Embedding high loading and uniform Ni nanoparticles into silicalite-1 zeolite for dry reforming of methane
Embedding high loading and uniform Ni nanoparticles into silicalite-1 zeolite for dry reforming of methane
复制标题
将高负载量且均匀的 Ni 纳米颗粒嵌入 Silalite-1 沸石中用于甲烷干重整
DOI：
10.1016/j.apcatb.2022.121202
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发表时间：
2022-02-15
影响因子：
22.1
通讯作者：
Shi, Chuan
中科院分区：
文献类型：
--
作者：
Liu, Yang;Chen, Yong;Shi, Chuan
将镍纳米颗粒(NPs)包埋到载体中作为镍限制的解决方案已被广泛接受，但高负载通常与良好的分散和包覆相反。为此，我们开发了一种可控的“溶解-再结晶”方法，将高负载量、均匀的纳米镍粒子嵌入到中空Silicalite-1(S-1)沸石的壳层中。当镍负载量从3%增加到20%时，镍纳米粒子的尺寸保持在约4-5 nm，TOF保持在约60 S(-1)(800？)在甲烷干法重整反应中。随着Ni负载量的增加，活性中心密度增大，在20%Ni@S-1上，反应速率达到20.0molCH(4)/g(CAT)/h。这种嵌入结构在运行150h时也具有良好的稳定性。本研究为在沸石中嵌入高负载、均匀的金属纳米颗粒铺平了道路，为在恶劣的反应条件下稳定金属提供了一种有效的策略。
Embedding Ni nanoparticles (NPs) into supports has been widely accepted as one of solutions for Ni confinement, but high loading usually stands on the opposite of being well dispersed and encapsulated. Herein, we developed a controlled 'dissolution-recrystallization' method of embedding high loading and uniform Ni NPs into the shell of hollow silicalite-1 (S-1) zeolite. The sizes of Ni NPs maintained at ca. 4-5 nm with increasing Ni loading from 3% to 20%, and the TOF kept at ca. 60 s(-1) (800 ?) in the dry reforming of methane reaction. The augmented density of active sites with Ni loading rendered an outstanding reaction rate of 20.0 molCH(4)/g(cat)/h over 20% Ni@S-1. The embedded structure also endowed a good stability upon running for 150 h. This study paves the way for embedding high loading and uniform metal nanoparticles inside the zeolite, providing an effective strategy to stabilize metals under harsh reaction conditions.