将 NiAl-citrate LDH 用作干重整反应催化剂前驱体的热研究

IF 3 3区 工程技术 Q2 CHEMISTRY, ANALYTICAL Journal of Thermal Analysis and Calorimetry Pub Date : 2024-08-08 DOI:10.1007/s10973-024-13457-1
Marco Fortunato, Marco Piccinni, Andrea Pastorino, Anna Maria Cardinale
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摘要

镍基层状双氢氧化物(LDHs)是众所周知的催化剂前体;事实上,它们的特性允许通过简单而经济的合成途径在基体上均匀分布镍。在这项工作中,柠檬酸镍铝双硬质合金是通过最近开发的合成途径合成的,从而形成了几乎单层的六角形纳米晶体。通过热解,层间柠檬酸盐可转化为 CO,同时将 Ni (II) 还原为 Ni (0),并将原始晶体炸开,因此这些晶体似乎有望生产出具有极高比表面积的 Ni (0) 基材料。在这一转化过程中,温度起着关键作用;因此,研究人员对加热过程中发生的过程进行了调查,以确定哪些过程有助于材料的还原。此外,还确定了适当的热解温度,以获得所需的化合物,即具有高比表面积(177m2g-1)的镍(0)和铝/镍混合氧化物纳米花纹微片的均匀分布。这种新材料的高比表面积和预期特性使其成为高温气体反应异相催化的理想候选材料,如干法重整,这是一种利用二氧化碳和甲烷这两种温室气体生产合成气的值得注意的工艺。DRM 的适用性受限于获得可接受的转化率所需的高温,以及催化剂上的固体碳沉积,这两个因素都会导致催化剂随着时间的推移而失活;因此,开发能够克服这些问题的新型催化剂非常重要。为此,我们对所获得的材料进行了一些初步测试,证实了它对 DRM 的催化性能,尤其是在 800 K 的温度下。
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A thermal study on NiAl-citrate LDH as catalyst precursor for dry reforming reaction

Ni-based layered double hydroxides (LDHs) are well-known as catalysts precursors; in fact, their properties allow for a homogeneous distribution of Ni on a matrix through simple and economic synthetic passages. In this work, NiAl-citrate LDH was synthetized through a recently developed synthetic pathway that led to the formation of almost single-layered hexagonal nanocrystals. These ones seem to be promising for the production of a Ni (0)-based material with a very high surface area, since through pyrolysis, the interlayered citrate could be turned into CO that simultaneously reduces the Ni (II) to Ni (0) and blow-up the original crystals. In this transformation, temperature plays a key role; therefore, the processes occurring during heating were investigated to discriminate which of them contribute to the material reduction. Additionally, the appropriate pyrolysis temperature was determined to achieve the desired compound that was a homogeneous distribution of nanopatterned micro-flakes of Ni (0) and Al/Ni mixed oxides, with a high specific surface area (177m2g−1). The high surface area and the expected properties of this new material make it an interesting candidate for heterogeneous catalysis of high-temperature gas reactions, such as dry reforming, a noteworthy process that produces syngas from the two greenhouse gases CO2 and CH4. DRM applicability is limited by high temperatures required to obtain acceptable conversion and by solid carbon deposition on catalyst, both leading to its deactivation over time; so, it is important to develop new catalysts able to overcome those problems. For these purposes, some preliminary tests on the obtained material were performed confirming its catalytic behavior for the DRM, especially at temperatures > 800 K.

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来源期刊
CiteScore
8.50
自引率
9.10%
发文量
577
审稿时长
3.8 months
期刊介绍: Journal of Thermal Analysis and Calorimetry is a fully peer reviewed journal publishing high quality papers covering all aspects of thermal analysis, calorimetry, and experimental thermodynamics. The journal publishes regular and special issues in twelve issues every year. The following types of papers are published: Original Research Papers, Short Communications, Reviews, Modern Instruments, Events and Book reviews. The subjects covered are: thermogravimetry, derivative thermogravimetry, differential thermal analysis, thermodilatometry, differential scanning calorimetry of all types, non-scanning calorimetry of all types, thermometry, evolved gas analysis, thermomechanical analysis, emanation thermal analysis, thermal conductivity, multiple techniques, and miscellaneous thermal methods (including the combination of the thermal method with various instrumental techniques), theory and instrumentation for thermal analysis and calorimetry.
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