Citation: Fan Yun, Chen Guodan, Xi Xiuan, Li Jun, Wang Qi, Luo Jingli, Fu Xianzhu. Co-Generation of Ethylene and Electricity from Ethane by CeO₂/RP-PSCFM@CoFe Anode Materials in Proton Conductive Fuel Cells[J]. Acta Physico-Chimica Sinica, ;2021, 37(7): 200910. doi: 10.3866/PKU.WHXB202009107 shu

Co-Generation of Ethylene and Electricity from Ethane by CeO₂/RP-PSCFM@CoFe Anode Materials in Proton Conductive Fuel Cells

Fan Yun ^1,† ,
Chen Guodan ^1,† ,
Xi Xiuan ¹ ,
Li Jun ¹ ,
Wang Qi ² ,
Luo Jingli ¹ ,
Fu Xianzhu ^1,,

1.
College of Material Science and Engineering, Shenzhen University, Shenzhen 518060, Guangdong Province, China
2.
School of Materials Science and Technology, China University of Geosciences, Beijing 100083, China

Corresponding author: Fu Xianzhu, xz.fu@szu.edu.cn

^†

Received Date: 30 September 2020
Revised Date: 30 October 2020
Accepted Date: 30 October 2020
Available Online: 5 November 2020
Fund Project: the National Natural Science Foundation of China 21975163The project was supported by the National Natural Science Foundation of China (21975163)

The continuous consumption and excessive use of fossil fuels promote the exploration of new energy conversion technologies. Meanwhile, the increase in the supply of ethane encourages the development of industrial technology for the production of ethylene chemical raw materials. Compared with traditional fossil fuel energy conversion equipment, solid oxide ethane cogeneration fuel cells are an efficient energy processing device. Through selective oxidation of fuel gas on the anode, the endothermic process of ethane dehydrogenation is converted into an exothermic oxidation reaction, which has a greater driving force for reaction thermodynamics, and simultaneously produces clean electricity and value-added chemicals without CO₂ emissions. The anode material used for the proton conductor ethane fuel cells needs to operate stably and efficiently under hydrocarbon fuel. Consequently, excellent catalytic activity, low polarization resistance, and anti-coking stability are essential. In this work, CeO₂ was uniformly impregnated into the surface of the porous cubic perovskite Pr_0.4Sr_0.6Co_0.2Fe_0.7Mo_0.1O_3−δ anode by wet impregnation, and then calcined and reduced to obtain a CeO₂/RP-PSCFM@CoFe composite anode embedded with nanoparticles, which was successfully used in electrolyte-supported proton conductor fuel cells. CeO₂ has a high ionic conductivity and transport capacity, which accelerates the transfer rate of protons on the anode and improves the catalytic reaction and transport process. Moreover, uniformly dispersed CeO₂ can effectively increase the three-phase interface of the anode reaction and increase the range of reaction activity. The peak power densities before and after wet impregnation reached 172 and 253 mW·cm⁻², respectively, at 750 ℃. When switching to ethane as the fuel, the peak power densities reached 136 and 183 mW·cm⁻², respectively. The polarization resistance of the impregnated single cell was significantly reduced, and the catalytic activity improved. Moreover, there was no attenuation for 10 h in the long-term test. Inversely, the current density increased with the continuous reduction of the composite anode. Product analysis revealed that the yield of ethylene increased from 23.52% at 650 ℃ to 34.09% at 750 ℃, and the ethylene selectivity exceeded 94%. These results clearly show that the impregnated anode exhibited excellent catalytic activity and anti-coking ability in hydrocarbon fuels at high temperatures. Combining CoFe nanoparticles with CeO₂ enhanced the electronic conductance and ionic conductance of the electrode, improved the transmission of electric energy and the efficient conversion of chemicals, thus successfully producing the cogeneration of electric energy and ethylene.
- Composite anode,
- Impregnation,
- Ethane,
- Cogeneration fuel cells,
- Anti-coking
1. [1]
  Atkinson, A.; Barnett, S.; Gorte, R. J.; Irvine, J. T.; McEvoy, A. J.; Mogensen, M.; Singhal, S. C.; Vohs, J. Nat. Mater. 2004, 3, 17. doi: 10.1038/nmat1040 doi: 10.1038/nmat1040
2. [2]
  Sun, W.; Shi, Z.; Liu, M.; Bi, L.; Liu, W. Adv. Funct. Mater. 2014, 24, 5695. doi: 10.1002/adfm.201401478 doi: 10.1002/adfm.201401478
3. [3]
  Sengodan, S.; Choi, S.; Jun, A.; Shin, T. H.; Ju, Y. W.; Jeong, H. Y.; Shin, J.; Irvine, J. T.; Kim, G. Nat. Mater. 2015, 14, 205. doi: 10.1038/nmat4166 doi: 10.1038/nmat4166
4. [4]
  Fu, X. Z.; Luo, J. L.; Sanger, A. R.; Luo, N. Chuang, K. T. J. Power Sources 2010, 195, 2659. doi: 10.1016/j.jpowsour.2009.10.069 doi: 10.1016/j.jpowsour.2009.10.069
5. [5]
  Wang, S. Y.; Luo, J. L.; Sanger, A. R.; Chuang, K. T. J. Phys. Chem. C 2007, 111, 5069. doi: 10.1021/jp066690w doi: 10.1021/jp066690w
6. [6]
  Fan, Y.; Wang, Q.; Li, J.; Luo, J. L.; Fu, X. Z. J. Electrochem. 2020, 26, 243. doi: 10.13208/j.electrochem.191145
7. [7]
  Wang, W.; Xu, M. G.; Xu, X. M.; Zhou, W.; Shao, Z. P. Angew. Chem. Int. Ed. 2020, 59, 136. doi: 10.1002/anie.201900292 doi: 10.1002/anie.201900292
8. [8]
  Li, Y. F.; Zhang, W. Q.; Zheng, Y.; Chen, J.; Yu, B.; Chen, Y.; Liu, M. L. Chem. Soc. Rev. 2017, 46, 6345. doi: 10.1039/c7cs00120g doi: 10.1039/c7cs00120g
9. [9]
  Xie, C.; Yan, D. F.; Chen, W.; Zou, Y. Q.; Chen, R.; Zang, S. Q.; Wang, Y. Y.; Yao, X. D.; Wang, S. Y. Mater. Today 2019, 31, 47. doi: 10.1016/j.mattod.2019.05.021 doi: 10.1016/j.mattod.2019.05.021
10. [10]
  Jarrige, I.; Ishii, K.; Matsumura, D.; Nishihata, Y.; Yoshida, M.; Kishi, H.; Taniguchi, M.; Uenishi, M.; Tanaka, H.; Kasai, H.; et al. ACS Catal. 2015, 5, 1112. doi: 10.1021/cs501608k doi: 10.1021/cs501608k
11. [11]
  Zhang, J.; Gao, M. R.; Luo, J. L. Chem. Mater. 2020, 32, 5424. doi: 10.1021/acs.chemmater.0c00721 doi: 10.1021/acs.chemmater.0c00721
12. [12]
  Zhang, X. R.; Ye, L. T.; Li, H.; Chen, F. L.; Xie, K. ACS Catal. 2020, 10, 3505. doi: 10.1021/acscaatal.9b05409 doi: 10.1021/acscaatal.9b05409
13. [13]
  Sun, Y. F.; Zhang, Y. Q.; Chen, J.; Li, J. H.; Zhu, Y. T.; Zeng, Y. M.; Amirkhiz, B. S.; Li, J.; Hua, B.; Luo, J. L. Nano Lett. 2016, 16, 5303. doi: 10.1021/acs.nanolett.6b02757 doi: 10.1021/acs.nanolett.6b02757
14. [14]
  Neagu, D.; Tsekouras, G.; Miller, D. N.; Menard, H.; Irvine, J. T. Nat. Chem. 2013, 5. doi: 10.1038/nchem.1773
15. [15]
  Liu, S.; Liu, Q.; Fu, X. Z.; Luo, J. L. Appl. Catal. B: Environ. 2018, 220, 283. doi: 10.1016/j.apcatb.2017.08.051 doi: 10.1016/j.apcatb.2017.08.051
16. [16]
  Lv, H. F.; Lin, L.; Zhang, X. M.; Song, Y. F.; Matsumoto, H.; Zeng, C. B.; Ta, N.; Liu, W.; Gao, D. F.; Wang, G. X.; et al. Adv. Mater. 2019, 32, 2063. doi: 10.1002/adma.201906193 doi: 10.1002/adma.201906193
17. [17]
  Shi, N.; Xue, S.; Xie, Y.; Yang, Y.; Huan, D.; Pan, Y.; Peng, R.; Xia, C.; Zhan, Z.; Lu, Y. Appl. Catal. B: Environ. 2020, 272, 118973. doi: 10.1016/j.apcatb.2020.118973 doi: 10.1016/j.apcatb.2020.118973
18. [18]
  Hua, B.; Yan, N.; Li, M.; Sun, Y. F.; Zhang, Y. Q.; Li, J.; Etsell, T.; Sarkar, P.; Luo, J. L. Adv. Mater. 2016, 28, 8922. doi: 10.1002/adma.201602103 doi: 10.1002/adma.201602103
19. [19]
  Xi, X.; Cao, Z. -S.; Shen, X. Q.; Lu, Y.; Li, J.; Luo, J. L.; Fu, X. Z. J. Power Sources 2020, 459, 228071. doi: 10.1016/j.jpowsour.2020.228071 doi: 10.1016/j.jpowsour.2020.228071
20. [20]
  Liu, S.; Chuang, K. T.; Luo, J. L. ACS Catal. 2015, 6, 760. doi: 10.1021/acscatal.5b02296 doi: 10.1021/acscatal.5b02296
21. [21]
  Lv, X.; Chen, H.; Zhou, W.; Cheng, F.; Li, S. D.; Shao, Z. Renewable Energy. 2020, 150, 334. doi: 10.1016/j.renene.2019.12.126 doi: 10.1016/j.renene.2019.12.126
22. [22]
  Ding, S.; Li, M.; Pang, W.; Hua, B.; Duan, N.; Zhang, Y. -Q.; Zhang, S. -N.; Jin, Z.; Luo, J. L. Electrochim. Acta 2020, 335, 135683. doi: 10.1016/j.electacta.2020.135683 doi: 10.1016/j.electacta.2020.135683
23. [23]
  Bian, L.; Duan, C.; Wang, L.; O'Hayre, R.; Cheng, J.; Chou, K. C. J. Mater. Chem. A. 2017, 5, 15253. doi: 10.1039/c7ta03001k doi: 10.1039/c7ta03001k
24. [24]
  Fu, X. Z.; Luo, X. X.; Luo, J. L.; Chuang, K. T.; Sanger, A. R.; Krzywicki, A. J. Power Sources 2011, 196, 1036. doi: 10.1016/j.jpowsour.2010.08.043 doi: 10.1016/j.jpowsour.2010.08.043
25. [25]
  McIntosh, S.; Gorte, R. J. Chem. Rev. 2004, 104, 4845. doi: 10.1021/cr020725g doi: 10.1021/cr020725g
26. [26]
  Silva, A. A. A.; Bion, N.; Epron, F.; Baraka, S.; Fonseca, F. C.; Rabelo, N. R. C.; Mattos, L. V.; Noronha, F. B. Appl. Catal. B: Environ. 2017, 206, 626. doi: 10.1016/j.apcatb.2017.01.069 doi: 10.1016/j.apcatb.2017.01.069
27. [27]
  Liu, Z.; Liu, B.; Ding, D.; Liu, M.; Chen, F.; Xia, C. J. Power Sources. 2013, 237, 243. doi: 10.1016/j.jpowsour.2013.03.025 doi: 10.1016/j.jpowsour.2013.03.025
28. [28]
  Lei, Z.; Zhu, Q. S.; Han, M. F. Acta Phys. -Chim. Sin. 2010, 26, 583. doi: 10.3866/PKU.WHXB20100323
29. [29]
  Mackenzie J. D.; Bescher E. P. Acc. Chem. Res. 2007, 40, 810. doi: 10.1021/ar7000149 doi: 10.1021/ar7000149
30. [30]
  Zuo, C.; Zha, S.; Liu, M.; Hatano, M.; Uchiyama, M. Adv. Mater. 2006, 18, 3318. doi: 10.1002/adma.200601366 doi: 10.1002/adma.200601366
31. [31]
  Zhang, L.; Yang, C.; Frenkel, A. I.; Wang, S.; Xiao, G.; Brinkman, K.; Chen, F. J. Power Sources. 2014, 262, 421. doi: 10.1016/j.jpowsour.2014.04.009 doi: 10.1016/j.jpowsour.2014.04.009
32. [32]
  Yang, C.; Li, J.; Lin, Y.; Liu, J.; Chen, F.; Liu, M. Nano Energy 2015, 11, 704. doi: 10.1016/j.nanoen.2014.12.001 doi: 10.1016/j.nanoen.2014.12.001
33. [33]
  Wang, Z.; Tian, Y.; Li, Y. J. Power Sources 2011, 196, 6104. doi: 10.1016/j.jpowsour.2011.03.053 doi: 10.1016/j.jpowsour.2011.03.053
34. [34]
  Song, Y.; Zhong, Q.; Tan, W.; Pan, C. Electrochim. Acta 2014, 139, 13. doi: 10.1016/j.electacta.2014.07.022 doi: 10.1016/j.electacta.2014.07.022
35. [35]
  Chen, D.; Chen, C.; Dong, F.; Shao, Z.; Ciucci, F. J. Power Sources 2014, 250, 188. doi: 10.1016/j.jpowsour.2013.11.010 doi: 10.1016/j.jpowsour.2013.11.010
36. [36]
  Pan, X.; Wang, Z.; He, B.; Wang, S.; Wu, X.; Xia, C. Int. J. Hydrog. Energy 2013, 38, 4108. doi: 10.1016/j.ijhydene.2013.01.121 doi: 10.1016/j.ijhydene.2013.01.121
37. [37]
  Osinkin, D. A.; Bogdanovich, N. M.; Gavrilyuk, A. L. Electrochim. Acta 2016, 199, 108. doi: 10.1016/j.electacta.2016.03.133 doi: 10.1016/j.electacta.2016.03.133
38. [38]
  Liu, S.; Behnamian, Y.; Chuang, K. T.; Liu, Q.; Luo, J. L. J. Power Sources 2015, 298, 23. doi: 10.1016/j.jpowsour.2015.08.032 doi: 10.1016/j.jpowsour.2015.08.032
39. [39]
  Fu, X. Z.; Lin, J. Y.; Xu, S.; Luo, J. L.; Chuang, K. T.; Sanger, A. R.; Krzywicki, A. Phys. Chem. Chem. Phys. 2011, 13, 19615. doi: 10.1039/c1cp22837d doi: 10.1039/c1cp22837d
1. [1]
  Yixin Lu , Minghan Qin , Shixian Zhang , Zhen Liu , Wang Sun , Zhenhua Wang , Jinshuo Qiao , Kening Sun . Triple-conducting heterostructure anodes for electrochemical ethane nonoxidative dehydrogenation by protonic ceramic electrolysis cells. Chinese Chemical Letters, 2025, 36(4): 110567-. doi: 10.1016/j.cclet.2024.110567
2. [2]
  Jiaxi Xu , Yuan Ma . Influence of Hyperconjugation on the Stability and Stable Conformation of Ethane, Hydrazine, and Hydrogen Peroxide. University Chemistry, 2024, 39(11): 374-377. doi: 10.3866/PKU.DXHX202402049
3. [3]
  Yao-Yu Ma , Wen-Juan Shi , Gang-Ding Wang , Xin Liu , Lei Hou , Yao-Yu Wang . Enhancing ethane/ethylene separation performance through the amino-functionalization of ethane-selective MOF. Chinese Chemical Letters, 2025, 36(3): 109729-. doi: 10.1016/j.cclet.2024.109729
4. [4]
  Lihua HUANG , Jian HUA . Denitration performance of HoCeMn/TiO₂ catalysts prepared by co-precipitation and impregnation methods. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 629-645. doi: 10.11862/CJIC.20230315
5. [5]
  Yaxin Sun , Huiyu Li , Shiquan Guo , Congju Li . Metal-based cathode catalysts for electrocatalytic ORR in microbial fuel cells: A review. Chinese Chemical Letters, 2024, 35(5): 109418-. doi: 10.1016/j.cclet.2023.109418
6. [6]
  Jiaqi Lin , Pupu Yang , Yimin Jiang , Shiqian Du , Dongcai Zhang , Gen Huang , Jinbo Wang , Jun Wang , Qie Liu , Miaoyu Li , Yujie Wu , Peng Long , Yangyang Zhou , Li Tao , Shuangyin Wang . Surface decoration prompting the decontamination of active sites in high-temperature proton exchange membrane fuel cells. Chinese Chemical Letters, 2024, 35(11): 109435-. doi: 10.1016/j.cclet.2023.109435
7. [7]
  Wenbiao Zhang , Bolong Yang , Zhonghua Xiang . Atomically dispersed Cu-based metal-organic framework directly for alkaline polymer electrolyte fuel cells. Chinese Chemical Letters, 2025, 36(2): 109630-. doi: 10.1016/j.cclet.2024.109630
8. [8]
  Shengfei Dong , Ziyu Liu , Xiaoyi Yang . Hydrothermal liquefaction of biomass for jet fuel precursors: A review. Chinese Chemical Letters, 2024, 35(8): 109142-. doi: 10.1016/j.cclet.2023.109142
9. [9]
  Rui Liu , Jinbo Pang , Weijia Zhou . Monolayer water shepherding supertight MXene/graphene composite films. Chinese Journal of Structural Chemistry, 2024, 43(10): 100329-100329. doi: 10.1016/j.cjsc.2024.100329
10. [10]
  Wendi Dou , Guangying Wan , Tiefeng Liu , Lin Han , Wu Zhang , Chuang Sun , Rensheng Song , Jianhui Zheng , Yujing Liu , Xinyong Tao . Conductive composite binder for recyclable LiFePO₄ cathode. Chinese Chemical Letters, 2024, 35(11): 109389-. doi: 10.1016/j.cclet.2023.109389
11. [11]
  Guilong Li , Wenbo Ma , Jialing Zhou , Caiqin Wu , Chenling Yao , Huan Zeng , Jian Wang . A composite hydrogel with porous and homogeneous structure for efficient osmotic energy conversion. Chinese Chemical Letters, 2025, 36(2): 110449-. doi: 10.1016/j.cclet.2024.110449
12. [12]
  Bingwei Wang , Yihong Ding , Xiao Tian . Benchmarking model chemistry composite calculations for vertical ionization potential of molecular systems. Chinese Chemical Letters, 2025, 36(2): 109721-. doi: 10.1016/j.cclet.2024.109721
13. [13]
  Jiale Zheng , Mei Chen , Huadong Yuan , Jianmin Luo , Yao Wang , Jianwei Nai , Xinyong Tao , Yujing Liu . Electron-microscopical visualization on the interfacial and crystallographic structures of lithium metal anode. Chinese Chemical Letters, 2024, 35(6): 108812-. doi: 10.1016/j.cclet.2023.108812
14. [14]
  Li Lin , Song-Lin Tian , Zhen-Yu Hu , Yu Zhang , Li-Min Chang , Jia-Jun Wang , Wan-Qiang Liu , Qing-Shuang Wang , Fang Wang . Molecular crowding electrolytes for stabilizing Zn metal anode in rechargeable aqueous batteries. Chinese Chemical Letters, 2024, 35(7): 109802-. doi: 10.1016/j.cclet.2024.109802
15. [15]
  Haixia Wu , Kailu Guo . Iodized polyacrylonitrile as fast-charging anode for lithium-ion battery. Chinese Chemical Letters, 2024, 35(10): 109550-. doi: 10.1016/j.cclet.2024.109550
16. [16]
  Haiying Lu , Weijie Li . The electrolyte solvation and interfacial chemistry for anode-free sodium metal batteries. Chinese Journal of Structural Chemistry, 2024, 43(11): 100334-100334. doi: 10.1016/j.cjsc.2024.100334
17. [17]
  Ze Liu , Xiaochen Zhang , Jinlong Luo , Yingjian Yu . Application of metal-organic frameworks to the anode interface in metal batteries. Chinese Chemical Letters, 2024, 35(11): 109500-. doi: 10.1016/j.cclet.2024.109500
18. [18]
  Wenfeng Shao , Chuanlin Li , Chenggang Wang , Guangsen Du , Shunshun Zhao , Guangmeng Qu , Yupeng Xing , Tianshuo Guo , Hongfei Li , Xijin Xu . Stabilization of zinc anode by trace organic corrosion inhibitors for long lifespan. Chinese Chemical Letters, 2025, 36(3): 109531-. doi: 10.1016/j.cclet.2024.109531
19. [19]
  Chengcheng Xie , Chengyi Xiao , Hongshuo Niu , Guitao Feng , Weiwei Li . Mesoporous organic solar cells. Chinese Chemical Letters, 2024, 35(11): 109849-. doi: 10.1016/j.cclet.2024.109849
20. [20]
  Wenqing Deng , Fanfeng Deng , Ting Zhang , Junjie Lin , Liang Zhao , Gang Li , Yi Pan , Jiebin Yang . Continuous measurement of reactive ammonia in hydrogen fuel by online dilution module coupled with Fourier transform infrared spectrometer. Chinese Chemical Letters, 2025, 36(3): 110085-. doi: 10.1016/j.cclet.2024.110085

Get Citation

PDF

XML

Metrics

PDF Downloads(22)
Abstract views(437)
HTML views(58)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Co-Generation of Ethylene and Electricity from Ethane by CeO2/RP-PSCFM@CoFe Anode Materials in Proton Conductive Fuel Cells

Metrics

通讯作者: 陈斌, bchen63@163.com

Co-Generation of Ethylene and Electricity from Ethane by CeO₂/RP-PSCFM@CoFe Anode Materials in Proton Conductive Fuel Cells