在超低铂负载的 Pt-Zn/HZSM-5 催化剂上进行轻烷脱氢芳构化反应

IF 2.8 3区 化学 Q2 CHEMISTRY, APPLIED Topics in Catalysis Pub Date : 2024-01-31 DOI:10.1007/s11244-023-01903-7
Genwei Chen, Anthony Griffin, Zhe Qiang, Hossein Toghiani, Yizhi Xiang
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引用次数: 0

摘要

尽量减少脱氢芳构化 (DHA) 催化剂中的铂负载量,对于经济高效地转化丰富的轻质烷烃用于能源和化工生产至关重要。我们小组最近的研究表明,铂负载量为 0.001-0.05 wt%(10-500 ppm)的 Pt-Zn/HZSM-5 催化剂对乙烷脱氢芳烃化具有很高的活性和稳定性(J Am Chem Soc 144(26):11831-11839, 2022)。在此,我们研究了此类催化剂的催化行为,尤其是在铂负载量进一步降低(10 ppm)的情况下,丙烷和乙烷 DHA 的催化行为。对于丙烷 DHA,我们发现铂负载量为 50-500 ppm 的双金属 Pt-Zn/HZSM-5 催化剂的活性和/或稳定性明显高于单金属催化剂。当铂负载量降低到 ≤10ppm 时,这种增强效果就不那么明显了。对于乙烷 DHA,Pt-Zn/HZSM-5 催化剂的质量比活性随着铂负载量从 10ppm 降低到 2.5ppm 几乎呈线性下降,显示出高达 132 s-1 (摩尔烷/摩尔铂)的恒定摩尔比活性 (TOF)。这一突破是由于在 ZSM-5 沸石的微孔中形成了 [Pt1-Znn]δ+ 组合。
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Light Alkane Dehydroaromatization over Pt-Zn/HZSM-5 Catalyst with Ultralow Pt Loading

Minimizing Pt loading in dehydroaromatization (DHA) catalysts is critical to the cost-efficient transformation of abundant light alkanes for energy and chemical production. Recent studies in our group show that Pt-Zn/HZSM-5 catalysts with Pt loading of 0.001–0.05 wt% (10–500 ppm) are highly active and stable for ethane DHA (J Am Chem Soc 144(26):11831–11839, 2022). Here, we investigated the catalytic behavior of such catalysts, especially with further decreased Pt loading (< 10 ppm), in both propane and ethane DHA. For propane DHA, we show that the bimetallic Pt-Zn/HZSM-5 catalysts with Pt loading of 50–500 ppm are significantly more active and/or stable than the monometallic counterparts. Such enhancement becomes less significant when decreasing Pt loading to ≤10 ppm. For ethane DHA, the mass-specific activity of the Pt-Zn/HZSM-5 catalysts decreases almost linearly with decreasing Pt loading from 10 to 2.5 ppm, indicating a constant molar-specific activity (TOF) of up to 132 s−1 (molethane/molPt). This breakthrough is achieved owing to the formation of [Pt1-Znn]δ+ ensemble in the micropores of ZSM-5 zeolite.

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来源期刊
Topics in Catalysis
Topics in Catalysis 化学-物理化学
CiteScore
5.70
自引率
5.60%
发文量
197
审稿时长
2 months
期刊介绍: Topics in Catalysis publishes topical collections in all fields of catalysis which are composed only of invited articles from leading authors. The journal documents today’s emerging and critical trends in all branches of catalysis. Each themed issue is organized by renowned Guest Editors in collaboration with the Editors-in-Chief. Proposals for new topics are welcome and should be submitted directly to the Editors-in-Chief. The publication of individual uninvited original research articles can be sent to our sister journal Catalysis Letters. This journal aims for rapid publication of high-impact original research articles in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis.
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