Progressive formation of active and stable PtZn bimetallic nanoclusters by exsolution during propane dehydrogenation

Min, Hyung‐Ki; Oh, Sohun; Kim, Young Woo; Kim, Eun-Jeong; Kweon, Sungjoon; Lee, Siyeon; Park, Kwangho; Jung, Kwang‐Deog; Hyeok, Seung; Yun, Gwang-Nam; Park, Min Bum; Shin, Chae‐Ho

doi:10.1016/j.cej.2023.143241

Cited by 8 publications

(3 citation statements)

References 29 publications

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“…Excessive and strong Lewis acid sites in S-1 and aSiO 2 enhance coke formation, and weak Brønsted acid sites in MCM-41 and SBA-15 are not responsible for coking. , There is a trade-off between propylene productivity and coking, which is determined by the number of Lewis acid sites . It implies that intensive control of unsaturated Si atoms on silica is essential for constructing a highly efficient anticoking PDH catalyst . Specifically, the deactivation rate of each sample follows the order of the amount of coke, indicating that coking is the major reason for the drops in the catalytic activity of silica-supported PDH catalysts.…”

Section: Resultsmentioning

confidence: 99%

“…49 It implies that intensive control of unsaturated Si atoms on silica is essential for constructing a highly efficient anticoking PDH catalyst. 50 Specifically, the deactivation rate of each sample follows the order of the amount of coke, indicating that coking is the major reason for the drops in the catalytic activity of silica-supported PDH catalysts. Despite coking, the sintering of metallic sites is another common issue for catalyst deactivation.…”

Section: Coking and Sintering Of Silica-supported Ptzn Catalystsmentioning

confidence: 93%

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Exploring the Properties of Silica Nanomaterials on Supporting Bimetallic PtZn Sites for Direct Propane Dehydrogenation

Gao,

Zong,

Yue

et al. 2024

ACS Appl. Nano Mater.

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The performance of metal sites in terms of their formation, evolution, and deactivation is strongly influenced by the properties of the supports during catalysis. Nanomaterials offer a tailorable size, shape, and composition, along with a large surface area, a high fraction of surface atoms, and unique electronic properties, thereby significantly improving the efficiency, selectivity, stability, and versatility of catalytic processes. In the direct dehydrogenation of propane (PDH) reactions, the activity, selectivity, and durability of catalysts face challenges due to the high reaction temperature and harsh atmosphere that accompanies the presence of reducible reactants. Herein, bimetallic platinum− zinc (PtZn) sites were synthesized on various silica nanomaterials to investigate the correlation between the nanoscale properties of silica and PDH performance. Among the supports being explored, including amorphous SiO 2 particles, mesoporous SBA-15, microporous silicate-1, and mesoporous MCM-41, MCM-41 stood out due to its distinctive advantages, including a large specific surface area, well-portioned pore size and distribution, and an appropriate amount and strength of acidic sites. Operating at a temperature of 600 °C, the catalyst exhibited a notable propene production rate of approximately 37.3 mmol•g cat −1•h −1 . This performance was coupled with an outstanding initial conversion (39.2%) and selectivity (97.7%) during the PDH reaction. The characterization results highlighted the exceptional dispersion of the PtZn sites on the MCM-41 support, showing remarkable resistance to coking and sintering throughout the reaction. These attributes exceeded those observed in other silica supports.

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Section: Resultsmentioning

confidence: 99%

Section: Coking and Sintering Of Silica-supported Ptzn Catalystsmentioning

confidence: 93%

Exploring the Properties of Silica Nanomaterials on Supporting Bimetallic PtZn Sites for Direct Propane Dehydrogenation

Gao,

Zong,

Yue

et al. 2024

ACS Appl. Nano Mater.

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“…For example, rare earth metals (La, Y, Ce), − transition metals (Ti, Cu, Zn, Co, etc. ), − and nonmetals (B, Si, S) − have been employed to improve strong metal–support interactions (SMSIs) or form alloys/intermetallics to suppress sintering or side reactions in many dehydrogenation studies. Among them, Sn and Ga, which act as promoters, have been successfully applied in commercial processes.…”

Section: Introductionmentioning

confidence: 99%

In Situ-Formed PtMn Intermetallic Subnanoclusters on Mn-Doped Mesoporous Al₂O₃ as Efficient Catalysts for Propane Dehydrogenation

Tian,

Cai,

Zhao

et al. 2024

ACS Appl. Nano Mater.

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Pt-based catalysts have been widely investigated for propane dehydrogenation (PDH) due to their superior activation of C−H bonds. It is still a challenge to develop highly dispersed Ptbased catalysts with an excellent PDH performance. Herein, we designed in situ-formed PtMn intermetallic nanoclusters on Mndoped mesoporous Al 2 O 3 as efficient catalysts for PDH. A series of characterizations demonstrated that well-dispersed PtMn intermetallic nanoclusters were in situ-formed and did not aggregate into large ensembles during PDH reactions. The PtMn intermetallic nanoclusters reduced the activation temperature of C−H cleavage and improved the PDH performance. The specific activity of the Pt/2Mn-Al 2 O 3 catalyst was 0.81 mol C3H6 mol Pt −1 s −1 at 600 °C, which is comparable to that of most of the state-of-theart PtM bimetallic nanocatalysts. Moreover, the catalyst exhibited better stability than the undoped catalyst, which resulted from the antisintering effect of the PtMn intermetallic nanoclusters and the migration of coke from the Pt sites to the support. Thus, the Pt/ 2Mn-Al 2 O 3 catalyst exhibited excellent regeneration stability with recoverable propane conversion and selectivity for propylene after removing coke.

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Elucidating the promoting advantages and fundamentals for their creation in Sn-modified commercial CrOx/Al2O3 catalyst for propane dehydrogenation

Zhang,

Chen,

Chen

et al. 2024

Chemical Engineering Journal

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Progressive formation of active and stable PtZn bimetallic nanoclusters by exsolution during propane dehydrogenation

Cited by 8 publications

References 29 publications

Exploring the Properties of Silica Nanomaterials on Supporting Bimetallic PtZn Sites for Direct Propane Dehydrogenation

Exploring the Properties of Silica Nanomaterials on Supporting Bimetallic PtZn Sites for Direct Propane Dehydrogenation

In Situ-Formed PtMn Intermetallic Subnanoclusters on Mn-Doped Mesoporous Al₂O₃ as Efficient Catalysts for Propane Dehydrogenation

Elucidating the promoting advantages and fundamentals for their creation in Sn-modified commercial CrOx/Al2O3 catalyst for propane dehydrogenation

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Progressive formation of active and stable PtZn bimetallic nanoclusters by exsolution during propane dehydrogenation

Cited by 8 publications

References 29 publications

Exploring the Properties of Silica Nanomaterials on Supporting Bimetallic PtZn Sites for Direct Propane Dehydrogenation

Exploring the Properties of Silica Nanomaterials on Supporting Bimetallic PtZn Sites for Direct Propane Dehydrogenation

In Situ-Formed PtMn Intermetallic Subnanoclusters on Mn-Doped Mesoporous Al2O3 as Efficient Catalysts for Propane Dehydrogenation

Elucidating the promoting advantages and fundamentals for their creation in Sn-modified commercial CrOx/Al2O3 catalyst for propane dehydrogenation

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Product

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In Situ-Formed PtMn Intermetallic Subnanoclusters on Mn-Doped Mesoporous Al₂O₃ as Efficient Catalysts for Propane Dehydrogenation