Electronic Tuning of Ni by Mo Species for Highly Efficient Hydroisomerization of n-Alkanes Comparable to Pt-Based Catalysts,ACS Catalysis

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Electronic Tuning of Ni by Mo Species for Highly Efficient Hydroisomerization of n-Alkanes Comparable to Pt-Based Catalysts
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-08-17 , DOI: 10.1021/acscatal.0c01159
Dongxu Wang ₁ , Xin Kang ₁ , Ying Gu ₁ , Hongyan Zhang ₁ , Jiancong Liu ₁ , Aiping Wu ₁ , Haijing Yan ₁ , Chungui Tian ₁ , Honggang Fu ₁

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Modulation of the electronic structure of metal-based catalysts is a key to optimize the catalytic activity. Here, we have shown the electronic tuning of Ni by Mo species anchored on SAPO-11 (Ni–Mo/S-11) enabling the high-efficient hydroisomerization of n-alkanes comparable to commercial Pt/S-11, which is of great importance in producing fuel oils. The well-dispersed Ni particles intimately contacted with MoO₂ are anchored on S-11 based on a vacuum-assisted route. There is the obvious presence of electron transfer from Mo species to Ni due to the intimate contact, which can increase the electron density around Ni and consequently promote H activation and desorption on Ni catalyst. Also, the good dispersion of Ni–Mo species on S-11 is favorable to expose more Brønsted acid sites of S-11, being responsible for the skeletal isomerization. These characteristics endow enhanced activity of 3.0Ni–0.5Mo/S-11 for the hydroisomerization of n-hexadecane with a high isomer yield of 81.4%, being comparable to 81.0% for 0.5 wt % Pt/S-11. The analysis of products showed similar isomerization and cracking mechanisms over 3.0Ni–0.5Mo/S-11 catalyst to Pt catalyst. Further, the presence of Mo species can enhance the stability, with no obvious change after 100 h continuous catalytic reaction. Both the catalytic activity and stability are much superior to those of monometallic Ni/S-11 and the reported non-noble-metal catalyst. This work focuses on developing high-effective non-noble-metal-based catalysts.

中文翻译：

Mo物种对Ni进行电子调谐，以实现与Pt基催化剂相当的n烷烃高效加氢异构化

金属基催化剂的电子结构的调节是优化催化活性的关键。在这里，我们显示了通过锚定在SAPO-11（Ni-Mo / S-11）上的Mo物种对Ni进行的电子调谐，可实现与商业Pt / S-11相当的正构烷烃的高效加氢异构化，在生产燃油中的重要性。分散良好的Ni颗粒与MoO ₂紧密接触根据真空辅助路线固定在S-11上。由于紧密接触，明显存在从Mo物种到Ni的电子转移，这可以增加Ni周围的电子密度，从而促进Ni催化剂上的H活化和脱附。同样，Ni-Mo物种在S-11上的良好分散有利于暴露S-11的更多布朗斯台德酸位，这是骨骼异构化的原因。这些特性赋予了3.0Ni–0.5Mo / S-11增强n的加氢异构化的活性。-异戊烷的异构体收率为81.4％，与0.5 wt％Pt / S-11的81.0％相当。产品分析表明，在3.0Ni–0.5Mo / S-11催化剂上，Pt催化剂具有相似的异构化和裂化机理。此外，Mo物种的存在可以提高稳定性，连续催化反应100小时后无明显变化。催化活性和稳定性都大大优于单金属Ni / S-11和报道的非贵金属催化剂。这项工作着重于开发高效的非贵金属基催化剂。

更新日期：2020-09-20

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