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Effect of interstitial carbon atoms in core-shell Ni3ZnC0.7/Al2O3 catalyst for high-performance dry reforming of methane
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2022-07-29 , DOI: 10.1016/j.apcatb.2022.121806
Qianqian Wang , Wu Wang , Min Cao , Sha Li , Pengfei Wang , Jiaqing He , Ruifeng Li , Xiaoliang Yan

Dry reforming of methane (DRM) on Ni-based catalysts provides an economically and environmentally pivotal route to generate synthesis gas. However, coke formation on Ni surface by the growth of carbon atoms is the main reason for catalyst deactivation and reactor blockage. Here, we propose a reaction-induced method to incorporate and store active carbon atoms into nickel octahedral sites in core-shell Ni3ZnC0.7/Al2O3. This strategy can fundamentally avoid C−C bond formation and feasible oxidation of Ni3ZnC0.7 in low-temperature DRM under CO2-rich condition. About 2 nm of thin-layer Al2O3 encapsulated Ni3ZnC0.7 is explored as the carbon reservoir to accommodate sufficient interstitial carbon atoms, and less than 5% Ni3Zn was observed under CH4/CO2 < 1/1 for 100 h. The dynamic balance of carbon atom storage and conversion in robust Ni3ZnC0.7 contributes to the enhanced activity, stability, coke and oxidation resistance, and distinct reaction pathway in low-temperature DRM.



中文翻译:

核壳型Ni3ZnC0.7/Al2O3催化剂中间隙碳原子对甲烷高​​效干重整的影响

在镍基催化剂上干法重整甲烷 (DRM) 为生产合成气提供了一种经济和环保的关键途径。然而,碳原子生长在镍表面形成焦炭是催化剂失活和反应器堵塞的主要原因。在这里,我们提出了一种反应诱导的方法,将活性碳原子结合并储存到核壳 Ni 3 ZnC 0.7 /Al 2 O 3的镍八面体位点中。该策略可以从根本上避免在富CO 2条件下在低温DRM中Ni 3 ZnC 0.7的CC键形成和可行的氧化。约 2 nm 的薄层 Al 2 O 3封装 Ni3 ZnC 0.7被探索作为碳储层以容纳足够的间隙碳原子,并且在CH 4 /CO 2 < 1/1 100 h下观察到小于5%的Ni 3 Zn。稳健的 Ni 3 ZnC 0.7中碳原子存储和转化的动态平衡有助于提高低温 DRM 中的活性、稳定性、抗焦化和抗氧化性以及独特的反应途径。

更新日期:2022-08-02
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