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Ultralow-Loading Pt/Zn Hybrid Cluster in Zeolite HZSM-5 for Efficient Dehydroaromatization
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2022-06-24 , DOI: 10.1021/jacs.2c04278
Genwei Chen 1 , Lingzhe Fang 2 , Tao Li 2, 3 , Yizhi Xiang 1
Affiliation  

Minimizing Pt loading without sacrificing catalytic performance is critical, particularly for designing cost-efficient hydrocarbon transformation catalysts. Here, we show that ultralow-loading (0.001–0.05 wt %) Pt- and Zn-functionalized HZSM-5 catalysts, prepared through simple ion exchange and impregnation, are highly active and stable for light alkane dehydroaromatization (DHA). The specific activity of benzene, toluene, and xylene is up to 8.2 mol/gPt/min (or 1592 min–1) over the 0.001 wt % Pt–Zn2/HZSM-5 catalyst during ethane DHA at 550 °C under atmospheric pressure. Additionally, such bimetallic Ptx–Zny/HZSM-5 catalysts are highly stable in contrast to the monometallic Pt/HZSM-5 catalysts. The rate constant of deactivation (kdeactiv), according to the first-order generalized power law equation model, for the bimetallic catalysts is up to 120 times lower than that of the monometallic counterparts, depending on the Pt loading. This breakthrough is achieved through the formation of the [Pt1–Znn]δ+ hybrid cluster, instead of Pt0 cluster–proton adducts, in the micropores of the ZSM-5 zeolite.

中文翻译:

沸石 HZSM-5 中的超低负载 Pt/Zn 杂化簇用于高效脱氢芳构化

在不牺牲催化性能的情况下最小化 Pt 负载至关重要,特别是对于设计具有成本效益的烃类转化催化剂而言。在这里,我们展示了通过简单的离子交换和浸渍制备的超低负载量(0.001-0.05 wt%)Pt 和 Zn 功能化 HZSM-5 催化剂对于轻质烷烃脱氢芳构化(DHA)具有高活性和稳定性。在 550 °C 常压条件下,乙烷 DHA中苯、甲苯和二甲苯的比活性比 0.001 wt % Pt–Zn 2 /HZSM-5 催化剂高达 8.2 mol/g Pt /min(或 1592 min –1 )压力。此外,这种双金属 Pt x –Zn y与单金属 Pt/HZSM-5 催化剂相比,/HZSM-5 催化剂高度稳定。根据一阶广义幂律方程模型,双金属催化剂的失活速率常数 ( k deactiv ) 比单金属催化剂低 120 倍,具体取决于 Pt 负载量。这一突破是通过在 ZSM-5 沸石的微孔中形成 [Pt 1 -Zn n ] δ+杂化簇而不是 Pt 0簇-质子加合物来实现的。
更新日期:2022-06-24
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