Chemical looping oxidative propane dehydrogenation controlled by oxygen bulk diffusion over FeVO4 oxygen carrier pellets

doi:10.1016/j.cjche.2022.10.006

Chinese Journal of Chemical Engineering ›› 2023, Vol. 53 ›› Issue (1): 409-420.DOI: 10.1016/j.cjche.2022.10.006

Chemical looping oxidative propane dehydrogenation controlled by oxygen bulk diffusion over FeVO₄ oxygen carrier pellets

Hongbo Song^1,2, Wei Wang^1,2,5,6, Jiachen Sun^1,2, Xianhui Wang^1,2, Xianhua Zhang^1,2, Sai Chen^1,2, Chunlei Pei^1,2,3,4, Zhi-Jian Zhao^1,2,3,4

1. Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
2. Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, China;
3. Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China;
4. Zhejiang Institute of Tianjin University, Ningbo, 315201, China;
5. Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, China;
6. Department of Chemistry, National University of Singapore, 3 Science Drive 3 117543, Singapore

Received:2022-09-23 Revised:2022-10-13 Online:2023-04-08 Published:2023-01-28
Contact: Chunlei Pei,E-mail:chunlei.pei@tju.edu.cn;Zhi-Jian Zhao,E-mail:zjzhao@tju.edu.cn
Supported by:
We acknowledge the National Key Research and Development Program of China (2021YFA1501302), the National Natural Science Foundation of China (22122808, U20B6002), the Haihe Laboratory of Sustainable Chemical Transformations and the Program of Introducing Talents of Discipline to Universities (BP0618007) for financial support. This work is supported by the XPLORER PRIZE by Tencent Foundation.

Chemical looping oxidative propane dehydrogenation controlled by oxygen bulk diffusion over FeVO₄ oxygen carrier pellets

Hongbo Song^1,2, Wei Wang^1,2,5,6, Jiachen Sun^1,2, Xianhui Wang^1,2, Xianhua Zhang^1,2, Sai Chen^1,2, Chunlei Pei^1,2,3,4, Zhi-Jian Zhao^1,2,3,4

1. Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
2. Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, China;
3. Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China;
4. Zhejiang Institute of Tianjin University, Ningbo, 315201, China;
5. Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, China;
6. Department of Chemistry, National University of Singapore, 3 Science Drive 3 117543, Singapore

通讯作者: Chunlei Pei,E-mail:chunlei.pei@tju.edu.cn;Zhi-Jian Zhao,E-mail:zjzhao@tju.edu.cn
基金资助:
We acknowledge the National Key Research and Development Program of China (2021YFA1501302), the National Natural Science Foundation of China (22122808, U20B6002), the Haihe Laboratory of Sustainable Chemical Transformations and the Program of Introducing Talents of Discipline to Universities (BP0618007) for financial support. This work is supported by the XPLORER PRIZE by Tencent Foundation.

Abstract

Abstract: The oxygen distribution and evolution within the oxygen carrier exert significant influence on chemical looping processes. This paper describes the influence of oxygen bulk diffusion within FeVO₄ oxygen carrier pellets on the chemical looping oxidative propane dehydrogenation (CL-ODH). During CL-ODH, the oxygen concentration at the pellet surface initially decreased and then maintained stable before the final decrease. At the stage with the stable surface oxygen concentration, the reaction showed a stable C₃H₆ formation rate and high C₃H₆ selectivity. Therefore, based on Fick’s second law, the oxygen distribution and evolution in the oxygen carrier at this stage were further analyzed. It was found that main reactions of selective oxidation and over-oxidation were controlled by the oxygen bulk diffusion. C₃H₈ conversion rate kept decreasing during this stage due to the decrease of the oxygen flux caused by the decline of oxygen gradient within the oxygen carrier, while C₃H₆ selectivity increased due to the decrease of over-oxidation. In addition, reaction rates could increase with the propane partial pressure due to the increase of the oxygen gradient within the oxygen carrier until the bulk transfer reached its limit at higher propane partial pressure. This study provides fundamental insights for the diffusion-controlled chemical looping reactions.

Key words: Chemical looping, Diffusion, Reaction kinetics, Oxygen carriers, Oxidation

摘要： The oxygen distribution and evolution within the oxygen carrier exert significant influence on chemical looping processes. This paper describes the influence of oxygen bulk diffusion within FeVO₄ oxygen carrier pellets on the chemical looping oxidative propane dehydrogenation (CL-ODH). During CL-ODH, the oxygen concentration at the pellet surface initially decreased and then maintained stable before the final decrease. At the stage with the stable surface oxygen concentration, the reaction showed a stable C₃H₆ formation rate and high C₃H₆ selectivity. Therefore, based on Fick’s second law, the oxygen distribution and evolution in the oxygen carrier at this stage were further analyzed. It was found that main reactions of selective oxidation and over-oxidation were controlled by the oxygen bulk diffusion. C₃H₈ conversion rate kept decreasing during this stage due to the decrease of the oxygen flux caused by the decline of oxygen gradient within the oxygen carrier, while C₃H₆ selectivity increased due to the decrease of over-oxidation. In addition, reaction rates could increase with the propane partial pressure due to the increase of the oxygen gradient within the oxygen carrier until the bulk transfer reached its limit at higher propane partial pressure. This study provides fundamental insights for the diffusion-controlled chemical looping reactions.

关键词: Chemical looping, Diffusion, Reaction kinetics, Oxygen carriers, Oxidation

Hongbo Song, Wei Wang, Jiachen Sun, Xianhui Wang, Xianhua Zhang, Sai Chen, Chunlei Pei, Zhi-Jian Zhao. Chemical looping oxidative propane dehydrogenation controlled by oxygen bulk diffusion over FeVO₄ oxygen carrier pellets[J]. Chinese Journal of Chemical Engineering, 2023, 53(1): 409-420.

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Chemical looping oxidative propane dehydrogenation controlled by oxygen bulk diffusion over FeVO₄ oxygen carrier pellets

Chemical looping oxidative propane dehydrogenation controlled by oxygen bulk diffusion over FeVO₄ oxygen carrier pellets

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