PtIn Alloy Supported on Y 2 O 3 ‑Modified δ‑Al 2 O 3 as a Propane Dehydrogenation Catalyst

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL
Jilei Lin, Meiqing Shen, Sifeng Bi, Gurong Shen, Feng Gao, Wei Li
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Abstract

Propylene production via propane dehydrogenation (PDH) over supported platinum (Pt) catalysts is a vital industrial process. However, rapid catalyst deactivation due to coking necessitates periodic regeneration under harsh oxidative conditions. While alloying Pt with transition metals significantly reduces coking, these alloy catalysts often exhibit poor regeneration stability. In this study, we demonstrate that supporting PtIn nanoparticles on Y2O3-modified δ-Al2O3 yields a PDH catalyst with significantly improved activity and stability. This catalyst achieves propane conversion rates close to the thermodynamic equilibrium at an ultralow Pt loading of 0.1 wt %, along with high propylene selectivity. Notably, this catalyst also exhibits remarkable regeneration stability. Through reaction-regeneration cycling experiments with various catalyst formulations, we reveal that the alloy effects between Pt and In are primarily responsible for enhanced catalyst stability under steady-state reaction conditions by suppressing coke formation. Meanwhile, the incorporation of Y2O3 as a support component significantly improves stability during regeneration. Density functional theory (DFT) calculations further elucidate the key factors contributing to the enhanced anticoking properties of the catalyst under PDH reaction conditions.
改性δ - al2o3负载PtIn合金丙烷脱氢催化剂
在负载型铂(Pt)催化剂上通过丙烷脱氢(PDH)生产丙烯是一个重要的工业过程。然而,由于焦化导致的催化剂快速失活需要在恶劣的氧化条件下定期再生。虽然将Pt与过渡金属合金化可以显著减少结焦,但这些合金催化剂通常表现出较差的再生稳定性。在这项研究中,我们证明了在y2o3修饰的δ-Al2O3上负载PtIn纳米颗粒可以得到活性和稳定性显著提高的PDH催化剂。该催化剂在0.1 wt %的超低铂负载下实现接近热力学平衡的丙烷转化率,同时具有很高的丙烯选择性。值得注意的是,该催化剂还表现出显著的再生稳定性。通过不同催化剂配方的反应-再生循环实验,我们发现Pt和In之间的合金效应是通过抑制焦炭形成来提高稳态反应条件下催化剂稳定性的主要原因。同时,Y2O3作为支撑组分的加入显著提高了再生过程中的稳定性。密度泛函理论(DFT)计算进一步阐明了PDH反应条件下催化剂抗结焦性能增强的关键因素。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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