Effective conversion of CO2 into lower olefins over GaCrZrOx/SAPO-34 tandem catalysts

[Display omitted] •GaCrZrOx(y%)/SAPO-34 was designed for efficient CO2 hydrogenation to C2=–C4=.•The addition of Cr strengthen the adsorption and activation of CO2 and H2.•The addition of Cr promote formation of formate and methoxy intermediates.•Integration manner of tandam catalyst is vital to pro...

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Veröffentlicht in:Separation and purification technology 2025-03, Vol.355, p.129743, Article 129743
Hauptverfasser: Wang, Ying, Liu, Fei, Yao, Mengqin, Ma, Jun, Geng, Shuo, Cao, Jianxin, Wang, Xiaodan
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Sprache:eng
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Zusammenfassung:[Display omitted] •GaCrZrOx(y%)/SAPO-34 was designed for efficient CO2 hydrogenation to C2=–C4=.•The addition of Cr strengthen the adsorption and activation of CO2 and H2.•The addition of Cr promote formation of formate and methoxy intermediates.•Integration manner of tandam catalyst is vital to promote catalytic performance.•The selectivity of C2=–C4= exceeds 85 % and CO2 conversion is close to 30 %. Promoting the efficient formation of methanol intermediates during CO2 hydrogenation to lower olefins plays a decisive role in improving the catalytic performance of a tandem catalyst. In this study, a series of chromium (Cr)-modified gallium–zirconium oxides with the formula GaCrZrOx(y%) were prepared via the sol–gel method. The characterization and experimental results show that the addition of moderate amounts of Cr not only facilitates the formation of more oxygen vacancies on the surface of GaZrOx but also strengthens the adsorption and activation ability of CO2 and H2, thereby promoting the generation of formate and methoxy intermediates. After coupling with SAPO-34 zeolite, the methanol intermediate produced on GaCrZrOx(y%) is rapidly converted into lower olefins. This integration manner oxide and zeolite catalysts is particularly important for catalytic performance because an appropriate affinity between components can induce the formation of methanol intermediates via the kinetic effect, which limits the reverse water–gas shift reaction at high temperature. The GaCrZrOx(3.0 %)/SAPO-34 tandem catalyst synthesized via grinding and mixing at 390 °C and 3 MPa exhibits remarkable stability and catalytic performance, achieving a CO2 conversion close to 30 %, a lower olefin selectivity of 85.8 %, and a lower olefin yield of 11.7 %.
ISSN:1383-5866
DOI:10.1016/j.seppur.2024.129743