Direct transformation of syngas to lower olefins synthesis over hybrid Zn–Al<sub>2</sub>O<sub>3</sub>/SAPO-34 catalysts

Raveendra, G.; Li, Congming; Cheng, Yong; Meng, Fanhui; Li, Zhong

doi:10.1039/c7nj04734g

Cited by 48 publications

(33 citation statements)

References 44 publications

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“…Different from FT reaction, which can only be catalyzed by Fe, Co and Ru, there are much more active catalysts for SMA process with methanol as intermediate. Besides typical Zn−Cr and Cu−Zn catalysts, actually many mixed oxides have been recently employed to combine with zeolite, to catalyze syngas to lower olefins, such as Zr−In, Zn−Al, Zn−Zr and Zn−Ga . Oxygen vacancies are often supposed to play a key role in the hydrogenation of CO to methanol over these mixed oxides, but there still requires substantial proof.…”

Section: Resultsmentioning

confidence: 99%

Selective Conversion of Syngas to Aromatics over a Mo−ZrO₂/H‐ZSM‐5 Bifunctional Catalyst

et al. 2019

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Direct conversion of syngas to aromatics is an extremely challenging target due to the complex reaction pathways. Herein, we present a well‐designed bifunctional catalyst composed of Mo‐doped ZrO2 nanoparticles and zeolite H‐ZSM‐5 for one‐step conversion of syngas to aromatics. The Mo−ZrO2 converts syngas to methanol as reaction intermediate, which can be successively converted to aromatics by H‐ZSM‐5. Hydrogenation ability of mixed oxides is pivotal to both selectivity and productivity of aromatics. We intensively clarify the individual role of catalyst components among CO activation, H2 activation and aromatization. With a Mo/Zr molar ratio of 1 : 68, the Mo−ZrO2/H‐ZSM‐5 resulted in 76 % selectivity of aromatics at 22 % CO conversion, and the productivity of aromatics reached 0.17 g gcat−1 h−1 at 400 °C and 4 MPa. Moreover, the distribution of aromatics can be tuned by surface modification of H‐ZSM‐5.

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Section: Resultsmentioning

confidence: 99%

Selective Conversion of Syngas to Aromatics over a Mo−ZrO₂/H‐ZSM‐5 Bifunctional Catalyst

et al. 2019

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“…More recently, using a bifunctional catalyst containing ZnCr oxide and SAPO-34 zeolite, Bao and coworkers 19 first reported direct synthesis of light olefins from syngas exhibiting an excellent selectivity of 80% (CO 2 free) for light olefins at ~17% CO conversion. Inspired by this pioneered work, several kinds of bifunctional catalysts to directly convert CO or CO 2 into light olefins were then developed, including ZnZr/SAPO-34 20 , ZnAl/SAPO-34 21 , MnO x /SAPO-34 22 , and InZr/SAPO-34 23 . Interestingly, as the selectivity of light olefins is close to that of the MTO reaction, this STO process therefore holds the potential to be a promising alternative to directly produce light olefins from syngas.…”

Section: Introductionmentioning

confidence: 99%

Syngas to light olefins conversion with high olefin/paraffin ratio using ZnCrOx/AlPO-18 bifunctional catalysts

Su¹,

Zhou²,

Liu³

et al. 2019

Nat Commun

135

113

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Direct synthesis of light olefins from syngas (STO) using a bifunctional catalyst composed of oxide and zeolite has attracted extensive attention in both academia and industry. It is highly desirable to develop robust catalysts that could enhance the CO conversion while simultaneously maintain high selectivity to C2-C4 olefins. Herein, we report a bifunctional catalyst consisting of ZnCr binary oxide (ZnCrOx) and low-Si AlPO-18 zeolite, showing both satisfying selectivity to C2-C4 olefins of 45.0% (86.7%, CO2 free) and high olefin/paraffin ratio of 29.9 at the CO conversion of 25.2% under mild reaction conditions (4.0 MPa, 390 °C). By optimizing the reaction conditions, the CO conversion could be markedly increased to 49.3% with a slight drop in selectivity. CD3CN/CO-FTIR characterizations and theoretical calculations demonstrate that low-Si AlPO-18 zeolite has lower acid strength, and is therefore less reactive toward the hydride transfer in the STO reaction, leading to a higher olefin/paraffin ratio.

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“…Besides the pioneer work reported by Jiao et al. on one step conversion of syngas to lower olefins using a bi‐functional catalyst (ZnCrO x &MSAPO), other works have been devoted to this bi‐functional catalyst method, including ZnZr&SAPO‐34, ZnAl&SAPO‐34, MnO x &SAPO‐34 and InZr&SAPO‐34 . Interestingly, all of these results exhibited an outstanding selectivity of lower olefins (about 70∼87 %) over the range of the Anderson‐Schulz‐Flory (ASF) distribution (∼58 %).…”

Section: Introductionmentioning

confidence: 96%

“…[3] Recently, bi-functional catalysts (Oxide-Zeolite concept) equipped with two kinds of active sites for the precise control of reaction process to achieve high selectivity of lower olefins have been attracted increasing attention due to this process is much more efficient in both economy and energy. [4] Besides the pioneer work reported by Jiao et al on one step conversion of syngas to lower olefins using a bi-functional catalyst (ZnCrO x &MSAPO), [5] other works have been devoted to this bi-functional catalyst method, including ZnZr&SAPO-34, [6] ZnAl&SAPO-34, [7] MnO x &SAPO-34 [8] and InZr&SAPO-34. [9] Interestingly, all of these results exhibited an outstanding selectivity of lower olefins (about 70~87 %) over the range of the Anderson-Schulz-Flory (ASF) distribution (~58 %).…”

Section: Introductionmentioning

confidence: 99%

Synthesis Gas Conversion to Lower Olefins over ZnCr‐SAPO‐34 Catalysts: Role of ZnO−ZnCr₂O₄ Interface

et al. 2020

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This work reports that the ZnO−ZnCr2O4 interface was constructed by tailoring the Zn/Cr ratio and the role of ZnO−ZnCr2O4 interface in activating CO molecule for the synthesis of lower olefins over a tandem catalyst was studied. A lower olefins selectivity of 71 % at a CO conversion of 34 % was achieving on Zn1Cr1&SAPO‐34. The presence of ZnO−ZnCr2O4 interface effectively reduces the activation energy of CO hydrogenation (from 51.8 kJ/mol to 33.6 kJ/mol) and subsequently leading to the triple increase of intrinsic activity. In situ DRIFTS and XPS studies demonstrate that the better catalytic activities of Zn1Cr1 catalyst are related to the presence of ZnO−ZnCr2O4 interface, which provides more oxygen vacancy sites for CO adsorption and activation. In this sense, the Zn1Cr1 catalyst with ZnO−ZnCr2O4 interface is more active than the simple physical mixture of ZnO and Cr2O3 catalyst separately and Zn1Cr2 catalyst. This work provides fundamental insights for a rational design of Zn−Cr based catalysts and even other heterogeneous catalysts by constructing oxide‐oxide interface.

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Direct transformation of syngas to lower olefins synthesis over hybrid Zn–Al₂O₃/SAPO-34 catalysts

Abstract: Syngas is a key platform chemical for the utilization of non-petroleum carbon resources.

Cited by 48 publications

References 44 publications

Selective Conversion of Syngas to Aromatics over a Mo−ZrO₂/H‐ZSM‐5 Bifunctional Catalyst

Selective Conversion of Syngas to Aromatics over a Mo−ZrO₂/H‐ZSM‐5 Bifunctional Catalyst

Syngas to light olefins conversion with high olefin/paraffin ratio using ZnCrOx/AlPO-18 bifunctional catalysts

Synthesis Gas Conversion to Lower Olefins over ZnCr‐SAPO‐34 Catalysts: Role of ZnO−ZnCr₂O₄ Interface

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Direct transformation of syngas to lower olefins synthesis over hybrid Zn–Al2O3/SAPO-34 catalysts

Abstract: Syngas is a key platform chemical for the utilization of non-petroleum carbon resources.

Cited by 48 publications

References 44 publications

Selective Conversion of Syngas to Aromatics over a Mo−ZrO2/H‐ZSM‐5 Bifunctional Catalyst

Selective Conversion of Syngas to Aromatics over a Mo−ZrO2/H‐ZSM‐5 Bifunctional Catalyst

Syngas to light olefins conversion with high olefin/paraffin ratio using ZnCrOx/AlPO-18 bifunctional catalysts

Synthesis Gas Conversion to Lower Olefins over ZnCr‐SAPO‐34 Catalysts: Role of ZnO−ZnCr2O4 Interface

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Direct transformation of syngas to lower olefins synthesis over hybrid Zn–Al₂O₃/SAPO-34 catalysts

Selective Conversion of Syngas to Aromatics over a Mo−ZrO₂/H‐ZSM‐5 Bifunctional Catalyst

Selective Conversion of Syngas to Aromatics over a Mo−ZrO₂/H‐ZSM‐5 Bifunctional Catalyst

Synthesis Gas Conversion to Lower Olefins over ZnCr‐SAPO‐34 Catalysts: Role of ZnO−ZnCr₂O₄ Interface