Dynamic Behavior of Pt Multimetallic Alloys for Active and Stable Propane Dehydrogenation Catalysts

IF 14.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2024-10-30 DOI:10.1021/jacs.4c0942410.1021/jacs.4c09424
Baraa Werghi, Shikha Saini, Pin-Hung Chung, Abinash Kumar, Amani M. Ebrahim, Kristen Abels, Miaofang Chi, Frank Abild-Pedersen, Simon R. Bare* and Matteo Cargnello*, 
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Abstract

Improving the use of platinum in propane dehydrogenation catalysts is a crucial aspect to increasing the efficiency and sustainability of propylene production. A known and practiced strategy involves incorporating more abundant metals in supported platinum catalysts, increasing its activity and stability while decreasing the overall loading. Here, using colloidal techniques to control the size and composition of the active phase, we show that Pt/Cu alloy nanoparticles supported on alumina (Pt/Cu/Al2O3) displayed elevated rates for propane dehydrogenation at low temperature compared to a monometallic Pt/Al2O3 catalyst. We demonstrate that the enhanced catalytic activity is correlated with a higher surface Cu content and formation of a Pt-rich core and Cu-rich shell that isolates Pt sites and increases their intrinsic activity. However, rates declined on stream because of dynamic metal diffusion processes that led to a more uniform alloy structure. This transformation was only partially inhibited by adding excess hydrogen to the feed stream. Instead, cobalt was introduced to provide trimetallic Pt/Cu/Co catalysts with stabilized surface structure and stable activity and higher rates than the original Pt/Cu system. The structure–activity relationship insights in this work offer improved knowledge of propane dehydrogenation catalyst development featuring reduced Pt loadings and notable thermal stability for propylene production.

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用于活性稳定丙烷脱氢催化剂的铂多金属合金的动态特性
改进丙烷脱氢催化剂中铂的使用是提高丙烯生产效率和可持续性的一个关键方面。一种已知且实用的策略是在支撑铂催化剂中掺入更丰富的金属,以提高其活性和稳定性,同时降低总负载量。在此,我们利用胶体技术控制活性相的大小和组成,结果表明,与单金属 Pt/Al2O3 催化剂相比,支撑在氧化铝上的 Pt/Cu 合金纳米颗粒(Pt/Cu/Al2O3)在丙烷低温脱氢过程中显示出更高的速率。我们证明,催化活性的提高与较高的表面铜含量以及富含铂的内核和富含铜的外壳的形成有关,后者可隔离铂位点并提高其内在活性。然而,由于金属的动态扩散过程导致合金结构更加均匀,其速率随流下降。在进料流中加入过量氢只能部分抑制这种转变。相反,通过引入钴,Pt/Cu/Co 三金属催化剂具有稳定的表面结构、稳定的活性和比原始 Pt/Cu 系统更高的速率。这项工作中对结构-活性关系的深入研究为丙烷脱氢催化剂的开发提供了更多的知识,这些催化剂具有降低铂载量和显著的热稳定性,可用于丙烯生产。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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