Development and Evaluation of Ni–Cu–Pt Monolithic Catalysts for Improved Ethanol Autothermal Reforming and Hydrogen Production

IF 5.2 3区 工程技术 Q2 ENERGY & FUELS Energy & Fuels Pub Date : 2024-11-12 DOI:10.1021/acs.energyfuels.4c0411310.1021/acs.energyfuels.4c04113
Jéssica F. Zeitoune, Camilla D. M. Nickel, Bruno L. D. Santos, Waldemar A. A. Macedo, Diego A. Duarte and Rafael C. Catapan*, 
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Abstract

This study investigates the development and characterization of Ni-based catalytic monoliths for ethanol reforming, focusing on the effects of incorporating Cu and Pt as promoters. Al2O3 monoliths were coated with α-Al2O3 and impregnated with Ni, Cu, and Pt by using a wet impregnation method. The catalysts were characterized by field-emission scanning electron microscopy (FESEM), energy-dispersive spectroscopy (EDS), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and temperature-programmed reduction (TPR). The multitechnique characterization results revealed differences between the monometallic Ni/α-Al2O3 catalyst and the trimetallic Ni-Cu-Pt/α-Al2O3 catalyst. A unique flower-like structure was identified in the trimetallic catalyst, formed due to acid leaching during the Pt impregnation step. The metal impregnation process did not alter the crystalline structure of the Al2O3 substrate with both catalysts primarily exhibiting oxide phases. The Ni-Cu-Pt/α-Al2O3 catalyst has surface concentrations of Cu and Pt around 1.3% or lower, while Ni concentration exceeds 4.8%, confirming the presence of all three metals at the catalyst surface, despite the acid leaching caused by the Pt impregnation. TPR analysis indicated complex metal-support interactions in the trimetallic catalyst, with distinct reduction peaks compared with the monometallic Ni/α-Al2O3 catalyst. Catalytic evaluation revealed that the trimetallic catalyst achieved similar ethanol conversion in comparison with the monometallic Ni/α-Al2O3 catalyst but exhibited lower hydrogen selectivity due to reduced C–C bond breaking, likely influenced by the presence of Cu. These findings highlight the potential and challenges of using trimetallic catalysts in ethanol reforming, with implications for optimizing catalyst composition and reaction conditions for hydrogen production.

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开发和评估用于改进乙醇自热转化和制氢的镍铜铂整体催化剂
本研究调查了用于乙醇重整的镍基催化单片的开发和特性,重点研究了加入铜和铂作为促进剂的效果。采用湿浸渍法在 Al2O3 单片上涂覆了 α-Al2O3,并浸渍了 Ni、Cu 和 Pt。催化剂的表征方法包括场发射扫描电子显微镜 (FESEM)、能量色散光谱 (EDS)、X 射线衍射 (XRD)、X 射线光电子能谱 (XPS) 和温度编程还原 (TPR)。多技术表征结果显示了单金属 Ni/α-Al2O3 催化剂与三金属 Nii-Cu-Pt/α-Al2O3 催化剂之间的差异。在三金属催化剂中发现了独特的花状结构,这是在铂浸渍步骤中酸浸出形成的。金属浸渍过程并没有改变 Al2O3 基质的晶体结构,两种催化剂都主要呈现出氧化物相。Ni-Cu-Pt/α-Al2O3 催化剂表面铜和铂的浓度约为 1.3% 或更低,而镍的浓度则超过了 4.8%,这证明尽管铂浸渍造成了酸浸出,但催化剂表面仍存在这三种金属。TPR 分析表明,与单金属 Ni/α-Al2O3 催化剂相比,三金属催化剂中的金属-支撑相互作用复杂,还原峰明显。催化评估显示,与单金属 Ni/α-Al2O3 催化剂相比,三金属催化剂实现了相似的乙醇转化率,但由于 C-C 键断裂减少,氢气选择性较低,这可能是受铜存在的影响。这些发现凸显了在乙醇转化过程中使用三金属催化剂的潜力和挑战,对优化催化剂组成和制氢反应条件具有重要意义。
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来源期刊
Energy & Fuels
Energy & Fuels 工程技术-工程:化工
CiteScore
9.20
自引率
13.20%
发文量
1101
审稿时长
2.1 months
期刊介绍: Energy & Fuels publishes reports of research in the technical area defined by the intersection of the disciplines of chemistry and chemical engineering and the application domain of non-nuclear energy and fuels. This includes research directed at the formation of, exploration for, and production of fossil fuels and biomass; the properties and structure or molecular composition of both raw fuels and refined products; the chemistry involved in the processing and utilization of fuels; fuel cells and their applications; and the analytical and instrumental techniques used in investigations of the foregoing areas.
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