Effect of metal-support interaction on activity and stability of Ni-CeO2 catalyst for partial oxidation of methane

被引:206
作者
Singha, Rajib Kumar [1 ]
Shukla, Astha [1 ]
Yadav, Aditya [1 ]
Konathala, L. N. Sivakumar [1 ]
Bal, Rajaram [1 ]
机构
[1] CSIR Indian Inst Petr, Refining Technol Div, Nanocatalysis Area, Dehra Dun 248005, Uttarakhand, India
关键词
Methane; Partial oxidation; Synthesis gas; Nickel; CeO2; nanoparticles; SOLID-SOLUTION CATALYSTS; SYNTHESIS GAS; LOW-TEMPERATURE; CARBON-DIOXIDE; NI NANOPARTICLES; SIO2-SUPPORTED NICKEL; MECHANISTIC ORIGINS; RH NANOPARTICLES; CO OXIDATION; NATURAL-GAS;
D O I
10.1016/j.apcatb.2016.09.060
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 objective of the current study was to synthesize a nickel based catalyst with high activity at low temperature for partial oxidation of methane (POM). Ni-nanoparticles supported on CeO2 nanoparticles were synthesized by two step preparation method. First, 30-50nm CeO2 was synthesized by solvo-thermal method and then Ni- nanoparticles were deposited over it following a newly developed procedure, where cetyltrimethylammonium bromide (CTAB) acted as morphology controlling agent and polyvinylpyrrolidone (PVP) as size controlling agent for nickel nanoparticles. The characterizations of synthesized catalysts were done by BET-Surface area, XRD, SEM, TEM, TPR, H-2-chemisorpton, TGA and XPS analysis. The catalysts showed excellent coke resisting ability during POM and produces synthesis gas with H-2/CO ratio almost 2. The catalyst activated methane at 400 degrees C with 10% methane conversion and converts methane almost completely at 800 degrees C. The catalyst showed above 98% methane conversion at 800 degrees C during 90 h of time on stream (TOS) reaction with H-2/CO ratio 1.98. Average 5.5 nm Ni particles, use of CeO2 as a support played a very crucial role for methane activation at such lower temperature. The synergistic effect between small Ni-nanoparticles and CeO2 nanoparticles of Ni-CeO2 catalyst is the main reason for such activity. Detailed study of other reaction parameters like temperature, Ni loading, weight hourly space velocity (WHSV) was also carried out and reported. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:473 / 488
页数:16
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