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Balancing free and confined metallic Ni for an active and stable catalyst—A case study of CO methanation over Ni/Ni–Al2O3
Journal of Energy Chemistry ( IF 14.0 ) Pub Date : 2020-03-07 , DOI: 10.1016/j.jechem.2020.02.053
Yong-Shan Xiao , Yong-Hong Song , Chang Liu , Xian-Ying Shi , Han-Qing Ge , Min-Li Zhu , Zhao-Tie Liu , Zhong-Wen Liu

We propose a new strategy to make an active and stable Ni-based catalyst which can be operated in a wide range of reaction temperatures. The ordered mesoporous alumina (OMA) with confined Ni in the pore wall (Ni-OMA) was prepared via the one-pot evaporation induced self-assembly method. By using the incipient impregnation method, different amounts of free Ni were loaded over Ni-OMA (Ni/Ni-OMA) at a fixed total NiO content of 15 wt%. Characterization results confirmed the formation of well-structured Ni-OMA, and the ordered structure was still well preserved even after impregnating NiO at a content of as high as 12 wt%. The catalysts were evaluated for the CO methanation as a model reaction under varied conditions. Importantly, the activity and stability of Ni/Ni-OMA for the titled reaction were significantly regulated by simply changing the ratio of the confined to free Ni. Over the optimum catalyst of NiO (2 wt%)/NiO (13 wt%)-OMA, the high activity at a temperature of as low as 300 °C was achieved with the space-time yield of methane over 7.6 g gcat−1 h−1 while a long-term stability for a time-on-stream of 400 h was confirmed without an observable deactivation under the conditions of 600 °C and an extremely high gas hourly space velocity of 120,000 mL g−1 h−1. The results were well explained as the integrated merits of the free Ni for a high dispersion and the confined Ni in OMA for the anti-sintering property.



中文翻译:

平衡游离和受限的金属Ni,以制得活性稳定的催化剂-以Ni / Ni–Al 2 O 3上的CO甲烷化为例

我们提出了一种新的策略来制备可以在广泛的反应温度范围内操作的活性稳定的Ni基催化剂。通过一锅蒸发诱导自组装法制备了孔壁中具有受限Ni的有序介孔氧化铝(OMA)。通过使用初始浸渍方法,将不同量的游离Ni负载在固定的总NiO含量为15 wt%的Ni-OMA(Ni / Ni-OMA)上。表征结果证实了结构良好的Ni-OMA的形成,并且即使在以高达12wt%的含量浸渍NiO之后,仍然很好地保留了有序结构。评价催化剂在不同条件下的甲烷化反应,作为模型反应。重要的,Ni / Ni-OMA对标题反应的活性和稳定性可通过简单地改变受限Ni与游离Ni的比例来显着调节。在NiO(2 wt%)/ NiO(13 wt%)-OMA的最佳催化剂上,在低至300°C的温度下实现了高活性,甲烷的时空产率超过7.6 ggcat -1 h -1,同时确认了在400 h的运行时间具有长期稳定性,而在600°C和120,000 mL g -1 h的极高气体时空速度条件下未观察到失活-1。结果得到了很好的解释,因为游离Ni具有较高的分散性,而受限的Ni在OMA中具有抗烧结性能。

更新日期:2020-03-07
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