Performance of Ni/MgO-AN catalyst in high pressure CO2 reforming of methane

被引:25
|
作者
Wang, YH
Wang, H
Li, Y
Zhu, QM
Xu, BQ [1 ]
机构
[1] Tsing Hua Univ, Dept Chem, Key Lab Organ Optoelect & Mol Engn, Innovat Catalysis Program, Beijing 100084, Peoples R China
[2] Harbin Normal Univ, Dept Chem, Harbin 150080, Peoples R China
关键词
Ni catalyst; methane dry reforming; carbon dioxide; high pressure reaction; catalyst deactivation; coking;
D O I
10.1007/s11244-005-2882-9
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The catalytic activity of 8.8 wt% Ni/MgO-AN prepared from alcogel derived MgO was studied for the dry reforming of methane under high Pressure (1.5 MPa). The catalyst showed a self-stabilization process during the reaction that lasted for 50 h, in which the catalytic activity decreased with increasing the reaction time on stream (TOS) up to 12 h, and then became stabilized thereafter. The activity decline during the initial 12 h of the reaction Was found closely related to an increase in the amount of carbon deposits or) the catalyst. which also became stabilized after the catalyst had served the reaction for 12 h. Comprehensive characterizations of the coked catalyst with Temprature programmed hydrogenation (TPH). X-ray photoelectron spectroscopy (XPS) and X-ray diffractometer (XRD) techniques revealed two kinds of carbon deposits (alpha-carbon and beta-carbon) on the used catalyst. The alpha-carbon deposits were found to be produced from CH4 decomposition while the beta-carbon deposits from CO disproportionation. It was revealed that the accumulation of beta-carbon deposits was a key cause for the activity decline and the self-stabilized catalysis during the initial 12 h of the high-pressure reaction. Moreover, it was also observed that an unavoidable sintering of metallic Ni particles from 6.5 to 11 nm, which happened within the very first hour of the reaction, was not directly related to the catalyst stability.
引用
收藏
页码:109 / 116
页数:8
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