Tailoring olefin distribution via tuning rare earth metals in bifunctional Cu-RE/beta-zeolite catalysts for ethanol upgrading

被引:7
作者
Li, Meijun [1 ]
Zhang, Junyan [2 ]
Purdy, Stephen C. [1 ]
Lin, Fan [3 ,4 ]
Unocic, Kinga A. [5 ]
Cordon, Michael [1 ]
Wu, Zili [2 ,5 ]
Wang, Huamin [3 ,4 ]
Hall, Jacklyn [6 ]
Kropf, A. Jeremy [6 ]
Krause, Theodore R. [6 ]
Davison, Brian [7 ]
Li, Zhenglong [1 ,8 ]
Sutton, Andrew D. [1 ]
机构
[1] Oak Ridge Natl Lab, Mfg Sci Div, Oak Ridge, TN 37830 USA
[2] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37830 USA
[3] Pacific Northwest Natl Lab, Energy Proc & Mat Div, Richland, WA 99354 USA
[4] Pacific Northwest Natl Lab, Inst Integrated Catalysis, Richland, WA 99354 USA
[5] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37830 USA
[6] Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
[7] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37830 USA
[8] Zhejiang Univ, Coll Biosyst Engn & Food Sci, Hangzhou 310058, Peoples R China
来源
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2024年 / 344卷
关键词
Ethanol; Alkenes; Rare earth metals; Lewis acid Zeolite catalysts; Decarbonization; BETA-ZEOLITE; CONVERSION; CONDENSATION; ACETALDEHYDE; BUTADIENE; AMMONIA; ACIDITY; SURFACE; SITES;
D O I
10.1016/j.apcatb.2023.123648
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Bioethanol to middle distillate technologies have offered a unique solution to produce renewable aviation fuel for decarbonizing the hard-to-electrify sectors. Here, we have developed the series of bimetallic Cu- and rare earth-containing (RE) Beta zeolite catalysts that yield high C3+ alkene selectivity from ethanol upgrading (>80% selectivity at similar to 100% conversion, 623 K). The formation rates of butene isomers to C5+ alkenes are linearly correlated with the strength of Lewis acidic RE identity, which follows the sequence of Yb-12/Beta >Y-7/Beta > Gd-12/Beta > Ce-10/Beta > La-12/Beta. Rate measurements indicate that the RE selection plays the vital role in altering the rate of the key competitive reactions within the ethanol-to-alkenes reaction network, namely C-4 alcohol dehydration and C-C chain growth, which dictate alkene product distributions. These findings indicate a feasible and promising method for tailoring alkene product distributions from ethanol upgrading, which is of notable significance to the generation of renewable middle distillates.
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页数:12
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