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High-efficiency catalytic reduction of residual oxygen for purification of carbon dioxide streams from high-pressure oxy-combustion systems
Reaction Chemistry & Engineering ( IF 3.9 ) Pub Date : 2021-4-26 , DOI: 10.1039/d0re00481b
Hong Lu 1, 2, 3, 4 , Luke Schideman 1, 2, 3, 4, 5 , Qing Ye 1, 2, 3, 4 , Yongqi Lu 1, 2, 3, 4
Affiliation  

Pressurized oxy-combustion is a promising technology for carbon capture, utilization, and storage. For the captured CO2 to be used for enhanced oil recovery or stored in geological formations, flue gas impurities, including residual O2 in the CO2 stream, must be purified to meet the purity specifications. A catalytic approach to reducing residual O2 with CH4 was investigated in this study. Five CoMn- and Cu-based catalysts were synthesized or acquired, and a reverse-flow fixed-bed reactor was used to assess their performance for O2 removal from a simulated oxy-combustion flue gas at 15 bar. The impacts of the operating parameters on O2 removal, such as temperature, gas hourly space velocity, O2/CH4 ratio, and gas pressure, were investigated. Among the tested catalysts, the two CoMn catalysts were superior in both activity and selectivity, with the reaction lighting off at about 350 °C and achieving 99% O2 removal at about 500 °C. The kinetics of the catalytic reaction is discussed, and the Mars–van Krevelen redox mechanism is deemed valid for describing the reaction pathway for the top-performing CoMn catalysts. The catalytic reaction was determined to be first order in CH4 and zero order in O2 under the test conditions.

中文翻译:

高效催化还原残留氧气,以净化高压氧气燃烧系统中的二氧化碳流

加压氧燃烧是一种用于碳捕获,利用和储存的有前途的技术。为了将捕获的CO 2用于提高石油采收率或将其存储在地质构造中,烟道气杂质(包括CO 2流中残留的O 2)必须进行净化,以满足纯度要求。在这项研究中研究了一种用CH 4还原残留O 2的催化方法。合成或获得了五种基于CoMn和Cu的催化剂,并使用逆流固定床反应器评估了它们在15 bar下从模拟的氧燃烧烟道气中去除O 2的性能。操作参数对O 2的影响研究了温度,气体时空速度,O 2 / CH 4比和气体压力等去除率。在所测试的催化剂中,两种CoMn催化剂在活性和选择性上均优异,反应在约350°C时熄灭,在约500°C时达到99%的O 2去除率。讨论了催化反应的动力学,并且认为Mars-van Krevelen氧化还原机理对于描述性能最佳的CoMn催化剂的反应途径是有效的。在测试条件下,确定催化反应在CH 4中为一级,在O 2中为零级。
更新日期:2021-04-30
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