Ultralow-Loading Pt/Zn Hybrid Cluster in Zeolite HZSM-5 for Efficient Dehydroaromatization

Chen, Genwei; Fang, Lingzhe; Li, Tao; Xiang, Yizhi

doi:10.1021/jacs.2c04278

Ultralow-Loading Pt/Zn Hybrid Cluster in Zeolite HZSM-5 for Efficient Dehydroaromatization

Journal Article · Fri Jun 24 00:00:00 EDT 2022 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.2c04278· OSTI ID:2000074

Chen, Genwei ^[1]; Fang, Lingzhe ^[2]; ^[3]; ^[1]

Mississippi State Univ., Mississippi State, MS (United States)
Northern Illinois Univ., DeKalb, IL (United States)
Northern Illinois Univ., DeKalb, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

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/g_Pt/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 Pt_x–Zn_y/HZSM-5 catalysts are highly stable in contrast to the monometallic Pt/HZSM-5 catalysts. The rate constant of deactivation (k_deactiv), 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. In conclusion, this breakthrough is achieved through the formation of the [Pt₁–Zn_n]^δ+ hybrid cluster, instead of Pt⁰ cluster–proton adducts, in the micropores of the ZSM-5 zeolite.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2000074

Alternate ID(s):: OSTI ID: 1876074

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 26 Vol. 144; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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cluster chemistry
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light alkanes
platinum

Ultralow-Loading Pt/Zn Hybrid Cluster in Zeolite HZSM-5 for Efficient Dehydroaromatization

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