N-doped carbon-coated Fe3N composite as heterogeneous electro-Fenton catalyst for efficient degradation of organics

doi:10.1016/S1872-2067(20)63719-6

Abstract

Abstract:

Herein, the application of a N-doped graphitic-carbon-coated iron nitride composite dispersed in a N-doped carbon framework (Fe₃N@NG/NC) is investigated as a heterogeneous electro-Fenton ( HE-EF) catalyst for the efficient removal of organics. The simultaneous carbonization and ammonia etching of iron-based metal organic framework (Fe-MOF) materials yielded well-dispersed N-doped carbon-coated Fe₃N nanoparticles with a diameter of ~70 nm. The Fe₃N and pyridinic N endowed the composite with high HE-EF activity for decomposing the electrogenerated H₂O₂ to^•OH. The Fe₃N@NG/NC exhibited outstanding HE-EF performance in removing various organic pollutants with low iron leaching. A removal rate of 97-100% could be obtained for rhodamine B (RhB), dimethyl phthalate, methylene blue, and orange II in 120 min at a pH of 5.0. When the solution pH was set to 3.0, 5.0, 7.0, and 9.0, the removal rate of RhB reached 100%, 96%, 92%, and 81%, respectively, in 60 min at an optimum voltage of 0.0 V (vs. reversible hydrogen electrode (RHE)). Moreover, the concentration of leached iron was expected to be below 0.03 mg/L in a wide pH range of 3.0-9.0. In addition, the RhB removal efficiency remained as high as 90% after six cycles in the reusability experiments. This work highlights the MOF-derived Fe₃N composite as an efficient HE-EF catalyst and the corresponding catalytic mechanism, which facilitates its application in wastewater treatment.

Key words: Fe₃N@NG/NC composite, Heterogeneous electro-Fenton, Metal-organic frameworks, Degradation, Organic pollutants

Juan Xiao, Junwei Chen, Zuqiao Ou, Junhang Lai, Tongwen Yu, Yi Wang. N-doped carbon-coated Fe₃N composite as heterogeneous electro-Fenton catalyst for efficient degradation of organics[J]. Chinese Journal of Catalysis, 2021, 42(6): 953-962.

×
share this article

Add to citation manager EndNote|Ris|BibTeX

URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63719-6

https://www.cjcatal.com/EN/Y2021/V42/I6/953

Figures/Tables 11

Fig. 1. (a) Schematic diagram of the synthesis procedure used for Fe3N@NG/NC; XRD patterns of MIL-101 (Fe) (b) and Fe3N@NG/NC (c).

Fig. 2. SEM (a) and corresponding elemental mapping (b-d) images of Fe3N@NG/NC.

Fig. 3. HAADF-STEM (a), TEM (b), HRTEM (c), and atomic-resolution HRTEM (d) images of Fe3N@NG/NC.

Fig. 4. Fe 2p (a), N 1s (b), C 1s (c) XPS spectra, and Raman spectrum (d) of Fe3N@NG/NC.

Fig. 5. RRDE polarization curves (a), n and H2O2 selectivity (b) of Fe3N@NG/NC at pH 5.0. Experimental conditions: scan rate of 10 mV/s, rotation rate of 1600 rpm, and [Na2SO4] = 0.1 M.

Fig. 6. RhB degradation efficiency (a) and corresponding k values (b) of different systems at a pH of 5.0. The effects of pH (c) and working potential (d) on RhB degradation. Experimental conditions: [RhB] = 10.0 mg/L, potential of 0.0 V, and [loaded catalyst] = 2.0 mg/cm2.

Fig. 7. Results of the recycling tests for HE-EF degradation of RhB at a pH of 5.0. Experimental conditions: [RhB] = 10.0 mg/L, potential of 0.0 V, and [loaded catalyst] = 2.0 mg/cm2.

Fig. 8. Removal efficiency for organics (a) and corresponding k values (b) in the HE-EF reaction at a pH of 5.0. Experimental conditions: [dimethyl phthalate] = [RhB] = [methylene blue] = [orange II] = 10.0 mg/L, potential of 0.0 V, and [loaded catalyst] = 2.0 mg/cm2.

Fig. 9. EPR spectra of ?OH in raw GF and Fe3N@NG/NC/GF systems.

Fig. 10. XRD patterns of the FeNC material (a) and k values for the RhB removal (b); (c,d) XPS spectra of Fe and corresponding Fe content of different Fe species; (e,f) N 1s XPS spectra and corresponding N content of different N species (FeNC materials).

Fig. 11. Possible HE-EF degradation mechanism for RhB with Fe3N@NG/NC/GF as the cathode.

References

[1]	H. Q. He, Z. Zhou, Crit. Rev. Environ. Sci. Technol., 2017,47, 2100-2131.
[2]	Y. Wang, Y. H. Liu, T. F. Liu, S. Q. Song, X. C. Gui, H. Liu, Appl. Catal. B, 2014,156-157, 1-7.
[3]	J. L. Yu, T. F. Liu, H. Y. Liu, Y. Wang, Chin. J. Catal., 2016,37, 2079-2085.
[4]	F. X. Deng, S. X. Li, M. H. Zhou, Y. S. Zhu, S. Qiu, H. K. Li, F. Ma, J. Z. Jiang, Appl. Catal. B, 2019,256, 117796.
[5]	C. Zhang, G. B. Ren, W. Wang, X. M. Yu, F. K. Yu, Q. Z. Zhang, M. H. Zhou, Sep. Purif. Technol., 2019,208, 76-82.
[6]	V. Poza-Nogueiras, E. Rosales, M. Pazos, M. A Sanromán, Chemosphere, 2018,201, 399-416.
[7]	X. Ding, S. Y. Wang, W. Q. Shen, Y. Mu, L. Wang, H. Chen, L. Z. Zhang, Water Res., 2017,112, 9-18.
[8]	P. Xu, H. Xu, D. Y. Zheng, Chem. Eng. J., 2019,361, 968-974.
[9]	S. O. Ganiyu, M. Zhou, C. A. Martínez-Huitle, Appl. Catal. B, 2018,235, 103-129.
[10]	P. Dong, W. J. Liu, S. J. Wang, H. L. Wang, Y. Q. Wang, C. C. Zhao, Electrochim. Acta, 2019,308, 54-63.
[11]	Q. S. Peng, H. Y. Zhao, L. Qian, Y. B. Wang, G. H. Zhao, Appl. Catal. B, 2015, 174-175, 157-166.
[12]	Y. Z. Wang, H. M. Zhang, B. K. Li, M. C. Yu, R. Zhao, X. T. Xu, L. Cai, Chem. Eng. J., 2019,359, 914-923.
[13]	L. Z. Huang, M. T. Zhu, Z. Z. Liu, Z. P. Wang, H. C. B. Hansen, J. Hazard. Mater., 2019,364, 39-47.
[14]	F. K. Yu, Y. Wang, H. R. Ma, M. H. Zhou, Sep. Purif. Technol., 2020,248, 117022.
[15]	P. Xu, D. Y. Zheng, Z. Y. Xie, J. W. Ma, J. Yu, B. L. Hou, Sep. Purif. Technol., 2020,234, 116103.
[16]	H. Y. Zhao, Q. N. Wang, Y. Chen, Q. L. Tian, G. H. Zhao, Carbon, 2017,124, 112-122.
[17]	W. Chen, X. L. Yang, J. F. Huang, Y. H. Zhu, Y. Zhou, Y. F. Yao, C. Z. Li, Electrochim. Acta, 2016,200, 75-83.
[18]	Y. M. Zhang, Z. Chen, P. P. Wu, Y. X. Duan, L. C. Zhou, Y. X. Lai, F. Wang, S. Li, J. Hazard. Mater., 2020,393, 120448.
[19]	T. X, Huong Le, M. Drobek, M. Bechelany, J. Motuzas, A. Julbe, M. Cretin, Microporous Mesoporous Mater., 2019,278, 64-69.
[20]	A. Özcan, A. Atilir Özcan, Y. Demirci, E. Şener, Appl. Catal. B, 2017,200, 361-371.
[21]	H. Y. Zhao, L. Qian, Y. Chen, Q. N. Wang, G. H. Zhao, Chem. Eng. J., 2018,332, 486-498.
[22]	T. Luo, H. P. Feng, L. Tang, Y. Lu, W. W. Tang, S. Chen, J. F. Yu, Q. Q. Xie, X. L. Ouyang, Z. M. Chen, Chem. Eng. J., 2020,382, 122970.
[23]	X. L. Zhou, D. Xu, Y. C. Chen, Y. Y. Hu, Chem. Eng. J., 2020,384, 123324.
[24]	S. O. Ganiyu, T. X. Huong Le, M. Bechelany, G. Esposito, E. D. van Hullebusch, M. A. Oturan, M. Cretin, J. Mater. Chem. A, 2017,5, 3655-3666.
[25]	Y. Wang, M. Yi, K. Wang, S. Q. Song, Chin. J. Catal., 2019,40, 523-533.
[26]	K. Zhao, Y. Su, X. Quan, Y. M. Liu, S. Chen, H. T. Yu, J. Catal., 2018,357, 118-126.
[27]	V. Perazzolo, C. Durante, R. Pilot, A. Paduano, J. Zheng, G. A. Rizzi, A. Martucci, G. Granozzi, A. Gennaro, Carbon, 2015,95, 949-963.
[28]	K. Q. Li, J. M. Liu, J. Li, Z. Q. Wan, Chemosphere, 2018,193, 800-810.
[29]	M. Cheng, C. Lai, Y. Liu, G. M. Zeng, D. L. Huang, C. Zhang, L. Qin, L. Hu, C. Y. Zhou, W. P. Xiong, Coord. Chem. Rev., 2018,368, 80-92.
[30]	J. T. Tang, J. L. Wang, Chemosphere, 2020,241, 125002.
[31]	V. K. Sharma, M. B. Feng, J. Hazard. Mater., 2019,372, 3-16.
[32]	Z. H. Ye, J. A. Padilla, E. Xuriguera, E. Brillas, I. Sires, Appl. Catal. B, 2020,266, 118604.
[33]	Z. H. Ye, J. A. Padilla, E. Xuriguera, J. L. Beltran, F. Alcaide, E. Brillas, I. Sires, Environ. Sci. Technol., 2020,54, 4664-4674.
[34]	P. K. Cao, X. Quan, K. Zhao, S. Chen, H. T. Yu, J. F. Niu, J. Hazard. Mater., 2020,382, 121102.
[35]	P. K. Cao, K. Zhao, X. Quan, S. Chen, H. T. Yu, Sep. Purif. Technol., 2020,238, 116424.
[36]	Y. Wang, Y. H. Liu, K. Wang, S. Q. Song, P. Tsiakaras, H. Liu, Appl. Catal. B, 2015,165, 360-368.
[37]	J. Xiao, J. H. Lai, R. C. Li, X. Fang, D. F. Zhang, P. Tsiakaras, Y. Wang, Ind. Eng. Chem. Res., 2020,59, 12431-12440.
[38]	K. Wang, H. X. Chen, X. F. Zhang, Y. X. Tong, S. Q. Song, P. Tsiakaras, Y. Wang, Appl. Catal. B, 2020,264, 118468.
[39]	J. Xiao, C. Wang, H. Liu, J. Hazard. Mater., 2020,382, 121007.
[40]	S. Bauer, C. Serre, T. Devic, P. Horcajada, J. Marrot, G. Férey, N. Stock, Inorg. Chem., 2008,47, 7568-7576.
[41]	H. W. Song, J. Su, C. X. Wang, ACS Appl. Energy Mater., 2018,1, 5008-5015.
[42]	M. M. Wu, K. Wang, M. Yi, Y. X. Tong, Y. Wang, S.Q. Song, ACS Catal., 2017,7, 6082-6088.
[43]	H. W. Song, N. Li, H. Cui, C. X. Wang, Nano Energy, 2014,4, 81-87.
[44]	X. D. Ma, X. H. Xiong, J. Q. Zeng, P. J. Zou, Z. Lin, M. L. Liu, J. Mater. Chem. A, 2020,8, 6768-6775.
[45]	T. F. Li, M. Li, M. R. Zhang, X. Li, K. H. Liu, M. Y. Zhang, X. Liu, D. M. Sun, L. Xu, Y. W. Zhang, Y.W. Tang, Carbon, 2019,153, 364-371.
[46]	P. Su, M. H. Zhou, X. Y. Lu, W. L. Yang, G. B. Ren, J. J. Cai, Appl. Catal. B, 2019,245, 583-595.
[47]	M. R. Haider, W. L. Jiang, J. L. Han, H. M. A. Sharif, Y. C. Ding, H. Y. Cheng, A. J. Wang, Appl. Catal. B, 2019,256, 117774.
[48]	Y. Q. Hua, T. T. Jiang, K. Wang, M. M. Wu, S. Q. Song, Y. Wang, P. Tsiakaras, Appl. Catal. B, 2016,194, 202-208.
[49]	J. T. Tang, J. L. Wang, Chem. Eng. J., 2019,375, 122007.
[50]	Y. L. Yang, Y. Liu, X. Fang, W. Miao, X. Y. Chen, J. Sun, B. J. Ni, S. Mao, Chemosphere, 2020,243, 125423.
[51]	S. Cheng, C. Shen, H. Zheng, F. Q. Liu, A. Li, Appl. Catal. B, 2020,269, 118785.
[52]	J. T. Tang, J. L. Wang, Environ. Sci. Technol., 2018,52, 5367-5377.
[53]	P. Su, M. H. Zhou, G. Song, X. D. Du, X. Y. Lu, J. Hazard. Mater., 2020,397, 122681.
[54]	J. Y. Lu, Y. R. Yuan, X. Hu, W. J. Liu, C. X. Li, H. Q. Liu, W. W. Li, Ind. Eng. Chem. Res., 2020,59, 1800-1808.
[55]	C. Liu, Y. Feng, Z. T. Han, Y. Sun, X. Q. Wang, Q. F. Zhang, Z. G. Zou, Chin. J. Catal., 2021,42, 164-174.
[56]	X. Han, S. Y. Liu, X. T. Huo, F. Q. Cheng, M. Zhang, M. Guo, J. Hazard. Mater., 2020,392, 122295.
[57]	S. Sahar, A. Zeb, Y. N. Liu, N. Ullah, A. W. Xu, Chin. J. Catal., 2017,38, 2110-2119.
[58]	J. Wu, K. Zhu, H. Xu, W. Yan, Chin. J. Catal., 2019,40, 917-927.
[59]	L. X. Hu, G. H Deng, W. C. Lu, Y. S. Lu, Y. Y. Zhang, Chin. J. Catal., 2017,38, 1360-1372.

N-doped carbon-coated Fe₃N composite as heterogeneous electro-Fenton catalyst for efficient degradation of organics

RichHTML

PDF (PC)

Knowledge

Supporting Information

Abstract

Cite this article

share this article

share this article

Figures/Tables 11

References

Related Articles 15

Recommended Articles

Metrics

[1]	Shijie Li, Chunchun Wang, Kexin Dong, Peng Zhang, Xiaobo Chen, Xin Li. MIL-101(Fe)/BiOBr S-scheme photocatalyst for promoting photocatalytic abatement of Cr(VI) and enrofloxacin antibiotic: Performance and mechanism [J]. Chinese Journal of Catalysis, 2023, 51(8): 101-112.
[2]	Ning Li, Xueyun Gao, Junhui Su, Yangqin Gao, Lei Ge. Metallic WO₂-decorated g-C₃N₄ nanosheets as noble-metal-free photocatalysts for efficient photocatalysis [J]. Chinese Journal of Catalysis, 2023, 47(4): 161-170.
[3]	Yujie Li, Yuanyuan Liu, Zeyan Wang, Peng Wang, Zhaoke Zheng, Hefeng Cheng, Ying Dai, Baibiao Huang. Enhanced photocatalytic H2O2 production over Pt(II) deposited boron containing metal-organic framework via suppressing the simultaneous decomposition [J]. Chinese Journal of Catalysis, 2023, 45(2): 132-140.
[4]	Haibo Chi, Wangyin Wang, Jiangping Ma, Ruizhi Duan, Chunmei Ding, Rui Song, Can Li. A synchronous defluorination-oxidation process for efficient mineralization of fluoroarenes with photoelectrocatalysis [J]. Chinese Journal of Catalysis, 2023, 55(12): 171-181.
[5]	Chun-Yu Qiu, Li-yang Wan, Yu-Cheng Wang, Muhammad Rauf, Yu-Hao Hong, Jia-yin Yuan, Zhi-You Zhou, Shi-Gang Sun. Revealing the concentration of hydrogen peroxide in fuel cell catalyst layers by an in-operando approach [J]. Chinese Journal of Catalysis, 2022, 43(7): 1918-1926.
[6]	Fenglei Lyu, Wei Hua, Huirong Wu, Hao Sun, Zhao Deng, Yang Peng. Structural and interfacial engineering of well-defined metal-organic ensembles for electrocatalytic carbon dioxide reduction [J]. Chinese Journal of Catalysis, 2022, 43(6): 1417-1432.
[7]	Boyu Zhang, Jiafu Shi, Yang Zhao, Han Wang, Ziyi Chu, Yu Chen, Zhenhua Wu, Zhongyi Jiang. Pickering interfacial biocatalysis with enhanced diffusion processes for CO₂ mineralization [J]. Chinese Journal of Catalysis, 2022, 43(4): 1184-1191.
[8]	Yaping Zhang, Jixiang Xu, Jie Zhou, Lei Wang. Metal-organic framework-derived multifunctional photocatalysts [J]. Chinese Journal of Catalysis, 2022, 43(4): 971-1000.
[9]	Junmin Huang, Jianmin Chen, Wangxi Liu, Jingwen Zhang, Junying Chen, Yingwei Li. Copper-doped zinc sulfide nanoframes with three-dimensional photocatalytic surfaces for enhanced solar driven H₂ production [J]. Chinese Journal of Catalysis, 2022, 43(3): 782-792.
[10]	Yiwei Fan, Helong Li, Shihao Su, Jinlei Chen, Chunquan Liu, Shuizhong Wang, Xiangya Xu, Guoyong Song. Integration of Ru/C and base for reductive catalytic fractionation of triploid poplar [J]. Chinese Journal of Catalysis, 2022, 43(3): 802-810.
[11]	Ling-Ling Zheng, Long-Shuai Zhang, Ying Chen, Lei Tian, Xun-Heng Jiang, Li-Sha Chen, Qiu-Ju Xing, Xiao-Zhen Liu, Dai-She Wu, Jian-Ping Zou. A new strategy for the fabrication of covalent organic framework-metal-organic framework hybrids via in-situ functionalization of ligands for improved hydrogen evolution reaction activity [J]. Chinese Journal of Catalysis, 2022, 43(3): 811-819.
[12]	Yingnan Zhao, Xing Qin, Xinyu Zhao, Xin Wang, Huaqiao Tan, Huiying Sun, Gang Yan, Haiwei Li, Wingkei Ho, Shun-cheng Lee. Polyoxometalates-doped Bi₂O_3-_x/Bi photocatalyst for highly efficient visible-light photodegradation of tetrabromobisphenol A and removal of NO [J]. Chinese Journal of Catalysis, 2022, 43(3): 771-781.
[13]	Zhen Liu, Jian Tian, Changlin Yu, Qizhe Fan, Xingqiang Liu. Solvothermal fabrication of Bi₂MoO₆ nanocrystals with tunable oxygen vacancies and excellent photocatalytic oxidation performance in quinoline production and antibiotics degradation [J]. Chinese Journal of Catalysis, 2022, 43(2): 472-484.
[14]	Ting Huang, Jiaqi Chen, Lili Zhang, Alireza Khataee, Qiaofeng Han, Xiaoheng Liu, Jingwen Sun, Junwu Zhu, Shugang Pan, Xin Wang, Yongsheng Fu. Precursor-modified strategy to synthesize thin porous amino-rich graphitic carbon nitride with enhanced photocatalytic degradation of RhB and hydrogen evolution performances [J]. Chinese Journal of Catalysis, 2022, 43(2): 497-506.
[15]	Jun Wan, Weijie Yang, Jiaqing Liu, Kailong Sun, Lin Liu, Feng Fu. Enhancing an internal electric field by a solid solution strategy for steering bulk-charge flow and boosting photocatalytic activity of Bi₂₄O₃₁Cl_xBr_10-_x [J]. Chinese Journal of Catalysis, 2022, 43(2): 485-496.