Synthesis and Characterization of AlPO4-18 Supported Mesoporous and Crystalline β-Mo2C, Ni3C, and WC Nanoparticles

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL Catalysis Letters Pub Date : 2024-07-30 DOI:10.1007/s10562-024-04791-y

Zinnabu T. Redda, Daniel Brennecke, Carsten Prinz, Abubeker Yimam, Mirko Barz, Steffen Kadow, Asnakech Laß-Seyoum

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Abstract

Developing high-efficiency, high-stability, and low-cost deoxygenation and hydrocracking catalysts could be considered one of the most significant breakthroughs in catalytic hydroprocessing. The present study utilized aluminophosphate (AlPO₄-18), a zeolite-like molecular sieve, as catalyst support for producing carbon-coated β-Mo₂C, Ni₃C, and WC nanoparticles. The synthesis used an incipient wetness impregnation followed by a temperature-programmed reduction-carburization approach which involved cracking a hydrocarbon gas, propane, in a hydrogen environment. The synthesis parameters were a 1:7 propane/hydrogen reductive-carburizing gas stream, 15 wt.% metal loading, an 800 °C carburization temperature ramped-up at a heating rate of 10 °C min⁻¹, a 2-h holding time, and a 1-h holding time in hydrogen. The synthesized catalysts were characterized using thermogravimetry mass spectroscopy/temperature-programmed oxidation (TPO TG-MS), nitrogen physisorption at 77 K, X-ray diffraction (XRD), and transmission electron microscopy/energy-dispersive X-ray spectroscopy (TEM EDS). TPO TG-MS, nitrogen physisorption, TEM, and XRD characterization results proved that atomic carbon was successfully incorporated into the lattice interstitials, resulting in thermally stable, well-dispersed, crystalline and mesoporous β-Mo₂C/AlPO₄-18, Ni₃C/AlPO₄-18, and WC/AlPO₄-18 nanoparticles. XRD analysis showed structural evolution during reduction-carburization, with average crystallite sizes of metal-containing particles of 8.2–9.22, 6.64–8.50, and 6.03–7.56 nm for β-Mo₂C/AlPO₄-18, Ni₃C/AlPO₄-18, and WC/AlPO₄-18, respectively. These values did not significantly deviate from high-resolution TEM analysis. The surface areas of the nanoparticles were categorized in decreasing order as WC/AlPO₄-18 > Ni₃C/AlPO₄-18 > β-Mo₂C/AlPO₄-18, with values of 193.79, 169.05, and 66.57 m² g⁻¹, respectively. In conclusion, these carbon-coated metal carbide nanoparticles with excellent thermal, structural, microscopic, and textural properties can be viable alternatives to noble metal catalysts for producing bio-jet fuel using the hydroprocessing pathway.

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以 AlPO4-18 为支撑的介孔和晶体 β-Mo2C、Ni3C 和 WC 纳米粒子的合成与表征

开发高效率、高稳定性和低成本的脱氧和加氢裂化催化剂可以说是催化加氢处理领域最重要的突破之一。本研究利用沸石类分子筛磷酸铝（AlPO4-18）作为催化剂载体，生产碳包覆的 β-Mo2C、Ni3C 和 WC 纳米颗粒。该合成采用了初湿浸渍法，然后是温度编程的还原-渗碳法，包括在氢气环境中裂解碳氢化合物气体丙烷。合成参数为：1:7 丙烷/氢气还原-渗碳气流、15 wt.% 金属负载、以 10 °C min-1 升温速率升高的 800 °C 渗碳温度、2 小时保温时间和 1 小时氢气保温时间。使用热重/温度编程氧化（TPO TG-MS）、77 K 下的氮物理吸附、X 射线衍射（XRD）和透射电子显微镜/能量色散 X 射线光谱（TEM EDS）对合成的催化剂进行了表征。TPO TG-MS、氮物理吸附、TEM 和 XRD 表征结果证明，原子碳成功地融入了晶格间隙，从而产生了热稳定、分散良好、结晶和介孔的β-Mo2C/AlPO4-18、Ni3C/AlPO4-18 和 WC/AlPO4-18 纳米粒子。XRD 分析表明还原-渗碳过程中的结构演变，β-Mo2C/AlPO4-18、Ni3C/AlPO4-18 和 WC/AlPO4-18 含金属颗粒的平均结晶尺寸分别为 8.2-9.22、6.64-8.50 和 6.03-7.56nm。这些数值与高分辨率 TEM 分析结果没有明显偏差。纳米颗粒的表面积按递减顺序分为 WC/AlPO4-18 >；Ni3C/AlPO4-18 >；β-Mo2C/AlPO4-18，其值分别为 193.79、169.05 和 66.57 m2 g-1。总之，这些碳包覆金属碳化物纳米颗粒具有优异的热性能、结构性能、微观性能和纹理性能，可以替代贵金属催化剂，利用加氢处理途径生产生物喷气燃料。图文摘要

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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.