Carbon dioxide reforming of methane over 5wt.% nickel calcium aluminate catalysts – effect of preparation method

Ni-C/SiO2 and Ni-G/SiO2 catalysts were prepared by a complexed-impregnation method using citric acid and glycine as complexing agents, respectively. Ni/SiO2 was also prepared by the conventional incipient impregnation method. All the catalysts were comparatively tested for carbon dioxide reforming of methane (CDR) at P = 1.0 atm, T = 750 °C, CO2/CH4 = 1.0, and GHSV = 60,000 mL·g−1·h−1. The results showed that Ni-C/SiO2 and Ni-G/SiO2 exhibited better CDR performance, especially regarding stability, than Ni/SiO2. The conversions of CH4 and CO2 were kept constant above 82% and 87% after 20 h of reaction over Ni-C/SiO2 and Ni-G/SiO2 while they were decreased from 81% and 88% to 56% and 59%, respectively, over the Ni/SiO2. The characterization results of the catalysts before and after the reaction showed that the particle size and the distribution of Ni, as well as the interactions between Ni and the support were significantly influenced by the preparation method. As a result, an excellent resistance to the coking deposition and the anti-sintering of Ni was obtained over the Ni-C/SiO2 and Ni-G/SiO2, leading to a highly active and stable CDR performance.

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The Effect of Preparation Method of Ni-Supported SiO2 Catalysts for Carbon Dioxide Reforming of Methane

Catalysts ◽

10.3390/catal11101221 ◽

2021 ◽

Vol 11 (10) ◽

pp. 1221

Author(s):

Hua-Ping Ren ◽

Si-Yi Ding ◽

Qiang Ma ◽

Wen-Qi Song ◽

Yu-Zhen Zhao ◽

...

Keyword(s):

Carbon Dioxide ◽

Particle Size ◽

Active Sites ◽

High Performance ◽

Preparation Method ◽

Complexing Agent ◽

Preparation Process ◽

Carbon Dioxide Reforming ◽

Preparation Methods ◽

Synthetic Strategy

Reforming methane to produce syngas is a subject that generates considerable interest. The process requires catalysts that possess high-performance active sites to activate stable C–H bonds. Herein, we report a facile synthetic strategy to prepare Ni-based catalysts by complexation–impregnation (Ni-G/SiO2-C) and precipitation–impregnation (Ni-G/SiO2-P) methods using glycine as a complexing agent. The particle size of Ni in both types of catalysts is decreased by adding glycine in the preparation process. Nevertheless, the preparation methods and amount of glycine play a significant role in the particle size and distribution of Ni over the Ni-based catalysts. The smaller particle size and narrower distribution of Ni were obtained in the Ni-G/SiO2-P catalyst. The catalysts were comparatively tested for carbon-dioxide reforming of methane (CDR). Ni-G/SiO2-P showed better CDR performance than Ni-G/SiO2-C and Ni/SiO2 and increased stability because of the smaller particle size and narrower distribution of Ni. Moreover, a high-performance Ni-based catalyst was prepared by optimizing the amount of glycine added. An unobservable deactivation was obtained over Ni-G-2/SiO2-P and Ni-G-3/SiO2-P for CDR during TOS = 20 h. Thus, a new promising method is described for the preparation of Ni-based catalysts for CDR.

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