Fuel-driven design of NiOx/AlOx catalysts for methane decomposition through tuning of metal-support interaction

IF 5.5 3区材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Carbon Letters Pub Date : 2025-01-17 DOI:10.1007/s42823-024-00856-5

Nodira Urol Kizi Saidova, So Yeong Yang, Jae Hoon Kim, Shaikh Shayan Siddiqui, Soo Hong Lee, Ji Sun Im

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Abstract

As the demand for sustainable hydrogen (H₂) production grows, catalytic decomposition of methane (CDM) has emerged as a CO₂-free pathway for H₂ generation, producing valuable multi-walled carbon nanotubes (MWCNTs) as byproducts. This study examines the role of fuel type in shaping the properties and performance of NiOx/AlOx catalysts synthesized via solution combustion synthesis (SCS). Catalysts prepared with citric acid, urea, hexamethylenetetramine (HMTA), and glycine exhibited varying NiO nanoparticle (NP) sizes and dispersions. Among them, the HMTA catalyst achieved the highest Ni dispersion (~ 3.2%) and specific surface area (21.6 m²/g_cat), attributed to vigorous combustion facilitated by its high pH and amino-group-based fuel. Catalytic tests showed comparable activation energy (55.7–59.7 kJ/mol) across all catalysts, indicating similar active site formation mechanisms. However, the HMTA catalyst demonstrated superior CH₄ conversion (~ 68%) and stability, maintaining performance for over 160 min under undiluted CH₄, while others deactivated rapidly. MWCNT characterization revealed consistent structural properties, such as graphitization degree and electrical conductivity, across all catalysts, emphasizing that fuel type influenced stability rather than MWCNT quality. H₂ temperature-programmed reduction (H₂-TPR) analysis identified moderate metal-support interaction (MSI) in the HMTA catalyst as a key factor for optimizing stability and active site utilization. These findings underscore the importance of fuel selection in SCS to control MSIs and dispersion, offering a strategy to enhance catalytic performance in CDM and other thermocatalytic applications.

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通过调节金属-载体相互作用设计燃料驱动的甲烷分解NiOx/AlOx催化剂

随着对可持续制氢（H₂）需求的增长，甲烷催化分解（CDM）已成为一种无二氧化碳的制氢途径，产生有价值的多壁碳纳米管（MWCNTs）作为副产品。本研究考察了燃料类型对通过溶液燃烧合成（SCS）合成的NiOx/AlOx催化剂的性能和性能的影响。由柠檬酸、尿素、六亚甲基四胺（HMTA）和甘氨酸制备的催化剂表现出不同的NiO纳米颗粒（NP）大小和分散性。其中，HMTA催化剂的Ni分散度最高（~ 3.2%），比表面积最高（21.6 m2/gcat），这是由于其高pH值和氨基基燃料促进了剧烈燃烧。催化试验表明，所有催化剂的活化能（55.7-59.7 kJ/mol）相似，表明活性位点形成机制相似。然而，HMTA催化剂表现出优异的CH4转化率（~ 68%）和稳定性，在未稀释的CH₄下保持性能超过160分钟，而其他催化剂则迅速失活。MWCNT的表征表明，所有催化剂的结构特性（如石墨化程度和导电性）都是一致的，强调燃料类型影响稳定性而不是MWCNT质量。H2程序升温还原（H2- tpr）分析发现，适度的金属-载体相互作用（MSI）是优化HMTA催化剂稳定性和活性位点利用率的关键因素。这些发现强调了燃料选择对控制msi和分散的重要性，为提高CDM和其他热催化应用的催化性能提供了策略。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Carbon Letters CHEMISTRY, MULTIDISCIPLINARY-MATERIALS SCIENCE, MULTIDISCIPLINARY

CiteScore

7.30

自引率

20.00%

发文量

118

期刊介绍： Carbon Letters aims to be a comprehensive journal with complete coverage of carbon materials and carbon-rich molecules. These materials range from, but are not limited to, diamond and graphite through chars, semicokes, mesophase substances, carbon fibers, carbon nanotubes, graphenes, carbon blacks, activated carbons, pyrolytic carbons, glass-like carbons, etc. Papers on the secondary production of new carbon and composite materials from the above mentioned various carbons are within the scope of the journal. Papers on organic substances, including coals, will be considered only if the research has close relation to the resulting carbon materials. Carbon Letters also seeks to keep abreast of new developments in their specialist fields and to unite in finding alternative energy solutions to current issues such as the greenhouse effect and the depletion of the ozone layer. The renewable energy basics, energy storage and conversion, solar energy, wind energy, water energy, nuclear energy, biomass energy, hydrogen production technology, and other clean energy technologies are also within the scope of the journal. Carbon Letters invites original reports of fundamental research in all branches of the theory and practice of carbon science and technology.