Confinement of Nickel Nanoparticles in Tailored MCF via Removable Carbon Template: Enhanced DRM Activity and Sintering Resistance

IF 2.5 4区 化学 Q3 CHEMISTRY, PHYSICAL
Chao Hu, Pengcheng Dai, Minghui Li, Yaoyao Xu, Ziwen Zhao, Dingyi Jing, ShenQiao Song
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引用次数: 0

Abstract

Nickel-based catalysts are widely employed in the dry reforming of methane (DRM) due to their superior intrinsic activity, yet they often undergo severe deactivation caused by sintering and carbon deposition. A key strategy to mitigate these issues is to achieve highly dispersed and strongly anchored nickel species on a tailored support. In this study, the structure of a mesoporous cellular foam silica (MCF) support was systematically engineered by adjusting the mass ratio of the swelling agent 1,3,5-trimethylbenzene (TMB) to the templating agent triblock copolymer P123 (EO20PO70EO20). An optimized MCF architecture obtained at a TMB/P123 ratio of 1.6 facilitated the formation of small and well-dispersed nickel nanoparticles. Furthermore, a removable carbon template method was utilized to confine nickel particles within the MCF framework, which significantly enhanced metal-support interaction and effectively suppressed nickel sintering. The unique structure also promoted the formation of additional oxygen vacancies and a higher concentration of active Ni0 sites, thereby accelerating CH4 activation and CO2 dissociation. Consequently, the designed catalyst exhibited markedly improved DRM activity and long-term stability, offering a rational structural-functional strategy for developing high-performance nicked-based DRM catalysts.

Graphical Abstract

通过可移动碳模板在定制MCF中限制镍纳米颗粒:增强DRM活性和抗烧结性能
镍基催化剂因其优异的本构活性被广泛应用于甲烷(DRM)的干重整反应中,但由于烧结和积碳等原因,镍基催化剂往往会发生严重的失活。缓解这些问题的一个关键策略是在定制的支架上实现高度分散和强锚定的镍。本研究通过调节膨胀剂1,3,5-三甲基苯(TMB)与模板剂三嵌段共聚物P123 (EO20PO70EO20)的质量比,系统地设计了介孔泡沫二氧化硅(MCF)载体的结构。在TMB/P123比为1.6时获得的优化MCF结构有利于形成小而分散的镍纳米颗粒。此外,利用可移动碳模板方法将镍颗粒限制在MCF框架内,显著增强了金属-载体相互作用,有效抑制了镍的烧结。这种独特的结构也促进了额外氧空位的形成和活性Ni0位点的高浓度,从而加速了CH4的活化和CO2的解离。结果表明,所设计的催化剂具有明显提高的DRM活性和长期稳定性,为开发高性能镍基DRM催化剂提供了合理的结构-功能策略。图形抽象
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来源期刊
Catalysis Letters
Catalysis Letters 化学-物理化学
CiteScore
5.70
自引率
3.60%
发文量
327
审稿时长
1 months
期刊介绍: Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.
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