Formation of active species for propane dehydrogenation with hydrogen sulfide co-feeding over transition metal catalyst

Watanabe, Ryo; Hirata, Naru; Miura, Kazuya; Yoda, Yuta; Fushimi, Yuya; Fukuhara, Choji

doi:10.1016/j.apcata.2019.117238

Cited by 29 publications

(26 citation statements)

References 53 publications

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“…Various metal oxides supported zeolite have been widely investigated for light alkane (i.e., methane, ethane, propane) conversion, including precious metal Pt [18,19] and transition metal Zn [20][21][22][23][24][25], Ga [26][27][28][29][30], Mo [31,32], Co [33], Zr [34][35][36] oxides, etc. Moreover, metal modification also has a potential effect on the acidity of ZSM-5.…”

Section: Introductionmentioning

confidence: 99%

Relationship between Acidity and Activity on Propane Conversion over Metal-Modified HZSM-5 Catalysts

Zhou

Zhang

et al. 2021

Catalysts

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A systematic study of the comparative performances of different metal-impregnated HZSM-5 catalysts (Zn, Ga, Mo, Co, and Zr) for propane conversion is presented. The physicochemical properties of catalysts were characterized by means of XRD, BET, SEM, TEM, FTIR, XPS, 27Al MAS NMR, NH3-TPD and Py-FTIR. It was found that the acidities of the catalysts were significantly influenced by loading metal. More specifically, Mo-, Co- or Zr-modified catalysts showed a large metal size and low acidic density, resulting high olefin selectivity, while Zn- or Ga-modified catalysts maintained their small metal size and acidic density, and mainly reduced B/L due to the Lewis acid sites created by Zn or Ga species, resulting in high aromatics selectivity. Experimental results also showed that there is a balance between metals size and medium and strong acidity on propane conversion. Moreover, based on the different acidity of metal-modified HZSM-5 catalysts, the mechanism of propane conversion was also discussed.

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Section: Introductionmentioning

confidence: 99%

Relationship between Acidity and Activity on Propane Conversion over Metal-Modified HZSM-5 Catalysts

Zhou

Zhang

et al. 2021

Catalysts

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“…Previous study shows that Co and Fe in transition metals exhibit well performance on oxidative dehydrogenation of higher alkanes. To compare the difference of catalytic effect between Cr, Co and Fe on the reaction between ethane andCO 2 , the catalytic performance of different transition metal catalysts with different temperature is displayed in Figure .…”

Section: Resultsmentioning

confidence: 92%

Research on the Selectivity and Activity of Ethane Oxidation Dehydrogenation with CO ₂ on Cr‐based Catalyst

Yang

Liu

et al. 2020

ChemistrySelect

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Catalysts containing different Cr load (5 %∼15 %) supported on SiO2 were prepared using the incipient wetness impregnation method. The influence of Cr load was investigated for the ethane oxidation dehydrogenation with CO2 and the difference between Co, Fe and Cr were compared. The catalytic activity is affected by the load of the Cr/SiO2.Cr‐10 %/SiO2 exhibits best catalytic performance, providing ethane conversion of 30.53 % as well as 98.64 % ethylene selectivity at 650 °C. Excessive load increases the aggregation and grain size of active phase, which goes against catalytic activity. Furthermore, overload increases the crystallization of α‐Cr2O3, which is difficult for reduction and is adverse for catalytic activity. Ethane conversion of Cr, Co and Fe based catalysts is corresponding to redox ability. Cr‐10 %/SiO2(30.53 %) takes the lead and Fe‐10 %/SiO2 is the least active (18.98 %). Co‐10 %/SiO2 is suitable for reforming reaction as its ethylene selectivity is only 19.60 % at 650 °C.

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“…Pure iron is known to suffer from runaway coking under PDH 44,60 conditions, while other Fe-based materials, such as Fe 3 C 44 and FeS, 50,51 have shown high coke resistance. Here, we perform GCMC and ab initio thermodynamics analyses to better understand why these materials are resistant to coke formation.…”

Section: Coke Formation On Iron Carbide Iron Sulfide and Fe/al Alloysmentioning

confidence: 99%

“…Coke formation on catalyst surfaces is a major cause of catalyst deactivation in several industrial reactions involving hydrocarbon-rich environments, such as Fischer-Tropsch synthesis, [33][34][35][36] methane reforming, [37][38][39][40] CO 2 reduction, 41 fluid catalytic cracking, 42,43 and hydrocarbon dehydrogenation. 44,45 Various strategies have been developed to suppress coke formation, typically by adding promoters and dopants, [46][47][48] forming metal phosphides or sulfides, [49][50][51][52] forming nitrides or carbides, 44,53 or alloying with less carbophilic metals. [54][55][56] The particular interest in this work is the suppression of coke formation during nonoxidative propane dehydrogenation (PDH).…”

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confidence: 99%

“…Sun et al 46,47,61 found that coke formation can be suppressed during PDH by either adding sulfate during the catalyst preparation stage or by cofeeding SO 2 with the hydrocarbon reactants. Watanabe et al 50,51 found that the iron sulfide formed in situ by cofeeding H 2 S can suppress coke build-up. Similarly, Tan et al 44 showed that adding phosphate during the catalyst preparation stage greatly increased the coking resistance of Fe-based PDH catalysts.…”

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confidence: 99%

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Modeling phase formation on catalyst surfaces: Coke formation and suppression in hydrocarbon environments

Wang

Senftle

2021

AIChE Journal

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We develop a simulation toolset employing density functional theory in conjunction with grand canonical Monte Carlo (GCMC) to study coke formation on Fe-based catalysts during propane dehydrogenation (PDH). As expected, pure Fe surfaces develop stable graphitic coke structures and rapidly deactivate. We find that coke formation is markedly less favorable on Fe 3 C and FeS surfaces. Fe-Al alloys display varying degrees of coke resistance, depending on their composition, suggesting that they can be optimized for coke resistance under PDH conditions. Electronic structure analyses show that both electron-withdrawing effects (on Fe 3 C and FeS) and electron-donating effects (on Fe-Al alloys) destabilize adsorbed carbon. On the alloy surfaces, a geometric effect also isolates Fe sites and disrupts the formation of graphitic carbon networks. This work demonstrates the utility of GCMC for studying the formation of disordered phases on catalyst surfaces and provides insights for improving the coke resistance of Fe-based PDH catalysts.

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Formation of active species for propane dehydrogenation with hydrogen sulfide co-feeding over transition metal catalyst

Cited by 29 publications

References 53 publications

Relationship between Acidity and Activity on Propane Conversion over Metal-Modified HZSM-5 Catalysts

Relationship between Acidity and Activity on Propane Conversion over Metal-Modified HZSM-5 Catalysts

Research on the Selectivity and Activity of Ethane Oxidation Dehydrogenation with CO ₂ on Cr‐based Catalyst

Modeling phase formation on catalyst surfaces: Coke formation and suppression in hydrocarbon environments

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Formation of active species for propane dehydrogenation with hydrogen sulfide co-feeding over transition metal catalyst

Cited by 29 publications

References 53 publications

Relationship between Acidity and Activity on Propane Conversion over Metal-Modified HZSM-5 Catalysts

Relationship between Acidity and Activity on Propane Conversion over Metal-Modified HZSM-5 Catalysts

Research on the Selectivity and Activity of Ethane Oxidation Dehydrogenation with CO 2 on Cr‐based Catalyst

Modeling phase formation on catalyst surfaces: Coke formation and suppression in hydrocarbon environments

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Research on the Selectivity and Activity of Ethane Oxidation Dehydrogenation with CO ₂ on Cr‐based Catalyst