IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Reaction Chemistry & Engineering Pub Date : 2024-11-14 DOI:10.1039/D4RE00464G
Haobin Hu, Ke Ma, Zhenyu Cheng, Xinyu Qi, Haiyan Song, Zhijun Li, Yufeng Wang, Penghui Zhang, Chengyi Dai and Xiaoxun Ma
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摘要

甲醇制烯烃反应是替代日益稀缺的石油资源的一条可行且前景广阔的技术路线。SAPO-34 沸石具有合适的酸性和孔结构,是甲醇制烯烃反应的理想催化剂。然而,单一的沸石催化剂性能有限,在这项工作中,在 SAPO-34 分子筛上引入了金属物种,通过调节酸度获得更高的低碳烯烃选择性。然而,由于金属的引入会促进芳烃循环,从而产生碳质前体,缩短催化剂的使用寿命。因此,在载气中引入二氧化碳可抑制碳质前体的生成,从而延长催化剂的使用寿命。通过 XPS 表征了金属物种的存在及其对 SAPO-34 孔隙和结构的影响,通过 NH3-TPD 确定了酸量的变化,通过 CO2-TPD 确定了催化剂对 CO2 的吸附强度,从而揭示了催化剂的活性位点。该催化剂还实现了高低碳烯烃选择性和长催化剂寿命,其中低碳烯烃选择性为 88.0%。
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Effect of the presence of CO2 on the stability of the methanol-to-olefins reaction catalyzed by Zn/SAPO-34 zeolite

The methanol-to-olefins reaction is a viable and promising technological route to replace increasingly scarce petroleum resources. SAPO-34 zeolite is an ideal catalyst for the methanol-to-olefins reaction due to its suitable acidity and pore structure. However, a single zeolite catalyst has limited performance, and in this work, metal species were introduced on SAPO-34 molecular sieves to achieve higher low-carbon olefin selectivity through the modulation of acidity. However, since the introduction of metals promotes aromatic cycling, it allows the creation of carbonaceous precursors and reduces the catalyst lifetime. Therefore, the introduction of CO2 into the carrier gas inhibited the generation of carbonaceous precursors and thus prolonged the catalyst life. The presence of the metal species and their effects on SAPO-34's pores and structure were characterized by XPS, the change in acid amount was determined by NH3-TPD, and the adsorption strength of the catalyst for CO2 was determined by CO2-TPD, revealing the active sites of the catalyst. High low-carbon olefin selectivity and long catalyst life were also achieved, with low-carbon olefin selectivity of 88.0%.

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来源期刊
Reaction Chemistry & Engineering
Reaction Chemistry & Engineering Chemistry-Chemistry (miscellaneous)
CiteScore
6.60
自引率
7.70%
发文量
227
期刊介绍: Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society. From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.
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Back cover Correction: Intensification of silver nanoparticle synthesis through continuous flow split and recombine microreactors Correction: Rare-earth doped hexagonal NaYbF4 nanoprobes with size-controlled and NIR-II emission for multifunctional applications Back cover Self-optimising continuous-flow hydrothermal reactor for nanoparticle synthesis†
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