杨仲卿, 牛浩男, 唐波, 李秀权, 冉景煜. ABO3载氧体A/B位金属对乙烷化学链氧化制乙烯性能影响实验研究[J]. 中国电机工程学报, 2024, 44(15): 6086-6094. DOI: 10.13334/j.0258-8013.pcsee.231193
引用本文: 杨仲卿, 牛浩男, 唐波, 李秀权, 冉景煜. ABO3载氧体A/B位金属对乙烷化学链氧化制乙烯性能影响实验研究[J]. 中国电机工程学报, 2024, 44(15): 6086-6094. DOI: 10.13334/j.0258-8013.pcsee.231193
YANG Zhongqing, NIU Haonan, TANG Bo, LI Xiuquan, RAN Jingyu. Experimental Study on the Effect of Metal at A/B Site of ABO3 Oxygen Carrier on the Performance of Chemical Chain Oxidation of Ethane to Ethylene[J]. Proceedings of the CSEE, 2024, 44(15): 6086-6094. DOI: 10.13334/j.0258-8013.pcsee.231193
Citation: YANG Zhongqing, NIU Haonan, TANG Bo, LI Xiuquan, RAN Jingyu. Experimental Study on the Effect of Metal at A/B Site of ABO3 Oxygen Carrier on the Performance of Chemical Chain Oxidation of Ethane to Ethylene[J]. Proceedings of the CSEE, 2024, 44(15): 6086-6094. DOI: 10.13334/j.0258-8013.pcsee.231193

ABO3载氧体A/B位金属对乙烷化学链氧化制乙烯性能影响实验研究

Experimental Study on the Effect of Metal at A/B Site of ABO3 Oxygen Carrier on the Performance of Chemical Chain Oxidation of Ethane to Ethylene

  • 摘要: 钙钛矿载氧体因其低廉的成本、A/B位掺杂金属的灵活多变、优良的氧储存释放性能而受到关注,被广泛应用于化学链式氧化反应中制备乙烯。该文采用柠檬酸络合法制备不同A/B位金属的ABO3钙钛矿型载氧体,通过研究A/B位金属变化对乙烷催化反应性能的影响,得到具有最佳反应活性的载氧体。运用XPS、O2-TPD等方法对催化剂的结构进行表征,为探究其本征反应特性规律,通过动力学研究发现,在形成钙钛矿载氧体的不同A/B位金属中,BaCoO3具有最佳的反应性能,其中乙烷转化率最高达到60%,乙烯选择性达到75%,乙烯收率最高为46%。BaCoO3经过12次循环反应后,乙烯选择性基本保持不变,乙烷转化率降低约4%。通过表征分析发现,比表面积和孔径略微减小,表明载氧体具有优良的稳定性。

     

    Abstract: Perovskite oxygen carriers have attracted much attention due to their low cost, variability of A/B-site metals, and excellent oxygen storage and release performance. They are widely used in the preparation of ethylene in chemical chain oxidation reactions. In this paper, different ABO3 perovskite oxygen carriers are prepared by using the citric acid complexation method. The effect of A/B metal on the reaction performance of oxygen carrier ethane is studied, and the oxygen carrier with the best reaction performance is obtained. The structure of the catalyst is characterized by XPS, O2-TPD and other methods. According to kinetic studies, BaCoO3 has the best reaction performance among the different A/B position metals forming perovskite oxygen carriers, with the highest ethane conversion of 60%, ethylene selectivity of 75% and ethylene yield of 46%, showing its intrinsic reaction characteristics. After 12 cycles of BaCoO3, the specific surface area and pore size decreases slightly, the ethane conversion decreases by about 4%, and the ethylene selectivity remains basically unchanged, indicating that the cycle stability of oxygen carrier is excellent.

     

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