Electrochemically reconstructed copper-polypyrrole modified graphite felt electrodes for efficiently electrocatalytic reduction of nitrate

doi:10.1016/j.cjche.2025.04.005

中国化学工程学报 ›› 2025, Vol. 83 ›› Issue (7): 51-61.DOI: 10.1016/j.cjche.2025.04.005

Electrochemically reconstructed copper-polypyrrole modified graphite felt electrodes for efficiently electrocatalytic reduction of nitrate

Ge Liu^1,2, Jiahong Wang^1,2, Zhi Hu^1,2, Tianjiao Lu^1,2, Hao Zhang^1,2, Jie Zhu^1,2

1 School of Environmental Science and Engineering, Shaanxi University of Science & Technology, Xi'an 710021, China;
2 Shaanxi Key Laboratory of Green Preparation and Functionalization of Inorganic Materials, Xi'an 710021, China

收稿日期:2024-12-23 修回日期:2025-03-04 接受日期:2025-04-01 出版日期:2025-07-28 发布日期:2025-07-28
通讯作者: Jiahong Wang,E-mail:wangjiahong@sust.edu.cn
基金资助:
This work was supported by the National Natural Science Foundation of China (22076111), and Key Research and Development Program of Shaanxi (2024 GX-YBXM-427), China.

Electrochemically reconstructed copper-polypyrrole modified graphite felt electrodes for efficiently electrocatalytic reduction of nitrate

Ge Liu^1,2, Jiahong Wang^1,2, Zhi Hu^1,2, Tianjiao Lu^1,2, Hao Zhang^1,2, Jie Zhu^1,2

1 School of Environmental Science and Engineering, Shaanxi University of Science & Technology, Xi'an 710021, China;
2 Shaanxi Key Laboratory of Green Preparation and Functionalization of Inorganic Materials, Xi'an 710021, China

Received:2024-12-23 Revised:2025-03-04 Accepted:2025-04-01 Online:2025-07-28 Published:2025-07-28
Contact: Jiahong Wang,E-mail:wangjiahong@sust.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China (22076111), and Key Research and Development Program of Shaanxi (2024 GX-YBXM-427), China.

摘要/Abstract

摘要： In this work, a simple two-step electrodeposition was employed to prepare PPy-Cu/GF (PPy, polypyrrole; GF, graphite felt) composite cathodes for the nitrate reduction. Characterized results revealed that the introduction of PPy as an intermediate layer resulted in the transformation of both granular and dendritic Cu in form of Cu⁺/Cu⁰, Cu²⁺ on the electrode surface. The NO₃^--N of 50 mg·L^-1 was almost completely removed (99.01%) using the PPy-Cu/GF cathode under the optimum condition, which is obviously higher than the GF, PPy/GF and Cu/GF electrodes. NO₃^--N removal was slightly affected over the pH scale of 3.0 e11.0, whereas increasing the current density from 10 to 25 mA·cm^-2 boosted the reduction of NO₃^--N. At a Cl concentration of 2000 mg·L1, the removal of NO₃^--N was slightly reduced, while the selectivity for N₂ increased dramatically due to the active chlorine could oxidize NH₄⁺-N to N₂. Meanwhile, PPy-Cu/ GF cathode exhibits an average removal rate of 97.83% within 12 cycles, highlighting its potential for application in actual water bodies. The EPR analysis and the active species trapping experiment confirmed that the nitrate reduction on the PPy-Cu/GF cathode mainly relies on direct reduction mediated by electron transfer, while ^*H influences the reduction of nitrite to ammonia.

关键词: Electrocatalytic nitrate reduction, Electrodeposition, PPy-Cu/GF cathode

Abstract: In this work, a simple two-step electrodeposition was employed to prepare PPy-Cu/GF (PPy, polypyrrole; GF, graphite felt) composite cathodes for the nitrate reduction. Characterized results revealed that the introduction of PPy as an intermediate layer resulted in the transformation of both granular and dendritic Cu in form of Cu⁺/Cu⁰, Cu²⁺ on the electrode surface. The NO₃^--N of 50 mg·L^-1 was almost completely removed (99.01%) using the PPy-Cu/GF cathode under the optimum condition, which is obviously higher than the GF, PPy/GF and Cu/GF electrodes. NO₃^--N removal was slightly affected over the pH scale of 3.0 e11.0, whereas increasing the current density from 10 to 25 mA·cm^-2 boosted the reduction of NO₃^--N. At a Cl concentration of 2000 mg·L1, the removal of NO₃^--N was slightly reduced, while the selectivity for N₂ increased dramatically due to the active chlorine could oxidize NH₄⁺-N to N₂. Meanwhile, PPy-Cu/ GF cathode exhibits an average removal rate of 97.83% within 12 cycles, highlighting its potential for application in actual water bodies. The EPR analysis and the active species trapping experiment confirmed that the nitrate reduction on the PPy-Cu/GF cathode mainly relies on direct reduction mediated by electron transfer, while ^*H influences the reduction of nitrite to ammonia.

Key words: Electrocatalytic nitrate reduction, Electrodeposition, PPy-Cu/GF cathode

Ge Liu, Jiahong Wang, Zhi Hu, Tianjiao Lu, Hao Zhang, Jie Zhu. Electrochemically reconstructed copper-polypyrrole modified graphite felt electrodes for efficiently electrocatalytic reduction of nitrate[J]. 中国化学工程学报, 2025, 83(7): 51-61.

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Electrochemically reconstructed copper-polypyrrole modified graphite felt electrodes for efficiently electrocatalytic reduction of nitrate

Electrochemically reconstructed copper-polypyrrole modified graphite felt electrodes for efficiently electrocatalytic reduction of nitrate

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