The Role of Pore Architect, Reducibility and Silica-Alumina Ratio over Ni-Containing Molecular Sieves for Methane Partial Oxidation

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL Catalysis Letters Pub Date : 2025-01-21 DOI:10.1007/s10562-024-04922-5

Kirankumar J. Chaudhary, Khaled M. Banabdwin, Abdulaziz A. M. Abahussain, Anis H. Fakeeha, Irfan Wazeer, Jehad K. Abu-Dahrieh, Syed Ul Hasnain Bakhtiar, Rawesh Kumar, Ahmed S. Al-Fatesh

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Abstract

The catalytic conversion of CH₄ by O₂ into syngas (known as partial oxidation of methane; POM) is a practical approach for depleting CH₄ concentration as well as achieving excellent H₂ yield with high H₂/CO ratio. The pentasil zeolite family having different SiO₂/Al₂O₃ ratios 10, 20, 25, and 30 (abbreviated as CBV10A, CBV20A, CP810E, and CBV3024E) is found to be an excellent carrier for Ni. These Ni-containing molecular sieves are investigated for POM and characterized by X-ray diffraction, Raman-infrared spectroscopy, thermogravimetry, temperature-programmed techniques, and transmission electron microscopy. 5Ni/CBV3024E catalyst has smaller number of active sites, 5Ni/CP810E contains unstable active site and mordenite-based Ni catalysts (5Ni/CBV10A and 5Ni/CBV20A) attain higher metal-support interaction. 5Ni/CBV20A outperforms others due to the presence of reducible NiO under moderate and strong interaction. It shows an initial 40% H₂ yield at 600 ^oC and 81% H₂ yield at 750 ^oC. The high-temperature POM reaction limits the H₂/CO ratio close to the stoichiometric value of POM (~ 2), indicating the direct pathways of POM reaction at high temperatures. The high POM activity with the option of a wide range of H₂/CO (4.12–2.26) using Ni-containing molecular sieve may gain industrial-level attention in the coming future.

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孔结构、还原性和硅铝比在含镍分子筛上对甲烷部分氧化的作用

甲烷被O2催化转化为合成气(称为甲烷部分氧化；POM是一种消耗CH4浓度和获得高H2/CO比的优异H2产率的实用方法。不同SiO2/Al2O3比值为10、20、25和30的五硫分子筛家族（简称CBV10A、CBV20A、CP810E和CBV3024E）是镍的优良载体。研究了这些含镍分子筛的POM，并通过x射线衍射，拉曼红外光谱，热重法，温度编程技术和透射电子显微镜进行了表征。5Ni/CBV3024E催化剂具有较少的活性位点，5Ni/CP810E含有不稳定的活性位点，而5Ni/CBV10A和5Ni/CBV20A基镍催化剂具有较高的金属负载相互作用。由于5Ni/CBV20A在中等和强相互作用下存在还原性NiO，因此性能优于其他材料。在600℃时H2产率为40%，750℃时H2产率为81%。高温POM反应使H2/CO比接近POM的化学计量值（~ 2），表明了高温下POM反应的直接途径。含镍分子筛具有较高的POM活性和较宽的H2/CO（4.12-2.26）选择范围，在未来可能会得到工业层面的关注。图形抽象

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来源期刊

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.