1. Facile synthesis of nickel phyllosilicate for enhanced CO2 methanation: Interrelationships of silicon-containing precursors and the formation of intermediates.
- Author
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Liu, Zeyu, Bi, Wenhui, Zhao, Wenyue, and Liu, Qing
- Subjects
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FOURIER transform infrared spectroscopy , *ACTIVATION energy , *CATALYTIC activity , *ETHYL silicate , *CARBON dioxide , *METHANATION - Abstract
In order to investigate the effect of silicon-containing precursors on the facile synthesis of Ni-phyllosilicate, Stöber SiO 2 , tetraethyl orthosilicate (TEOS), sodium metasilicate (Na 2 SiO 3 ⋅9H 2 O) was used. Na 2 SiO 3 successfully reacts with the nickel nitrate to form nickel phyllosilicate at ambient temperature, owing to its strong basicity and easy hydrolysis to generate intermediates of H 4 SiO 4 and Ni(OH) 2. Stöber SiO 2 and TEOS can only convert to Ni-phyllosilicate with the assistance of NH 4 F and urea, because of the limitation of intermediates formation. The Na 2 SiO 3 -based Ni-phyllosilicate NiPs-M-12 shows the highest catalytic activity for CO 2 methanation among all the samples, whose maximum CO 2 conversion reaches 71.0% at 450 °C, 0.1 MPa, 60 L g−1·h−1 with a TOF CO2 of 2.6 ± 0.1 × 10−3 s−1 and activation energy of 83.19 kJ mol−1. The active intermediates of *HCOO and *CO are observed by in-situ diffuse reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS) analysis, which can be hydrogenated to CH 3 O species with the further hydrogenation to produce the target products CH 4 and H 2 O. It also displays high long-term stability up to 100 h with high anti-sintering property. In conclusion, the recognition of the interrelationships of silicon-containing precursors and the formation of intermediates can shed light on the facile synthesis of Ni-phyllosilicate with high catalytic performance. • The room-temperature synthesis of Ni-phyllosilicate was proposed. • The properties of silicon-containing precursors were important for Ni-phyllosilicate synthesis. • The strong basicity and easy hydrolysis of Na 2 SiO 3 were the main reasons for the formation of intermediates of H 4 SiO 4 and Ni(OH) 2. • The Na 2 SiO 3 -based Ni-phyllosilicate showed high catalytic activity and stability. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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