Boosting the catalytic performance of core-shell structured Ru@Pd/SBA-15 in 2-ethyl-anthraquinone hydrogenation by tuning d-band center

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Catalysis Pub Date : 2024-10-15 DOI:10.1016/j.jcat.2024.115793

Yue Zhang , Rongrong Zhang , Guozhu Liu , Li Wang , Zhiyong Pan

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Abstract

Core-shell Ru@Pd/SBA-15 catalysts with various atomic layer numbers of Pd were prepared by changing the Pd/Ru ratio and Pd coating temperature. The results of characterizations show that the compressive strain of Pd atoms and electron transfer from Ru to Pd result in a downward shift in the d-band center of core–shell catalysts. Density functional theory calculations further reveal that the reduced d-band center of Pd via strain and electronic effects weakens the adsorption ability of Pd. A roughly volcano-shaped correlation between the d-band center and 2-ethyl-anthraquinone (EAQ) hydrogenation activity is experimentally observed. The catalyst with Pd shell of 2 atomic layers provides medium adsorption strength for EAQ and hydrogenated product, thereby exhibiting the highest activity of 0.37 molH₂·gMet⁻¹·min⁻¹, with a selectivity of 97.3%. This work provides a facile strategy for optimizing hydrogenation performance by modulating the strain and electron effects between the Ru core and Pd shell through regulating the number of shell layers.

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通过调整 d 带中心提高核壳结构 Ru@Pd/SBA-15 在 2-乙基蒽醌加氢反应中的催化性能

通过改变 Pd/Ru 比率和 Pd 涂层温度，制备了具有不同 Pd 原子层数的核壳 Ru@Pd/SBA-15 催化剂。表征结果表明，Pd 原子的压缩应变和电子从 Ru 转移到 Pd 导致核壳催化剂的 d 带中心下移。密度泛函理论计算进一步表明，由于应变和电子效应，钯的 d 带中心下移，从而削弱了钯的吸附能力。实验观察到，d-带中心与 2-乙基蒽醌（EAQ）氢化活性之间大致呈火山状相关。具有 2 个原子层钯壳的催化剂对 EAQ 和氢化产物具有中等吸附强度，因此活性最高，达到 0.37 molH2-gMet-1-min-1，选择性为 97.3%。这项工作提供了一种简便的策略，通过调节外壳层数来调节 Ru 内核与 Pd 外壳之间的应变和电子效应，从而优化氢化性能。

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来源期刊

Journal of Catalysis 工程技术-工程：化工

CiteScore

12.30

自引率

5.50%

发文量

447

审稿时长

31 days

期刊介绍： The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.