The dry reforming of methane has received notable attention as a chemical process to convert natural gas into value‐added chemicals and fuels. Ni‐based exsolution catalysts using perovskite oxides supports have been used for their attractive sinter‐resistance and coke‐resistance properties. The perovskite oxide in itself has unique defect chemistry that can be used to manipulate and control the properties of the catalyst nanoparticles exsolved on the surface, therefore influencing both the nanoparticle and support characteristics. In this study, the La:Fe ratio of Ni‐doped LaFeO₃ was used to manipulate and control the properties of exsolved Ni‐Fe alloy nanoparticles. The Ni‐Fe nanoparticles consisted of different sizes ranging from 10 to 380 nm. Temperature programmed surface reaction studies along with materials characterization with SEM, STEM‐HAADF, XRD, and BET showed that the Ni‐Fe nanoparticles from different solid precursors have the same active sites for methane activation but differ in performance and stability because of size effects, metal‐support strength, composition and support basicity. A mechanism is proposed to decipher the merits of the Ni‐Fe nanoparticles with the best activity, selectivity, and stability in this study.

中文翻译：

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化学计量学对干式甲烷重整用溶解的Ni-Fe合金纳米粒子性能的影响

甲烷的干法重整作为将天然气转化为增值化学品和燃料的化学过程而受到了广泛关注。使用具有钙钛矿氧化物载体的镍基脱附催化剂具有出色的耐烧结性和耐焦炭性能。钙钛矿氧化物本身具有独特的缺陷化学，可用于操纵和控制溶解在表面上的催化剂纳米颗粒的性质，因此影响纳米颗粒和载体特性。在这项研究中，掺Ni的LaFeO ₃的La：Fe比用于控制和控制溶解的镍铁合金纳米粒子的性能。Ni-Fe纳米粒子的大小从10到380 nm不等。程序升温的表面反应研究以及使用SEM，STEM-HAADF，XRD和BET进行的材料表征表明，来自不同固体前体的Ni-Fe纳米粒子具有相同的甲烷活化活性位，但由于尺寸效应而在性能和稳定性上存在差异，金属支撑强度，成分和支撑碱度。在本研究中，提出了一种机制来解释具有最佳活性，选择性和稳定性的Ni-Fe纳米颗粒的优点。