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Direct Conversion of Syngas to Light Olefins over a ZnCrO _x + H-SSZ-13 Bifunctional Catalyst.

ABSTRACT: In recent years, bifunctional catalysts for the syngas-to-olefins (STO) reaction via the oxide-zeolite (OX-ZEO) strategy has been intensively investigated. However, the bifunctional catalyst containing H-SSZ-13 with a 100% H⁺-exchanging degree for the STO reaction has not been developed because of the high selectivity to paraffin. Here, we report a ZnCrO _x + H-SSZ-13 bifunctional catalyst, which contains the submicron H-SSZ-13 with adequate acidic strength. Light olefins in hydrocarbon reached 70.8% at a CO conversion of 20.9% over the ZnCrO _x + H-SSZ-13(23S) bifunctional catalyst at 653 K, 1.0 MPa, and GHSV = 6000 mL·g^-1·h^-1 after 800 min of STO reaction. The effect of CO and H₂ on the C-C coupling was discussed by carrying out the methanol-to-olefins (MTO) reaction under a similar atmosphere as that of the STO reaction. H₂ and CO should play a more dominant role than the conventional hydrogen transfer reaction on the undesired high selectivity of paraffins. These findings provide new insight into the design of the bifunctional catalyst for the STO process via the OX-ZEO strategy.

SUBMITTER: Huang Y

PROVIDER: S-EPMC8153927 | biostudies-literature | 2021 Apr

REPOSITORIES: biostudies-literature

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Direct Conversion of Syngas to Light Olefins over a ZnCrO x + H-SSZ-13 Bifunctional Catalyst.

Huang Yuxuan Y Ma Hongfang H Xu Zhiqiang Z Qian Weixin W Zhang Haitao H Ying Weiyong W

ACS omega 20210419 16

In recent years, bifunctional catalysts for the syngas-to-olefins (STO) reaction via the oxide-zeolite (OX-ZEO) strategy has been intensively investigated. However, the bifunctional catalyst containing H-SSZ-13 with a 100% H+-exchanging degree for the STO reaction has not been developed because of the high selectivity to paraffin. Here, we report a ZnCrO x + H-SSZ-13 bifunctional catalyst, which contains the submicron H-SSZ-13 with adequate acidic strength. Light ole ...[more]

PMID: 34056248

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Project description:The effect of the phase transformation of a FePO4 catalyst material from the tridymite-like (tdm) FePO4 to the α-domain (α-Fe3(P2O7)2) during the direct selective oxidation of methane to methanol was studied using oxidant species O2, H2O and N2O. The main reaction products were CH3OH, carbon dioxide and carbon monoxide, whereas formaldehyde was produced in rather minute amounts. Results showed that the single-step non-syngas activation of CH4 to oxygenate(s) on a solid FePO4 phase-specific catalyst was influenced by the nature of the oxidizer used for the CH4 turnover. Fresh and activated FePO4 powder samples and their modified physicochemical surface and bulk properties, which affected the conversion and selectivity in the partial oxidation (POX) mechanism of CH4, were investigated. Temperature-programmed re-oxidation (TPRO) profiles indicated that the type of moieties utilised in the procedures, determined the re-oxidizing pathway of the reduced multiphase FePO4 system. Mössbauer spectroscopy measurements along with X-ray diffraction (XRD) examination of neat, hydrogenated and spent catalytic compounds, demonstrated a variation of the phosphate into a mixture of crystallites, which depended on operating process conditions (for example time-on-stream). The Mössbauer spectra revealed the change of the initial ferric orthophosphate, FePO4 (tdm), to the divalent metal form, iron(ii) pyrophosphate (Fe2P2O7); thereafter, reactivity was governed by the interaction (strength) with individual oxidizing agents. The Fe3+ ↔ Fe2+ chemical redox cycle can play a key mechanistic role in tailored multistep design, while the advantage of iron-based heterogeneous catalysis primarily lies in being inexpensive and comprising non-critical raw resources. When compared to the other catalysts reported in the literature, the FePO4-tdm phase catalysts showed in this work exhibited a high activity towards methanol i.e., 12.3 × 10-3 μmolMeOH gcat h-1 using N2O as an oxidant. This catalyst also showed a high activity with O2 as an oxidant (5.3 × 10-3 μmolMeOH gcat h-1). Further investigations will include continuous reactor unit engineering optimisation.

Dataset Information

Direct Conversion of Syngas to Light Olefins over a ZnCrO _x + H-SSZ-13 Bifunctional Catalyst.

Publications

Direct Conversion of Syngas to Light Olefins over a ZnCrO <sub><i>x</i></sub> + H-SSZ-13 Bifunctional Catalyst.

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