Ultra-small Metallic Nickel Nanoparticles on Dealuminated Zeolite for Active and Durable Catalytic Dehydrogenation

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Huixin Wu, Hai Wang, Yating Lv, Yuexin Wu, Yike Wang, Qingsong Luo, Yu Hui, Lujie Liu, Mengting Zhang, Kunming Hou, Prof. Lina Li, Jianrong Zeng, Prof. Weili Dai, Prof. Liang Wang, Prof. Feng-Shou Xiao
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Abstract

Each step in the catalyst synthesis process plays an important role in tuning the catalyst structures. For zeolite-supported nickel catalysts, we found the conventional calcination-reduction method typically leads to the formation of large nickel particles, but a pre-aging in hydrogen or nitrogen at a low temperature prior to final reduction can result in ultra-small nickel nanoparticles in a metallic state. This pre-aging treatment facilitates the interaction between Ni2+ cations and silanol nests on zeolite before the decomposition of the metal salt, leading to the formation of nanoparticles with an average diameter of ~1.2 nm. In contrast, the pre-calcination in oxygen caused the Ni2+ aggregation before the decomposition of the metal salt precursor, yielding nickel nanoparticles larger than 5 nm. Given the structure sensitivity of nickel in cyclohexane dehydrogenation for hydrogen production, the ultra-small nickel nanoparticles exhibited significantly enhanced activity and durability compared to previous nickel catalysts.

Abstract Image

超小金属镍纳米颗粒在脱铝沸石上的活性持久催化脱氢
催化剂合成过程中的每一步都对催化剂结构的调整起着重要的作用。对于沸石负载的镍催化剂,我们发现传统的煅烧-还原方法通常会导致大镍颗粒的形成,但在最终还原之前,在氢气或氮气中低温预老化可以导致处于金属状态的超小镍纳米颗粒。这种预时效处理促进了Ni2+阳离子与沸石上硅醇巢在金属盐分解前的相互作用,形成了平均直径约为1.2 nm的纳米颗粒。相比之下,在氧气中预煅烧导致Ni2+在金属盐前驱体分解前聚集,生成大于5 nm的纳米镍。考虑到镍在环己烷脱氢制氢过程中的结构敏感性,超小镍纳米颗粒的活性和耐用性比之前的镍催化剂显著增强。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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