Silicon: A Surface Dopant for Stable Alumina-Supported PtGa Propane Dehydrogenation Catalysts by Favoring Redox and Carbon Dynamics

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Kazutaka Sakamoto, Milivoj Plodinec, Christoph R. Müller* and Christophe Copéret*, 
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引用次数: 0

Abstract

The exploitation of shale gas has stimulated the use of on-purpose propane dehydrogenation (PDH) technologies. These technologies rely on continuous and rapid catalyst regeneration to maintain high propene production. For Pt-based catalysts, metal promotors and additives, such as Ga and Si, have been shown to enhance the catalyst productivity and stability. While most studies have focused on understanding the role of Ga as a promoter, the effect and role of Si on the catalytic properties are less explored and understood. Therefore, tailored monometallic Pt and bimetallic Pt–Ga catalysts supported on alumina or Si-doped alumina are prepared via surface organometallic chemistry and evaluated under PDH conditions. The Pt catalyst containing both Ga and Si displays the highest propene productivity (1970 molC3= molPt–1 h–1 after 2 h) and the lowest deactivation constant (0.31 h–1 after 2 h), pointing out the critical role of both Ga and Si. While scanning transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy and X-ray absorption spectroscopy show that the catalyst structures of the as-reduced Pt–Ga catalysts are similar, postmortem analyses reveal that Si-doping of the alumina-supported Pt–Ga PDH catalyst modifies redox and carbon dynamics. This modification maintains Pt-active sites by yielding interfaces between Pt and GaOx domains along with a surface PtC structure that is correlated with increased structural dynamics and slower deactivation.

Abstract Image

Abstract Image

硅:一种支持氧化还原和碳动力学的稳定铝负载PtGa丙烷脱氢催化剂的表面掺杂剂
页岩气的开发促进了丙烷脱氢(PDH)技术的使用。这些技术依靠连续和快速的催化剂再生来保持高丙烯产量。对于pt基催化剂,金属促进剂和添加剂,如Ga和Si,已被证明可以提高催化剂的生产率和稳定性。虽然大多数研究都集中在了解Ga作为促进剂的作用,但Si对催化性能的影响和作用却很少被探索和了解。因此,通过表面有机金属化学制备了氧化铝或硅掺杂氧化铝负载的单金属Pt和双金属Pt - ga催化剂,并在PDH条件下进行了评价。同时含有Ga和Si的Pt催化剂表现出最高的丙烯产率(2h后为1970 molC3= molPt-1 h - 1)和最低的失活常数(2h后为0.31 h - 1),说明Ga和Si的作用至关重要。扫描透射电子显微镜、能量色散x射线光谱和x射线吸收光谱分析表明,还原态Pt-Ga催化剂的催化剂结构相似,事后分析表明,si掺杂的氧化铝负载的Pt-Ga PDH催化剂改变了氧化还原和碳动力学。这种修饰通过产生Pt和GaOx结构域之间的界面以及表面PtC结构来维持Pt活性位点,该结构与结构动力学增加和慢失活相关。
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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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