].A promising route for the broad adoption of fuel cells is through the so-called onboard fuel cell technology where H2 is obtained via real-time steam reforming of hydrocarbon, such as methanol, which is liquid at room temperature and normal pressure [3,4].Cu is the most commonly used commercial catalyst for the methanol steam reforming (MSR), CH3 OH + H2 O CO2 + 3H2. To overcome the drawbacks of Cu catalyst, numerous alternative materials have been examined, including noble metal catalysts [8,9,10], Ni-Cu alloy-based catalysts [11,12,13], and Ni-based catalysts [7,14,15,16]. Noble metals (Pd, Pt) are known to be the most active catalysts for MSR [8,9,10], but the high prices limit their large-scale industrial applications. Together with the observed high CH3 OH conversion activities of Ni-catalysts [14,15,16,17], and considering their low prices, Ni-based catalysts appear to be promising industrial catalysts for MSR
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