A tandem system of Cr/HZSM-5 and bismuth-modified CeZrO2 for coupling of ethane dehydrogenation to selective H2 combustion

IF 6.7 1区 工程技术 Q2 ENERGY & FUELS
Fuel Pub Date : 2025-05-28 DOI:10.1016/j.fuel.2025.135819
Ying Li, Haibo Zhao
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引用次数: 0

Abstract

Ethylene production via chemical looping oxidative dehydrogenation (CL-ODH) of ethane faces a critical challenge in balancing conversion efficiency and selectivity due to competing oxygen species requirements. Here, we present a bifunctional composite catalyst (CrH/BiCZ) by physically integrating a Cr-HZSM5 (Cr-H) dehydrogenation (DH) catalyst with a Bi2O3-Ce0.4Zr0.6O2 (Bi-CZ) selective hydrogen combustion (SHC) catalyst. This tandem system decouples ethane activation and hydrogen combustion, promoting the DH process of ethane through the in situ hydrogen combustion of the SHC catalyst. The Ce-Zr solid solution in Bi-CZ acts as an oxygen reservoir, enabling complete H2 combustion within 3 min and suppressing carbon deposition. This rapid hydrogen combustion shifts the reaction equilibrium towards ethylene production. At 650 °C, the optimized CrH/BiCZ catalyst achieves 84.1 % ethylene selectivity at 43.0 % ethane conversion, and maintains exceptional stability over 36 redox cycles. This work establishes a scalable chemical looping strategy for efficient ethylene synthesis.
Cr/HZSM-5与铋改性CeZrO2串联体系耦合乙烷脱氢与选择性H2燃烧
乙烷化学环氧化脱氢(CL-ODH)制乙烯面临着平衡转化效率和选择性的关键挑战。本文通过物理整合Cr-HZSM5 (Cr-H)脱氢(DH)催化剂和Bi2O3-Ce0.4Zr0.6O2 (Bi-CZ)选择性氢燃烧(SHC)催化剂,制备了一种双功能复合催化剂(CrH/BiCZ)。该串联系统将乙烷活化与氢燃烧解耦,通过SHC催化剂的原位氢燃烧促进乙烷的DH过程。Ce-Zr固溶体在Bi-CZ中充当氧气储存器,使H2在3分钟内完全燃烧,并抑制碳沉积。这种快速的氢燃烧使反应平衡转向乙烯生产。在650℃下,优化后的CrH/BiCZ催化剂在43.0%的乙烷转化率下,乙烯选择性达到84.1%,并且在36个氧化还原循环中保持了优异的稳定性。这项工作为高效乙烯合成建立了一个可扩展的化学环策略。
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来源期刊
Fuel
Fuel 工程技术-工程:化工
CiteScore
12.80
自引率
20.30%
发文量
3506
审稿时长
64 days
期刊介绍: The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.
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