Regulating the location relationship between Cu nanoparticles and Pt atoms to enhance the catalytic hydroisomerization performance: Together or apart?

IF 3.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2024-10-17 DOI:10.1016/j.mcat.2024.114620
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Abstract

Single atom catalysts have been recently reported as the efficient catalysts for hydroisomerization compared to the conventional nanoparticle catalyst. Despite the fascinating advantage in enhancing the metal activity or reducing the catalyst cost, the long-term stability of the single atom catalyst seemed not that satisfactory, especially when reacting under atmospheric pressure. Herein, Pt single atom catalysts were combined with Cu nanoparticles by different means to explore a new way to improve the catalytic performance. Cu nanoparticles were located away from Pt sites to form a binary catalyst, or acted as the support of Pt atoms to form a single atom alloy (SAA) catalyst. With the binary catalyst Pt1–0.1Cu@CS, the conversion of the n-heptane after time on stream of 50 h increased to 70.3 %, higher than Pt1@CS (47.3 %). Besides, excessive Cu nanoparticles in the binary catalyst were found rather harmful to the catalysis instead. However, the SAA catalyst Pt1Cu@SAPO-11 showed a poor activity in hydroisomerization compared to Pt1@CS, indicating that the alloy structure should go against the activation of reactant. The roles of Pt atoms and Cu nanoparticles in different catalysts were discussed in detail. The reaction mechanism of hydroisomerization was refined with the different functions of the dual metal sites. This work might be instructive for the design of single atom catalysts combined with metal nanoparticles.

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调节铜纳米颗粒与铂原子之间的位置关系,提高催化加氢异构化性能:在一起还是分开?
据报道,与传统的纳米颗粒催化剂相比,单原子催化剂是一种高效的加氢异构化催化剂。尽管单原子催化剂在提高金属活性或降低催化剂成本方面具有令人着迷的优势,但其长期稳定性似乎并不令人满意,尤其是在常压下反应时。在此,我们采用不同的方法将铂单原子催化剂与铜纳米颗粒结合起来,探索提高催化性能的新途径。铜纳米颗粒远离铂位点形成二元催化剂,或作为铂原子的支撑形成单原子合金(SAA)催化剂。在二元催化剂 Pt1-0.1Cu@CS 的作用下,正庚烷的转化率在流动 50 小时后提高到 70.3%,高于 Pt1@CS(47.3%)。此外,二元催化剂中过多的纳米铜颗粒反而对催化有害。然而,与 Pt1@CS 相比,SAA 催化剂 Pt1Cu@SAPO-11 的加氢异构化活性较差,这表明合金结构不利于反应物的活化。详细讨论了铂原子和铜纳米颗粒在不同催化剂中的作用。根据双金属位点的不同作用,完善了加氢异构化反应机理。这项工作可能对设计与金属纳米颗粒相结合的单原子催化剂具有指导意义。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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