One-step conversion of syngas to light olefins over bifunctional metal-zeolite catalyst

Du, Ce; Chizema, Linet Gapu; Hondo, Emmerson; Tong, Ming‐Liang; Ma, Qingxiang; Gao, Xinhua; Yang, Renqiang; Lu, Peng; Tsubaki, Noritatsu

doi:10.1016/j.cjche.2020.09.004

Cited by 11 publications

(5 citation statements)

References 35 publications

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“…When the reaction pressure was further increased, the CO conversion significantly increased to 20.3%, and the lower olefins selectivity slightly decreased to 80%. According to earlier reports, 30,70 the reaction pressures has a significant effect on the activation of surface carbon species because it increases the probability of the reaction. In contrast, the active catalyst surfaces increase the interaction rate and product selectivity.…”

Section: Catalytic Activity Studymentioning

confidence: 93%

A bifunctional Zn/ZrO₂–SAPO-34 catalyst for the conversion of syngas to lower olefins induced by metal promoters

et al. 2023

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Section: Catalytic Activity Studymentioning

confidence: 93%

A bifunctional Zn/ZrO₂–SAPO-34 catalyst for the conversion of syngas to lower olefins induced by metal promoters

et al. 2023

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“…Hence, it is quite challenging to design and develop metal oxides that can effectively activate CO 2 and inhibit the formation of CO. Naturally, molecular sieves also have a significant impact on the performance of bifunctional catalysts, which is in addition to the metal oxides [25–26] . According to Kolboe's [27] proposed hydrocarbon pool mechanism (HCP), lower olefins produced by the MTO reaction first form a ring of organic intermediate species inside the molecular sieve cage before diffusing out through the pore channels.…”

Section: Introductionmentioning

confidence: 99%

“…Naturally, molecular sieves also have a significant impact on the performance of bifunctional catalysts, which is in addition to the metal oxides. [25][26] According to Kolboe's [27] proposed hydrocarbon pool mechanism (HCP), lower olefins produced by the MTO reaction first form a ring of organic intermediate species inside the molecular sieve cage before diffusing out through the pore channels. Since the SAPO-34 molecular sieve has strong shape selectivity and stable hydrothermal properties, the pore diameter inside the cage of the SAPO-34 molecular sieve is comparable to the kinetic diameter of tiny molecules like ethylene and propylene, [28] it has been widely employed in MTO processes.…”

Section: Introductionmentioning

confidence: 99%

Highly Active Catalytic CO₂ Hydrogenation to Lower Olefins via Spinel ZnGaO_x Combined with SAPO‐34

Yuan

Zheng

Ren

et al. 2023

Chemistry An Asian Journal

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A key primary method for creating a carbon cycle and carbon neutrality is the catalytic hydrogenation of CO 2 into high value-added chemicals or fuels. In this work, ZnGaO x oxides were prepared by parallel co-precipitation and physically mixed with SAPO-34 molecular sieves prepared by hydrothermal synthesis to produce ZnGaO x /SAPO-34 bifunctional catalysts, which were evaluated for the catalytic synthesis of lower olefins (C 2 = À C 4 = ) from carbon dioxide hydrogenation. It was demonstrated that the reaction process requires oxygen defect activation, synergistic hydrogenation, and CO 2 alkaline adsorption of ZnGaO x . The spinel structure of ZnGaO x has more abundant oxygen defects and alkaline adsorption sites than the ZnGaO x solid solution, which effectively enhances the catalytic performance. The CO 2 conversion was 28.52%, the selectivity of C 2 = À C 4 = in hydrocarbons reached 70.01%, and the single-pass yield of C 2 = À C 4 = was 10.95% at 370 °C, 3.0 MPa, and 4800 mL/g cat /h.

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“…Du and co-workers reported that the MnO x /H-SAPO-34 composite showed a CO 2 selectivity of 24.3% at 380 °C, 2.5 MPa and H 2 /CO ratio of 2, although MnZrO x (Mn/Zr = 4/1)/H-SAPO-34 gave a CO 2 selectivity of 48.4% at the same conditions . This indicates that metal oxide compositions considerably influence the amount of CO 2 formation.…”

mentioning

confidence: 99%

“…The preparation method of metal oxide also has a great effect on the catalytic performance. Upon coupling with H-SAPO-34, MnO x oxides prepared by precipitating an aqueous manganese nitrate solution with sodium carbonate, by precipitating a manganese sulfate water-glycerol solution with ammonium carbonate, and by precipitating an aqueous manganese nitrate solution with ammonium bicarbonate show a CO 2 selectivity of 24.3%, ∼33% and 43.4%, respectively, at similar conditions (380–410 °C, 2.5 MPa and H 2 /CO = 2.0–2.5) due to the different electronic structure and/or particle size of MnO x oxides. − …”

mentioning

confidence: 99%

Reply to the Comment on “Direct Conversion of Syngas into Light Olefins with Low CO₂ Emission”

Wang,

Fan

2023

ACS Catal.

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The purpose of this Reply is to account for the possible reasons for the difference in catalytic performance of ZnCeZrO x /H-SAPO-34 composites prepared by Loridant et al. and our group. Loridant et al. assumed that CO 2 formation is dominantly controlled by thermodynamics, viz., CO 2 selectivity is in the range of 42−51% regardless of sample compositions and reaction conditions. However, this assumption contradicts with many reported catalytic results that the CO 2 selectivity is less than 40% in syngas conversion to hydrocarbons, and it is highly dependent on the structure, chemical compositions, elemental distributions, and particle size of the metal oxide; the pore structure, crystal morphology, and acidity of the zeolite component; the distance between metal oxide and zeolite particles; and the reaction conditions. This is obviously manifested by the seriously different catalytic results obtained on Loridant's and our ZnCeZrO x /H-SAPO-34 composites; Loridant's samples show far higher selectivity to CH 4 and CO 2 but lower selectivity to C 2 = -C 4 = and lower O/P ratio than our samples. This is because Loridant's and our samples have significantly different metal oxide crystalline structure, particle size, and elemental distributions as well as zeolite acidity that determines MTO and further CO-to-olefins catalytic performance.

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One-step conversion of syngas to light olefins over bifunctional metal-zeolite catalyst

Cited by 11 publications

References 35 publications

A bifunctional Zn/ZrO₂–SAPO-34 catalyst for the conversion of syngas to lower olefins induced by metal promoters

A bifunctional Zn/ZrO₂–SAPO-34 catalyst for the conversion of syngas to lower olefins induced by metal promoters

Highly Active Catalytic CO₂ Hydrogenation to Lower Olefins via Spinel ZnGaO_x Combined with SAPO‐34

Reply to the Comment on “Direct Conversion of Syngas into Light Olefins with Low CO₂ Emission”

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One-step conversion of syngas to light olefins over bifunctional metal-zeolite catalyst

Cited by 11 publications

References 35 publications

A bifunctional Zn/ZrO2–SAPO-34 catalyst for the conversion of syngas to lower olefins induced by metal promoters

A bifunctional Zn/ZrO2–SAPO-34 catalyst for the conversion of syngas to lower olefins induced by metal promoters

Highly Active Catalytic CO2 Hydrogenation to Lower Olefins via Spinel ZnGaOx Combined with SAPO‐34

Reply to the Comment on “Direct Conversion of Syngas into Light Olefins with Low CO2 Emission”

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A bifunctional Zn/ZrO₂–SAPO-34 catalyst for the conversion of syngas to lower olefins induced by metal promoters

A bifunctional Zn/ZrO₂–SAPO-34 catalyst for the conversion of syngas to lower olefins induced by metal promoters

Highly Active Catalytic CO₂ Hydrogenation to Lower Olefins via Spinel ZnGaO_x Combined with SAPO‐34

Reply to the Comment on “Direct Conversion of Syngas into Light Olefins with Low CO₂ Emission”