Rational design of silica nanoreactor encapsulated Ni for reinforcing coke-resistance in dry reforming of methane

IF 4.7 2区 化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2024-04-25 DOI:10.1016/j.apcata.2024.119759
Songbai Qiu , Ling Lan , Zheng Liang , Xian Xu , Linlu Tan , Haowen Yang , Qian Zhang , Tiejun Wang
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Abstract

Dry reforming of methane (DRM) provides a desired approach to produce valuable syngas in tackling greenhouse gases. Yet it faces a formidable challenge in the design and synthesis of high coke-resistant Ni-based catalysts. Herein, we report a nanoreactor strategy to construct a supported Ni catalyst (Ni@SiO2@SiO2) for reinforcing coke-resistance during DRM, by effectively encapsulating small Ni nanoparticles into dendritic fibrous silica (SiO2) nanospheres and coating SiO2 shell layers. Taking advantage of chemical characteristics of citric acid (CA), CA-chelated Ni impregnation enables the uniform immobilization of Ni species into the radial SiO2 framework, then following carbonization produces protective carbon layers on the Ni nanoparticle surface during SiO2 coating, which can be removed via oxidizing calcination. The resultant pomegranate-like nanoreactor catalyst possesses outstanding coke-resistance, without any detectable coke deposition after 200 h of DRM reaction at 700 ℃, benefiting from effectively restricting metal sintering and fully preventing formation of inert carbon species.

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合理设计包裹镍的二氧化硅纳米反应器,增强甲烷干转化过程中的抗焦性能
甲烷干重整(DRM)为解决温室气体问题提供了一种生产有价值合成气的理想方法。然而,它在设计和合成高抗焦性镍基催化剂方面面临着严峻的挑战。在此,我们报告了一种纳米反应器策略,通过有效地将小镍纳米颗粒封装到树枝状纤维状二氧化硅(SiO2)纳米球中并包覆 SiO2 壳层,构建了一种支撑型镍催化剂(Ni@SiO2@SiO2),用于增强 DRM 过程中的抗焦性。利用柠檬酸(CA)的化学特性,CA包覆镍浸渍能使镍均匀地固定在径向SiO2框架中,然后在碳化过程中在SiO2包覆过程中在镍纳米粒子表面产生保护性碳层,这些碳层可通过氧化煅烧去除。由于有效限制了金属烧结,并完全阻止了惰性碳的形成,因此生成的石榴状纳米反应器催化剂具有出色的抗焦性,在 700 ℃ 下进行 DRM 反应 200 小时后,未发现任何焦炭沉积。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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