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Enhancement of hydrothermal synthesis of FDU-12-derived nickel phyllosilicate using double accelerators of ammonium fluoride and urea for CO2 methanation
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2021-08-16 , DOI: 10.1016/j.jcou.2021.101677
Hai Li 1 , Yaqi Chen 1 , Shuqi Liu 1, 2 , Qing Liu 1
Affiliation  

Nickel phyllosilicate materials were usually prepared by the hydrothermal method under severe conditions with high hydrothermal temperature and long hydrothermal time. In order to obtain Ni-phyllosilicate under mild hydrothermal conditions, a modified hydrothermal method assisted by double accelerators of ammonium fluoride and urea was proposed in this work. The N/F-A100-12 catalyst was prepared by the modified hydrothermal method at 100 °C for 12 h with similar Ni content and morphology as N/F-H220-48 prepared by the conventional hydrothermal method at 220 °C for 48 h. The improvement derived from that ammonium fluoride accelerated the etching of FDU-12 to form the intermediate of H4SiO4, and urea could facilitate the formation of Ni(OH)2, resulting in the quick formation of Ni-phyllosilicate under mild conditions. N/F-A100-12 exhibited high TOFCO2 (220 °C) value of 3.05 × 10−3 s−1 and low activation energy of 96.5 kJ mol−1 for CO2 methanation due to the small Ni particle size and enhanced CO2 and H2 adsorption property. In addition, N/F-A100-12 also displayed high long-term stability and anti-sintering property. In all, the modified hydrothermal method was highly efficient to synthesize Ni-phyllosilicate material under mild hydrothermal conditions.



中文翻译:

使用氟化铵和尿素双促进剂促进水热合成 FDU-12 衍生的页硅酸镍 CO2 甲烷化

镍页硅酸盐材料通常在水热温度高、水热时间长的恶劣条件下采用水热法制备。为了在温和的水热条件下获得Ni-页硅酸盐,本文提出了一种改进的水热法,在氟化铵和尿素双重促进剂的辅助下。N/FA 100 -12 催化剂是通过改进的水热法在 100 °C 下 12 h 制备的,其 Ni 含量和形貌与通过常规水热法在 220 °C 下 48 h 制备的N/FH 220 -48相似。源自氟化铵的改进加速了 FDU-12 的蚀刻形成 H 4 SiO 4中间体, 尿素可以促进 Ni(OH) 2的形成,导致在温和条件下快速形成 Ni-页硅酸盐。N/FA 100 -12由于小的 Ni 粒径和增强的 CO 2表现出3.05 × 10 -3 s -1 的高 TOF CO2 (220 °C) 值和 96.5 kJ mol -1 的低CO 2甲烷化活化能和H 2吸附性能。此外,N/FA 100 -12 还表现出较高的长期稳定性和抗烧结性。总之,改进的水热法在温和的水热条件下非常有效地合成镍-页硅酸盐材料。

更新日期:2021-08-17
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