Stability investigation and techno-economic assessment of gliding arc plasma coupled electrocatalytic ammonia synthesis system

doi:10.1016/j.cjche.2025.04.014

中国化学工程学报 ›› 2025, Vol. 85 ›› Issue (9): 251-259.DOI: 10.1016/j.cjche.2025.04.014

Stability investigation and techno-economic assessment of gliding arc plasma coupled electrocatalytic ammonia synthesis system

Yang Lv, Gaoyang Li, Jianpeng Sun, Honghui Ou, Yang Li, Guidong Yang

State Key Laboratory of Fluorine & Nitrogen Chemicals, School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an 710049, China

收稿日期:2025-03-23 修回日期:2025-04-21 接受日期:2025-04-22 出版日期:2025-09-28 发布日期:2025-05-17
通讯作者: Yang Li,E-mail:yangli0528@xjtu.edu.cn;Guidong Yang,E-mail:guidongyang@xjtu.edu.cn
基金资助:
This research was financially supported by National Key Research and Development Program of China (2020YFA0710000), National Natural Science Foundation of China (U22A20391, 22308274), Postdoctoral Fellowship Program of CPSF (GZB20240600, 2023TQ0265, 2024M752589), Innovation Capability Support Program of Shaanxi (NO. 2023-CX-TD-26), and the Programme of Introducing Talents of Discipline to Universities (B23025).

Stability investigation and techno-economic assessment of gliding arc plasma coupled electrocatalytic ammonia synthesis system

Yang Lv, Gaoyang Li, Jianpeng Sun, Honghui Ou, Yang Li, Guidong Yang

State Key Laboratory of Fluorine & Nitrogen Chemicals, School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an 710049, China

Received:2025-03-23 Revised:2025-04-21 Accepted:2025-04-22 Online:2025-09-28 Published:2025-05-17
Contact: Yang Li,E-mail:yangli0528@xjtu.edu.cn;Guidong Yang,E-mail:guidongyang@xjtu.edu.cn
Supported by:
This research was financially supported by National Key Research and Development Program of China (2020YFA0710000), National Natural Science Foundation of China (U22A20391, 22308274), Postdoctoral Fellowship Program of CPSF (GZB20240600, 2023TQ0265, 2024M752589), Innovation Capability Support Program of Shaanxi (NO. 2023-CX-TD-26), and the Programme of Introducing Talents of Discipline to Universities (B23025).

摘要/Abstract

摘要： The plasma-coupled electrocatalytic cascade technology with NO_x^- as intermediate product is a potential method to realize green ammonia synthesis. The matching of the formation rate and consumption rate of NO₂^- as the main absorption product is an important prerequisite for the system to achieve stable operation. Therefore, this paper firstly emphasizes the importance of operating parameters on the cascade system based on the single factor experiment. Secondly, the empirical equation between electrocatalytic operating conditions and NO₂^- consumption rate was established by response surface analysis. Based on this equation, the electrocatalytic operating parameters were optimized to achieve the dynamic equilibrium between NO₂^- formation rate and consumption rate. Finally, the techno-economic assessment model was established to calculate the levelized cost of ammonia based on the cascade system, and the single-variable sensitivity analysis was performed to provide the clear guidance for cost reduction.

关键词: Ammonia synthesis, Plasma, Electrochemistry, Equilibrium, Response surface analysis, Economics

Abstract: The plasma-coupled electrocatalytic cascade technology with NO_x^- as intermediate product is a potential method to realize green ammonia synthesis. The matching of the formation rate and consumption rate of NO₂^- as the main absorption product is an important prerequisite for the system to achieve stable operation. Therefore, this paper firstly emphasizes the importance of operating parameters on the cascade system based on the single factor experiment. Secondly, the empirical equation between electrocatalytic operating conditions and NO₂^- consumption rate was established by response surface analysis. Based on this equation, the electrocatalytic operating parameters were optimized to achieve the dynamic equilibrium between NO₂^- formation rate and consumption rate. Finally, the techno-economic assessment model was established to calculate the levelized cost of ammonia based on the cascade system, and the single-variable sensitivity analysis was performed to provide the clear guidance for cost reduction.

Key words: Ammonia synthesis, Plasma, Electrochemistry, Equilibrium, Response surface analysis, Economics

Yang Lv, Gaoyang Li, Jianpeng Sun, Honghui Ou, Yang Li, Guidong Yang. Stability investigation and techno-economic assessment of gliding arc plasma coupled electrocatalytic ammonia synthesis system[J]. 中国化学工程学报, 2025, 85(9): 251-259.

参考文献

[1] V. Jain, S. Tyagi, P. Roy, P.P. Pillai, Ammonia synthesis with visible light and quantum dots, J. Am. Chem. Soc. 146 (47) (2024) 32356-32365.
[2] Q.K. Hu, O.W. Peng, J. Liu, D.R. Chen, K.P. Loh, Low power consumption ammonia electrosynthesis using hydrogen-nitrate flow electrolyzer, ACS Energy Lett. 9 (5) (2024) 2303-2309.
[3] X. Fu, J.B. Pedersen, Y. Zhou, M. Saccoccio, S. Li, R. Sazinas, K. Li, S.Z. Andersen, A. Xu, N.H. Deissler, J.B.V. Mygind, C. Wei, J. Kibsgaard, P.C.K. Vesborg, J.K. Noerskov, I. Chorkendorff, Continuous-flow electrosynthesis of ammonia by nitrogen reduction and hydrogen oxidation, Science 379 (6633) (2023) 707-712.
[4] K.E. Lamb, M.D. Dolan, D.F. Kennedy, Ammonia for hydrogen storage; A review of catalytic ammonia decomposition and hydrogen separation and purification, Int. J. Hydrog. Energy 44 (7) (2019) 3580-3593.
[5] S.L. Foster, S.I.P. Bakovic, R.D. Duda, S. Maheshwari, R.D. Milton, S.D. Minteer, M.J. Janik, J.N. Renner, L.F. Greenlee, Catalysts for nitrogen reduction to ammonia, Nat. Catal. 1 (7) (2018) 490-500.
[6] Y.C. Wan, J.C. Xu, R.T. Lv, Heterogeneous electrocatalysts design for nitrogen reduction reaction under ambient conditions, Mater. Today 27 (2019) 69-90.
[7] S. Padinjarekutt, H.Z. Li, S.J. Ren, P. Ramesh, F.L. Zhou, S.G. Li, G. Belfort, M. Yu, Na+-gated nanochannel membrane for highly selective ammonia (NH3) separation in the Haber-Bosch process, Chem. Eng. J. 454 (2023) 139998.
[8] J. Emsley, Going one better than nature? Nature 410 (6829) (2001) 633-634.
[9] S. Samaroo, D.P. Hickey, Electrochemical ammonia production from nitrates in agricultural tile drainage: Technoeconomic and global warming analysis, AlChE. J. 69 (2) (2023) e17969.
[10] K. Dong, Y.C. Yao, H.B. Li, H. Li, S.J. Sun, X. He, Y. Wang, Y.S. Luo, D.D. Zheng, Q. Liu, Q. Li, D.W. Ma, X.P. Sun, B. Tang, H2O2-mediated electrosynthesis of nitrate from air, Nat. Synth 3 (6) (2024) 763-773.
[11] A.J. Martin, T. Shinagawa, J. Perez-Ramirez, Electrocatalytic reduction of nitrogen: From Haber-Bosch to ammonia artificial leaf, Chem 5 (2) (2019) 263-283.
[12] X.L. Xue, R.P. Chen, C.Z. Yan, P.Y. Zhao, Y. Hu, W.J. Zhang, S.Y. Yang, Z. Jin, Review on photocatalytic and electrocatalytic artificial nitrogen fixation for ammonia synthesis at mild conditions: Advances, challenges and perspectives, Nano Res. 12 (6) (2019) 1229-1249.
[13] H.M. Liu, N. Guijarro, J.S. Luo, The pitfalls in electrocatalytic nitrogen reduction for ammonia synthesis, J. Energy Chem. 61 (2021) 149-154.
[14] M. Hattori, S. Iijima, T. Nakao, H. Hosono, M. Hara, Solid solution for catalytic ammonia synthesis from nitrogen and hydrogen gases at 50 ℃, Nat. Commun. 11 (1) (2020) 2001.
[15] S. Feng, W.B. Gao, J.P. Guo, H.J. Cao, P. Chen, Electrodriven chemical looping ammonia synthesis mediated by lithium imide, ACS Energy Lett. 8 (3) (2023) 1567-1574.
[16] Y.W. Ren, C. Yu, L.S. Wang, X.Y. Tan, Z. Wang, Q.B. Wei, Y.F. Zhang, J.S. Qiu, Microscopic-level insights into the mechanism of enhanced NH3 synthesis in plasma-enabled cascade N2 oxidation-electroreduction system, J. Am. Chem. Soc. 144 (23) (2022) 10193-10200.
[17] W. Liu, M.Y. Xia, C. Zhao, B. Chong, J.H. Chen, H. Li, H.H. Ou, G.D. Yang, Efficient ammonia synthesis from the air using tandem non-thermal plasma and electrocatalysis at ambient conditions, Nat. Commun. 15 (1) (2024) 3524.
[18] I. Muzammil, Y.N. Kim, H. Kang, D.K. Dinh, S. Choi, C. Jung, Y.H. Song, E. Kim, J.M. Kim, D.H. Lee, Plasma catalyst-integrated system for ammonia production from H2O and N2 at atmospheric pressure, ACS Energy Lett. 6 (8) (2021) 3004-3010.
[19] X.Q. Yan, Y. Zhao, Y.Z. Zhang, B.W. Wang, H.H. Fan, H.H. Ou, X.L. Hou, Q.Z. Huang, H.G. Hu, G.D. Yang, A five-fold twin structure copper for enhanced electrocatalytic nitrogen reduction to sustainable ammonia, AlChE. J. 71 (3) (2025) e18654.
[20] J. Yang, T.Y. Li, C.S. Zhong, X.X. Guan, C. Hu, Nitrogen fixation in water using air phase gliding arc plasma, J. Electrochem. Soc. 163 (10) (2016) E288-E292.
[21] A.J. Wu, J. Yang, B. Xu, X.Y. Wu, Y.H. Wang, X.J. Lv, Y.C. Ma, A.N. Xu, J.G. Zheng, Q.H. Tan, Y.Q. Peng, Z.F. Qi, H.F. Qi, J.F. Li, Y.L. Wang, J. Harding, X. Tu, A.Q. Wang, J.H. Yan, X.D. Li, Direct ammonia synthesis from the air via gliding arc plasma integrated with single atom electrocatalysis, Appl. Catal. B Environ. 299 (2021) 120667.
[22] J. Ding, W.Y. Li, Q.Q. Chen, J.F. Liu, S. Tang, Z.W. Wang, L.W. Chen, H.M. Zhang, Sustainable ammonia synthesis from air by the integration of plasma and electrocatalysis techniques, Inorg. Chem. Front. 10 (19) (2023) 5762-5771.
[23] Y. Lv, J.H. Chen, P.W. Bai, T. Xie, J.J. Liu, H.H. Ou, G.D. Yang, Mass transfer and electrochemical behavior of nitrate reduction to ammonia in electrocatalytic flow cell reactor, AlChE. J. 70 (1) (2024) e18262.
[24] Y.T. Wang, C.H. Wang, M.Y. Li, Y.F. Yu, B. Zhang, Nitrate electroreduction: Mechanism insight, in situ characterization, performance evaluation, and challenges, Chem. Soc. Rev. 50 (12) (2021) 6720-6733.
[25] X.Y. Dai, L. Tian, Z.X. Liu, W.S. Xu, Y.P. Liu, Y. Liu, Nanoreactor based on cyclodextrin for direct electrocatalyzed ammonia synthesis, ACS Nano 16 (11) (2022) 18398-18407.
[26] D. Yin, D. Chen, Y.X. Zhang, W.J. Wang, Q. Quan, W. Wang, Y. Meng, Z.X. Lai, Z. Yang, S. Yip, C.Y. Wong, X.M. Bu, X.Y. Wang, J.C. Ho, Synergistic active phases of transition metal oxide heterostructures for highly efficient ammonia electrosynthesis, Adv. Funct. Mater. 33 (50) (2023) 2303803.
[27] Y.F. Zhang, C. Zhu, H.X. Wei, Y. Tian, W.D. Xia, C. Wang, A highly effective N2 fixation method based on reverse vortex flow gliding arc plasma under water, J. Clean. Prod. 452 (2024) 142158.
[28] Y. Lv, W.K. Teng, Y. Li, H.H. Ou, T. Xie, X.Q. Yan, G.D. Yang, Electrochemical macrokinetics analysis of nitrite electrocatalytic reduction to ammonia, AlChE. J. 70 (12) (2024) e18578.
[29] B.S. Patil, F.J.J. Peeters, G.J. van Rooij, J.A. Medrano, F. Gallucci, J. Lang, Q. Wang, V. Hessel, Plasma assisted nitrogen oxide production from air: Using pulsed powered gliding arc reactor for a containerized plant, AlChE. J. 64 (2) (2018) 526-537.
[30] S. Yang, A. Chen, Z.J. Tang, Z.X. Wu, P. Li, Y.B. Wang, X.Q. Wang, X. Jin, S.C. Bai, C.Y. Zhi, Regulating the electrochemical reduction kinetics by the steric hindrance effect for a robust Zn metal anode, Energy Environ. Sci. 17 (3) (2024) 1095-1106.
[31] A.A. Shah, M.J. Watt-Smith, F.C. Walsh, A dynamic performance model for redox-flow batteries involving soluble species, Electrochim. Acta 53 (27) (2008) 8087-8100.
[32] O.A. El-Shafie, R.M. El-Maghraby, J. Albo, S.K. Fateen, A. Abdelghany, Modeling and numerical investigation of the performance of gas diffusion electrodes for the electrochemical reduction of carbon dioxide to methanol, Ind. Eng. Chem. Res. 59 (47) (2020) 20929-20942.
[33] H. Bouaboula, M. Ouikhalfan, I. Saadoune, J. Chaouki, A. Zaabout, Y. Belmabkhout, Addressing sustainable energy intermittence for green ammonia production, Energy Rep. 9 (2023) 4507-4517.
[34] L. Hatton, R. Banares-Alcantara, S. Sparrow, F. Lott, N. Salmon, Assessing the impact of climate change on the cost of production of green ammonia from offshore wind, Int. J. Hydrog. Energy 49 (2024) 635-643.

Stability investigation and techno-economic assessment of gliding arc plasma coupled electrocatalytic ammonia synthesis system

Stability investigation and techno-economic assessment of gliding arc plasma coupled electrocatalytic ammonia synthesis system

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